Molecular Scaffolding Strategy with Synergistic Active Centers To Facilitate Electrocatalytic CO Reduction to Hydrocarbon/Alcohol.
A major impediment to the electrocatalytic CO reduction reaction (CRR) is the lack of electrocatalysts with both high efficiency and good selectivity toward liquid fuels or other valuable chemicals. Effective strategies for the design of electrocatalysts are yet to be discovered to substitute the co...
| Publicado en: | Journal of the American Chemical Society Vol. 139; no. 49; pp. 18093 - 18101 |
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| Autores principales: | , , , , |
| Formato: | Artículo |
| Publicado: |
American Chemical Society
12/13/2017
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| Materias: | |
| Acceso en línea: | Ver este registro en EBSCOhost |
| fields | @attributes: recordID: 1 pdfLink: plink: https://search.ebscohost.com/login.aspx?direct=true&db=hlh&AN=126761890&site=ehost-live header: @attributes: shortDbName: hlh uiTerm: 126761890 longDbName: Humanities International Complete uiTag: AN controlInfo: bkinfo: jinfo: jid: 00027863 ACS jtl: Journal of the American Chemical Society issn: 00027863 maglogo: N pubinfo: dt: 12/13/2017 vid: 139 iid: 49 pid: 997 pub: American Chemical Society artinfo: ui: 126761890 10.1021/jacs.7b10817 ppf: 18093 ppct: 8 formats: tig: atl: Molecular Scaffolding Strategy with Synergistic Active Centers To Facilitate Electrocatalytic CO Reduction to Hydrocarbon/Alcohol. aug: au: Yan Jiao Yao Zheng Ping Chen Jaroniec, Mietek Shi-Zhang Qiao affil: School of Chemical Engineering, The University of Adelaide, Adelaide, South Australia 5005, Australia School of Chemistry and Chemical Engineering, Anhui University, Hefei 230000, P. R. China Department of Chemistry and Biochemistry, Kent State University, Kent, Ohio 44242, United States School of Materials Science and Engineering, Tianjin University, Tianjin 300072, P. R. China su: Carbon dioxide reduction Electrocatalysis Scaffold proteins Hydrocarbons Alcohols (Chemical class) Density functional theory sug: subj: Carbon dioxide reduction Electrocatalysis Scaffold proteins Hydrocarbons Alcohols (Chemical class) Density functional theory ab: A major impediment to the electrocatalytic CO reduction reaction (CRR) is the lack of electrocatalysts with both high efficiency and good selectivity toward liquid fuels or other valuable chemicals. Effective strategies for the design of electrocatalysts are yet to be discovered to substitute the conventional trial-and-error approach. This work shows that a combination of density functional theory (DFT) computation and experimental validation of molecular scaffolding to coordinate the metal active centers presents a new molecular-level strategy for the development of electrocatalysts with high CRR selectivity toward hydrocarbon/ alcohol. Taking the most widely investigated Cu as a probe, our study reveals that the use of graphitic carbon nitride (g-CN) as a molecular scaffold allows for an appropriate modification of the electronic structure of Cu in the resultant Cu-CN complex. As a result, the adsorption behavior of some key reaction intermediates can be optimized on the Cu-CN surface, which greatly benefits the activation of CO and leads to a more facile CO reduction to desired products as compared with those on the Cu(111) surface and other kinds of Cu complexes formed on nitrogen-doped carbons. Remarkably, different from the most studied elementary metal surfaces, an intramolecular synergistic catalysis with dual active centers was for the first time observed on the Cu-CN complex model, which possesses a unique capability to generate C products. A good agreement between electrochemical measurements and the DFT analysis of the CRR has been achieved on the basis of the newly designed and synthesized Cu-CN electrocatalyst. pubtype: Academic Journal doctype: Article src: R language: English refInfo: copyright: @attributes: flag: Y dt: @attributes: year: 2017 holdings: @attributes: islocal: N |
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