Hot Papers
Hot Papers werden von der Redaktion aufgrund ihrer Bedeutung in einem sich schnell entwickelnden Feld von hoher aktueller Bedeutung ausgewählt. Dieses Kriterium trifft sicher auch auf viele der "Very Important Papers" zu, aber eine solche Doppelung wird vermieden.
Proton Channels
A Molecular Staircase Built from Hydrazide-Linked Pyridines as an Artificial Proton Channel
Jianhe Xu, Yanbin Chen, Jianru Wang, Dr. Wenju Chang, Prof. Dr. Jie Shen, Prof. Dr. Huaqiang Zeng
Hydrazide-bridged pyridine moieties have been used to generate a staircase-shaped artificial proton channel that exhibits excellent proton transport performance. The proton channel shows an EC₅₀ value of 0.33 mol% relative to lipids while demonstrating exceptional selectivity over Na⁺ and K⁺ ions, with selectivity values of 90.5 and 160.3, respectively.
Organometallic Chemistry
Synthesis and Structure of Neopentyl Sodium: A Hydrocarbon-Soluble Reagent for Controlled Sodiation of Non-Activated Substrates
David E. Anderson, Dr. Lorraine A. Malaspina, PD Dr. Simon Grabowsky, Prof. Dr. Eva Hevia
Displaying strong controlled metalating power, hydrocarbon-soluble sodium neopentyl can deprotonate challenging non-activated arenes and alkenes, with sodiated intermediates successfully undergoing onward functionalisation reactions. By characterising key reaction intermediates, and running computational studies on models, insight has been gained on the structure, bonding, and special reactivity of this promising new reagent.
Polymer Chemistry
On-Demand Photodegradable and Thermo-Reversible, Soft, Transparent Dithioacetal Hydrogels
Dr. Maria Psarrou, Ioanna Chatzaki, Antonis Mavromanolakis, Dr. Theodore Manouras, Prof. Dimitris Vlassopoulos, Prof. Maria Vamvakaki
A versatile chemical platform for the development of photodegradable and thermally-reversible hydrogels is presented. The hydrogels were synthesized via a step-growth reaction of a difunctional PEG-thiol with an aromatic dialdehyde cross-linker. The photosensitive dithioacetal bonds endowed the material with photodegradable and thermo-reversible properties.
Batteries
Boosting Performance of Quasi-Solid-State Zinc Ion Batteries via Zincophilic Solubilization
Yifan Wang, Weilin Yan, Xuejun Zhu, Jinghao Li, Prof. Zhaoqian Li, Hong Zhang, Yingke Ren, Lie Mo, Prof. Yang Huang, Prof. Lei Zhang, Prof. Linhua Hu
In this paper, a zincophilic solubilization strategy was proposed to break the concentration limit in Zn(Ac)2 hydrogel electrolytes. Based on the salting-out effect, this provides high mechanical durability for AZIBs, enabling in situ polyurea-based solid electrolyte interphase (SEI) layer. The assembled batteries have high platting/stripping reversibility and high capacity.
Electrocatalytic Acetonitrile Hydrogenation
Spillover-Mediated H* Redistribution Promotes Electrocatalytic Acetonitrile Hydrogenation in PEM Reactors
Shan Huang, Dr. Bingying Han, Ye Liu, Zijie Cheng, Prof. Huibin Ge, Prof. Lianbing Zhang, Prof. Riguang Zhang, Prof. Baojun Wang, Prof. Jie Kong, Prof. Jiayuan Li
Palladium with high H* coverage is partnered with copper with low H* coverage to enable palladium-to-copper hydrogen spillover, which reduces H* coverage on Pd to mitigate H2 evolution and increases H* availability on Cu to promote ethylamine productivity. Utilization of these catalysts into a proton exchange membrane electrolyzer enabled an expected improvement in ethylamine production rate, HER suppression, and energy efficiency.
Methanol Synthesis
Engineering PdAu/CeO₂ Alloy/Oxide Interfaces for Selective Methane-to-Methanol Conversion with Water
Dr. Estefanía Fernández-Villanueva, Dr. Pedro J. Ramírez, Dr. Pablo G. Lustemberg, Prof. Rubén Pérez, Prof. M. Verónica Ganduglia-Pirovano, Prof. José A. Rodriguez
Selective methane-to-methanol conversion at 500 K over Pd0.3Au0.7/CeO2. The synergistic interaction between alloyed Pd-Au sites and the CeO2 support enhances catalytic performance, enabling highly selective methane-to-methanol under mild conditions. The reaction of CH4 with H2O produces CH3OH and H2, achieving ∼80% selectivity under mild conditions while maintaining stable long-term activity.
Hydrophobic Ru Catalysts for Hydrogenation
Hydrophobic Poly(divinylbenzene) Polymer-Supported Ruthenium Catalysts for Efficient Hydrogenation of Pyridines in Water
Qingsong Luo, Hai Wang, Yating Lv, Jinghao Fan, Huixin Wu, Wei Fang, Lujie Liu, Pei Liu, Liang Wang, Feng-Shou Xiao
This study demonstrates that the pyridine hydrogenation in water is greatly enhanced over the hydrophobic Ru/PDVB catalyst, where nanopores in the PDVB are empty for hydrogen storage, enabling the enrichment of abundant hydrogen around active Ru sites for hydrogenation.
Organic Materials
Unconventional Fast Room Temperature Synthesis of Covalent Organic Framework Single Crystals Unveiling Precise Structural Insights
Miguel Jiménez-Duro, Dr. Marcos Martínez-Fernández, Dr. Jorge J. Cabrera-Trujillo, Eva Osuna, Miguel Fernández-Ramos Humanes, Prof. Cristina Gómez-Navarro, Prof. Julio Gómez-Herrero, Prof. Félix Zamora, Prof. José L. Segura
This work presents a fast, room-temperature synthesis of single-crystalline, highly fluorinated 2D covalent organic frameworks (COFs). We achieved the growth of 3-micron-long COF rods, enabling the precise study of their mechanical properties and aggregation states. The crystallization process was computationally elucidated, revealing the critical roles of trifluoroacetic acid and 2,3,5,6-tetrafluoroaniline in promoting Schiff base bond formation and improving COF crystallinity. This study offers new insights into the controlled synthesis of 2D COFs, with implications for their use in a range of advanced materials applications.
Light-Ultrasound-Driven Hydrogen
Synergistic Light-Ultrasound-Driven Hydrogen Production by Hydrogen Iodide Decomposition Over Dual-Molecular Ferroelectric Heterostructure
Zi Ning Zhou, Qing Dian Chong, Ya Wen Yang, Zong Wei Hu, Wei Ren, Prof. Sheng Sen Zhang, Prof. Qiong Ye
A dual molecular ferroelectric heterojunction [(4,4-DFPD)2PbI4/(4,4-DFCHA)2PbI4], synthesized via a simple one-pot method, achieves a high H₂ evolution rate of 5.26 mmol·g−1·h−1 under light and ultrasound, significantly outperforming its individual components. Polarization-coupled energy-level alignment and Pb-I bond-driven charge transfer enhance directional carrier migration and suppress recombination.
Multisite Proton-Coupled Electron Transfer
Multisite Proton-Coupled Electron Transfer Facilitates Oxidative Photocatalysis in a Molecular Zr-Based Coordination Compound
Mercedes Moreno-Albarracín, Alvaro M. Rodriguez-Jimenez, Omar Nuñez, Pablo Garrido-Barros
Deprotonation of the hydroxy ligand in the Zr3(O)(OH)3 nodes of a molecular cage unlocks photo-oxidative catalysis via multisite proton-coupled electron transfer (PCET), complementing previous findings in the reductive counterpart. This platform offers valuable insights into the excited-state reactivity of photoredox catalysts and stands as a promising tool with unprecedented ambipolar reactivity for solar-to-chemical conversion.
Nanovaccine
Atorvastatin-Loaded Mineralized Vaccine Reprograms Endosomal Trafficking to Amplify STING-Driven Cancer Immunotherapy
Yuhan Yang, Wei Long, Xiangyu Pei, Shangfei Li, Bowen Fu, Hao Zhai, Xiaoyi Zhang, Ying Wan, Prof. Yayun Peng, Ting Cai
A biomineralized nanovaccine (OVA-ATV@MnO₂) spatiotemporally co-delivers and releases tumor antigen, atorvastatin, and Mn adjuvants in dendritic cells. Atorvastatin reprograms endosomal trafficking to delay lysosomal degradation, enhancing antigen cross-presentation via MHC-I, while Mn2+ activates the cGAS-STING pathway, amplifying dendritic cell maturation and antitumor T-cell responses. This dual-action strategy achieves potent tumor regression, suppresses metastasis, and establishes durable anticancer immunity.
Atomic Precision
Hydrogen-Bonding-Assisted Assembly of Stable High-Nuclearity Copper(I)-Alkyne Nanoclusters for X-Ray Scintillation
Bao-Liang Han, Fahri Alkan, Zhi-Rui Yuan, Paritosh Mahato, Zhi Wang, Chen-Ho Tung, Di Sun
A novel hydrogen-bonding-assisted assembly strategy has been developed for the construction of high-nuclearity copper nanoclusters. Furthermore, the X-ray scintillation properties of the high-nuclearity nanocluster are investigated for the first time, demonstrating their potential for advanced radiation detection applications.
Electrochemical C─H Chlorination
Alkali Metal Cations Impact the Selectivity of Radical-Mediated Electrochemical C─H Chlorination
Bo Wu, Ruihu Lu, Tenghui Yuan, Beijing Cai, Bingqing Wang, Bote Zhao, Shibo Xi, Ziyun Wang, Yanwei Lum
In this work, we found that alkali metal cations in the electrolyte can impact the *Cl binding energy, which controls selectivity between radical-mediated electrochemical C─H chlorination and competing Cl2 formation.
CO2 Hydrogenation
Establishing 3d-4d Orbital Hybridization for Efficient Photothermal Catalytic CO2 Hydrogenation
Yisi Yang, Dr. Fengliang Wang, Wenyuan Lyu, Dawang Tang, Datong Chen, Dr. Xin Zhao, Prof. Ruiqi Fang, Prof. Yingwei Li
The d-d hybridization between 3d and 4d metals can induce the modulation of the affinity of *CO intermediate, thereby accelerating the *CO hydrogenation process in photothermal CO2 methanation.
Porous Organic Salts
Constructing Water-Stable Porous Organic Salts via Suppressed Proton Integration Using Fluorinated Tetrazole Tectons
Dr. Errui Li, Dr. Xian Suo, Yujing Tong, Dr. Phattananawee Nalaoh, Dr. David M. Jenkins, Dr. Carlos Alberto Steren, Dr. Lilin He, Alexander S. Ivanov, Dr. Leighanne C. Gallington, Dr. Victoria Cooley, Dr. Bo Li, Dr. Xin Wang, Dr. Kai Li, Dr. Juntian Fan, Dr. Liqi Qiu, Dr. De-en Jiang, Dr. Katherine R. Johnson, Dr. Takeshi Kobayashi, Dr. Murillo L. Martins, Dr. Shannon M. Mahurin, Dr. Zhenzhen Yang, Dr. Sheng Dai
Porous organic salts featuring hydrophobic channels and minimal hydrogen bonding were constructed using a fluorinated tetrazole as a weak acid tecton and a tetra-substituted imidazole precursor lacking active protons as the base. These materials exhibited exceptional robustness and structural integrity under both aqueous and water-lean conditions, maintaining their stacking mode and crystal structure even at elevated temperatures.
Fluoroalkenes
Platinum-Catalysed Hydrofluorination of Alkynes at Room Temperature Promoted by a Fluoride Shuttle
Ouchan He, Dr. Froze Jameel, Hannah Flammang, Smrithi Suresh Babu, Prof. Dr. Martin Kaupp, Prof. Dr. Thomas Braun
This work presents an air and moisture tolerant platinum-catalysed hydrofluorination system that gives selectively (Z)-fluoroalkenes. Experimental and computational investigation on the mechanism allowed for the identification of catalytic species. The hydrofluorination is mediated by complexes between the fluorinated anion and HF, resulting into BF3, PF5 and HF serving as fluoride shuttles.
Heterometallic Complex
C(sp2)─H Bond Activation with a Heterometallic Nickel-Aluminium Complex
Joseph A. Zurakowski, Dr. Benedek Stadler, Prof. Dr. Marcus W. Drover, Prof. Dr. Mark R. Crimmin
Despite the prevalence of Ni/Al catalysts for pyridine C─H functionalization, mechanistic details of such systems remain scarce. Herein, we present the discovery of PCy3-catalyzed bond-breaking and making processes that occur in the coordination sphere of a novel Ni─Al heterometallic complex. The reaction is 1st order in PCy3 and proceeds with a low KIE of 0.9-1.1. These data suggest that both C─H activation and H2 reductive elimination steps in this system are low energy, are readily accessible, and are not rate limiting.
Magnetic Resonance Imaging
Scalable Hyperpolarized MRI Enabled by Ace-SABRE of [1-13C]Pyruvate
Stephen J. McBride, Megan Pike, Erica Curran, Alexander Zavriyev, Bukola Adebesin, Luke Tucker, Jared M. Harzan, Ishani M. Senanayake, Mustapha Abdulmojeed, Franziska Theiss, Sheng Shen, Thomas Boele, Simon B. Duckett, Boyd M. Goodson, Matthew S. Rosen, Eduard Y. Chekmenev, Hong Yuan, Carlos Dedesma, Terence Gade, Stephen Kadlecek, Thomas Theis, Patrick TomHon
Ace-SABRE overcomes previous biocompatibility challenges associated with the Signal Amplification By Reversible Exchange (SABRE) hyperpolarization technique. The employed acetone-water mixtures greatly simplify separation of the hyperpolarized compound (e.g., pyruvate) from solvents and catalysts delivering a biocompatible injectable. Ace-SABRE retains high polarization during processing and enables effective metabolic characterization in vivo.
Radicals
Feedstock-Derived Thiophene Radical Anions Exhibiting Redox Stability at Extreme Potentials
Aurelio C. Gasser, Daniel Käch, Prof. Dr. Máté J. Bezdek
Although organic redox systems are emerging as next-generation energy storage media, stability at high cell voltage is often achieved at the expense of synthetic accessibility. Here, we isolate and characterize a feedstock-derived thiophene radical anion bearing simple ester groups. Despite a minimalist design, the radical and its derivatives are stable at extreme potentials, enabling their use as readily accessible electrolytes for electron storage.
Triarylmethyl Radicals
Chloromethoxytrityls: Tuning the SOMO Level of Stable Luminescent Radicals
Hannah E. Hackney, Cory Ruchlin, Emil Stahle, Dmytro F. Perepichka
In this work, we use chlorine and methoxy groups to control the singly occupied molecular orbital level of triarylmethyl radicals within a wide range of 1.8 eV and establish structure-properties relationships between the substituents and photophysical properties of triarylmethyl radicals.
Vibrational Strong Coupling
The Diels-Alder Reaction as a Mechanistic Probe for Vibrational Strong Coupling
Dr. Cyprien Muller, Dr. Maciej Piejko, Sinan Bascil, Prof. Dr. Joseph Moran
Vibrational Strong Coupling (VSC) was recently shown to modify chemical reactivity, but it is unclear why. We introduce the Diels-Alder (DA) reaction as a mechanistic probe for some of the most popular hypotheses and provide the first experimental investigation of the DA reaction under VSC by measuring the kinetics of six different DA reactions under various coupling conditions. No significant change in kinetics was observed.
Perovskite Solar Cells
Monodisperse Regulation of Self-Assembled Monolayer Via Dipole Molecules for Efficient Perovskite Solar Cells
Zhinan Zhang, Yinghao Xu, Sifan Chen, Wenbo Li, Shaofu Wang, Chuan Peng, Shengjie Du, Sixiong Li, Xingzhong Zhao, Ti Wang, Zhenhua Yu
Strong dipole molecules are employed to regulate the monodispersity of self-assembled monolayer (SAM) micelles and coverage distribution of the resulting SAM films, achieving an efficiency of 26.58%.
Total Synthesis
Ligand Type Guided Keto-Arylation Enables Modular Total Synthesis of Polycyclic CBS Xanthones
Jonas W. Meringdal, Vivienne Prangenberg, Tim Treiber, Andreas J. Schneider, Leon Honsdorf, Dirk Menche
A ligand type concept guided a central aromatic keto-arylation in the first total syntheses of CBS72, CBS87 and CBS100. Davis oxidation with catalytic base and late-stage aminolysis completed the route. This strategy provides modular, concise and high-yielding access to uncharted polycyclic xanthones. Meanwhile, ligand types emerge as a powerful design tool in sophisticated cross couplings.
