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

被引：239

作者：

Zhang, Xu ^{[1
]}

Su, Hui ^{[2
,3
]}

Cui, Peixin ^{[4
]}

Cao, Yongyong ^{[5
]}

Teng, Zhenyuan ^{[6
]}

Zhang, Qitao ^{[7
]}

Wang, Yang ^{[8
]}

Feng, Yibo ^{[1
]}

Feng, Ran ^{[1
]}

Hou, Jixiang ^{[1
]}

Zhou, Xiyuan ^{[1
]}

Ma, Peijie ^{[1
]}

Hu, Hanwen ^{[1
]}

Wang, Kaiwen ^{[1
]}

Wang, Cong ^{[1
]}

Gan, Liyong ^{[8
]}

Zhao, Yunxuan ^{[9
]}

Liu, Qinghua ^{[2
]}

Zhang, Tierui ^{[9
]}

Zheng, Kun ^{[1
]}

机构：

[1] Beijing Univ Technol, Fac Mat & Mfg, Beijing Key Lab Microstruct & Properties Solid, Beijing 100124, Peoples R China

[2] Univ Sci & Technol China, Natl Synchrotron Radiat Lab, Hefei 230029, Anhui, Peoples R China

[3] Hunan Normal Univ, Coll Chem & Chem Engn, Changsha 410081, Hunan, Peoples R China

[4] Chinese Acad Sci, Inst Soil Sci, Key Lab Soil Environm & Pollut Remediat, Nanjing 210008, Peoples R China

[5] Jiaxing Univ, Coll Biol Chem Sci & Engn, Jiaxing 314001, Zhejiang, Peoples R China

[6] Nanyang Technol Univ, Sch Chem Chem Engn & Biotechnol, Singapore 637459, Singapore

[7] Shenzhen Univ, Inst Microscale Optoelect, Int Collaborat Lab 2D Mat Optoelect Sci & Tech, Minist Educ, Shenzhen 518060, Peoples R China

[8] Chongqing Univ, Coll Phys & Inst Adv Interdisciplinary Studies, Chongqing 400044, Chongqing, Peoples R China

[9] Chinese Acad Sci, Tech Inst Phys & Chem, Key Lab Photochem Convers & Optoelect Mat, Beijing, Peoples R China

来源：

NATURE COMMUNICATIONS | 2023年 / 14卷 / 01期

基金：

中国国家自然科学基金;

关键词：

HYDROGEN-PEROXIDE PRODUCTION; ELECTROCHEMICAL SYNTHESIS; GENERAL-SYNTHESIS; WATER; CATALYSTS; IDENTIFICATION; CONVERSION; OXYGEN;

D O I：

10.1038/s41467-023-42887-y

中图分类号：

O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];

学科分类号：

07 ; 0710 ; 09 ;

摘要：

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 420nm 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-N-3 sites dynamically transform into high-valent O-1-Ni-N-2 sites after O-2 adsorption and further evolve to form a key *OOH intermediate before finally forming HOO-Ni-N-2. 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.

引用

页数：13

共 56 条

[1] PROJECTOR AUGMENTED-WAVE METHOD [J].