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DOI10.1039/d0ee03731a
Bifunctional single-molecular heterojunction enables completely selective CO2-to-CO conversion integrated with oxidative 3D nano-polymerization
Ma D.-D.; Han S.-G.; Cao C.; Wei W.; Li X.; Chen B.; Wu X.-T.; Zhu Q.-L.
发表日期2021
ISSN17545692
起始页码1544
结束页码1552
卷号14期号:3
英文摘要Herein, for the first time, an active and stable bifunctional electrocatalyst has been elaborately designed to achieve the integration of CO2 reduction and anodic non-classical reaction to efficiently yield products of high value at both electrodes, which was constructed by surface anchoring of a novel multi-azido-group-bearing nickel phthalocyanine onto carbon nanotubes at the single-molecule level via strong interactions. Concretely, the obtained heterojunction-type electrocatalyst exhibits ultrahigh activity for completely selective CO2-to-CO conversion with a 100% faradaic efficiency in a wide potential window, large partial current density (>200 mA cm-2) and turnover frequency, and remarkable stability. Particularly, a mass of azido-derived amine groups around the nickel phthalocyanine centers increase the local concentration of CO2via chemisorption, thus boosting the formation of the key intermediate. Unprecedentedly, an exotic electrolytic system integrating CO2 reduction with oxidative nano-polymerization was further conceptually developed using this individual bifunctional electrocatalyst for both the cathode and anode. Besides the high-performance CO2 reduction at the cathode, a unique porous 3D polymer nano-framework was obtained in the anode chamber instead of low-value O2, while the cell voltage was significantly reduced by 1.05 V to achieve 10 mA cm-2. © 2021 The Royal Society of Chemistry.
英文关键词Anodes; Cathodes; Electrocatalysts; Heterojunctions; Nickel; Polymerization; Bifunctional electrocatalysts; Classical reactions; Electrolytic system; Faradaic efficiencies; Nickel phthalocyanines; Single molecule level; Strong interaction; Turnover frequency; Carbon dioxide; carbon dioxide; carbon monoxide; oxidation; polymerization; three-dimensional modeling
语种英语
来源期刊Energy & Environmental Science
文献类型期刊论文
条目标识符http://gcip.llas.ac.cn/handle/2XKMVOVA/190753
作者单位State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences (CAS), Fuzhou, 350002, China; University of Chinese Academy of Sciences, Beijing, 100049, China; School of Materials Science and Engineering, Nanyang Technological University, Singapore, 639798, Singapore; Fujian Science and Technology Innovation Laboratory for Optoelectronic Information of China, Fuzhou, 350108, China
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GB/T 7714
Ma D.-D.,Han S.-G.,Cao C.,et al. Bifunctional single-molecular heterojunction enables completely selective CO2-to-CO conversion integrated with oxidative 3D nano-polymerization[J],2021,14(3).
APA Ma D.-D..,Han S.-G..,Cao C..,Wei W..,Li X..,...&Zhu Q.-L..(2021).Bifunctional single-molecular heterojunction enables completely selective CO2-to-CO conversion integrated with oxidative 3D nano-polymerization.Energy & Environmental Science,14(3).
MLA Ma D.-D.,et al."Bifunctional single-molecular heterojunction enables completely selective CO2-to-CO conversion integrated with oxidative 3D nano-polymerization".Energy & Environmental Science 14.3(2021).
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