Thermoelectrics
Conduction Band Convergence and Modular Nanostructures: Driving High Thermoelectric Performance in n-Type PbSe
Indrajit Haldar, Vaishali Taneja, Naveen Goyal, Mohammad Ubaid, Debattam Sarkar, Dinesh Kumar Kedia, Kumar Saurabh, Surjeet Singh, Koushik Pal, N. Ravishankar, Kanishka Biswas
Mo 4d orbital hybridized with the Se 4p-Pb 6p to provide conduction band convergence, and PbSe-MoSe2 modular nanostructures lead to high thermoelectric performance in MoCl5 doped n-type PbSe.
Spitzenverstärkte Raman-Spektroskopie
Winkelaufgelöste Spitzenverstärkte Ramanspektroskopie
Felix Schneider, Tim Parker, Dr. Liangxuan Wang, Michel Rebmann, Yang Zhao, Eric Juriatti, Prof. Heiko Peisert, Prof. Alfred J. Meixner, Dr. Johannes Gierschner, Prof. Lingyan Meng, Prof. Dai Zhang
Wir haben beobachtet, dass das spitzenverstärkte Ramansignal (TERS) winkelverteilt und modenspezifisch ist. Das Strahlungsmuster in der hinteren Brennebene von vertikalen bzw. parallelen Dipolen wird stark vom Nahfeld in der TERS Nanolücke beeinflusst, während die Emission mit großer Direktionalität von der Spitzen-Proben Antenne ins Fernfeld geführt wird, jedoch mit signifikanten Unterschieden in Emissionswinkel, Intensität und der Winkeldivergenz.
Facet-Dependent Photocatalytic HER
Crystal Facet-Dependent Photocatalytic Hydrogen Evolution From Ultra-Stable Cu-Zr/Hf Heterobimetallic Metal-Organic Frameworks
Hang Lei, Dr. Jieping Zhang, Zhiyuan Wu, Yangxingyu Ye, Dr. Zhijia Li, Yunfang Zhao, Prof. Lian Chen, Prof. Yongsheng Liu, Prof. Maochun Hong
Crystal engineering and facet engineering were concurrently employed to develop a series of precious-metal-free heterobimetallic MOFs (M-BCA-M', M = Cu+, M' = Zr4+ or Hf4+) for record-high photocatalytic hydrogen production in pristine MOFs. The high performance and crystal-facet dependent behaviors were investigated to provide molecular-level insights into the coordination regulation and morphology control of pristine MOFs for efficient photocatalysis.
Perovskite Solar Cells
Antisolvent-Bathing Strategy with Ultra-Wide Processing Window for Making High-efficiency Perovskite Solar Cells in Ambient Air
Lixiu Zhang, Chuantian Zuo, Mei Zhang, Ruihao Chen, Xiangyu Chen, Ke Jin, Feng Hao, Keyou Yan, Zuo Xiao, Congcong Wu, Jingjing Chang, Yong Ding, Liming Ding
Antisolvent bathing strategy with ultra-wide processing window (10 s-10 min) is proposed to achieve high-performance perovskite solar cells (PSCs). The bathing process is in situ monitored via time-resolved UV-Vis spectroscopy, systematically unrevealing the crystallization kinetics for different antisolvents. The PCE of CF-bathed device achieves 24.49% in ambient air, representing the record for antisolvent bathing method.
Organosilicon Chemistry
Nickel-Catalyzed Sila-Cycloaddition of Dichlorodisilanes: Selective Si─Cl Activation for Cyclic Disilanes and Enantioenriched Synthesis
Dr. Liangliang Qi, Shaojie Xu, Prof. Xiaobo Pang, Yu-Ke Wu, Prof. Xiaotai Wang, Prof. Xing-Zhong Shu
A nickel-catalyzed [4 + 2] sila-cycloaddition between dichlorodisilanes and 1,3-dienes enables efficient access to diverse cyclic disilanes via selective Si─Cl activation. The method tolerates broad diene scope, offers an enantioselective variant, and reveals a unique Ni⁰-mediated SN2-type activation pathway.
Circularly Polarized Luminescence
Chiral Tin-Oxo Cluster Matrices with Fluorophore Embedment for Multichromatic Circularly Polarized Luminescence
Gui-Xin Yan, Dr. Er-Xia Chen, Dr. Jin-Xia Yang, Prof. Jian Zhang, Prof. Qipu Lin
Enantiomeric tin-oxo clusters form helical supramolecular matrices through directional intermolecular interactions, enabling efficient transfer of optical handedness to encapsulated non-chiral fluorophores via spatial confinement. These assemblies exhibit tunable circularly polarized luminescence (CPL) emissions.
CO2 Reduction
Ordered Copper Triangular Atomic Sites for Industrial-Grade Electromethanation of CO2 via Self-Regulated Adsorption of Reactants
Dr. Fanglei Yao, Dr. Yuntong Sun, Long Nie, Dr. Cheng Zhang, Dr. Hongwei Shou, Zhiming Li, Prof. Xiaoping Gao, Prof. Jin Wang
Ordered copper triangular atomic site motifs loaded on poly(heptazine imide) (Cu TAS/PHI) were synthesized via a precise ion exchange strategy. Cu TAS/PHI enables enhanced CO2 coverage and activation with balanced proton supply through self-regulated adsorption of reactants, as well as unlocks an energetically favorable *C(OH)2 pathway, achieving an FECH4 of 80.5% at 400 mA cm−2 and an FECD4 of 75.1% at 700 mA cm−2.
Cobalt Catalysis
A Homobimetallic Frustrated Lewis Pair Cobalt Catalyst for the Methanolysis of Hydrosilanes
Dr. Ana Luque-Gómez, Daniel Barrena-Espés, Dr. Pilar García-Orduña, Andrea Pérez-García, Miguel A. Casado, Dr. Julen Munarriz, Dr. Manuel Iglesias
The bimetallic Co(I)/Co(-I) complex [Co(CO)2(κ3-P,N,P-PNHP)][Co(CO)4] shows excellent activities in the methanolysis of hydrosilanes, reaching TOF values of ca. 50 000 h−1. This behavior can be ascribed to the presence of the [Co(CO)4]- anion, which allows for a frustrated Lewis pair mechanism, resulting in a low energy pathway for the heterolytic splitting of the Si─H bond, as substantiated by DFT calculations.
Homichiral Ferroelectric
Mathematical Double-Matrix Switchable Homochiral Ferroelectric
Dr. Xian-Jiang Song, Dr. Yan Qin, Prof. Yong Ai, Dr. Xiao-Gang Chen, Dr. Yan-Ran Weng, Dr. Hang Peng, Dr. Hui-Peng Lv, Dr. Ren-Gen Xiong, Dr. Wei-Qiang Liao
We reported the first homochiral metal halide ferroelectrics showing on/off switchable second-harmonic generation circular dichroism (SHG-CD) response. They exhibit strong SHG-CD with the anisotropy factor (gSHG-CD) up to 1.28 and a 432F2 ferroelectric phase transition, enabling the unprecedented on/off switching of both SHG-CD and piezoelectric response between the SHG-CD/piezoelectric active and SHG-CD/piezoelectric inactive states.
Phototheranostics
Doping Bulky Fluorinated Organic Anion to Construct Highly Efficient Anion-π+ Type Photosensitizers for Cancer Phototheranostics
Lingxiu Liu, Jianye Gong, Xue Wang, Prof. Guoyu Jiang, Prof. Ben Zhong Tang, Prof. Jianguo Wang
A facile strategy to enhance the fluorescence intensity and to modulate cellular uptake of anion-π+ AIE PSs by doping bulky fluorinated anions tetrakis(pentafluorophenyl)borate (FTB) into nanoparticles was proposed. The optimized DF-FTB8 (FTB:DPBCF-Br = 8:1) exhibited superior cellular uptake, outstanding imaging capabilities and high intracellular reactive oxygen species generation level, enabling efficient cancer photodynamic therapy.
