Elucidating the Copper–Hägg Iron Carbide Synergistic Interactions for Selective CO Hydrogenation to Higher Alcohols
CO hydrogenation to higher alcohols (C(2+)OH) provides a promising route to convert coal, natural gas, shale gas, and biomass feedstocks into value-added chemicals and transportation fuels. However, the development of nonprecious metal catalysts with satisfactory activity and well-defined selectivit...
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| Published in | ACS catalysis Vol. 7; no. 8; pp. 5500 - 5512 |
|---|---|
| Main Authors | , , , , , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
United States
American Chemical Society (ACS)
04.08.2017
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| Subjects | |
| Online Access | Get full text |
| ISSN | 2155-5435 2155-5435 |
| DOI | 10.1021/acscatal.7b01469 |
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| Abstract | CO hydrogenation to higher alcohols (C(2+)OH) provides a promising route to convert coal, natural gas, shale gas, and biomass feedstocks into value-added chemicals and transportation fuels. However, the development of nonprecious metal catalysts with satisfactory activity and well-defined selectivity toward C(2+)OH remains challenging and impedes the commercialization of this process. Here, we show that the synergistic geometric and electronic interactions dictate the activity of Cu(0)–χ-F(e)5C(2) binary catalysts for selective CO hydrogenation to C(2+)OH, outperforming silica-supported precious Rh-based catalysts, by using a combination of experimental evidence from bulk, surface-sensitive, and imaging techniques collected on real and high-performance Cu–Fe binary catalytic systems coupled with density functional theory calculations. The closer is the d-band center to the Fermi level of Cu(0)–χ-Fe(5)C(2)(510) surface than those of χ-Fe(5)C(2)(510) and Rh(111) surface, and the electron-rich interface of Cu0–χ-Fe(5)C(2)(510) due to the delocalized electron transfer from Cu0 atoms, facilitates CO activation and CO insertion into alkyl species to C2-oxygenates at the interface of Cu(0)–χ-Fe(5)C(2)(510) and thus enhances C(2)H(5)OH selectivity. Starting from the CHCO intermediate, the proposed reaction pathway for CO hydrogenation to C(2)H(5)OH on Cu0–χ-Fe(5)C(2)(510) is CHCO + (H) → CH(2)CO + (H) → CH(3)CO + (H) → CH(3)CHO + (H) → CH(3)CH2O + (H) → C(2)H(5)OH. This study may guide the rational design of high-performance binary catalysts made from earth-abundant metals with synergistic interactions for tuning selectivity. |
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| AbstractList | CO hydrogenation to higher alcohols (C(2+)OH) provides a promising route to convert coal, natural gas, shale gas, and biomass feedstocks into value-added chemicals and transportation fuels. However, the development of nonprecious metal catalysts with satisfactory activity and well-defined selectivity toward C(2+)OH remains challenging and impedes the commercialization of this process. Here, we show that the synergistic geometric and electronic interactions dictate the activity of Cu(0)–χ-F(e)5C(2) binary catalysts for selective CO hydrogenation to C(2+)OH, outperforming silica-supported precious Rh-based catalysts, by using a combination of experimental evidence from bulk, surface-sensitive, and imaging techniques collected on real and high-performance Cu–Fe binary catalytic systems coupled with density functional theory calculations. The closer is the d-band center to the Fermi level of Cu(0)–χ-Fe(5)C(2)(510) surface than those of χ-Fe(5)C(2)(510) and Rh(111) surface, and the electron-rich interface of Cu0–χ-Fe(5)C(2)(510) due to the delocalized electron transfer from Cu0 atoms, facilitates CO activation and CO insertion into alkyl species to C2-oxygenates at the interface of Cu(0)–χ-Fe(5)C(2)(510) and thus enhances C(2)H(5)OH selectivity. Starting from the CHCO intermediate, the proposed reaction pathway for CO hydrogenation to C(2)H(5)OH on Cu0–χ-Fe(5)C(2)(510) is CHCO + (H) → CH(2)CO + (H) → CH(3)CO + (H) → CH(3)CHO + (H) → CH(3)CH2O + (H) → C(2)H(5)OH. This study may guide the rational design of high-performance binary catalysts made from earth-abundant metals with synergistic interactions for tuning selectivity. CO hydrogenation to higher alcohols (C2+OH) provides a promising route to convert coal, natural gas, shale gas, and biomass feedstocks into value-added chemicals and transportation fuels. However, the development of nonprecious metal catalysts with satisfactory activity and well-defined selectivity toward C2+OH remains challenging and impedes the commercialization of this process. Here, we show that the synergistic geometric and electronic interactions dictate the activity of Cu-0-chi-Fe5C2 binary catalysts for selective CO hydrogenation to C2+OH, outperforming silica-supported precious Rh-based catalysts, by using a combination of experimental evidence from