Number of Reactive Charge Carriers-A Hidden Linker between Band Structure and Catalytic Performance in Photocatalysts

doi:10.1021/acscatal.9b02426

	Number of Reactive Charge Carriers-A Hidden Linker between Band Structure and Catalytic Performance in Photocatalysts
	Xiao, Jiadong 1,2,3,4; Hang, Qingzhen 2; Cao, Hongbin 2; Rabeah, Jabor 1; Yang, Jin 2; Guo, Zhuang 2,3; Zhou, Linbi 2; Xie, Yongbing 2; Brueckner, Angelika 1
刊名	ACS CATALYSIS
	2019-10-01
卷号	9 期号:10 页码:8852-8861
关键词	g-C3N4 photocatalysis photocatalytic ozonation band structure number of reactive charge carriers in situ EPR
ISSN号	2155-5435
DOI	10.1021/acscatal.9b02426
英文摘要	Tailoring the band structure of a photocatalyst without causing significant changes in further properties and deriving unambiguous relationship between the number of charge carriers (CB-e(-) and VB-h(+)) and their reactivity in a photocatalytic reaction are very challenging, but highly important for rational catalyst design. In this work, semiquantitative relationships among the band structure, number of reactive charge carriers, yield of hydroxyl ((OH)-O-center dot) and superoxide (O-center dot(2)-) radicals, and degradation rate of oxalic acid as a model pollutant have been discovered in g-C3N4 photocatalysts by in situ electron paramagnetic resonance (EPR) coupled with an online spin trapping technique. We demonstrate that it is the number of reactive charge carriers which links the band structure of a photocatalyst with its catalytic performance. An optimum balance between the number and reducing ability of conduction band (CB) electrons (CB-e(-)), which depends on the interplay between the band gap and CB edge potential, is a key property for highly efficient g-C3N4 photocatalysts. A combination of (i) narrowing of the band gap and upshift of the CB edge at the same time, and (ii) using O-3 instead of O-2 as CB-e(-) trap would lead to the maximum number of reactive CB-e(-) and (OH)-O-center dot and, hence, to optimal photocatalytic activity.
资助项目	Natural Science Foundation of Beijing Municipality[8172043] ; National Science Fund for Distinguished Young Scholars of China[51425405] ; National Key Research and Development Program of China[2017YFC0210304] ; CAS-DAAD fellowship (Regierungsstipendien VR China-Programme for the Promotion of Outstanding Young Scholars)[91637735]
WOS关键词	GRAPHITIC CARBON NITRIDE ; VISIBLE-LIGHT ; HYDROXYL RADICALS ; POROUS G-C3N4 ; SUPER SYNERGY ; WASTE-WATER ; OXALIC-ACID ; OZONATION ; OXIDATION ; NANOPARTICLES
WOS研究方向	Chemistry
语种	英语
出版者	AMER CHEMICAL SOC
WOS记录号	WOS:000489204000001
资助机构	Natural Science Foundation of Beijing Municipality ; National Science Fund for Distinguished Young Scholars of China ; National Key Research and Development Program of China ; CAS-DAAD fellowship (Regierungsstipendien VR China-Programme for the Promotion of Outstanding Young Scholars)
内容类型	期刊论文
源URL	[http://ir.ipe.ac.cn/handle/122111/31134]
专题	中国科学院过程工程研究所
通讯作者	Rabeah, Jabor; Xie, Yongbing; Brueckner, Angelika
作者单位	1.Univ Rostock, Leibniz Inst Catalysis eV, Albert Einstein Str 29a, D-18059 Rostock, Germany 2.Chinese Acad Sci, Beijing Engn Res Ctr Proc Pollut Control, Inst Proc Engn, Div Environm Technol & Engn, Beijing 100190, Peoples R China 3.Univ Chinese Acad Sci, Beijing 100049, Peoples R China 4.Univ Utrecht, Debye Inst Nanomat Sci, Inorgan Chem & Catalysis, Univ Weg 99, Utrecht, Netherlands
推荐引用方式 GB/T 7714	Xiao, Jiadong,Hang, Qingzhen,Cao, Hongbin,et al. Number of Reactive Charge Carriers-A Hidden Linker between Band Structure and Catalytic Performance in Photocatalysts[J]. ACS CATALYSIS,2019,9(10):8852-8861.
APA	Xiao, Jiadong.,Hang, Qingzhen.,Cao, Hongbin.,Rabeah, Jabor.,Yang, Jin.,...&Brueckner, Angelika.(2019).Number of Reactive Charge Carriers-A Hidden Linker between Band Structure and Catalytic Performance in Photocatalysts.ACS CATALYSIS,9(10),8852-8861.
MLA	Xiao, Jiadong,et al."Number of Reactive Charge Carriers-A Hidden Linker between Band Structure and Catalytic Performance in Photocatalysts".ACS CATALYSIS 9.10(2019):8852-8861.