Gold(0) Complexes
Dinuclear Au(0) Complex Supported by Tridentate P-Mg-P Ligands
Yafei Li, Tianze Xu, Xinggao Ji, Jie Zeng, Jin Xie, Jing Ma, Congqing Zhu, Qin Zhu
A complex featuring an Au(0)-Au(0) σ-bond is stabilized by tridentate P-Mg-P ligands, with the σ-bond serving as a two-electron donor to the Mg centers and enabling two-electron reductions of various substrates. This work highlights the significance of ligand design for stabilizing low-valent Au center and provides new cases to explore the properties of dinuclear Au(0) complexes.
CO2 Electroreduction
Enhanced Active Hydrogen Absorption and Stabilized Cu(I) Species Over Cu-O-Ce Bridges Boosting Electrocatalytic CO2 Reduction to Ethylene
Zhenwei Zhao, Yu Zhang, Junjun Li, Bingqing Yao, Hui Zhang, Zhicheng Zhang
The as-synthesized CuxO-CeO2 composites exhibit enhanced Faradaic efficiency and partial current density of C2H4 compared with Cu2O cubes. In situ spectroscopies and theoretical calculations confirm that the Cu-O-Ce bridges in CuxO-CeO2 composite can effectively enhance *H absorption and stabilize Cu(I) species, facilitating subsequent C-C coupling and further protonation into the key *COCHO intermediate of C2H4.
Supramolecular Polymers
Mechanically Tunable Slide-Ring Polymers via Photo-Regulated Topological Control
Xiaoqing Wang, Chenjuan Yu, Maolin Wang, Shiyu Zhao, Qimo Mao, Prof. Yuping Wang
We developed light-responsive slide-ring polymer networks whose mechanical properties can be tuned through photoisomerization of the incorporated azobenzene units. The trans-state permits unhindered macrocycle sliding, yielding ductile materials, while UV-induced cis-configuration restricts macrocycle mobility to double Young's modulus. Furthermore, the azobenzene linkage confers controlled degradability under mild conditions.
Anion Channels
Dual-Function Tetrabenzylphosphonium Groups as Mitochondria-Targeting Artificial Anion Channels
Dr. Fei Gou, Xinlei Huangfu, Qiuting Wang, Zihong Yang, Xiyu Yuan, Dr. Wenju Chang, Prof. Dr. Jie Shen, Prof. Dr. Wen-Xiong Zhang, Prof. Dr. Huaqiang Zeng
A series of mitochondriotropic artificial anion channels have been constructed from a self-assembled tetrabenzylphosphonium framework with an inherent ability to autonomously target mitochondria. Anion transport is mediated by multiple intermolecular C─H⋯anion H─bonds and electrostatic ion pair interactions. The highly efficient transmembrane anion transport is demonstrated by low micromolar anticancer activity against three cancer cell lines.
Supramolecular Chemistry
Macromolecule-Driven Supramolecular Polymerization Induced by Crowding Effects
Dr. Joost J. B. v. d. Tol, Magda M. J. Dekker, Ádám Müller, Puck Springintveld, Prof. Dr. E. W. Meijer, Prof. Dr. Ghislaine Vantomme
A systematic study is presented that investigates the influence of the excluded volume effect by macromolecules on supramolecular polymerizations in organic media. Upon crowding, the discotic supramolecular monomers sequentially assemble into polymers and higher-order aggregates (HOAs), affected by the macromolecule's concentration, size and polarity. The proven tunability and general applicability of this entropically driven assembly open new avenues for applying macromolecular crowding beyond aqueous systems.
Organic Photovoltaics
Prolonging Exciton Diffusion Length via Modulating Aggregation Structures for Binary Organic Photovoltaics Approaching 20% Certified Efficiency
Jiayou Zhang, Fang Fang, Bending Zhang, Dr. Lifu Zhang, Houdong Mao, Lin Wen, Dr. Dou Luo, Chongbin Yu, Prof. Zhen Yang, Prof. Yiwang Chen
The exciton diffusion length (LD) and fluid mechanics were effectively optimized by modulating the polymer aggregation structure. The printing PPHJ flexible OPVs exhibits more than 18% efficiency, and the flexible device maintained 90.4% of the initial PCE after 2000 bending cycles, showing excellent mechanical stability. Meanwhile, the rigid device exhibits 20% efficiency (certified19.68%, the highest value for the eco-friendly solvent system). Notably, the fabricated 23.60 cm2 large-area module was 15.60% PCE.
Photocages
Unveiling the Power of Dark State Photocages: An Efficient Pathway to Triplet State Under Near-Infrared Light Irradiation
Qiao Hu, Prof. Jianjun Du, Syed Ali Abbas Abedi, Prof. Xiaogang Liu, Saran Long, Prof. Wen Sun, Prof. Jiangli Fan, Prof. Xiaojun Peng
The concept of a dark state photocage was proposed based on near-infrared light-activated leuco dyes. The dark state enhances triplet-state formation, enabling the release of dyes and functional molecules under red light irradiation. This platform exhibited excellent “OFF”-to-“ON” tumor imaging contrast and effective tumor inhibition against triple-negative breast cancer and lung metastases.
Supramolecular Chemistry
Tailoring Tubular Supramolecular Polymers with Polar Lumens to Host Hydrophilic Dye Molecules
Irene Sancho-Casado, Dr. Fátima Aparicio, Dr. Marina González-Sánchez, Dr. Raquel Chamorro, Dr. Víctor Vega-Mayoral, Dr. Juan Cabanillas-González, Prof. David González-Rodríguez
A unique class of tubular polymer structures that are soluble in apolar organic solvents but are endowed with polar pores has been created through the rational design of the monomer units, which self-assemble in amphiphilic cyclic entities that then stack into tubular architectures. These tailored assemblies are able to selectively host hydrophilic dye molecules that are complementary in size and chemical affinity for the pore coating, providing containers for the study of energy transfer processes.
InP QD-LEDs
Dual-Mode Strain Relief via Zinc Acetate Enables High-Efficiency InP Quantum Dot Light-Emitting Diodes
Changwei Yuan, Prof. Qun Wan, Xinrong Liao, Mengda He, Canan Li, Prof. Zhemin Shen, Prof. Baoquan Sun, Prof. Zan Qu, Prof. Long Kong, Prof. Liang Li
This study presents a novel strain engineering strategy that enables stress relief and uniform shell growth at the InP quantum dot coreshell interface using a small-molecule Zn(Ac)2 precursor. This approach significantly reduces interfacial strain and boosts the PLQY to nearly 100%. The resulting QLEDs demonstrate enhanced charge injection and energy level alignment, achieving an external quantum efficiency of up to 26.3%, offering a scalable platform for advanced quantum dot and device development.
Urea Electrosynthesis
Atomic-Scale Mott-Schottky Analogy in SnCu Nanoalloy Promote High-Efficiency Urea Electrosynthesis at Ultralow Potential
Pingyi Feng, Buqi Ke, Shao Wang, Yanxu Chen, Mingyu Cheng, Zechuan Dai, Bocheng Zhang, Yifan Li, Prof. Genqiang Zhang
Electron-enriched Cu active sites arising from an atomic-scale Mott-Schottky analogy in SnCu nanoalloy catalyst, exhibited quadruple synergism: enhanced CO2 and NO3− co-adsorption, elevated *CO surface coverage, accelerated *NHO-*CO coupling, and concurrent HER suppression, collectively achieving a twofold enhancement in urea yield compared to pristine Cu.
Photocatalysis
Light-Induced Fe-LMCT Catalysis for Redox-Coupled Conversion of NOx and SO2 Mixture
Ruimin Chen, Jielin Wang, Taobo Huang, Chunling Zhang, Xiuping Zhu, Jieyuan Li, Fan Dong
A light-induced Fe-LMCT (ligand-to-metal charge transfer) catalytic system is demonstrated, whereby continuous conversion of NO to N2 and SO2 to SO42− is achieved, with the formation of N2O byproducts suppressed via LMCT-driven spatial segregation of redox pathways.
