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Crystal‐Phase‐Engineered PdCu Electrocatalyst for Enhanced Ammonia Synthesis
Author(s) -
Tong Wu,
Huang Bolong,
Wang Pengtang,
Li Leigang,
Shao Qi,
Huang Xiaoqing
Publication year - 2020
Publication title -
angewandte chemie
Language(s) - English
Resource type - Journals
eISSN - 1521-3757
pISSN - 0044-8249
DOI - 10.1002/ange.201913122
Subject(s) - electrocatalyst , faraday efficiency , ammonia production , reversible hydrogen electrode , catalysis , electrochemistry , electrolysis , chemistry , selectivity , bulk electrolysis , redox , ammonia , crystal structure , nanoparticle , inorganic chemistry , combinatorial chemistry , materials science , nanotechnology , electrode , crystallography , cyclic voltammetry , organic chemistry , working electrode , electrolyte
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 NH 3 yield of 35.7 μg h −1 mg −1 cat , Faradaic efficiency of 11.5 %, and high selectivity (no N 2 H 4 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.