Dual effect of the coordination field and sulphuric acid on the properties of a single-atom catalyst in the electrosynthesis of H2O2

文献情報

出版日 2021-09-06

DOI 10.1039/D1CP03189A

インパクトファクター 3.676

著者

Jinkong Pan, Qiaojun Fang, Qian Xia, Anfu Hu, Fuli Sun, Wei Zhang, Yifan Yu, Guilin Zhuang, Jian Jiang, Jianguo Wang

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要旨

Electrocatalytic synthesis of hydrogen peroxide (H2O2) via the two-electron oxygen reduction reaction (2e− ORR) is the ideal solution for on-site H2O2 production. Herein, we propose a new strategy for creating new 2e− ORR catalysts by introducing electron-deficient B atoms and electron-rich N atoms to regulate the coordination field of metal ions on a graphene substrate. Through the first-principles density functional theory (DFT) calculations, NiN2B2-h was screened out as it had a low overpotential (0.12 V) for 2e− ORR. The Bader charge analysis revealed that B atoms increased the charge density of Ni atoms, leading to moderate binding of O2. Furthermore, the combination of ab initio molecular dynamic (AIMD) calculations and DFT calculations in an H2SO4 environment revealed a new reaction mechanism of H2O2 synthesis, involving proton-transfer between activated O2 and HSO4−. Moreover, the rate-determining step (0.63 eV) of H2O2 desorption in the presence of H2SO4 was different from that of OOH* protonation (0.45 eV) under the gas phase. This difference is attributed to the hydrogen-bond network in the acid solution.

掲載誌

Physical Chemistry Chemical Physics

CiteScore: 5.5

自己引用率: 10.3%

年間論文数: 3036

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.

Dual effect of the coordination field and sulphuric acid on the properties of a single-atom catalyst in the electrosynthesis of H2O2

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掲載誌

Physical Chemistry Chemical Physics

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