文献类型：期刊文献

英文题名：Boron-Sulfur Pairs for Highly Active 2e- Oxygen Reduction Reaction to Electrochemically Synthesize Hydrogen Peroxide

作者：Wu, Yuhan[1] Yuan, Qixin[1] Zhao, Yuying[2] Xu, Xiang[1] Xu, Jing[1] Wang, Yan[1] Sun, Kang[2] Wang, Ao[2] Sun, Hao[2] Li, Bei[2] Xu, Ruting[2] Wang, Zeming[3] Jiang, Jianchun[2] Fan, Mengmeng[1,2]

第一作者：Wu, Yuhan

机构：[1] Jiangsu Co-Innovation Center of Efficient Processing and Utilization of Forest Resources, International Innovation Center for Forest Chemicals and Materials, College of Chemical Engineering, Nanjing Forestry University, Nanjing, 210037, China; [2] Key Lab of Biomass Energy and Material, Jiangsu Province, Jiangsu Co-Innovation Center of Efficient Processing and Utilization of Forest Resources, Institute of Chemical Industry of Forest Products, Chinese Academy of Forestry, Nanjing, 210042, China; [3] Institute of Nanochemistry and Nanobiology, School of Environmental and Chemical Engineering, Shanghai University, Shanghai, 200444, China

年份：2023

卷号：11

期号：36

起止页码：13363-13373

外文期刊名：ACS Sustainable Chemistry and Engineering

收录：EI(收录号：20233914774557);Scopus(收录号：2-s2.0-85171732346)

语种：英文

外文关键词：Boron - Carbon - Catalyst selectivity - Density functional theory - Electrocatalysts - Electrodes - Electrolytic reduction - Hydrogen peroxide - Oxidation - Oxygen

摘要：Past decade has witnessed the great improvement of carbon-based dual-single metal-site electrocatalysts. However, there are rare reports exploring the enhanced effect of a nonmetallic "dual-site" in carbon-based catalysts. Herein, a "H3BO3 template" method is proposed to fabricate highly active B-S pairs dispersed on a hierarchically microporous/mesoporous carbon matrix to electrochemically synthesize hydrogen peroxide by two-electron oxygen reduction reaction. Under the synergistic effect of B-S pairs and advantageous nanostructures, the catalytic performance outperforms the reported metal-free carbon catalysts in alkaline electrolytes, especially, with a high HO2- selectivity of 90-94% at a wide potential range of 0.3-0.7 V versus reversible hydrogen electrode (RHE) using a rotating ring-disk electrode, Faradaic efficiency of over 90% during 11 h stability testing, and high mass activity of 756 mmol gcatalyst-1 h-1 in a flow cell. Density functional theory demonstrates that the carbon atoms nearby B-S pairs exhibit predominant catalytic sites. This paper proposes a new approach to distinctly improve the catalytic performance by dual heteroatom pairs. ? 2023 American Chemical Society