High-efficiency Electroreduction of O2 into H2O2 over ZnCo Bimetallic Triazole Frameworks Promoted by Ligand Activation
Zi-Meng Li
College of Chemical Engineering, National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fuzhou, 350002 China
These authors contributed equally to this work.
Search for more papers by this authorDr. Chao-Qi Zhang
School of Chemistry and Molecular Engineering, East China Normal University, Shanghai, 200241 China
These authors contributed equally to this work.
Search for more papers by this authorCorresponding Author
Prof. Chao Liu
School of Chemistry and Molecular Engineering, East China Normal University, Shanghai, 200241 China
Search for more papers by this authorProf. Hong-Wei Zhang
College of Chemical Engineering, National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fuzhou, 350002 China
Search for more papers by this authorDr. Hao Song
Australian Institute for Bioengineering and Nanotechnology, The University of Queensland, Brisbane, Queensland, 4072 Australia
Search for more papers by this authorProf. Zhi-Qiang Zhang
Shanghai Key Laboratory of Chemical Assessment and Sustainability, School of Chemical Science and Engineering, College of Environmental Science and Engineering, Tongji University, Shanghai, 200092 China
Search for more papers by this authorCorresponding Author
Prof. Guang-Feng Wei
Shanghai Key Laboratory of Chemical Assessment and Sustainability, School of Chemical Science and Engineering, College of Environmental Science and Engineering, Tongji University, Shanghai, 200092 China
Search for more papers by this authorProf. Xiao-Jun Bao
College of Chemical Engineering, National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fuzhou, 350002 China
Qingyuan Innovation Laboratory, Quanzhou, 362801 China
Search for more papers by this authorCorresponding Author
Prof. Cheng-Zhong Yu
School of Chemistry and Molecular Engineering, East China Normal University, Shanghai, 200241 China
Australian Institute for Bioengineering and Nanotechnology, The University of Queensland, Brisbane, Queensland, 4072 Australia
Search for more papers by this authorCorresponding Author
Prof. Pei Yuan
College of Chemical Engineering, National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fuzhou, 350002 China
Qingyuan Innovation Laboratory, Quanzhou, 362801 China
Search for more papers by this authorZi-Meng Li
College of Chemical Engineering, National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fuzhou, 350002 China
These authors contributed equally to this work.
Search for more papers by this authorDr. Chao-Qi Zhang
School of Chemistry and Molecular Engineering, East China Normal University, Shanghai, 200241 China
These authors contributed equally to this work.
Search for more papers by this authorCorresponding Author
Prof. Chao Liu
School of Chemistry and Molecular Engineering, East China Normal University, Shanghai, 200241 China
Search for more papers by this authorProf. Hong-Wei Zhang
College of Chemical Engineering, National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fuzhou, 350002 China
Search for more papers by this authorDr. Hao Song
Australian Institute for Bioengineering and Nanotechnology, The University of Queensland, Brisbane, Queensland, 4072 Australia
Search for more papers by this authorProf. Zhi-Qiang Zhang
Shanghai Key Laboratory of Chemical Assessment and Sustainability, School of Chemical Science and Engineering, College of Environmental Science and Engineering, Tongji University, Shanghai, 200092 China
Search for more papers by this authorCorresponding Author
Prof. Guang-Feng Wei
Shanghai Key Laboratory of Chemical Assessment and Sustainability, School of Chemical Science and Engineering, College of Environmental Science and Engineering, Tongji University, Shanghai, 200092 China
Search for more papers by this authorProf. Xiao-Jun Bao
College of Chemical Engineering, National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fuzhou, 350002 China
Qingyuan Innovation Laboratory, Quanzhou, 362801 China
Search for more papers by this authorCorresponding Author
Prof. Cheng-Zhong Yu
School of Chemistry and Molecular Engineering, East China Normal University, Shanghai, 200241 China
Australian Institute for Bioengineering and Nanotechnology, The University of Queensland, Brisbane, Queensland, 4072 Australia
Search for more papers by this authorCorresponding Author
Prof. Pei Yuan
College of Chemical Engineering, National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fuzhou, 350002 China
Qingyuan Innovation Laboratory, Quanzhou, 362801 China
Search for more papers by this authorAbstract
Co-based metal–organic frameworks (MOFs) as electrocatalysts for two-electron oxygen reduction reaction (2e− ORR) are highly promising for H2O2 production, but suffer from the intrinsic activity-selectivity trade-off. Herein, we report a ZnCo bimetal-triazole framework (ZnCo-MTF) as high-efficiency 2e− ORR electrocatalysts. The experimental and theoretical results demonstrate that the coordination between 1,2,3-triazole and Co increases the antibonding-orbital occupancy on the Co−N bond, promoting the activation of Co center. Besides, the adjacent Zn−Co sites on 1,2,3-triazole enable an asymmetric “side-on” adsorption mode of O2, favoring the reduction of O2 molecules and desorption of OOH* intermediate. By virtue of the unique ligand effect, the ZnCo-MTF exhibits a 2e− ORR selectivity of ≈100 %, onset potential of 0.614 V and H2O2 production rate of 5.55 mol gcat−1 h−1, superior to the state-of-the-art zeolite imidazole frameworks. Our work paves the way for the design of 2e− ORR electrocatalysts with desirable coordination and electronic structure.
Conflict of interest
The authors declare no conflict of interest.
Open Research
Data Availability Statement
The data that support the findings of this study are available from the corresponding author upon reasonable request.
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