High-efficiency Electroreduction of O 2 into H 2 O 2 over ZnCo Bimetallic Triazole Frameworks Promoted by Ligand Activation.

Autor: Li ZM; College of Chemical Engineering, National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fuzhou, 350002, China., Zhang CQ; School of Chemistry and Molecular Engineering, East China Normal University, Shanghai, 200241, China., Liu C; School of Chemistry and Molecular Engineering, East China Normal University, Shanghai, 200241, China., Zhang HW; College of Chemical Engineering, National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fuzhou, 350002, China., Song H; Australian Institute for Bioengineering and Nanotechnology, The University of Queensland, Brisbane, Queensland, 4072, Australia., Zhang ZQ; 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., Wei GF; 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., Bao XJ; College of Chemical Engineering, National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fuzhou, 350002, China.; Qingyuan Innovation Laboratory, Quanzhou, 362801, China., Yu CZ; 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., Yuan P; College of Chemical Engineering, National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fuzhou, 350002, China.; Qingyuan Innovation Laboratory, Quanzhou, 362801, China.
Jazyk: angličtina
Zdroj: Angewandte Chemie (International ed. in English) [Angew Chem Int Ed Engl] 2024 Jan 08; Vol. 63 (2), pp. e202314266. Date of Electronic Publication: 2023 Dec 01.
DOI: 10.1002/anie.202314266
Abstrakt: Co-based metal-organic frameworks (MOFs) as electrocatalysts for two-electron oxygen reduction reaction (2e - ORR) are highly promising for H 2 O 2 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 O 2 , favoring the reduction of O 2 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 H 2 O 2 production rate of 5.55 mol g cat -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.
(© 2023 Wiley-VCH GmbH.)
Databáze: MEDLINE
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