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Isolated Tin(IV) Active Sites for Highly Efficient Electroreduction of CO2 to CH4 in Neutral Aqueous Solution.
Zhao, Zhen-Hua; Huang, Jia-Run; Liao, Pei-Qin; Chen, Xiao-Ming.
Afiliación
  • Zhao ZH; MOE Key Laboratory of Bioinorganic and Synthetic Chemistry, School of Chemistry, Sun Yat-Sen University, Guangzhou, 510275, China.
  • Huang JR; MOE Key Laboratory of Bioinorganic and Synthetic Chemistry, School of Chemistry, Sun Yat-Sen University, Guangzhou, 510275, China.
  • Liao PQ; MOE Key Laboratory of Bioinorganic and Synthetic Chemistry, School of Chemistry, Sun Yat-Sen University, Guangzhou, 510275, China.
  • Chen XM; MOE Key Laboratory of Bioinorganic and Synthetic Chemistry, School of Chemistry, Sun Yat-Sen University, Guangzhou, 510275, China.
Angew Chem Int Ed Engl ; 62(22): e202301767, 2023 May 22.
Article en En | MEDLINE | ID: mdl-36823343
The development of efficient electrocatalysts with non-copper metal sites for electrochemical CO2 reduction reactions (eCO2 RR) to hydrocarbons and oxygenates is highly desirable, but still a great challenge. Herein, a stable metal-organic framework (DMA)4 [Sn2 (THO)2 ] (Sn-THO, THO6- = triphenylene-2,3,6,7,10,11-hexakis(olate), DMA = dimethylammonium) with isolated and distorted octahedral SnO6 2- active sites is reported as an electrocatalyst for eCO2 RR, showing an exceptional performance for eCO2 RR to the CH4 product rather than the common products formate and CO for reported Sn-based catalysts. The partial current density of CH4 reaches a high value of 34.5 mA cm-2 , surpassing most reported copper-based and all non-Cu metal-based catalysts. Our experimental and theoretical results revealed that the isolated SnO6 2- active site favors the formation of key *OCOH species to produce CH4 and can greatly inhibit the formation of *OCHO and *COOH species to produce *HCOOH and *CO, respectively.
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Angew Chem Int Ed Engl Año: 2023 Tipo del documento: Article País de afiliación: China Pais de publicación: Alemania
Texto completo
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XML
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Angew Chem Int Ed Engl Año: 2023 Tipo del documento: Article País de afiliación: China Pais de publicación: Alemania