Phase-Dependent Electrocatalytic CO2 Reduction on Pd3Bi Nanocrystals

Lin Jia, Mingzi Sun, Jie Xu, Xuan Zhao, Rui Zhou, Binbin Pan, Lu Wang, Na Han, Bolong Huang, Yanguang Li

Research output: Journal article publicationJournal articleAcademic researchpeer-review

12 Citations (Scopus)

Abstract

Alloying is a general strategy for modulating the electronic structures of catalyst materials. Compared to more common solid–solution alloys, intermetallic alloys feature well-defined atomic arrangements and provide the unique platform for studying the structure-performance correlations. It is, unfortunately, synthetically challenging to prepare the nanostructures of intermetallic alloys for catalysis research. In this contribution, we prepare intermetallic Pd3Bi nanocrystals of a uniform size via a facile solvothermal method. These nanocrystals can phase-transform into solid solution alloy via thermal annealing while retaining a similar composition and size. In 0.1 M KHCO3 aqueous solution, the intermetallic Pd3Bi can selectively reduce CO2 to formate with high selectivity (≈100 %) and stability even at <-0.35 V versus reversible hydrogen electrode, whereas the solid solution alloy has limited formate selectivity of <60 %. Such unique phase-dependence is understood via theoretical simulations showing that the crystallographic ordering of Pd and Bi atoms within intermetallic alloys can suppress CO poisoning and enhance the *OCHO adsorption during electrochemical CO2 reduction to formate.

Original languageEnglish
Pages (from-to)21741-21745
Number of pages5
JournalAngewandte Chemie - International Edition
Volume60
Issue number40
DOIs
Publication statusPublished - 27 Sep 2021

Keywords

  • electrochemical CO reduction
  • formate
  • intermetallic alloy
  • phase dependence
  • selectivity

ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)

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