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

Xu Zhang, Hui Su, Peixin Cui, Yongyong Cao, Zhenyuan Teng, Qitao Zhang, Yang Wang, Yibo Feng, Ran Feng, Jixiang Hou, Xiyuan Zhou, Peijie Ma, Hanwen Hu, Kaiwen Wang, Cong Wang, Liyong Gan, Yunxuan Zhao, Qinghua Liu (), Tierui Zhang () and Kun Zheng ()
Additional contact information
Xu Zhang: Beijing University of Technology
Hui Su: University of Science and Technology of China
Peixin Cui: Key Laboratory of Soil Environment and Pollution Remediation, Institute of Soil Science, Chinese Academy of Sciences
Yongyong Cao: Jiaxing University
Zhenyuan Teng: Nanyang Technological University
Qitao Zhang: Shenzhen University
Yang Wang: Chongqing University
Yibo Feng: Beijing University of Technology
Ran Feng: Beijing University of Technology
Jixiang Hou: Beijing University of Technology
Xiyuan Zhou: Beijing University of Technology
Peijie Ma: Beijing University of Technology
Hanwen Hu: Beijing University of Technology
Kaiwen Wang: Beijing University of Technology
Cong Wang: Beijing University of Technology
Liyong Gan: Chongqing University
Yunxuan Zhao: Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry, Chinese Academy of Sciences
Qinghua Liu: University of Science and Technology of China
Tierui Zhang: Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry, Chinese Academy of Sciences
Kun Zheng: Beijing University of Technology

Nature Communications, 2023, vol. 14, issue 1, 1-13

Abstract: 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.

Date: 2023
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DOI: 10.1038/s41467-023-42887-y

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