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- Title
Developing Ni single-atom sites in carbon nitride for efficient photocatalytic H<sub>2</sub>O<sub>2</sub> production.
- Authors
Zhang, Xu; Su, Hui; Cui, Peixin; Cao, Yongyong; Teng, Zhenyuan; Zhang, Qitao; Wang, Yang; Feng, Yibo; Feng, Ran; Hou, Jixiang; Zhou, Xiyuan; Ma, Peijie; Hu, Hanwen; Wang, Kaiwen; Wang, Cong; Gan, Liyong; Zhao, Yunxuan; Liu, Qinghua; Zhang, Tierui; Zheng, Kun
- 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. Here, the authors explore how Ni single-atom sites on carbon nitride evolve under photocatalytic conditions. They show that this evolution plays a pivotal role in enhancing photocatalytic H2O2 production.
- Subjects
NITRIDES; RAMAN spectroscopy; ACTIVATION energy; X-ray absorption; HYDROGEN peroxide; X-ray spectroscopy; OXYGEN reduction
- Publication
Nature Communications, 2023, Vol 14, Issue 1, p1
- ISSN
2041-1723
- Publication type
Article
- DOI
10.1038/s41467-023-42887-y