A Full-Spectrum ZnS Photocatalyst with Gradient Distribution of Atomic Copper Dopants and Concomitant Sulfur Vacancies for Highly Efficient Hydrogen Evolution

doi:10.1021/acsnano.3c12773

IMR OpenIR

	A Full-Spectrum ZnS Photocatalyst with Gradient Distribution of Atomic Copper Dopants and Concomitant Sulfur Vacancies for Highly Efficient Hydrogen Evolution
	Bao, Linping 1; Ali, Sajjad 2; Dai, Chunhui 3; Zeng, Qing 4,5; Zeng, Chao 1; Jia, Yushuai 1; Liu, Xin 1; Wang, Ping 1; Ren, Xiaohui 6; Yang, Teng 9; Bououdina, Mohamed 7; Lu, Zhang-Hui 1; Wei, Yuechang 10; Yu, Xuan 8; Zhou, Yingtang 8
通讯作者	Zeng, Chao(czeng@jxnu.edu.cn) ; Yang, Teng(yangteng@imr.ac.cn) ; Wei, Yuechang(weiyc@cup.edu.cn) ; Zhou, Yingtang(zhouyingtang@zjou.edu.cn)
	2024-02-06
发表期刊	ACS NANO
ISSN	1936-0851
卷号	18 期号:7 页码:5878-5889
摘要	A rarely discussed phenomenon in the realm of photocatalytic materials involves the presence of gradient distributed dopants and defects from the interior to the surface. This intriguing characteristic has been successfully achieved in the case of ZnS through the incorporation of atomic monovalent copper ions (Cu+) and concurrent sulfur vacancies (V-s), resulting in a photocatalyst denoted as G-CZS(1-x). Through the cooperative action of these atomic Cu dopants and Vs, G-CZS(1-x) significantly extends its photoabsorption range to encompass the full spectrum (200-2100 nm), which improves the solar utilization ability. This alteration enhances the efficiency of charge separation and optimizes Delta(H) (free energy of hydrogen adsorption) to approach 0 eV for the hydrogen evolution reaction (HER). It is noteworthy that both surface-exposed atomic Cu and V-s act as active sites for photocatalysis. G-CZS(1-x) exhibits a significant H-2 evolution rate of 1.01 mmol h(-1) in the absence of a cocatalyst. This performance exceeds the majority of previously reported photocatalysts, exhibiting approximately 25-fold as ZnS, and 5-fold as H-CZS(1-x) with homogeneous distribution of equal content Cu dopants and Vs. In contrast to G-CZS(1-x), the H adsorption on Cu sites for H-CZS(1-x) (Delta G(H) = -1.22 eV) is excessively strong to inhibit the H-2 release, and the charge separation efficiency for H-CZS(1-x) is relatively sluggish, revealing the positive role of a gradient distribution model of dopants and defects on activity enhancement. This work highlights the synergy of atomic dopants and defects in advancing photoactivity, as well as the significant benefit of the controllable distribution model of dopants and defects for photocatalysis.
关键词	photocatalysis hydrogen evolution atomicCu doping sulfur vacancy full-spectrum
资助者	National Natural Science Foundation of China ; National Natural Science Foundation of China ; Zhejiang Province key research and development project
DOI	10.1021/acsnano.3c12773
收录类别	SCI
语种	英语
资助项目	National Natural Science Foundation of China[52002158] ; National Natural Science Foundation of China[52031014] ; National Natural Science Foundation of China[2023 C01191] ; Zhejiang Province key research and development project
WOS研究方向	Chemistry ; Science & Technology - Other Topics ; Materials Science
WOS类目	Chemistry, Multidisciplinary ; Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary
WOS记录号	WOS:001163380800001
出版者	AMER CHEMICAL SOC
引用统计
文献类型	期刊论文
条目标识符	http://ir.imr.ac.cn/handle/321006/184290
专题	中国科学院金属研究所
通讯作者	Zeng, Chao; Yang, Teng; Wei, Yuechang; Zhou, Yingtang
作者单位	1.Jiangxi Normal Univ, Inst Adv Mat, Coll Chem & Chem Engn, Nanchang 330224, Peoples R China 2.Prince Sultan Univ, Coll Humanities & Sci, Energy Water & Environm Lab, Riyadh 11586, Saudi Arabia 3.East China Univ Technol, Sch Chem Biol & Mat Sci, Jiangxi Key Lab Mass Spectrometry & Instrumentat, Nanchang 330013, Jiangxi, Peoples R China 4.Fudan Univ, Dept Mat Sci, Shanghai 200433, Peoples R China 5.Fudan Univ, Adv Coatings Res Ctr, Minist Educ, Shanghai 200433, Peoples R China 6.Wuhan Univ Sci & Technol, Sch Mat & Met, State Key Lab Refractories & Met, Wuhan 430081, Peoples R China 7.Prince Sultan Univ, Coll Humanities & Sci, Dept Math & Sci, Riyadh 11586, Saudi Arabia 8.Zhejiang Ocean Univ, Marine Sci & Technol Coll, Natl Engn Res Ctr Marine Aquaculture, Zhejiang Key Lab Petrochem Environm Pollut Control, Zhoushan 316022, Peoples R China 9.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110017, Peoples R China 10.China Univ Petr, Key Lab Opt Detect Technol Oil & Gas, State Key Lab Heavy Oil Proc, Beijing 102249, Peoples R China
推荐引用方式 GB/T 7714	Bao, Linping,Ali, Sajjad,Dai, Chunhui,et al. A Full-Spectrum ZnS Photocatalyst with Gradient Distribution of Atomic Copper Dopants and Concomitant Sulfur Vacancies for Highly Efficient Hydrogen Evolution[J]. ACS NANO,2024,18(7):5878-5889.
APA	Bao, Linping.,Ali, Sajjad.,Dai, Chunhui.,Zeng, Qing.,Zeng, Chao.,...&Zhou, Yingtang.(2024).A Full-Spectrum ZnS Photocatalyst with Gradient Distribution of Atomic Copper Dopants and Concomitant Sulfur Vacancies for Highly Efficient Hydrogen Evolution.ACS NANO,18(7),5878-5889.
MLA	Bao, Linping,et al."A Full-Spectrum ZnS Photocatalyst with Gradient Distribution of Atomic Copper Dopants and Concomitant Sulfur Vacancies for Highly Efficient Hydrogen Evolution".ACS NANO 18.7(2024):5878-5889.