Au-activated N motifs in non-coherent cupric porphyrin metal organic frameworks for promoting and stabilizing ethylene production

Xulan Xie, Xiang Zhang, Miao Xie, Likun Xiong, Hao Sun, Yongtao Lu, Qiaoqiao Mu, Mark H. Rummeli, Jiabin Xu, Shuo Li, Jun Zhong, Zhao Deng, Bingyun Ma, Tao Cheng (), William A. Goddard () and Yang Peng ()
Additional contact information
Xulan Xie: Soochow University
Xiang Zhang: Soochow University
Miao Xie: Soochow University
Likun Xiong: Shanghai Institute of Technology
Hao Sun: Soochow University
Yongtao Lu: Soochow University
Qiaoqiao Mu: Soochow University
Mark H. Rummeli: Soochow University
Jiabin Xu: Soochow University
Shuo Li: Soochow University
Jun Zhong: Soochow University
Zhao Deng: Soochow University
Bingyun Ma: Soochow University
Tao Cheng: Soochow University
William A. Goddard: California Institute of Technology
Yang Peng: Soochow University

Nature Communications, 2022, vol. 13, issue 1, 1-11

Abstract: Abstract Direct implementation of metal-organic frameworks as the catalyst for CO2 electroreduction has been challenging due to issues such as poor conductivity, stability, and limited > 2e− products. In this study, Au nanoneedles are impregnated into a cupric porphyrin-based metal-organic framework by exploiting ligand carboxylates as the Au3+ -reducing agent, simultaneously cleaving the ligand-node linkage. Surprisingly, despite the lack of a coherent structure, the Au-inserted framework affords a superb ethylene selectivity up to 52.5% in Faradaic efficiency, ranking among the best for metal-organic frameworks reported in the literature. Through operando X-ray, infrared spectroscopies and density functional theory calculations, the enhanced ethylene selectivity is attributed to Au-activated nitrogen motifs in coordination with the Cu centers for C-C coupling at the metalloporphyrin sites. Furthermore, the Au-inserted catalyst demonstrates both improved structural and catalytic stability, ascribed to the altered charge conduction path that bypasses the incoherent framework. This study underlines the modulation of reticular metalloporphyrin structure by metal impregnation for steering the CO2 reduction reaction pathway.

Date: 2022
References: View complete reference list from CitEc
Citations:

Downloads: (external link)
https://www.nature.com/articles/s41467-021-27768-6 Abstract (text/html)

Related works:
This item may be available elsewhere in EconPapers: Search for items with the same title.

Export reference: BibTeX RIS (EndNote, ProCite, RefMan) HTML/Text

Persistent link: https://EconPapers.repec.org/RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-021-27768-6

Ordering information: This journal article can be ordered from
https://www.nature.com/ncomms/

DOI: 10.1038/s41467-021-27768-6

Access Statistics for this article

Nature Communications is currently edited by Nathalie Le Bot, Enda Bergin and Fiona Gillespie

More articles in Nature Communications from Nature
Bibliographic data for series maintained by Sonal Shukla () and Springer Nature Abstracting and Indexing ().