ZrO2/Ni Inverse Catalysts
Spontaneous Nano-ZrO2 Exsolution from Ni-Zr-O Mixed Oxides Enables Facile Fabrication of ZrO2/Ni Inverse Catalysts for Efficient COx Methanation
Xin Tang, Yuanchang Wang, Jinrong Zhang, Cheng Yu, Mengyao Cheng, Shiqing Yang, Xuguang Yang, Liangwei Liu, Lili Han, Yao Xu, Chuqiao Song, Lili Lin
A spontaneous nano-oxide exsolution strategy was reported as a facile engineering of ZrO2/Ni inverse catalyst, involving the one-step co-precipitation synthesis of Ni-Zr-O mixed oxide with monodispersed Zr species followed by H₂-induced in situ oxide segregation. The prepared ZrO2/Ni inverse catalyst was demonstrated to exhibit near-thermodynamic-equilibrium COx conversions at 200 °C, while maintaining robust stability under complex simulated syngas conditions.
Small Molecule Activation
Cooperative Activation of CO and Pyridine by an Aluminum(I) Complex Ligated with a Silylene-Borane Ligand
Jinghuang Lv, Xiao Fang, Fanshu Cao, Prof. Dr. Zhenbo Mo
A silylene-borane-ligated aluminum(I) complex featuring Si(II)→Al(I) and Al(I)→B(III) donor-acceptor interactions were synthesized and structurally characterized. The ambiphilic ligand- aluminum cooperation enables C≡O bond cleavage and pyridine dearomatization, uncovering new avenues in low-valent aluminum chemistry.
Rotaxanes
Logic-Gated Release of a Dual Payload from a β-Lactam Mechanophore with a Rotaxane Actuator
Dr. Lei Chen, Prof. Dr. Guillaume De Bo
A rotaxane device operates as a logic AND gate to release a single or dual cargo payload upon application of force in the absence or the presence of water, respectively. This concept was demonstrated with the release of a ketene and varied drugs, paving the way for precision release applications.
Ferroptosis
EDTA-Mg Nano-Chelators Amplify Ferroptosis by Artificially Simulating the Epithelial-Mesenchymal Transition Process and Endogenous Iron Deprivation
Yulin Xie, Tengfei Jiang, Junrong Wang, Yanrong Qian, Wencheng Xu, Guanghui Zhao, Prof. Haidong Gao, Prof. Chunxia Li
Based on metal chelation therapy, we utilize the chelation performance of ethylene diamine tetraacetic acid (EDTA) for different divalent metal ions to achieve the precise regulation of the epithelial-mesenchymal transition (EMT) process in tumors and simultaneously synergize ferroptosis and immunotherapy to effectively inhibit the growth and metastasis of tumors.
Batteries
Amorphous Nitride-chloride Solid-State Electrolytes for High Performance All-Solid-State Lithium Batteries
Ting-Ting Wu, Dr. Si-Jie Guo, Dr. Hong-Shen Zhang, Yue Jiang, Jun Wang, Jiacheng Zhu, Dr. Xusheng Zhang, Dr. Pengfei Wei, Dr. Ziyang Hu, Rongzhi Gao, Prof. GuanHua Chen, Prof. Rui Wen, Prof. Xuefeng Wang, Prof. An-Min Cao
An amorphous nitrogenchloride dual-anion solid-state electrolyte (Li1.3ZrN0.4Cl4.1) with high ionic conductivity (3.01 mS cm−1 at 25 °C) and broad electrochemical stability is developed. When paired with LiNi0.83Co0.06Mn0.11O2, it enables all-solid-state batteries (ASSBs) with high capacity (200.1 mAh g−1 at 4.5 V), excellent cycle retention (95.1% after 150 cycles), and long-term durability (3,000 cycles at 3 C). The electrolyte remains stable under extreme conditions, operating at 4.8 V and 50 °C, demonstrating strong potential for high-energy, long-life ASSBs.
Pt-Based Hydrogen Oxidation
Site-Blocking Strategy Boosts H2S Tolerance in Platinum-Based Hydrogen Oxidation Catalysts
Wei Kang, Dr. Tao Shen, Ying Wang, Jilong Xu, Chuansheng Ma, Yue Wang, Dr. Yue-Jiao Zhang, Prof. Jia-Bo Le, Prof. Yifan Ye, Prof. Jian-Feng Li, Prof. Jin-Chao Dong
The in situ Raman spectroscopy reveals that the S-contained poisoning intermediates formed on pure Pt could be limited on PtRu alloy to enhance the H2S tolerance in hydrogen-oxygen fuel cells, which originates from the site-blocking effect and electronic tuning effect induced by Ru.
Bioorthogonal Reactions
Tuning Encodable Tetrazine Chemistry for Site-Specific Protein Bioorthogonal Ligations
Subhashis Jana, Alex J. Eddins, Yogesh M. Gangarde, P. Andrew Karplus, Ryan A. Mehl
We expand the bioorthogonal chemistry toolkit by synthesizing and characterizing 29 tetrazine ncAAs and evaluating their genetic encoding into proteins. Site-specific incorporation was achieved, and tools to assess efficiency, fidelity, stability, and reactivity were applied. This roadmap enabled the design of tunable tetrazines and the fastest quantitative labeling at 10⁶ M⁻¹s⁻¹ without compromising stability.
Polymer Chemistry
Catalytic Polymerization of n-Doped Poly(benzodifurandione) (n-PBDF) Using Parts Per Million (ppm) Levels of Molybdenum Trioxide
Dr. Guangchao Liu, Uttam Pal, Dr. Sanket Samal, Michael F. Espenship, Dr. Yuanhe Li, Dr. Won-June Lee, Lawal Adewale Ogunfowora, Dr. Liyan You, Prof. Julia Laskin, Prof. Jianguo Mei
An efficient, scalable, and cost-effective catalytic polymerization of n-PBDF using ppm levels of MoO3 was developed in this study. Kinetic studies reveal that this polymerization demonstrates chain-growth characteristics, enabling the preparation of high-quality n-PBDF polymers. Mechanistic investigations reveal that MoO3 mediates an oxidative pathway involving dimethyl sulfoxide (DMSO), with dimethyl sulfide (DMS) identified as the reduction product. This method eliminates the need for purification process, demonstrating the potential for large-scale production of high-quality n-PBDF ink.
Room-Temperature Phosphorescence
Molecular Engineering of Plant Polyphenols Into Amorphous Room-Temperature Phosphorescent Materials
Guobin Yang, Yajing Zhang, Chuang Lei, Dr. Yunxiang He, Yizhen Wang, Prof. Huijing Li, Prof. Yanchao Wu, Prof. Junling Guo
A phenolic-mediated molecular splicing and ring-locking strategy enables the fabrication of amorphous RTP systems with lifetimes up to 124 ms. The resulting phosphorescent nanoparticles exhibit exceptional biocompatibility, enabling high-contrast, time-resolved luminescence imaging, offering a sustainable approach for biomedical RTP applications.
Organic Materials
Chiral Co-Assembled Liquid Crystal Polymer Network Enabled by In-Situ Photopolymerization for High-Performance CP-OLEDs
Chunya Fu, Dong Li, Chao Liu, Yu Zhang, Junsheng Zhang, Yixiang Cheng
This work developed a facile in situ photopolymerization approach to construct rigid cholesteric liquid crystal polymer network (ChLC-PN) as the emitting layers (EML) for CP-OLEDs through chiral co-assembly strategy in cholesteric liquid crystal matrices.
DNAzyme
Framework Nucleic Acid-Mediated DNAzyme Chaperoning for Sensitive Trace Metal Ion Mapping on Live Neuronal Cell Membranes
Tianqi Xu, Fan Li, Yichao Jin, Feng Jia, Yu Wang, Tao Lv, Yueyue Zhang, Min Li, Chunhai Fan, Mingqiang Li, Xiaohua Zhang, Shaopeng Wang, Xiaolei Zuo
Inspired by the beneficial effects of molecular chaperones on the stability and functionality of proteins, we present in this study the development of tetrahedral DNA frameworks (TDF) as chaperones for DNAzymes. Integration of TDF with DNAzymes significantly improves sensitivity and stability, facilitating precise and quantitative mapping of local trace metal ion concentrations on live neuronal cell membranes. This adaptable approach sets a foundation for developing sensitive nanodevices based on DNAzymes.
