Influence of Anchoring Groups on the Charge Transfer and Performance of p-Si/TiO2/Cobaloxime Hybrid Photocathodes for Photoelectrochemical H-2 Production

doi:10.1021/acsami.9b12182

	Influence of Anchoring Groups on the Charge Transfer and Performance of p-Si/TiO2/Cobaloxime Hybrid Photocathodes for Photoelectrochemical H-2 Production
	Gong, Lunlun 1; Yin, Heng 2; Nie, Chengming 1; Sun, Xuran 1; Wang, Xiuli 2; Wang, Mei 1
刊名	ACS APPLIED MATERIALS & INTERFACES
	2019-09-18
卷号	11 期号:37 页码:34010-34019
关键词	anchoring group cobaloxime hydrogen production photocathode photoelectrochemistry silicon
ISSN号	1944-8244
DOI	10.1021/acsami.9b12182
通讯作者	Wang, Xiuli(xiuliwang@dicp.ac.cn) ; Wang, Mei(symbueno@dlut.edu.cn)
英文摘要	Although hybrid photocathodes built by immobilizing molecular catalysts to the surface of semiconductors through chemical linkages have been reported in recent years, systematic and comparative studies remain scarce about the impact of various anchoring groups on the performance, stability, and charge-transfer kinetics of molecular catalyst-decorated hybrid photocathodes for photoelectrochemical (PEC) H-2 production. In this study, the molecular cobaloxime catalysts, CoPy-4-X (Py = pyridine, X = PO3H2, COOH, and CONH(OH)), bearing different anchoring groups were synthesized and covalently immobilized to the surface of the porous TiO2 layer coated on a p-Si plate or a fluorine-doped tin oxide glass. The influence of the anchoring groups on the performance of p-Si/TiO2/CoPy-4-X photocathodes was comparatively studied for PEC H-2 evolution. Among the tested hybrid photocathodes, the one with a hydroxamate as an anchoring group displayed higher activity and lower charge-transfer resistance than that observed for the electrode with a carboxylate or a phosphonate as the anchoring group. Notably, the catalytic current of p-Si/Ti-2/CoPy-4-CONH(OH) was attenuated only by 2.9% in the controlled potential photoelectrolysis tests in borate buffer solution at pH 9 at 0 V versus a reversible hydrogen electrode over 6 h. Moreover, the influence of anchoring groups on the interfacial electron transfer from the TiO2 layer to the immobilized cobaloxime catalyst and electron-hole recombination was studied by transient absorption spectroscopy. These results revealed that the hydroxamate as an anchoring group is superior to the carboxylate and phosphonate groups for speeding up the interfacial electron transfer and firmly immobilizing the molecular catalysts to the metal oxide semiconductors to build efficient and stable hybrid photoelectrodes.
资助项目	National Natural Science Foundation of China[21673028] ; National Natural Science Foundation of China[21373040] ; Basic Research Program of China[2014CB239402]
WOS关键词	SOLAR HYDROGEN-PRODUCTION ; VISIBLE-LIGHT ; EVOLUTION CATALYST ; WATER ; TIO2 ; SI ; ACID
WOS研究方向	Science & Technology - Other Topics ; Materials Science
语种	英语
出版者	AMER CHEMICAL SOC
WOS记录号	WOS:000487179900051
资助机构	National Natural Science Foundation of China ; National Natural Science Foundation of China ; Basic Research Program of China ; Basic Research Program of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Basic Research Program of China ; Basic Research Program of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Basic Research Program of China ; Basic Research Program of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Basic Research Program of China ; Basic Research Program of China
内容类型	期刊论文
源URL	[http://cas-ir.dicp.ac.cn/handle/321008/172741]
专题	大连化学物理研究所_中国科学院大连化学物理研究所
通讯作者	Wang, Xiuli; Wang, Mei
作者单位	1.Dalian Univ Technol, State Key Lab Fine Chem, Dalian 116024, Peoples R China 2.Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy, State Key Lab Catalysis, Dalian 116023, Peoples R China
推荐引用方式 GB/T 7714	Gong, Lunlun,Yin, Heng,Nie, Chengming,et al. Influence of Anchoring Groups on the Charge Transfer and Performance of p-Si/TiO2/Cobaloxime Hybrid Photocathodes for Photoelectrochemical H-2 Production[J]. ACS APPLIED MATERIALS & INTERFACES,2019,11(37):34010-34019.
APA	Gong, Lunlun,Yin, Heng,Nie, Chengming,Sun, Xuran,Wang, Xiuli,&Wang, Mei.(2019).Influence of Anchoring Groups on the Charge Transfer and Performance of p-Si/TiO2/Cobaloxime Hybrid Photocathodes for Photoelectrochemical H-2 Production.ACS APPLIED MATERIALS & INTERFACES,11(37),34010-34019.
MLA	Gong, Lunlun,et al."Influence of Anchoring Groups on the Charge Transfer and Performance of p-Si/TiO2/Cobaloxime Hybrid Photocathodes for Photoelectrochemical H-2 Production".ACS APPLIED MATERIALS & INTERFACES 11.37(2019):34010-34019.