DICP OpenIR
Selective Hydrodeoxygenation of Guaiacol to Phenolics by Ni/Anatase TiO2 Catalyst Formed by Cross-Surface Migration of Ni and TiO2
Zhang, Xiaoqiang1,2; Yan, Peifang1; Zhao, Bin3; Liu, Kairui1,2; Kung, Mayfair C.4; Kung, Harold H.4; Chen, Shanyong5; Zhang, Z. Conrad1
Corresponding AuthorKung, Harold H.(hkung@northwestern.edu) ; Zhang, Z. Conrad(zczhang@yahoo.com)
Keywordguaiacol hydrodeoxygenation phenol SMSI or strong metal-support interaction titania and nickel lignin
Source PublicationACS CATALYSIS
2019-04-01
ISSN2155-5435
DOI10.1021/acscatal.9b00400
Volume9Issue:4Pages:3551-3563
Funding ProjectGlobal Expert program of China ; National Natural Science Foundation of China[21690084] ; National Natural Science Foundation of China[21721004] ; U.S. Department of Energy[DE-FG02-03ER15457]
Funding OrganizationGlobal Expert program of China ; Global Expert program of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; U.S. Department of Energy ; U.S. Department of Energy ; Global Expert program of China ; Global Expert program of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; U.S. Department of Energy ; U.S. Department of Energy ; Global Expert program of China ; Global Expert program of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; U.S. Department of Energy ; U.S. Department of Energy ; Global Expert program of China ; Global Expert program of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; U.S. Department of Energy ; U.S. Department of Energy
WOS SubjectChemistry, Physical
WOS Research AreaChemistry
WOS KeywordMETAL-SUPPORT INTERACTIONS ; CO METHANATION ; NI/TIO2 CATALYST ; CARBON NANOTUBES ; BIO-OIL ; LIGNIN ; HYDROGENATION ; CONVERSION ; BIOMASS ; SPILLOVER
AbstractThe catalytic properties of physical mixtures of Ni particles (100-200 nm) with nanoparticles of anatase TiO2 (TiO2-A), ZrO2, Al2O3, rutile TiO 2 (TiO2-R), and CeO2 were investigated for the hydrodeoxygenation (HDO) of guaiacol. High selectivities to phenolics were obtained only for Ni mixed with anatase TiO2 (Ni and TiO2-A), while saturated hydro- carbons were the main products for the mixtures with other supports. By thermal treatment in hydrogen gas only at 300 degrees C or higher and subsequently separating the large Ni particles from the TiO2-A particles with a magnet, it was further discovered that there was migration of TiO 2 from TiO2-A onto the large Ni particles, resulting in an amorphous TiO2 overlayer on the Ni particles as evidenced by high-resolution TEM, and vice versa, migration of Ni onto TiO2-A. The TiO2 overlayer rendered the Ni particles completely inactive as a hydrogenation/hydrodeoxygenation catalyst. Conversely, the small amounts of Ni (<1.5 wt %) migrated onto TiO2-A formed highly dispersed Ni, undetectable by high-resolution TEM (<2 nm), that were remarkably highly active for HDO of guaiacol, producing selectively phenolics. Such highly selective HDO catalysts could also be formed by incipient wetness impregnation of Ni in loadings above 2 wt % onto the TiO2-A, but it was essential to pretreat the sample in H-2 at 300 degrees C or higher. Pretreatment in H-2 at 200 degrees C generated catalysts that produced saturated ring products. The activity of the impregnated catalysts, as measured by guaiacol conversion, increased linearly with Ni loading below 0.5 wt %. The activity continued to increase with Ni loading but more slowly up to 2 wt %, beyond which there was little further change. The results suggested that two types of Ni species existed on the TiO2-A surface. One type consisted of a cluster of Ni atoms that were dominant on larger Ni particles that were active in aromatic ring hydrogenation and hydrodeoxygenation. They were readily covered by reducible TiO2-A at 300 degrees C or higher due to the traditional strong metal support interaction (SMSI) effect and became inactive. Another type was clusters of a very small number of Ni atoms, perhaps one atom, that were present as highly dispersed Ni clusters interacting strongly with the defect sites of TiO2-A. The strong interaction of this type of Ni with the TiO2 defect deterred TiO, migration allowing surface exposed Ni atoms to catalyze the HDO of guaiacol with very high selectivities that were not characteristic of typical Ni particles.
Language英语
Funding OrganizationGlobal Expert program of China ; Global Expert program of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; U.S. Department of Energy ; U.S. Department of Energy ; Global Expert program of China ; Global Expert program of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; U.S. Department of Energy ; U.S. Department of Energy ; Global Expert program of China ; Global Expert program of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; U.S. Department of Energy ; U.S. Department of Energy ; Global Expert program of China ; Global Expert program of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; U.S. Department of Energy ; U.S. Department of Energy
WOS IDWOS:000464075700082
PublisherAMER CHEMICAL SOC
Citation statistics
Document Type期刊论文
Identifierhttp://cas-ir.dicp.ac.cn/handle/321008/165569
Collection中国科学院大连化学物理研究所
Corresponding AuthorKung, Harold H.; Zhang, Z. Conrad
Affiliation1.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China
2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
3.Dalian Univ Technol, Sch Chem Engn, PSU DUT Joint Ctr Energy Res, State Key Lab Fine Chem, Dalian 116024, Peoples R China
4.Northwestern Univ, Dept Chem Engn, Evanston, IL 60208 USA
5.Nanjing Univ, Sch Chem & Chem Engn, Key Lab Mesoscop Chem MOE, Nanjing 210023, Jiangsu, Peoples R China
Recommended Citation
GB/T 7714
Zhang, Xiaoqiang,Yan, Peifang,Zhao, Bin,et al. Selective Hydrodeoxygenation of Guaiacol to Phenolics by Ni/Anatase TiO2 Catalyst Formed by Cross-Surface Migration of Ni and TiO2[J]. ACS CATALYSIS,2019,9(4):3551-3563.
APA Zhang, Xiaoqiang.,Yan, Peifang.,Zhao, Bin.,Liu, Kairui.,Kung, Mayfair C..,...&Zhang, Z. Conrad.(2019).Selective Hydrodeoxygenation of Guaiacol to Phenolics by Ni/Anatase TiO2 Catalyst Formed by Cross-Surface Migration of Ni and TiO2.ACS CATALYSIS,9(4),3551-3563.
MLA Zhang, Xiaoqiang,et al."Selective Hydrodeoxygenation of Guaiacol to Phenolics by Ni/Anatase TiO2 Catalyst Formed by Cross-Surface Migration of Ni and TiO2".ACS CATALYSIS 9.4(2019):3551-3563.
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