Sustainable Carbon Sequestration
Long-Range Electronically Polarized Fe-N5 Catalysts Redirect Polymerization-Driven Phenolic Pollutant Removal Toward Sustainable Carbon Sequestration
Yanchun Deng, Prof. Yingtang Zhou, Dr. Zilong Song, Prof. Xin Yang
A long-range electronically polarized Fe-N5 catalyst is developed, enabling specific and efficient peroxymonosulfate (PMS)-catalyst complex generation. BPA removal is redirected by tailored PMS complexes from conventional radical-mediated mineralization pathways to interfacial polymerization. A 4-668 times higher total organic carbon (TOC) removal than reported for iron-based single-atom catalysts (Fe-SACs) is achieved, with sustainable practical wastewater treatment and carbon sequestration observed (>1700 h operation).
Direct X-ray Detectors
Solution-Processed Amorphous Zero-Dimensional Organic Metal Halide Hybrid Films for Direct X-Ray Detectors
Oluwadara J Olasupo, Abiodun M. Adewolu, Mohammad Khizr, Tarannuma F. Manny, He Liu, Tunde B. Shonde, Md S. Islam, Sahel Moslemi, Ethan Kim, J.S. Raaj V Winfred, Thilina N.D.D. Gamaralalage, Yan-Yan Hu, Ranjan Das, Biwu Ma
The use of solution-processed amorphous zero-dimensional organic metal halide hybrid (TPPCarz)2ZnBr4 films for direct X-ray detection is demonstrated. The amorphous films exhibit efficient molecular sensitization, with ZnBr42− species serving as X-ray absorbers and TPPCarz⁺ moieties as charge transporters. The resulting detectors achieve a detection sensitivity of 2165 µC Gyair−1cm−2 at 20 V mm−1 and a detection limit of 6.01 nGyair s−1.
Batteries
Local Electric Field Microenvironment-Induced Dynamic Spatial Confinement to Stabilize I+ Toward High-Mass-Loading and Stable Zinc-Iodine Batteries
Liting Chen, Song Huang, Zhenfeng Feng, Zhenxin Lin, Haolong Huang, Minghui Ye, Yufei Zhang, Zhipeng Wen, Yongchao Tang, Xiaoqing Liu, Cheng Chao Li
A local electric field (LEF) microenvironment is induced by the abundant polyquaternary ammonium cations in polydimethylammonium iodide (PDDA-I), which effectively spatially confine nucleophilic species (Cl−) on the cathode.This design dynamically coordinates the dense ligand sites around I+, ensuring the stable conversion of I+ ion even under high iodine mass loading conditions.
Metal Clusters for Catalysis
Photocatalytic Reduction of CO2 to CO in 100%: The Synergistic Effect of Nickel and Europium in Heterometallic Clusters
Kai-Peng Bai, Dr. Wei-Peng Chen, Meng-Di Cui, Prof. Yan-Zhen Zheng
Two series of 3d-4f nanoclusters with analogous structures were synthesized, and the {Ni24Eu10} cluster demonstrates high stability and exceptional performance in the photocatalytic reduction of CO2 to CO, which can be attributed to the synergistic interaction between the Ni(II) and Eu(III) metal centers within its [Ni4Eu] assembly units.
Electrophilic Functionalization
Reductive N2 Cleavage and Nitride Insertion Reactivity at Molybdenum Complexes Supported by a Rigid PNP Pincer
Minjun Kim, Jeewhan Oh, Sanha Park, Hankyul Lee, Prof. Dr. Zee Hwan Kim, Prof. Dr. Jin Kim, Dr. Heui Beom Lee, Prof. Dr. Jonghoon Choi, Prof. Dr. Yunho Lee
Reductive N2 cleavage at an acridane PNP pincer-supported Mo center leads to the first crystallographically characterized example of an unusual Mo(IV) nitride species featuring a bridging N2 coordination stabilized via Mo-N2 dπ-pπ backbonding interactions. Nitride functionalization with CO leads to Mo(II) isocyanate species.
Batteries
Symmetry Breaking Enabled Stable Oxygen Redox in Li-Rich Cathodes via π-Type Interaction
Dr. Fu-Da Yu, Zhe-Jian Yi, Hai-Nan Wang, Jia-Zhen Zhao, Yang-Qian Zhang, Prof. Yang Ren, Dr. Ji-Gang Zhou, Prof. Ji-Huai Wu, Prof. Zhang Lan, Prof. Yi-Ming Xie, Dr. Lan-Fang Que, Dr. Yun-Shan Jiang, Prof. Zhen-Bo Wang
Interfacial Li/Ni disordered via hydrothermal treatment is achieved in Li-rich cathode materials to trigger a robust π-type interaction between metal and ligand. The reductive coupling (charge transfer from O 2p to Ni t2g) and induced symmetry breaking of NiO6 is confirmed by X-ray absorption spectroscopy and theoretical calculations, which avoids excessive irreversible oxygen release from non-bonding O 2p state.
Batteries
Nuclear Quantum Confinement Enables Robust Deuterium Bonds for Highly Reversible Aluminum Anodes
Hao Cheng, Yao Lu, Zheng Li, Zibo Chen, Chao Chen, Xinyi Li, Hailin Yu, Adham Hashibon, Zhongliang Tian, Guanjie He
Quantum confinement by leveraging D as a quantum bridge is engineered to tailor stronger intra- and intermolecular D-bonds, effectively suppressing water reactivity and achieving exceptional HER inhibition. The induced Al3+ solvation structures further inhibit the decomposition of water at the interface and improve Al redox reversibility.
Graphene Nanoribbons
Engineering Graphene Nanoribbons via Periodically Embedding Oxygen Atoms
Dr. Yan Zhao, Dr. Li-Xia Kang, Yi-Jun Wang, Yi Wu, Guang-Yan Xing, Dr. Shi-Wen Li, Dr. Jinliang Pan, Nie-Wei Wang, Dr. Yin-Ti Ren, Ying Wang, Dr. Ya-Cheng Zhu, Prof. Xing-Qiang Shi, Dr. Mengxi Liu, Prof. Xiaohui Qiu, Prof. Pei-Nian Liu, Prof. Deng-Yuan Li
Two types of oxygen-doped graphene nanoribbons (O-doped chevron-GNR and O-doped chiral (2,1)-GNR) were synthesized on Au(111) via in situ formation of pyrans. Both O-doped GNRs are direct bandgap semiconductors but exhibit different sensitivities to oxygen dopants, which is attributed to the difference in the density of states near the Fermi level between the substituted intrinsic carbon atoms and their pristine counterparts.
Vibrational Strong Coupling
A Phenomenological Symmetry Rule for Chemical Reactivity Under Vibrational Strong Coupling
A. Jayachandran, B. Patrahau, J. G. Ricca, M. K. Mahato, Y. Pang, K. Nagarajan, A. Thomas, C. Genet, T. W. Ebbesen
A general symmetry rule emerges from the study of charge transfer complexes in cavities that points to an underlying framework to the predict the outcome of chemical reactivity under vibrational strong coupling.
Wastewater Treatment
Electron-Delocalized Cu2+ Activates Spin Channels in Spinel Oxides to Selectively Produce 1O2 for Wastewater Treatment
Le-Yang Hao, Zi-Jun Tang, Chu-Yi Cai, Yu-Chen Zhao, Dr. Lei Tian, Prof. Nan Li, Prof. Zhao-Qing Liu
This work proposes an electron-delocalized strategy to unlock FeTd2+─O─FeOh3+ spin channel, inducing intermolecular electron transfer of two PMS for selective 1O2 generation. The directed electron transfer behavior not only maintains the catalyst stability, but also immensely reduces the 1O2 generation energy barrier and improves the PMS utilization.
Asymmetrische Katalyse
Steuerbare endo/exo-Selektivität in direkten katalytisch- asymmetrischen 1,3-dipolaren Cycloadditionen mit polyfunktionellen Lewis-Säure-/Azolium-Aryloxid-Katalysatoren
Adrian Bürstner, Patrick M. Becker, Alexander Allgaier, Lucca Pfitzer, Dr. Daniel M. Wanner, Johanna Dollinger, Dr. Felix Willig, Justin Herrmann, Dr. Vukoslava Miskov-Pajic, Dr. Andreas C. Hans, Wolfgang Frey, Prof. Dr. Joris van Slageren, Prof. Dr. Johannes Kästner, Prof. Dr. René Peters
Ein neuartiges Konzept für katalytische asymmetrische 1,3-dipolare Cycloadditionen mit Iminoestern verwendet modulare polyfunktionelle Lewis-Säure-/Azolium-Aryloxid-Betain-Katalysatoren, die die endo- und exo-Selektivität durch Anpassungen des Metallzentrums, des Azoliums und der Sterik steuern. DFT-Studien zeigen eine nahezu perfekte räumliche Passung der funktionellen Einheiten, die eine präzise Orchestrierung der beteiligten katalytisch relevanten Einheiten ermöglicht, ähnlich enzymatischen Maschinerien.
