Boosting selective nitrogen reduction to ammonia on electron-deficient copper nanoparticles

• Published in: Nature communications Vol. 10; no. 1; pp. 4380 - 7
• Main Authors: Lin, Yun-Xiao, Zhang, Shi-Nan, Xue, Zhong-Hua, Zhang, Jun-Jun, Su, Hui, Zhao, Tian-Jian, Zhai, Guang-Yao, Li, Xin-Hao, Antonietti, Markus, Chen, Jie-Sheng
• Format: Journal Article
• Language: English
• Published: London Nature Publishing Group UK 26.09.2019; Nature Publishing Group; Nature Portfolio
• