Atomic high-spin cobalt(II) center for highly selective electrochemical CO reduction to CH3OH

Research output: Journal Publications and Reviews (RGC: 21, 22, 62)21_Publication in refereed journalpeer-review

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Author(s)

  • Jie Ding
  • Zhiming Wei
  • Fuhua Li
  • Jincheng Zhang
  • Qiao Zhang
  • Jing Zhou
  • Weijue Wang
  • Yuhang Liu
  • Zhen Zhang
  • Xiaozhi Su
  • Runze Yang
  • Wei Liu
  • Chenliang Su
  • Hong Bin Yang
  • Yanqiang Huang
  • Yueming Zhai

Detail(s)

Original languageEnglish
Article number6550
Journal / PublicationNature Communications
Volume14
Online published17 Oct 2023
Publication statusPublished - 2023

Link(s)

Abstract

In this work, via engineering the conformation of cobalt active center in cobalt phthalocyanine molecular catalyst, the catalytic efficiency of electrochemical carbon monoxide reduction to methanol can be dramatically tuned. Based on a collection of experimental investigations and density functional theory calculations, it reveals that the electron rearrangement of the Co 3d orbitals of cobalt phthalocyanine from the low-spin state (S = 1/2) to the high-spin state (S = 3/2), induced by molecular conformation change, is responsible for the greatly enhanced CO reduction reaction performance. Operando attenuated total reflectance surface-enhanced infrared absorption spectroscopy measurements disclose accelerated hydrogenation of CORR intermediates, and kinetic isotope effect validates expedited proton-feeding rate over cobalt phthalocyanine with high-spin state. Further natural population analysis and density functional theory calculations demonstrate that the high spin Co2+ can enhance the electron backdonation via the dxz/dyz−2π* bond and weaken the C-O bonding in *CO, promoting hydrogenation of CORR intermediates. © 2023, Springer Nature Limited.

Research Area(s)

Citation Format(s)

Atomic high-spin cobalt(II) center for highly selective electrochemical CO reduction to CH3OH. / Ding, Jie; Wei, Zhiming; Li, Fuhua et al.
In: Nature Communications, Vol. 14, 6550, 2023.

Research output: Journal Publications and Reviews (RGC: 21, 22, 62)21_Publication in refereed journalpeer-review

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