Efficient multicarbon formation in acidic CO2 reduction via tandem electrocatalysis

Yuanjun Chen, Xiao Yan Li, Zhu Chen, Adnan Ozden, Jianan Erick Huang, Pengfei Ou, Juncai Dong, Jinqiang Zhang, Cong Tian, Byoung Hoon Lee, Xinyue Wang, Shijie Liu, Qingyun Qu, Sasa Wang, Yi Xu, Rui Kai Miao, Yong Zhao, Yanjiang Liu, Chenyue Qiu, Jehad AbedHengzhou Liu, Heejong Shin, Dingsheng Wang, Yadong Li, David Sinton, Edward H. Sargent*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

16 Scopus citations

Abstract

The electrochemical reduction of CO2 in acidic conditions enables high single-pass carbon efficiency. However, the competing hydrogen evolution reaction reduces selectivity in the electrochemical reduction of CO2, a reaction in which the formation of CO, and its ensuing coupling, are each essential to achieving multicarbon (C2+) product formation. These two reactions rely on distinct catalyst properties that are difficult to achieve in a single catalyst. Here we report decoupling the CO2-to-C2+ reaction into two steps, CO2-to-CO and CO-to-C2+, by deploying two distinct catalyst layers operating in tandem to achieve the desired transformation. The first catalyst, atomically dispersed cobalt phthalocyanine, reduces CO2 to CO with high selectivity. This process increases local CO availability to enhance the C–C coupling step implemented on the second catalyst layer, which is a Cu nanocatalyst with a Cu–ionomer interface. The optimized tandem electrodes achieve 61% C2H4 Faradaic efficiency and 82% C2+ Faradaic efficiency at 800 mA cm−2 at 25 °C. When optimized for single-pass utilization, the system reaches a single-pass carbon efficiency of 90 ± 3%, simultaneous with 55 ± 3% C2H4 Faradaic efficiency and a total C2+ Faradaic efficiency of 76 ± 2%, at 800 mA cm−2 with a CO2 flow rate of 2 ml min−1.

Original languageEnglish (US)
Pages (from-to)311-318
Number of pages8
JournalNature nanotechnology
Volume19
Issue number3
DOIs
StatePublished - Mar 2024

ASJC Scopus subject areas

  • Condensed Matter Physics
  • Bioengineering
  • Atomic and Molecular Physics, and Optics
  • Electrical and Electronic Engineering
  • Biomedical Engineering
  • General Materials Science

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