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

Wang, YR (Wang, Yi-Rong)[ 1 ] ; Huang, Q (Huang, Qing)[ 1 ] ; He, CT (He, Chun-Ting)[ 2 ] ; Chen, YF (Chen, Yifa)[ 1 ] ; Liu, J (Liu, Jiang)[ 1 ] ; Shen, FC (Shen, Feng-Cui)[ 1 ] ; Lan, YQ (Lan, Ya-Qian)[ 1 ]*（兰亚乾）

[ 1 ] Nanjing Normal Univ, Jiangsu Collaborat Innovat Ctr Biomed Funct Mat, Sch Chem & Mat Sci, Jiangsu Key Lab New Power Batteries, Nanjing 210023, Jiangsu, Peoples R China

[ 2 ] Jiangxi Normal Univ, MOE Key Lab Funct Small Organ Mol, Coll Chem & Chem Engn, Nanchang 330022, Jiangxi, Peoples R China

NATURE COMMUNICATIONS，201810,9

The design of highly stable, selective and efficient electrocatalysts for CO2 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 {epsilon-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 CO2 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).

文章链接：

https://www.nature.com/articles/s41467-018-06938-z

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