Nanograin-Boundary-Abundant Cu2O-Cu Nanocubes with High C2+ Selectivity and Good Stability during Electrochemical CO2 Reduction at a Current Density of 500 mA/cm2

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

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Author(s)

  • Qiqi Wu
  • Ruian Du
  • Peng Wang
  • Geoffrey I. N. Waterhouse
  • Jia Li
  • Yongcai Qiu
  • Keyou Yan
  • Yun Zhao
  • Wei-Wei Zhao
  • Hsin-Jung Tsai
  • Meng-Cheng Chen
  • Sung-Fu Hung
  • Guangxu Chen

Related Research Unit(s)

Detail(s)

Original languageEnglish
Pages (from-to)12884–12894
Journal / PublicationACS Nano
Volume17
Issue number13
Online published20 Jun 2023
Publication statusPublished - 11 Jul 2023

Abstract

Surface and interface engineering, especially the creation of abundant Cu0/Cu+ interfaces and nanograin boundaries, is known to facilitate C2+ production during electrochemical CO2 reductions over copper-based catalysts. However, precisely controlling the favorable nanograin boundaries with surface structures (e.g., Cu(100) facets and Cu[n(100)×(110)] step sites) and simultaneously stabilizing Cu0/Cu+ interfaces is challenging, since Cu+ species are highly susceptible to be reduced into bulk metallic Cu at high current densities. Thus, an in-depth understanding of the structure evolution of the Cu-based catalysts under realistic CO2RR conditions is imperative, including the formation and stabilization of nanograin boundaries and Cu0/Cu+ interfaces. Herein we demonstrate that the well-controlled thermal reduction of Cu2O nanocubes under a CO atmosphere yields a remarkably stable Cu2O-Cu nanocube hybrid catalyst (Cu2O(CO)) possessing a high density of Cu0/Cu+ interfaces, abundant nanograin boundaries with Cu(100) facets, and Cu[n(100)×(110)] step sites. The Cu2O(CO) electrocatalyst delivered a high C2+ Faradaic efficiency of 77.4% (56.6% for ethylene) during the CO2RR under an industrial current density of 500 mA/cm2. Spectroscopic characterizations and morphological evolution studies, together with in situ time-resolved attenuated total reflection–surface enhanced infrared absorption spectroscopy (ATR-SEIRAS) studies, established that the morphology and Cu0/Cu+ interfacial sites in the as-prepared Cu2O(CO) catalyst were preserved under high polarization and high current densities due to the nanograin-boundary-abundant structure. Furthermore, the abundant Cu0/Cu+ interfacial sites on the Cu2O(CO) catalyst acted to increase the *CO adsorption density, thereby increasing the opportunity for C–C coupling reactions, leading to a high C2+ selectivity. © 2023 American Chemical Society.

Research Area(s)

  • C2+ products, Cu+/Cu0 interface, electrochemical CO2 reduction, high current density, nanograin boundary

Citation Format(s)

Nanograin-Boundary-Abundant Cu2O-Cu Nanocubes with High C2+ Selectivity and Good Stability during Electrochemical CO2 Reduction at a Current Density of 500 mA/cm2. / Wu, Qiqi; Du, Ruian; Wang, Peng et al.
In: ACS Nano, Vol. 17, No. 13, 11.07.2023, p. 12884–12894.

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