Raman Scattering
Transfer Learning-Assisted SERS: Predicting Molecular Identity and Concentration in Mixtures Using Pure Compound Spectra
Dr. Emily Xi Tan, Jaslyn Ru Ting Chen, Desmond Wei Cheng Pang, Prof. Nguan Soon Tan, Prof. In Yee Phang, Prof. Xing Yi Ling
Transfer learning-driven SERS to elucidate mixtures with unknown composition and ratios.
Helicene
Federartiges Verhalten in [8]Helicendiimiden: Wie die Ganghöhe die optische Anisotropie und die elektronische Konjugation steuert
Fridolin Saal, Vincenzo Brancaccio, Dr. Krzysztof Radacki, Prof. Dr. Holger Braunschweig, Dr. Prince Ravat
Die Verbrückung der Stickstoffatome von [8]Helicendiimiden mit verschiedenen Alkylketten ermöglicht präzise Kontrolle der Ganghöhe ihrer Rückgrate. Dies hat tiefgreifende Auswirkungen auf die Molekülpackung, die Chiroptik und die elektronische Konjugation durch den Raum hindurch. Dieser Ansatz ermöglicht die Feinabstimmung der Eigenschaften dieser neuen Materialklasse und steigert die optische Anisotropie und die elektronische Kommunikation.
Oxygen Reduction Reaction
A Dual-Atom La2 Catalyst for the Oxygen Reduction Reaction
Jingru Sun, Tianmi Tang, Siying Zhang, Siyu Chen, Yingying Duan, Xue Bai, Xiaoqin Xu, Xiaodi Niu, Zhenlu Wang, Jingqi Guan
Using an ultra-fast printing technology, we have successfully embedded diatomic lanthanum sites onto a graphene framework, which shows excellent ORR performance. The La2-N6 configuration structure can effectively reduce the reaction barrier of RDS and promote effective charge transfer, thus enhancing the catalytic process, on which the intermediates and structural evolution were well uncovered by combining advanced characterizations and theoretical calculations.
Hydrogen Evolution Reaction
Ultrathin PtSe2 Nanowires in Single-Walled Carbon Nanotubes for Hydrogen Evolution Reaction
Nan Si, Rui Wang, Xianyu Hu, Yide Chang, Qingyuan He, Yang Wang, Yakui Mu, Yanming Wang, Siyu Liu, Qinglin Yuan
PtSe2 NWs grow anisotropically along the <110> direction inside the SWCNTs, and expose abundant zigzag edges, which contribute to the higher catalytic activity for HER. The as-prepared PtSe2 NWs exhibit excellent HER activity at extremely low Pt loading of 4.684 wt%, with an overpotential of 47 mV@10 mA cm−2 and a Tafel slope of 41.7 mV dec−1.
DNA Nanotechnology
Complex Donuts: Small Variations in DNA Sequence Dictate Pathway Complexity in DNA Nanotoroids
Muhammad Ghufran Rafique, Yihao Wu, Yutong Shi, Quentin Laurent, Abdelrahman Elmanzalawy, Christopher Saab, Yu Shi, Dmytro F. Perepichka, Jianing Li, Hanadi F. Sleiman
Chemical information encoded in the sequence of DNA amphiphiles enables the selective formation of kinetically trapped DNA nanotoroids through a complex self-assembly pathway. The toroids are formed as on-pathway structures via a competitive mechanism only when a toroid-selective DNA sequence is used.
Aluminiumchemie
Bemerkenswerte Reaktivität eines 1,2-Dihydrodialans mit organischen Aziden - vom terminalen Diazido-Dialuman zur pendeluhrartigen Azidbrücke
Dr. Xiaobai Wang, Dr. Franziska Traeger, Raphael F. Ligorio, Dr. Nico Graw, Dr. Regine Herbst-Irmer, Prof. Dr. Anna Krawczuk, Prof. Dr. Malte Fischer, Prof. Dr. Dietmar Stalke
Die Reaktion eines Dihydro-Dialans, das von einem Hybridliganden (DNI) koordiniert wird, mit organischen Aziden ergibt strukturell unterschiedliche Aluminiumspezies mit Aluminium in niedriger Oxidationsstufe: das erste Diazido-Dialan, ein Aluminium-Tetrazol und Produkte der Azid-Aluminierung. Spektroskopische Untersuchungen zeigen ein dynamisches Verhalten in Lösung mit einer Pendeluhr-ähnlichen Bewegung eines Benzylazids und Nα-Oszillation zwischen zwei Aluminiumatomen.
Ammonia Production
Ru Single Atoms Anchored in Metal Borides Enable Hydrogen Spillover for Superior Electrochemical Ammonia Production
Yuanguo Chen, Dr. Haoyun Bai, Dr. Jiao Lan, Dr. Cheng-Wei Kao, Dr. Feng Xie, Dr. Linghu Meng, Dr. Jilong Li, Dr. Ying-Rui Lu, Dr. Ming Peng, Prof. Hui Pan, Prof. Yongwen Tan
Single-atom Ru-decorated nanoporous metal borides are developed as high-performance electrochemical nitrate reduction electrocatalysts utilizing an atomic-scale hydrogen spillover effect. This strategy facilitates dissociation of water into *H and promotes the *H spillover for increasing *H coverage on the surface, thereby synergistically reducing the hydrogenation energy barrier for converting nitrate into valuable ammonia products.
Siloxane Electrolytes
Origin of Anion-Rich Solvation Structures in Siloxane Electrolytes
Yao-Peng Chen, Yi-Lin Niu, Dr. Zhao Zheng, Dr. Xiang Chen, Yu-Chen Gao, Nan Yao, Dr. Rui Zhang, Prof. Qiang Zhang
Siloxane electrolytes exhibit anion-rich solvation structures due to their large steric hindrance. The lower Pauli repulsion of Si─O bond compared to C─O bond leads to higher intrinsic stability than corresponding ethers.
Fuel Cells
Copper-Tailored Molybdenum-Nickel Catalyst Boosts Hydrogen Oxidation and Suppresses Parasitic Oxygen Reduction for Durable Fuel Cells
Lei Zhu, Xiao-Long Zhang, Yu Yang, Ye-Cheng Li, Ye-Hua Wang, Hui-Kun Yan, Fei-Yue Gao, Yu-Cai Zhang, Zhi-Zheng Wu, Shu-Ping Sun, Pu-Gan Lu, Wanjie Song, Prof. Xiaolin Ge, Prof. Tongwen Xu, Prof. Kai-Bin Tang, Prof. Min-Rui Gao
A copper-tailored MoNi4 alloyed catalyst (MoNi3.6Cu0.4) showing high hydrogen oxidation activity but low oxygen reduction activity in alkali has been developed. Such dual functionality tackles the issue of reverse-current decay—the harmful potential jump from parasitic anodic oxygen reduction during startup/shutdown events. When integrating into an anion-exchange membrane fuel cell, this catalyst demonstrates superior corrosion resistance and durability compared with the Pt/C counterpart over repeated startup/shutdown cycles.
Electrocatalysis
Catalyst-Engineered Proton Transfer Pathways for Selective Hydrogen Peroxide Electrosynthesis in Solid-State Electrolytes
Jun Wang, Dr. Junheng Huang, Chunguang Jia, Wenxing Chen, Junxiang Chen, Shengjian Lin, Yangjie Liu, Kai Chen, Yiqi Liang, Dr. Suqin Ci, Prof. Zhenhai Wen
We developed a rationally designed catalyst integrating Ni single atoms and NiO nanoclusters on porous carbon nanosheets for electrochemical H2O2 synthesis in solid electrolytes. This catalyst achieves 97% Faradaic efficiency and 356 mA cm−2 partial current density for pure H2O2 production. The study addresses a critical gap in elucidating proton transfer pathways in solid electrolytes during two-electron oxygen reduction reaction.
