Synergistic enhancement of electrocatalytic CO2 reduction to C2 oxygenates at nitrogen-doped nanodiamonds/Cu interface

Hongxia Wang, Yan Kai Tzeng, Yongfei Ji, Yanbin Li, Jun Li, Xueli Zheng, Ankun Yang, Yayuan Liu, Yongji Gong, Lili Cai, Yuzhang Li, Xiaokun Zhang, Wei Chen, Bofei Liu, Haiyu Lu, Nicholas A. Melosh, Zhi Xun Shen, Karen Chan, Tianwei Tan, Steven ChuYi Cui

Research output: Contribution to journalArticle

Abstract

To date, effective control over the electrochemical reduction of CO2 to multicarbon products (C ≥ 2) has been very challenging. Here, we report a design principle for the creation of a selective yet robust catalytic interface for heterogeneous electrocatalysts in the reduction of CO2 to C2 oxygenates, demonstrated by rational tuning of an assembly of nitrogen-doped nanodiamonds and copper nanoparticles. The catalyst exhibits a Faradaic efficiency of ~63% towards C2 oxygenates at applied potentials of only −0.5 V versus reversible hydrogen electrode. Moreover, this catalyst shows an unprecedented persistent catalytic performance up to 120 h, with steady current and only 19% activity decay. Density functional theory calculations show that CO binding is strengthened at the copper/nanodiamond interface, suppressing CO desorption and promoting C2 production by lowering the apparent barrier for CO dimerization. The inherent compositional and electronic tunability of the catalyst assembly offers an unrivalled degree of control over the catalytic interface, and thereby the reaction energetics and kinetics.

Original languageEnglish (US)
Pages (from-to)131-137
Number of pages7
JournalNature Nanotechnology
Volume15
Issue number2
DOIs
StatePublished - Feb 1 2020
Externally publishedYes

ASJC Scopus subject areas

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

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  • Cite this

    Wang, H., Tzeng, Y. K., Ji, Y., Li, Y., Li, J., Zheng, X., Yang, A., Liu, Y., Gong, Y., Cai, L., Li, Y., Zhang, X., Chen, W., Liu, B., Lu, H., Melosh, N. A., Shen, Z. X., Chan, K., Tan, T., ... Cui, Y. (2020). Synergistic enhancement of electrocatalytic CO2 reduction to C2 oxygenates at nitrogen-doped nanodiamonds/Cu interface. Nature Nanotechnology, 15(2), 131-137. https://doi.org/10.1038/s41565-019-0603-y