Identification and Characteristics of Catalytic Quad-Functions on Au/Anatase TiO2

doi:10.1021/acscatal.9b02090

	Identification and Characteristics of Catalytic Quad-Functions on Au/Anatase TiO2
	Mao, Jingbo 1,2,3; Zhao, Bin 1,2; Zhou, Jinxia 3; Zhang, Li 3; Yang, Fan 3; Guo, Xinwen 1; Zhang, Z. Conrad 2
刊名	ACS CATALYSIS
	2019-09-01
卷号	9 期号:9 页码:7900-7911
关键词	gold catalyst catalysis functions hydrogenation dehydration dehydrogenation hydroquinone hydrogenation
ISSN号	2155-5435
DOI	10.1021/acscatal.9b02090
通讯作者	Guo, Xinwen(guoxw@dlut.edu.cn) ; Zhang, Z. Conrad(zczhang@dicp.ac.cn)
英文摘要	Mechanistic pathways of catalytic hydrodeoxygenation determine the portfolios of biomass-derived platform chemicals. Bifunctional catalysts involving active metals on acidic supports are known to catalyze the hydrogenation of unsaturated chemical bonds on the metal surfaces and dehydration at acid sites of the supports. For poorly active hydrogenation metals such as Au, the effect of support became crucially important. In this work, the catalytic functions and the associated active sites in anatase TiO2 (TiO2-A)-supported Au nanoparticles (Au/TiO2-A) for hydrogenation and hydrodeoxygenation are determined in the conversion of catechol, hydroquinone, and other select oxygenate molecules under hydrogen pressure. Four catalytic functions are identified on Au/TiO2-A; these are labeled I-IV. While the Au/TiO2-A exhibited a single-site hydrodeoxygenation function [I] at a reduced TiOx site that converts catechol directly to phenol via spilt-over hydrogen from Au nanoparticles as the only product, hydroquinone conversion was catalyzed by three other functions, i.e., dehydrogenation [II], hydrogenation [III], and dehydration [IV], resulting in cyclohexane as the final product under the same conditions. In the hydrogenation of hydroquinone over Au/TiO2-A, the dehydrogenation [II] of hydroquinone to benzoquinone on the surface of TiO2-A and at the interface of Au and TiO2-A, but not on the Au surface, has been found to be the critical initiation step, followed by hydrogenation [III] of isolated C=C and C=O bonds on the surface of Au nanoparticles. A dehydration [IV] of alcohol happens on the surface of TiO2-A and at the interface between Au/TiO2-A. The synergism of these functions distinguishes the Au/TiO2-A catalyst from the Au/Al2O3, Au/ SiO2, and Au/TiO2-R (R = rutile) in catechol and the hydrogenation of hydroquinone. Particularly, Au/TiO2-R does not exhibit the hydrodeoxygenation and dehydrogenation functions, which are the unique catalytic characteristics of Au/TiO2-A. Unlike supported noble metals, gold shows little dehydrogenation activity for hydroquinone, as demonstrated on Au/Al2O3, Au/SiO2, and Au/TiO2-R.
资助项目	National Natural Science Foundation of China[21690084] ; National Natural Science Foundation of China[21721004] ; National Natural Science Foundation of China[21673229] ; DICP Innovation Fund ; DICP[1201936]
WOS关键词	LIQUID-PHASE HYDROGENATION ; METAL-SUPPORT INTERACTION ; SELECTIVE HYDROGENATION ; MODEL COMPOUNDS ; HYDRODEOXYGENATION ; GOLD ; SURFACE ; NANOPARTICLES ; HYDROQUINONE ; OXIDATION
WOS研究方向	Chemistry
语种	英语
出版者	AMER CHEMICAL SOC
WOS记录号	WOS:000485090400028
资助机构	National Natural Science Foundation of China ; National Natural Science Foundation of China ; DICP Innovation Fund ; DICP Innovation Fund ; DICP ; DICP ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; DICP Innovation Fund ; DICP Innovation Fund ; DICP ; DICP ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; DICP Innovation Fund ; DICP Innovation Fund ; DICP ; DICP ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; DICP Innovation Fund ; DICP Innovation Fund ; DICP ; DICP
内容类型	期刊论文
源URL	[http://cas-ir.dicp.ac.cn/handle/321008/173150]
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	Guo, Xinwen; Zhang, Z. Conrad
作者单位	1.Dalian Univ Technol, Sch Chem Engn, PSU DUT Joint Ctr Energy Res, State Key Lab Fine Chem, Dalian 116024, Peoples R China 2.Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy, State Key Lab Catalysis, Dalian 116023, Peoples R China 3.Dalian Univ, Coll Environm & Chem Engn, Dalian 116622, Peoples R China
推荐引用方式 GB/T 7714	Mao, Jingbo,Zhao, Bin,Zhou, Jinxia,et al. Identification and Characteristics of Catalytic Quad-Functions on Au/Anatase TiO2[J]. ACS CATALYSIS,2019,9(9):7900-7911.
APA	Mao, Jingbo.,Zhao, Bin.,Zhou, Jinxia.,Zhang, Li.,Yang, Fan.,...&Zhang, Z. Conrad.(2019).Identification and Characteristics of Catalytic Quad-Functions on Au/Anatase TiO2.ACS CATALYSIS,9(9),7900-7911.
MLA	Mao, Jingbo,et al."Identification and Characteristics of Catalytic Quad-Functions on Au/Anatase TiO2".ACS CATALYSIS 9.9(2019):7900-7911.