Crystal-Phase-Engineered PdCu Electrocatalyst for Enhanced Ammonia Synthesis
Wu Tong1,+ , Bolong Huang2,+ , Pengtang Wang1, Leigang Li1, Qi Shao1, and Xiaoqing Huang1,*（黄小青）
1 College of Chemistry, Chemical Engineering and Materials Science Soochow University No.199, Ren’ai Road, Suzhou 215123, Jiangsu (China)
2 Department of Applied Biology and Chemical Technology The Hong Kong Polytechnic University Hung Hom, Kowloon, Hong Kong SAR (Hong Kong)
+ These authors contributed equally to this work.
Angew. Chem. Int. Ed. 2020, 59，2649-2653
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.
链接：https://onlinelibrary.wiley.com/doi/full/10.1002/anie.201913122
