Facile formation of CoN4 active sites onto a SiO2 support to achieve robust CO2 and proton reduction in a noble-metal-free photocatalytic system

doi:10.1039/c9ta00949c

	Facile formation of CoN4 active sites onto a SiO2 support to achieve robust CO2 and proton reduction in a noble-metal-free photocatalytic system
	Hu, Jun-Chao 2; Gui, Meng-Xi 2; Xia, Wu 2; Wu, Jin 2; Zhou, Yong-Ning 3; Feng, Ningdong 1; Xiao, Junwu 2; Liu, Hongfang 2; Tung, Chen-Ho 4; Wu, Li-Zhu 4
刊名	JOURNAL OF MATERIALS CHEMISTRY A
	2019-05-07
卷号	7 期号:17 页码:10475-10482
ISSN号	2050-7488
DOI	10.1039/c9ta00949c
英文摘要	The conversion of CO2 and protons to solar fuels (CO and H2) is the basis of artificial photosynthesis. To date, most of the reported cobalt-based molecular catalysts or single-atom catalysts (SAC) feature a CoN4 core structure. However, the preparation of these metal complex catalysts or SACs requires either a complicated organic ligand synthesis method or harsh material fabrication conditions. In this study, the facile formation of an active CoN4 structure onto a SiO2 support was achieved via selfcoordination of Co2+ ions with aminated SiO2 nanoparticles. The formation of the CoN4 structure was identified by synchrotron-based X-ray absorption spectroscopy. The CoN4-SiO2 catalyst exhibited exceptional bifunctional activity of mediating the CO2-to-CO and 2H+-to-H2 conversions in a photochemical system containing g-C3N4 as a photosensitizer. The system robustly produced syngas (CO + H2, CO/H 2 = 1 : 1-1 : 2) with a high activity (5053 mmol g-1 and 36 mmol g-1 h-1 based on the catalyst) and remarkable stability (durability > 120 h). Mechanistic studies reveal that the Co(I)-species is the active species generated via a photoinduced electron transfer from g-C3N4 to CoN4-SiO2. The dissociation of Co2+ from the aminated SiO2 support and the decomposition of g-C3N4 under irradiation are the main reasons for the inactivation of the system after long-time photocatalysis.
资助项目	National Natural Science Foundation of China[21871102] ; National Natural Science Foundation of China[U1662114]
WOS关键词	VISIBLE-LIGHT ; SYNGAS PRODUCTION ; HIGHLY EFFICIENT ; COBALT COMPLEXES ; H-2 ; CATALYSTS ; HYDROGEN ; TIO2 ; IRON ; H2O
WOS研究方向	Chemistry ; Energy & Fuels ; Materials Science
语种	英语
出版者	ROYAL SOC CHEMISTRY
WOS记录号	WOS:000472183200034
资助机构	National Natural Science Foundation of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China
内容类型	期刊论文
源URL	[http://ir.wipm.ac.cn/handle/112942/14489]
专题	中国科学院武汉物理与数学研究所
通讯作者	Wang, Feng
作者单位	1.Chinese Acad Sci, State Key Lab Magnet Resonance & Atom & Mol Phys, Wuhan Inst Phys & Math, Wuhan 430071, Hubei, Peoples R China 2.Huazhong Univ Sci & Technol, Key Lab Mat Chem Energy Convers & Storage, Hubei Key Lab Mat Chem & Serv Failure, Minist Educ,Sch Chem & Chem Engn, Wuhan 430074, Hubei, Peoples R China 3.Fudan Univ, Dept Mat Sci, Shanghai 200433, Peoples R China 4.Chinese Acad Sci, Tech Inst Phys & Chem, Beijing 100190, Peoples R China
推荐引用方式 GB/T 7714	Hu, Jun-Chao,Gui, Meng-Xi,Xia, Wu,et al. Facile formation of CoN4 active sites onto a SiO2 support to achieve robust CO2 and proton reduction in a noble-metal-free photocatalytic system[J]. JOURNAL OF MATERIALS CHEMISTRY A,2019,7(17):10475-10482.
APA	Hu, Jun-Chao.,Gui, Meng-Xi.,Xia, Wu.,Wu, Jin.,Zhou, Yong-Ning.,...&Wang, Feng.(2019).Facile formation of CoN4 active sites onto a SiO2 support to achieve robust CO2 and proton reduction in a noble-metal-free photocatalytic system.JOURNAL OF MATERIALS CHEMISTRY A,7(17),10475-10482.
MLA	Hu, Jun-Chao,et al."Facile formation of CoN4 active sites onto a SiO2 support to achieve robust CO2 and proton reduction in a noble-metal-free photocatalytic system".JOURNAL OF MATERIALS CHEMISTRY A 7.17(2019):10475-10482.