Surprisingly big linker-dependence of activity and selectivity in CO2 reduction by an iridium(I) pincer complex

Gongfang Hu; Jianbing “Jimmy” Jiang; H. Ray Kelly; Adam J. Matula; Yueshen Wu; Neyen Romano; Brandon Q. Mercado; Hailiang Wang; Victor S. Batista; Robert H. Crabtree; Gary W. Brudvig

doi:10.1039/D0CC03207G

Surprisingly big linker-dependence of activity and selectivity in CO₂ reduction by an iridium(i) pincer complex†

Gongfang Hu,

‡^ab Jianbing “Jimmy” Jiang,‡*^c H. Ray Kelly,^ab Adam J. Matula,^ab Yueshen Wu,^ab Neyen Romano,^ab Brandon Q. Mercado,^a Hailiang Wang,

*^ab Victor S. Batista,*^ab Robert H. Crabtree

^ab and Gary W. Brudvig

*^ab

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* Corresponding authors

^a Department of Chemistry, Yale University, New Haven, Connecticut, USA
E-mail: victor.batista@yale.edu, hailiang.wang@yale.edu, gary.brudvig@yale.edu

^b Energy Sciences Institute, Yale University, West Haven, Connecticut, USA

^c Department of Chemistry, University of Cincinnati, P.O. Box 210172, Cincinnati, Ohio 45221-0172, USA
E-mail: jianbing.jiang@uc.edu

Abstract

Here, we report the quantitative electroreduction of CO₂ to CO by a PNP-pincer iridium(I) complex bearing amino linkers in DMF/water. The electrocatalytic properties greatly depend on the choice of linker within the ligand. The complex 3-N is far superior to the analogues with methylene and oxygen linkers, showing higher activity and better selectivity for CO₂ over proton reduction.

This article is part of the themed collection: (Photo)electrocatalysis for renewable energy

Chemical Communications

Surprisingly big linker-dependence of activity and selectivity in CO₂ reduction by an iridium(i) pincer complex†

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Surprisingly big linker-dependence of activity and selectivity in CO₂ reduction by an iridium(I) pincer complex

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