Volume 61, Issue 45 e202209693
Communication

Engineering Support and Distribution of Palladium and Tin on MXene with Modulation of the d-Band Center for CO-resilient Methanol Oxidation

Shufen Chen

Shufen Chen

State Key Laboratory of Optoelectronic Materials and Technologies, Guangzhou Key Laboratory of Flexible Electronic Materials and Wearable Devices, Nanotechnology Research Center, School of Materials Science and Engineering, Sun Yat-sen University, Guangzhou, 510275 China

School of Biomedical Science, The Chinese University of Hong Kong, Hong Kong, 999077 China

These authors contributed equally to this work.

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Ning Liu

Ning Liu

State Key Laboratory of Optoelectronic Materials and Technologies, Guangzhou Key Laboratory of Flexible Electronic Materials and Wearable Devices, Nanotechnology Research Center, School of Materials Science and Engineering, Sun Yat-sen University, Guangzhou, 510275 China

These authors contributed equally to this work.

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Junjie Zhong

Junjie Zhong

State Key Laboratory of Optoelectronic Materials and Technologies, Guangzhou Key Laboratory of Flexible Electronic Materials and Wearable Devices, Nanotechnology Research Center, School of Materials Science and Engineering, Sun Yat-sen University, Guangzhou, 510275 China

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Dr. Rongliang Yang

Dr. Rongliang Yang

State Key Laboratory of Optoelectronic Materials and Technologies, Guangzhou Key Laboratory of Flexible Electronic Materials and Wearable Devices, Nanotechnology Research Center, School of Materials Science and Engineering, Sun Yat-sen University, Guangzhou, 510275 China

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Dr. Bo Yan

Dr. Bo Yan

State Key Laboratory of Optoelectronic Materials and Technologies, Guangzhou Key Laboratory of Flexible Electronic Materials and Wearable Devices, Nanotechnology Research Center, School of Materials Science and Engineering, Sun Yat-sen University, Guangzhou, 510275 China

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Prof. Liyong Gan

Prof. Liyong Gan

Institute for Structure and Function, Department of Physics, Chongqing University, Chongqing, 400044 China

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Prof. Peng Yu

Prof. Peng Yu

State Key Laboratory of Optoelectronic Materials and Technologies, Guangzhou Key Laboratory of Flexible Electronic Materials and Wearable Devices, Nanotechnology Research Center, School of Materials Science and Engineering, Sun Yat-sen University, Guangzhou, 510275 China

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Prof. Xuchun Gui

Prof. Xuchun Gui

State Key Laboratory of Optoelectronic Materials and Technologies, School of Electronics and Information Technology, Sun Yat-sen University, Guangzhou, 510275 China

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Prof. Hongbin Yang

Corresponding Author

Prof. Hongbin Yang

School of Materials Science and Engineering, Suzhou University of Science and Technology, Suzhou, 215009 China

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Prof. Dingshan Yu

Corresponding Author

Prof. Dingshan Yu

Key Laboratory for Polymeric Composite and Functional Materials of Ministry of Education, Key Laboratory of High Performance Polymer-Based Composites of Guangdong Province, School of Chemistry, Sun Yat-sen University, Guangzhou, 510275 China

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Prof. Zhiping Zeng

Corresponding Author

Prof. Zhiping Zeng

State Key Laboratory of Optoelectronic Materials and Technologies, Guangzhou Key Laboratory of Flexible Electronic Materials and Wearable Devices, Nanotechnology Research Center, School of Materials Science and Engineering, Sun Yat-sen University, Guangzhou, 510275 China

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Prof. Guowei Yang

Prof. Guowei Yang

State Key Laboratory of Optoelectronic Materials and Technologies, Guangzhou Key Laboratory of Flexible Electronic Materials and Wearable Devices, Nanotechnology Research Center, School of Materials Science and Engineering, Sun Yat-sen University, Guangzhou, 510275 China

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First published: 16 September 2022
Citations: 61

Graphical Abstract

Boosted electron interaction of metal nano-alloy with Se-doped MXene and optimized distribution of Pd−Sn sites on PdSn0.5/Se−Ti3C2 can modulate the d band center, decrease adsorption energies of CO* at Pd site and enhance OH* generation at Sn site, thus removing CO poisonous intermediates, and thereby significantly enhancing methanol oxidation reaction (MOR) efficiency and durability of the anodic catalyst for a direct methanol fuel cell (DMFC).

Abstract

The efficiency of direct methanol fuel cell (DMFC) is largely determined by the activity and durability of methanol oxidation reaction (MOR) catalysts. Herein, we present a CO-resilient MOR catalyst of palladium-tin nano-alloy anchored on Se-doped MXene (PdSn0.5/Se−Ti3C2) via a progressive one-step electrochemical deposition strategy. MOR mass activity resulting from Pd/Se−Ti3C2 catalyst (1046.2 mA mg−1) is over 2-fold larger than that of Pd/Ti3C2, suggesting that the introduction of Se atoms on MXene might accelerate the reaction kinetics. PdSn0.5/Se−Ti3C2 with Se-doping progress of MXene and the cooperated Pd−Sn sites has a superior MOR mass activity (4762.8 mA mg−1), outperforming many other reported Pd-based catalysts. Both experimental results and theoretical calculation reveal that boosted electron interaction of metal crystals with Se-doped MXene and optimized distribution of Pd−Sn sites can modulate the d band center, reduce adsorption energies of CO* at Pd site and enhance OH* generation at Sn site, resulting in highly efficient removal of CO intermediates by reaction with neighboring OH species on adjacent Sn sites.

Data Availability Statement

The data that support the findings of this study are available in the supplementary material of this article.

The full text of this article hosted at iucr.org is unavailable due to technical difficulties.