Oriented electron transmission in polyoxometalate-metalloporphyrin organic framework for highly selective electroreduction of CO2

• Published in: Nature communications Vol. 9; no. 1; pp. 1 - 8
• Main Authors: Wang, Yi-Rong, Huang, Qing, He, Chun-Ting, Chen, Yifa, Liu, Jiang, Shen, Feng-Cui, Lan, Ya-Qian
• Format: Journal Article
• Language: English
• Published: London Nature Publishing Group UK 26.10.2018; Nature Publishing Group; Nature Portfolio
• Subjects: 639/301/299/921; 639/638/161/886; 639/638/77/887; 639/925/357/404; Carbon dioxide; Catalysis; Catalysts; Chemical reduction; Density functional theory; Electrocatalysts; Electrons; Humanities and Social Sciences; Metal-organic frameworks; Migration; multidisciplinary; Science; Science (multidisciplinary)
• ISSN: 2041-1723; 2041-1723
• DOI: 10.1038/s41467-018-06938-z

The design of highly stable, selective and efficient electrocatalysts for CO 2 reduction reaction is desirable while largely unmet. In this work, a series of precisely designed polyoxometalate-metalloporphyrin organic frameworks are developed. Noted that the integration of {ε-PMo 8 V Mo 4 VI O 40 Zn 4 } cluster and metalloporphyrin endows these polyoxometalate-metalloporphyrin organic frameworks greatly advantages in terms of electron collecting and donating, electron migration and electrocatalytic active component in the CO 2 reduction reaction. Thus-obtained catalysts finally present excellent performances and the mechanisms of catalysis processes are discussed and revealed by density functional theory calculations. Most importantly, Co-PMOF exhibits remarkable faradaic efficiency ( > 94%) over a wide potential range (−0.8 to −1.0 V). Its best faradaic efficiency can reach up to 99% (highest in reported metal-organic frameworks) and it exhibits a high turnover frequency of 1656 h −1 and excellent catalysis stability ( > 36 h). While CO2 reduction provides a way to remove carbon from the atmosphere, it is challenging to design effective, selective materials for this process. Here, authors construct metal-organic frameworks from polyoxometalates and porphryins to direct electron flow and improve CO2 reduction efficiencies.