Crystal‐Phase‐Engineered PdCu Electrocatalyst for Enhanced Ammonia Synthesis

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...

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Bibliographic Details
Published in:Angewandte Chemie International Edition 2020-02, Vol.59 (7), p.2649-2653
Main Authors: Tong, Wu, Huang, Bolong, Wang, Pengtang, Li, Leigang, Shao, Qi, Huang, Xiaoqing
Format: Article
Language:English
Subjects:
Ammonia
ammonia synthesis
Catalysis
Chemical reduction
crystal phase engineering
Density functional theory
Electrocatalysts
Electrolysis
electroreduction
Engineering
Face centered cubic lattice
Nanoparticles
Nitrogen
nitrogen fixation
ordered structures
Selectivity
Synthesis
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Summary: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. At face value: The body‐centered cubic (BCC) PdCu nanoparticles that were constructed and adopted as an active, selective, and stable electrocatalyst for the nitrogen reduction reaction display far better performance than the conventional face‐centered cubic (FCC) PdCu electrocatalyst.
ISSN:1433-7851
1521-3773
DOI:10.1002/anie.201913122