DICP OpenIR
The synergistic effect between Ni sites and Ni-Fe alloy sites on hydrodeoxygenation of lignin-derived phenols
Han, Qiao1; Rehman, Mooeez Ur1; Wang, Junhu2; Rykov, Alexandre2; Gutierrez, Oliver Y.3; Zhao, Yujun1; Wang, Shengping1; Ma, Xinbin1; Lercher, Johannes A.3,4,5
Corresponding AuthorZhao, Yujun(yujunzhao@tju.edu.cn)
KeywordPhenol Hydrodeoxygenation Cyclohexane Ni-Fe alloy Kinetics
Source PublicationAPPLIED CATALYSIS B-ENVIRONMENTAL
2019-09-15
ISSN0926-3373
DOI10.1016/j.apcatb.2019.04.065
Volume253Pages:348-358
Funding ProjectNational Natural Science Foundation of China[21878227] ; National Natural Science Foundation of China[U1510203] ; U.S. Department of Energy (DOE), Office of Basic Energy Sciences (BES), Division of Chemical Sciences, Geosciences and Biosciences
Funding OrganizationNational Natural Science Foundation of China ; National Natural Science Foundation of China ; U.S. Department of Energy (DOE), Office of Basic Energy Sciences (BES), Division of Chemical Sciences, Geosciences and Biosciences ; U.S. Department of Energy (DOE), Office of Basic Energy Sciences (BES), Division of Chemical Sciences, Geosciences and Biosciences ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; U.S. Department of Energy (DOE), Office of Basic Energy Sciences (BES), Division of Chemical Sciences, Geosciences and Biosciences ; U.S. Department of Energy (DOE), Office of Basic Energy Sciences (BES), Division of Chemical Sciences, Geosciences and Biosciences ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; U.S. Department of Energy (DOE), Office of Basic Energy Sciences (BES), Division of Chemical Sciences, Geosciences and Biosciences ; U.S. Department of Energy (DOE), Office of Basic Energy Sciences (BES), Division of Chemical Sciences, Geosciences and Biosciences ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; U.S. Department of Energy (DOE), Office of Basic Energy Sciences (BES), Division of Chemical Sciences, Geosciences and Biosciences ; U.S. Department of Energy (DOE), Office of Basic Energy Sciences (BES), Division of Chemical Sciences, Geosciences and Biosciences
WOS SubjectChemistry, Physical ; Engineering, Environmental ; Engineering, Chemical
WOS Research AreaChemistry ; Engineering
WOS KeywordGAS-PHASE HYDRODEOXYGENATION ; BIO-OIL ; MODEL-COMPOUND ; CATALYTIC HYDRODEOXYGENATION ; M-CRESOL ; SELECTIVE HYDRODEOXYGENATION ; HETEROGENEOUS CATALYSTS ; SUPPORT INTERACTIONS ; PRODUCE HYDROGEN ; METHYL LAURATE
AbstractThe catalytic hydrodeoxygenation (HDO) of lignin-derived phenolic compounds is a critical step in the upgrading of bio-oil. Here, bimetallic Ni-Fe nanoparticles supported on mesoporous carbon spheres (MCSs) were fabricated and applied in HDO of phenol. In comparison with monometallic Ni and Fe catalysts, the bimetallic Ni-Fe catalyst exhibited better performance for phenol HDO due to the formation of Ni-Fe alloy phase identified by X-ray powder diffraction (XRD) and Mossbauer spectroscopy techniques. Among several explored ratios, the catalysts with Ni/Fe ratio of 3/1 presented the highest cyclohexane yield. The reaction occurred in two consecutive steps: the hydrogenation of phenol to cyclohexanol and the further hydrogenolysis of cyclohexanol to cyclohexane. Kinetic studies showed that the hydrogenolysis of cyclohexanol controlled the overall reaction rate of phenol HDO due to the lower reaction rate of this step. Indeed, the turnover frequency (TOF) values of cyclohexanol normalized by surface metallic Ni sites exhibited a linear correlation with Ni-Fe alloy sites. The alloying of iron in the bimetallic Ni-Fe catalysts significantly enhanced the adsorption strength of cyclohexanol, which is the reason of the high activity of the Ni-Fe alloy particles. Thus, Fe-containing sites adsorb the hydroxyl species while Ni sites perform the H-2 activation, their synergistic effect plays a key role in phenol HDO process.
Language英语
Funding OrganizationNational Natural Science Foundation of China ; National Natural Science Foundation of China ; U.S. Department of Energy (DOE), Office of Basic Energy Sciences (BES), Division of Chemical Sciences, Geosciences and Biosciences ; U.S. Department of Energy (DOE), Office of Basic Energy Sciences (BES), Division of Chemical Sciences, Geosciences and Biosciences ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; U.S. Department of Energy (DOE), Office of Basic Energy Sciences (BES), Division of Chemical Sciences, Geosciences and Biosciences ; U.S. Department of Energy (DOE), Office of Basic Energy Sciences (BES), Division of Chemical Sciences, Geosciences and Biosciences ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; U.S. Department of Energy (DOE), Office of Basic Energy Sciences (BES), Division of Chemical Sciences, Geosciences and Biosciences ; U.S. Department of Energy (DOE), Office of Basic Energy Sciences (BES), Division of Chemical Sciences, Geosciences and Biosciences ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; U.S. Department of Energy (DOE), Office of Basic Energy Sciences (BES), Division of Chemical Sciences, Geosciences and Biosciences ; U.S. Department of Energy (DOE), Office of Basic Energy Sciences (BES), Division of Chemical Sciences, Geosciences and Biosciences
WOS IDWOS:000469904500040
PublisherELSEVIER SCIENCE BV
Citation statistics
Document Type期刊论文
Identifierhttp://cas-ir.dicp.ac.cn/handle/321008/171952
Collection中国科学院大连化学物理研究所
Corresponding AuthorZhao, Yujun
Affiliation1.Tianjin Univ, Sch Chem Engn & Technol, Collaborat Innovat Ctr Chem Sci & Engn, Key Lab Green Chem Technol,Minist Educ, Tianjin 300072, Peoples R China
2.Chinese Acad Sci, Dalian Inst Chem Phys, Mossbauer Effect Data Ctr, Dalian 116023, Peoples R China
3.Pacific Northwest Natl Lab, Inst Integrated Catalysis, Richland, WA 99352 USA
4.Tech Univ Munich, Dept Chem, D-85748 Garching, Germany
5.Tech Univ Munich, Catalysis Res Ctr, D-85748 Garching, Germany
Recommended Citation
GB/T 7714
Han, Qiao,Rehman, Mooeez Ur,Wang, Junhu,et al. The synergistic effect between Ni sites and Ni-Fe alloy sites on hydrodeoxygenation of lignin-derived phenols[J]. APPLIED CATALYSIS B-ENVIRONMENTAL,2019,253:348-358.
APA Han, Qiao.,Rehman, Mooeez Ur.,Wang, Junhu.,Rykov, Alexandre.,Gutierrez, Oliver Y..,...&Lercher, Johannes A..(2019).The synergistic effect between Ni sites and Ni-Fe alloy sites on hydrodeoxygenation of lignin-derived phenols.APPLIED CATALYSIS B-ENVIRONMENTAL,253,348-358.
MLA Han, Qiao,et al."The synergistic effect between Ni sites and Ni-Fe alloy sites on hydrodeoxygenation of lignin-derived phenols".APPLIED CATALYSIS B-ENVIRONMENTAL 253(2019):348-358.
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