DICP OpenIR
Freezing copper as a noble metal-like catalyst for preliminary hydrogenation
Sun, Jian1; Yu, Jiafeng1; Ma, Qingxiang2; Meng, Fanqiong1; Wei, Xiaoxuan3; Sun, Yannan1,4; Tsubaki, Noritatsu5
Corresponding AuthorSun, Jian(sunj@dicp.ac.cn) ; Wei, Xiaoxuan(xxwei@zjnu.edu.cn)
Source PublicationSCIENCE ADVANCES
2018-12-01
ISSN2375-2548
DOI10.1126/sciadv.aau3275
Volume4Issue:12Pages:10
Funding ProjectFoundation of State Key Laboratory of High-Efficiency Coal Utilization and Green Chemical Engineering[2016-04] ; Hundred-Talent Program of Dalian Institute of Chemical Physics ; Youth Innovation Promotion Association of the Chinese Academy of Sciences[2018214]
Funding OrganizationFoundation of State Key Laboratory of High-Efficiency Coal Utilization and Green Chemical Engineering ; Foundation of State Key Laboratory of High-Efficiency Coal Utilization and Green Chemical Engineering ; Hundred-Talent Program of Dalian Institute of Chemical Physics ; Hundred-Talent Program of Dalian Institute of Chemical Physics ; Youth Innovation Promotion Association of the Chinese Academy of Sciences ; Youth Innovation Promotion Association of the Chinese Academy of Sciences ; Foundation of State Key Laboratory of High-Efficiency Coal Utilization and Green Chemical Engineering ; Foundation of State Key Laboratory of High-Efficiency Coal Utilization and Green Chemical Engineering ; Hundred-Talent Program of Dalian Institute of Chemical Physics ; Hundred-Talent Program of Dalian Institute of Chemical Physics ; Youth Innovation Promotion Association of the Chinese Academy of Sciences ; Youth Innovation Promotion Association of the Chinese Academy of Sciences ; Foundation of State Key Laboratory of High-Efficiency Coal Utilization and Green Chemical Engineering ; Foundation of State Key Laboratory of High-Efficiency Coal Utilization and Green Chemical Engineering ; Hundred-Talent Program of Dalian Institute of Chemical Physics ; Hundred-Talent Program of Dalian Institute of Chemical Physics ; Youth Innovation Promotion Association of the Chinese Academy of Sciences ; Youth Innovation Promotion Association of the Chinese Academy of Sciences ; Foundation of State Key Laboratory of High-Efficiency Coal Utilization and Green Chemical Engineering ; Foundation of State Key Laboratory of High-Efficiency Coal Utilization and Green Chemical Engineering ; Hundred-Talent Program of Dalian Institute of Chemical Physics ; Hundred-Talent Program of Dalian Institute of Chemical Physics ; Youth Innovation Promotion Association of the Chinese Academy of Sciences ; Youth Innovation Promotion Association of the Chinese Academy of Sciences
WOS SubjectMultidisciplinary Sciences
WOS Research AreaScience & Technology - Other Topics
WOS KeywordSURFACE-PLASMON RESONANCE ; DIMETHYL OXALATE ; CU/SIO2 CATALYSTS ; CHEMOSELECTIVE SYNTHESIS ; SELECTIVE HYDROGENATION ; GOLD NANOPARTICLES ; METHYL GLYCOLATE ; ETHYLENE-GLYCOL ; HMS CATALYST ; PERFORMANCE
AbstractThe control of product distribution in a multistep catalytic selective hydrogenation reaction is challenging. For instance, the deep hydrogenation of dimethyl oxalate (DMO) is inclined to proceed over Cu/SiO2 catalysts because of inevitable coexistence of Cu+ and Cu-0, leading to hard acquisition of the preliminary hydrogenation product, methyl glycolate (MG). Here, the oriented DMO hydrogenation into MG is achieved over the sputtering (SP) Cu/SiO2 catalysts with a selectivity of more than 87% via freezing Cu in a zero-valence state. Our density functional theory calculation results revealed that Cu-0 is the active site of the preliminary hydrogenation step, selectively converting DMO to MG via center dot H addition, while Cu+ is a key factor for deep hydrogenation. The prominent Coster-Kronig transition enhancement is observed over SP-Cu/SiO2 from Auger spectra, indicating that the electron density of inner shells in Cu atoms is enhanced by high-energy argon plasma bombardment during the SP process. Thus, the "penetration effect" of outermost electrons could also be enhanced, making these Cu nanoparticles exhibit high oxidation resistance ability and present noble metal-like behaviors as Au or Ag. Therefore, the regulation of Cu chemical properties by changing the electron structure is a feasible strategy to control the hydrogenation products, inspiring the rational design of selective hydrogenation catalysts.
