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Multiscale modifications of carbon nitride to strengthen reaction kinetics and lower thermodynamic barriers for efficient photocatalytic oxygen evolution
Zhang, Yang1; Cao, Ning1; Wang, Caihao1; Zhao, Chaocheng1; Wang, Yongqiang1; Zhao, Shiyong2; Zhang, Jinqiang3
通讯作者Wang, Yongqiang(wangyq@upc.edu.cn) ; Zhang, Jinqiang(jinqiang.zhang@adelaide.edu.au)
2025-04-01
发表期刊JOURNAL OF COLLOID AND INTERFACE SCIENCE
ISSN0021-9797
卷号683页码:954-963
摘要Photocatalytic oxygen evolution reaction (OER) is pivotal for sustainable energy systems yet lacks high-performance catalysts capable of strong visible light absorption, robust charge dynamics, fast reaction kinetics, and high oxidation capability. Herein, we report the multiscale optimization of carbon nitride through the construction of porous curled carbon nitride nanosheets (CNA-B30) incorporating boron center/cyano group Lewis acid-base pairs (LABPs). The unique chemical and structural features of CNA-B30 extended the photoabsorption edges of pi -> pi* and n -> pi* electronic transitions to 470 nm and 715 nm, respectively. Planar distortion and LABPs induced charge redistribution, enhancing the built-in electric field to promote efficient charge dissociation and transport. Moreover, boron atoms elevated the valence band of carbon nitride and served as active oxidation sites, effectively lowering the thermodynamic barrier for water oxidation. As a result, CNA-B30 demonstrated outstanding OER activity, achieving 586.5 mu mol g(-1) h(-1) (lambda > 420 nm) without co-catalysts. With the addition of a Co co-catalyst, the oxygen evolution rate increased to 2085.5 mu mol g(-1) h(-1) (lambda > 420 nm), and an apparent quantum efficiency of 5.8 % at 420 nm, surpassing most state-of-the-art OER photocatalysts. This work offers valuable insights into designing advanced OER photocatalysts for efficient solar fuel production.
关键词Carbon nitride Multiscale modifications Photocatalysis Oxygen evolution Overall enhancement
资助者National Science and Technology Major Project
DOI10.1016/j.jcis.2024.12.144
收录类别SCI
语种英语
资助项目National Science and Technology Major Project[2016ZX05040003]
WOS研究方向Chemistry
WOS类目Chemistry, Physical
WOS记录号WOS:001395106100001
出版者ACADEMIC PRESS INC ELSEVIER SCIENCE
引用统计
文献类型期刊论文
条目标识符http://ir.imr.ac.cn/handle/321006/180944
专题中国科学院金属研究所
通讯作者Wang, Yongqiang; Zhang, Jinqiang
作者单位1.China Univ Petr East China, State Key Lab Petr Pollut Control, 66 West Changjiang Rd, Qingdao 266580, Peoples R China
2.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Peoples R China
3.Univ Adelaide, Sch Chem Engn, North Terrace, Adelaide, SA 5005, Australia
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Zhang, Yang,Cao, Ning,Wang, Caihao,et al. Multiscale modifications of carbon nitride to strengthen reaction kinetics and lower thermodynamic barriers for efficient photocatalytic oxygen evolution[J]. JOURNAL OF COLLOID AND INTERFACE SCIENCE,2025,683:954-963.
APA Zhang, Yang.,Cao, Ning.,Wang, Caihao.,Zhao, Chaocheng.,Wang, Yongqiang.,...&Zhang, Jinqiang.(2025).Multiscale modifications of carbon nitride to strengthen reaction kinetics and lower thermodynamic barriers for efficient photocatalytic oxygen evolution.JOURNAL OF COLLOID AND INTERFACE SCIENCE,683,954-963.
MLA Zhang, Yang,et al."Multiscale modifications of carbon nitride to strengthen reaction kinetics and lower thermodynamic barriers for efficient photocatalytic oxygen evolution".JOURNAL OF COLLOID AND INTERFACE SCIENCE 683(2025):954-963.
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