Crystal-Phase-Engineered PdCu Electrocatalyst for Enhanced Ammonia Synthesis

Wu Tong, Bolong Huang, Pengtang Wang, Leigang Li, Qi Shao, Xiaoqing Huang

Research output: Journal article publicationJournal articleAcademic researchpeer-review

31 Citations (Scopus)

Abstract

Crystal phase engineering is a powerful strategy for regulating the performance of electrocatalysts towards many electrocatalytic reactions, while its impact on the nitrogen electroreduction has been largely unexplored. Herein, we demonstrate that structurally ordered body-centered cubic (BCC) PdCu nanoparticles can be adopted as active, selective, and stable electrocatalysts for ammonia synthesis. Specifically, the BCC PdCu exhibits excellent activity with a high NH3 yield of 35.7 μg h−1 mg−1cat, Faradaic efficiency of 11.5 %, and high selectivity (no N2H4 is detected) at −0.1 V versus reversible hydrogen electrode, outperforming its counterpart, face-centered cubic (FCC) PdCu, and most reported nitrogen reduction reaction (NRR) electrocatalysts. It also exhibits durable stability for consecutive electrolysis for five cycles. Density functional theory calculation reveals that strong orbital interactions between Pd and neighboring Cu sites in BCC PdCu obtained by structure engineering induces an evident correlation effect for boosting up the Pd 4d electronic activities for efficient NRR catalysis. Our findings open up a new avenue for designing active and stable electrocatalysts towards NRR.

Original languageEnglish
Pages (from-to)2649-2653
Number of pages5
JournalAngewandte Chemie - International Edition
Volume59
Issue number7
DOIs
Publication statusPublished - 10 Feb 2020

Keywords

  • ammonia synthesis
  • crystal phase engineering
  • electroreduction
  • nitrogen fixation
  • ordered structures

ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)

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