Cyano group modified carbon nitride with enhanced photoactivity for selective oxidation of benzylamine

doi:10.1016/j.apcatb.2018.09.084

IMR OpenIR

	Cyano group modified carbon nitride with enhanced photoactivity for selective oxidation of benzylamine
	Tan, Hao 1,2; Gu, Xianmo 1; Kong, Peng 1; Lian, Zan 3; Li, Bo 3; Zheng, Zhanfeng 1
通讯作者	Li, Bo(boli@imr.ac.cn) ; Zheng, Zhanfeng(zfzheng@sxicc.ac.cn)
	2019-03-01
发表期刊	APPLIED CATALYSIS B-ENVIRONMENTAL
ISSN	0926-3373
卷号	242 页码:67-75
摘要	Polymeric graphitic carbon nitride (g-C3N4) is a promising photocatalyst but suffers from the high recombination rate of photogenerated carriers. Many strategies for introducing active "sites", such as heteroatom doping and defect creation, which can hinder recombination by capturing the separated electrons or holes, have been developed to solve the problem. As a polymeric organic material, it is possible to alter the electron structure and improve the charge separation by introducing organic groups with different electronegativities or conjugation properties to the side chains. Herein, we report a facile and efficient -C equivalent to N group modification strategy using the thermal condensation of the thiocyanuric acid (TA) precursor. The sulfur content in the precursor forms -C=N=S and then transforms to -C equivalent to N. The -C equivalent to N group introduced catalyst exhibits enhanced light absorption and a low carrier recombination rate based on optical and photoelectrical measurements. This is due to the formation of a -C equivalent to N group related midgap state between the bandgap of g-C3N4, according to a density functional theory (DFT) calculation. The -C equivalent to N groups can also loosen the stacking texture of g-C3N4 and result in a thinner layer structure during the post-thermal treatment, which can shorten the distance of photogenerated carrier transfer from the bulk to the surface. The -C equivalent to N group introduced photocatalyst is efficient for the selective oxidation of benzylamine to imine, even under green light irradiation. This result demonstrates that the introduction of an electron rich conjugation group such as -C equivalent to N into the edge chain of polymeric carbon nitride is efficient for better photoactivity.
关键词	Cyano group Carbon nitride Midgap state Benzylamine Thin-layered structure
资助者	National Natural Science Foundation of China ; Shanxi Science and Technology Department ; Foundation of State Key Laboratory of Coal Conversion ; Hundred Talents Program of the Chinese Academy of Sciences ; Hundred Talents Program of the Shanxi Province
DOI	10.1016/j.apcatb.2018.09.084
收录类别	SCI
语种	英语
资助项目	National Natural Science Foundation of China[21773284] ; National Natural Science Foundation of China[21503258] ; Shanxi Science and Technology Department[2015081044] ; Shanxi Science and Technology Department[201601D021032] ; Foundation of State Key Laboratory of Coal Conversion[J17-18-605] ; Hundred Talents Program of the Chinese Academy of Sciences ; Hundred Talents Program of the Shanxi Province
WOS研究方向	Chemistry ; Engineering
WOS类目	Chemistry, Physical ; Engineering, Environmental ; Engineering, Chemical
WOS记录号	WOS:000450135000008
出版者	ELSEVIER SCIENCE BV
引用统计	被引频次：103[WOS] [WOS记录] [WOS相关记录]
文献类型	期刊论文
条目标识符	http://ir.imr.ac.cn/handle/321006/130615
专题	中国科学院金属研究所
通讯作者	Li, Bo; Zheng, Zhanfeng
作者单位	1.Chinese Acad Sci, Inst Coal Chem, State Key Lab Coal Convers, Taiyuan 030001, Shanxi, Peoples R China 2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China 3.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Liaoning, Peoples R China
推荐引用方式 GB/T 7714	Tan, Hao,Gu, Xianmo,Kong, Peng,et al. Cyano group modified carbon nitride with enhanced photoactivity for selective oxidation of benzylamine[J]. APPLIED CATALYSIS B-ENVIRONMENTAL,2019,242:67-75.
APA	Tan, Hao,Gu, Xianmo,Kong, Peng,Lian, Zan,Li, Bo,&Zheng, Zhanfeng.(2019).Cyano group modified carbon nitride with enhanced photoactivity for selective oxidation of benzylamine.APPLIED CATALYSIS B-ENVIRONMENTAL,242,67-75.
MLA	Tan, Hao,et al."Cyano group modified carbon nitride with enhanced photoactivity for selective oxidation of benzylamine".APPLIED CATALYSIS B-ENVIRONMENTAL 242(2019):67-75.