COFs for Gold Recovery
Stable Acrylamide-Linked Covalent Organic Frameworks via Mannich Polymerization for Efficient Gold Recovery from Complex E-Waste Leachates
Rui Zhang, Cheng-Peng Niu, Nai-Huai Dong, Prof. Ru-Ping Liang, Li-Ling Chen, Yun-Peng Wu, Ying-Ying Xiao, Ying-Ao Wang, Xiao-Xing Wang, Zhi-Hai Peng, Prof. Jian-Ding Qiu
Acrylamide-linked covalent organic frameworks (COFs) were synthesized through a one-step Mannich-type three-component polymerization. The resulting frameworks feature irreversible linkages, extended π-conjugation, and dual C═O/N─H coordination sites, enabling exceptional stability and highly selective gold recovery from complex electronic waste leachates.
Photoswitches
Conditional Stabilization of the Hypoxia-Inducible Factor HIF1α— Photoswitchable Stapled Peptides Prevent Elongin BC-Mediated Degradation
Dr. Van Tuan Trinh, Dr. Sabrina Fischer, Dr. Lei Zhang, Dr. Heiko Geisler, Belen Pardo, Dr. Robert Liefke, Dr. Frank Abendroth, Prof. Dr. Olalla Vázquez
Visible-light photoswitchable peptides enable the stabilization of the hydroxylated hypoxia transcription factor 1α (HIF1α—OH) by targeting the pVHL-EloBC interaction. Significant differences in conformation, binding, and transcription of HIF-targeted genes between the photostationary states (PSS) were demonstrated.
Organocatalysis
A Bioinspired Diazafluorenone Catalytic System for Aerobic Oxidative Deamination of Primary Amines
Sheng Gong, Wenhu Zhang, Yongchang Song, Jianfeng Chen, Baoguo Zhao
A highly efficient biomimetic aerobic oxidation of α-amino amides and benzylamines into α-keto amides and aromatic aldehydes is enabled by 1,8-diazafluoren-9-one (DFO), a new organocatalyst with a simple structure, high robustness, and strong electrophilicity.
MOFs for Upconversion
Upconversion Lanthanide-Based 2D Metal-Organic Frameworks for Multimode Information Encryption
Jiabo Chen, Yao Xie, Wanjun Yang, Renrui Sun, Prof. Feifei Xing, Gabrielle A. Mandl, Prof. John A. Capobianco, Prof. Lining Sun
A novel 2D Yb-PMA MOFs were synthesized, and upconversion luminescence under 980 nm excitation was successfully achieved by introducing Ho3+, Tb3+, or Eu3+ as the luminescence center and using Yb3+ as the sensitizer. The upconversion/down-shifting luminescent lanthanide-based 2D MOFs designed in this work show good potential for application in the field of information encryption.
Photoredox Catalysis
Counterintuitive Photochemistry of an Isolated Acridinyl Radical: ConPET via Preassembly, Solvated Electrons or a Long-Lived Excited State?
Dr. Samuel J. Horsewill, Katherine M. M. Sharrock, Dr. Péter P. Fehér, Dr. Jack M. Woolley, Dr. Imre Pápai, Dr. Daniel J. Scott
In this paper, we isolate the reduced form of a commonly used acridinium photocatalyst (acridinyl, Acr•) and investigate its photochemistry using transient absorption, analysed alongside TD-DFT calculations. We show that despite the apparent long lifetime of the fluorescent state of Acr•, it is not relevant to reactivity. Instead, reactivity occurs through counterintuitive preassembly and solvated electron-based mechanisms.
Photochemistry
Dynamic Regulation of Radical Photochromism and Photoluminescence via Polymer Polarity
Quanchi Tian, Qiuyue Ding, Chao Xu, Dr. Lunjun Qu, Dr. Kaiti Wang, Prof. Dr. Chaolong Yang, Prof. Yanli Zhao
The polarity of polymer matrices not only plays a crucial role in inducing room-temperature phosphorescence by protecting the naphthalene diimide core structure from quenching by oxygen and moisture, but also facilitates the generation of stable anion radicals through photoinduced electron transfer, even in the absence of UV irradiation.
Mechanically Interlocked Molecules
Is the Smallest Molecular Trefoil Knot Actually the Tightest One?
Wei-Tao Xu, Chenxing Guo, Yefei Jiang, Wei-Jian Li, Xiao-Qin Xu, Xue Li, Siqi Luo, Prof. Dr. Lianrui Hu, Prof. Dr. Xiujun Yu, Prof. Dr. Xiaopeng Li, Prof. Dr. Hai-Bo Yang, Prof. Dr. Wei Wang
The use of a modular self-assembly strategy has enabled the successful synthesis of a new family of molecular trefoil knots with varied backbone-atom numbers. An interesting odd-even effect of alkyl chain linkers on their tightness was demonstrated, which not only provides key insights into size-tightness relationships but also guides further development of knotted, woven, and entangled molecules and materials.
Room-Temperature Phosphorescence
N─B─N Isomer Induced Room Temperature Phosphorescence: Expression, Mechanistic Insights, and Multi-Level Anti-Counterfeiting Applications
Dr. Jianhua Liu, Junxiong Yao, Ruping Mu, Xinyi Mao, Haihua Li, Prof. Jianqi Sun, Jifeng Huang, Dr. Qiang Feng, Prof. Xiaohua Cao, Prof. Jianguo Wang, Prof. Huanan Huang
This study introduces an N─B─N unit-based strategy to enhance room temperature phosphorescence (RTP), highlighting that 1,1-DB shows strong RTP property, unlike its isomer 1,2-DB. The contrast in their performance aids in understanding the relationship between molecular structure and phosphorescence, offering insights for designing and optimizing RTP materials.
Nanomotors
Communicative Nanomotors Reprogram Cancer Cell Death via Pyroptosis
Mingchen Sun, Luc van Oss, Chenxuan Wan, Daniela A. Wilson
Communicative nanomotors respond to elevated ROS in the tumor microenvironment, enabling active communication and selective mitochondrial targeting through non-covalent surface engineering. Their precise interaction with cells induces mitochondrial damage, cytochrome c release, and pyroptotic cell death, while chemotactic motility ensures deeper tumor penetration, advancing intelligent cancer therapeutics.
Chiral Metal Halides
First Chiral Catalan Solid Based on Molybdenum Halide with Efficient Circularly Polarized Luminescence in the Deep-Red Region
Sehrish Gull, Wenkai Zhao, Zhaoyu Wang, Yunxin Zhang, Haolin Lu, Xinyi Niu, Tianjiao Qiao, Hebin Wang, Tianyin Shao, Wenting Liu, Prof. Bing Sun, Prof. Hao-Li Zhang, Prof. Yongsheng Chen, Prof. Guankui Long
The first chiral molybdenum halide tetrakis hexahedra was successfully synthesized via a solvothermal method. This unique Catalan solid structure exhibits efficient deep-red circularly polarized emission, enhanced stability, and improved photoluminescence quantum yield. The proposed system provides a novel platform for advancing the research on chiral metal halides and paves the way for their application toward chiral optoelectronics.
Homogeneous Catalysis
Stable Yet Strongly Lewis-Acidic Anions Enabling Cooperative Catalysis with Cationic Transition-Metal Complexes
Ryo Mandai, Prof. Dr. Takanori Iwasaki, Prof. Dr. Kyoko Nozaki
A stable tetraarylborate anion, BBcat, possessing strong Lewis acidity was synthesized. BBcat serves as a weakly coordinating counteranion for the cationic transition-metal complex, and its Ir complex exhibited up to 8.2-fold higher reaction rate than the common counteranion BArF in the hydrogen isotope exchange of 1,2-disubstituted arenes by cooperative catalysis of the cationic transition-metal complex and the Lewis-acidic counteranion.
Covalent Organic Frameworks
Stepwise Post-Modification of Pyridine-Imine COFs for Enhanced Hydrolytic Stability and Proton Conductivity
Hongfei Wang, Wen-Na Jiao, Wei-De Zhu, Si Huang, Xiao-Chun Lin, Ting Chen, Yanan Fan, Fangzheng Chen, Prof. Hai-Sen Xu, Prof. Mei Pan, Prof. Cheng-Yong Su
The self-condensation reaction of bifunctional monomers containing both amino and acetal groups yielded COF-LIFM7. Via subsequent amidation and N-oxidation modifications, the pore polarity and hydrophilicity of the post-modified COFs were progressively enhanced, consequently leading to a significant increase in proton conductivity.