Language英语
Funding OrganizationFoundation of State Key Laboratory of High-Efficiency Coal Utilization and Green Chemical Engineering ; Foundation of State Key Laboratory of High-Efficiency Coal Utilization and Green Chemical Engineering ; Hundred-Talent Program of Dalian Institute of Chemical Physics ; Hundred-Talent Program of Dalian Institute of Chemical Physics ; Youth Innovation Promotion Association of the Chinese Academy of Sciences ; Youth Innovation Promotion Association of the Chinese Academy of Sciences ; Foundation of State Key Laboratory of High-Efficiency Coal Utilization and Green Chemical Engineering ; Foundation of State Key Laboratory of High-Efficiency Coal Utilization and Green Chemical Engineering ; Hundred-Talent Program of Dalian Institute of Chemical Physics ; Hundred-Talent Program of Dalian Institute of Chemical Physics ; Youth Innovation Promotion Association of the Chinese Academy of Sciences ; Youth Innovation Promotion Association of the Chinese Academy of Sciences ; Foundation of State Key Laboratory of High-Efficiency Coal Utilization and Green Chemical Engineering ; Foundation of State Key Laboratory of High-Efficiency Coal Utilization and Green Chemical Engineering ; Hundred-Talent Program of Dalian Institute of Chemical Physics ; Hundred-Talent Program of Dalian Institute of Chemical Physics ; Youth Innovation Promotion Association of the Chinese Academy of Sciences ; Youth Innovation Promotion Association of the Chinese Academy of Sciences ; Foundation of State Key Laboratory of High-Efficiency Coal Utilization and Green Chemical Engineering ; Foundation of State Key Laboratory of High-Efficiency Coal Utilization and Green Chemical Engineering ; Hundred-Talent Program of Dalian Institute of Chemical Physics ; Hundred-Talent Program of Dalian Institute of Chemical Physics ; Youth Innovation Promotion Association of the Chinese Academy of Sciences ; Youth Innovation Promotion Association of the Chinese Academy of Sciences
WOS IDWOS:000454369600023
PublisherAMER ASSOC ADVANCEMENT SCIENCE
Citation statistics
Document Type期刊论文
Identifierhttp://cas-ir.dicp.ac.cn/handle/321008/166343
Collection中国科学院大连化学物理研究所
Corresponding AuthorSun, Jian; Wei, Xiaoxuan
Affiliation1.Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy DNL, Dalian 116023, Peoples R China
2.Ningxia Univ, State Key Lab High Efficiency Utilizat Coal & Gre, Yinchuan 750021, Peoples R China
3.Zhejiang Normal Univ, Coll Geog & Environm Sci, Yingbin Ave 688, Jinhua 321004, Peoples R China
4.Dalian Univ Technol, Sch Chem, Dalian 116023, Peoples R China
5.Univ Toyama, Dept Appl Chem, Grad Sch Engn, Toyama 9308555, Japan
Recommended Citation
GB/T 7714
Sun, Jian,Yu, Jiafeng,Ma, Qingxiang,et al. Freezing copper as a noble metal-like catalyst for preliminary hydrogenation[J]. SCIENCE ADVANCES,2018,4(12):10.
APA Sun, Jian.,Yu, Jiafeng.,Ma, Qingxiang.,Meng, Fanqiong.,Wei, Xiaoxuan.,...&Tsubaki, Noritatsu.(2018).Freezing copper as a noble metal-like catalyst for preliminary hydrogenation.SCIENCE ADVANCES,4(12),10.
MLA Sun, Jian,et al."Freezing copper as a noble metal-like catalyst for preliminary hydrogenation".SCIENCE ADVANCES 4.12(2018):10.
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