Developing Ni single-atom sites in carbon nitride for efficient photocatalytic H2O2 production - Details

Author：

Indexed by：

Scopus SCIE

Abstract：

Photocatalytic　two-electron　oxygen　reduction　to　produce　high-value　hydrogen　peroxide　(H2O2)　is　gaining　popularity　as　a　promising　avenue　of　research.　However,　structural　evolution　mechanisms　of　catalytically　active　sites　in　the　entire　photosynthetic　H2O2　system　remains　unclear　and　seriously　hinders　the　development　of　highly-active　and　stable　H2O2　photocatalysts.　Herein,　we　report　a　high-loading　Ni　single-atom　photocatalyst　for　efficient　H2O2　synthesis　in　pure　water,　achieving　an　apparent　quantum　yield　of　10.9%　at　420　nm　and　a　solar-to-chemical　conversion　efficiency　of　0.82%.　Importantly,　using　in　situ　synchrotron　X-ray　absorption　spectroscopy　and　Raman　spectroscopy　we　directly　observe　that　initial　Ni-N3　sites　dynamically　transform　into　high-valent　O1-Ni-N2　sites　after　O2　adsorption　and　further　evolve　to　form　a　key　*OOH　intermediate　before　finally　forming　HOO-Ni-N2.　Theoretical　calculations　and　experiments　further　reveal　that　the　evolution　of　the　active　sites　structure　reduces　the　formation　energy　barrier　of　*OOH　and　suppresses　the　O=O　bond　dissociation,　leading　to　improved　H2O2　production　activity　and　selectivity.　©　2023,　The　Author(s).

Keyword：

Author Community：

[ 1 ] [Zhang X.]Beijing Key Laboratory of Microstructure and Properties of Solids, Faculty of Materials and Manufacturing, Beijing University of Technology, Beijing, 100124, China
[ 2 ] [Su H.]National Synchrotron Radiation Laboratory, University of Science and Technology of China, Anhui, Hefei, 230029, China
[ 3 ] [Su H.]College of Chemistry and Chemical Engineering, Hunan Normal University, Hunan, Changsha, 410081, China
[ 4 ] [Cui P.]Key Laboratory of Soil Environment and Pollution Remediation, Institute of Soil Science, Chinese Academy of Sciences, Nanjing, 210008, China
[ 5 ] [Cao Y.]College of Biological, Chemical Science and Engineering, Jiaxing University, Zhejiang, Jiaxing, 314001, China
[ 6 ] [Teng Z.]School of Chemistry, Chemical Engineering and Biotechnology, Nanyang Technological University, Singapore, 637459, Singapore
[ 7 ] [Zhang Q.]International Collaborative Laboratory of 2D Materials for Optoelectronics Science and Technology of Ministry of Education, Institute of Microscale Optoelectronics, Shenzhen University, Shenzhen, 518060, China
[ 8 ] [Wang Y.]College of Physics and Institute of Advanced Interdisciplinary Studies, Chongqing University, Chongqing, 400044, China
[ 9 ] [Feng Y.]Beijing Key Laboratory of Microstructure and Properties of Solids, Faculty of Materials and Manufacturing, Beijing University of Technology, Beijing, 100124, China
[ 10 ] [Feng R.]Beijing Key Laboratory of Microstructure and Properties of Solids, Faculty of Materials and Manufacturing, Beijing University of Technology, Beijing, 100124, China
[ 11 ] [Hou J.]Beijing Key Laboratory of Microstructure and Properties of Solids, Faculty of Materials and Manufacturing, Beijing University of Technology, Beijing, 100124, China
[ 12 ] [Zhou X.]Beijing Key Laboratory of Microstructure and Properties of Solids, Faculty of Materials and Manufacturing, Beijing University of Technology, Beijing, 100124, China
[ 13 ] [Ma P.]Beijing Key Laboratory of Microstructure and Properties of Solids, Faculty of Materials and Manufacturing, Beijing University of Technology, Beijing, 100124, China
[ 14 ] [Hu H.]Beijing Key Laboratory of Microstructure and Properties of Solids, Faculty of Materials and Manufacturing, Beijing University of Technology, Beijing, 100124, China
[ 15 ] [Wang K.]Beijing Key Laboratory of Microstructure and Properties of Solids, Faculty of Materials and Manufacturing, Beijing University of Technology, Beijing, 100124, China
[ 16 ] [Wang C.]Beijing Key Laboratory of Microstructure and Properties of Solids, Faculty of Materials and Manufacturing, Beijing University of Technology, Beijing, 100124, China
[ 17 ] [Gan L.]College of Physics and Institute of Advanced Interdisciplinary Studies, Chongqing University, Chongqing, 400044, China
[ 18 ] [Zhao Y.]Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry, Chinese Academy of Sciences, Beijing, China
[ 19 ] [Liu Q.]National Synchrotron Radiation Laboratory, University of Science and Technology of China, Anhui, Hefei, 230029, China
[ 20 ] [Zhang T.]Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry, Chinese Academy of Sciences, Beijing, China
[ 21 ] [Zheng K.]Beijing Key Laboratory of Microstructure and Properties of Solids, Faculty of Materials and Manufacturing, Beijing University of Technology, Beijing, 100124, China

Reprint Author's Address：

Email：

Show more details

Related Keywords：

Source ：

Nature Communications

ISSN： 2041-1723

Year： 2023

Issue： 1

Volume： 14

1 6 . 6 0 0

JCR@2022

ESI Discipline： Multidisciplinary;

ESI HC Threshold：20

Cited Count：

WoS CC Cited Count： 0

SCOPUS Cited Count： 148

ESI Highly Cited Papers on the List： 0 Unfold All

WanFang Cited Count：

Chinese Cited Count：

30 Days PV： 6

Affiliated Colleges：

Get Fulltext

DOI Library Discovery Baidu Scholar Search SCOPUS

Type
Departments

All Years Choose Year From to