bulk, surface-sensitive, and imaging techniques collected on real and high-performance Cu-Fe binary catalytic systems coupled with density functional theory calculations. The closer is the d-band center to the Fermi level of Cu-0-chi-Fe5C2(510) surface than those of chi-Fe5C2(510) and Rh(111) surface, and the electron-rich interface of Cu-0-chi-Fe5C2(510) due to the delocalized electron transfer from Cu-0 atoms, facilitates CO activation and CO insertion into alkyl species to C-2-oxygenates at the interface of Cu-0-chi-Fe5C2(510) and thus enhances C2H5OH selectivity. Starting from the CHCO intermediate, the proposed reaction pathway for CO hydrogenation to C2H5OH on Cu-0-chi-Fe5C2(510) is CHCO + (H) -> CH2CO + (H) -> CH3CO + (H) -> CH3CHO + (H) -> CH3CH2O + (H) -> C2H5OH. This study may guide the rational design of high-performance binary catalysts made from earth-abundant metals with synergistic interactions for tuning selectivity. |
| Author | Tao, Franklin Feng Lu, Yongwu Shan, Junjun Wu, Tianpin Cao, Baobao Pote, Jonathan W. Yu, Fei Bao, Zhenghong Ge, Binghui Zhang, Riguang Nguyen, Luan Wang, Baojun |
| Author_xml | – sequence: 1 givenname: Yongwu orcidid: 0000-0003-0858-8315 surname: Lu fullname: Lu, Yongwu organization: Department of Agricultural and Biological Engineering, Mississippi State University, Mississippi State, Mississippi 39762, United States – sequence: 2 givenname: Riguang surname: Zhang fullname: Zhang, Riguang organization: Key Laboratory of Coal Science and Technology of Ministry of Education and Shanxi Province, Taiyuan University of Technology, Taiyuan, Shanxi 030024, People’s Republic of China – sequence: 3 givenname: Baobao surname: Cao fullname: Cao, Baobao organization: School of Materials Science and Engineering, Southwest Jiaotong University, Chengdu, Sichuan 610031, People’s Republic of China – sequence: 4 givenname: Binghui surname: Ge fullname: Ge, Binghui organization: Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Science, Beijing 100190, People’s Republic of China – sequence: 5 givenname: Franklin Feng orcidid: 0000-0002-4916-6509 surname: Tao fullname: Tao, Franklin Feng organization: Department of Chemical and Petroleum Engineering and Department of Chemistry, University of Kansas, Lawrence, Kansas 66045, United States – sequence: 6 givenname: Junjun surname: Shan fullname: Shan, Junjun organization: Department of Chemical and Petroleum Engineering and Department of Chemistry, University of Kansas, Lawrence, Kansas 66045, United States – sequence: 7 givenname: Luan surname: Nguyen fullname: Nguyen, Luan organization: Department of Chemical and Petroleum Engineering and Department of Chemistry, University of Kansas, Lawrence, Kansas 66045, United States – sequence: 8 givenname: Zhenghong surname: Bao fullname: Bao, Zhenghong organization: Department of Agricultural and Biological Engineering, Mississippi State University, Mississippi State, Mississippi 39762, United States – sequence: 9 givenname: Tianpin surname: Wu fullname: Wu, Tianpin organization: X-ray Science Division, Advanced Photon Source, Argonne National Laboratory, Argonne, Illinois 60439, United States – sequence: 10 givenname: Jonathan W. surname: Pote fullname: Pote, Jonathan W. organization: Department of Agricultural and Biological Engineering, Mississippi State University, Mississippi State, Mississippi 39762, United States – sequence: 11 givenname: Baojun surname: Wang fullname: Wang, Baojun organization: Key Laboratory of Coal Science and Technology of Ministry of Education and Shanxi Province, Taiyuan University of Technology, Taiyuan, Shanxi 030024, People’s Republic of China – sequence: 12 givenname: Fei orcidid: 0000-0001-5595-6147 surname: Yu fullname: Yu, Fei organization: Department of Agricultural and Biological Engineering, Mississippi State University, Mississippi State, Mississippi 39762, United States |
| BackLink | https://www.osti.gov/biblio/1481734$$D View this record in Osti.gov |
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| Snippet | CO hydrogenation to higher alcohols (C(2+)OH) provides a promising route to convert coal, natural gas, shale gas, and biomass feedstocks into value-added... CO hydrogenation to higher alcohols (C2+OH) provides a promising route to convert coal, natural gas, shale gas, and biomass feedstocks into value-added... |
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| SubjectTerms | biomass catalytic activity CO hydrogenation coal commercialization copper density functional theory electron transfer feedstocks Hagg iron carbide higher alcohols hydrogenation natural gas reaction mechanism shale gas synergistic effect value added |
| Title | Elucidating the Copper–Hägg Iron Carbide Synergistic Interactions for Selective CO Hydrogenation to Higher Alcohols |
| URI | https://www.proquest.com/docview/2636484747 https://www.osti.gov/biblio/1481734 |
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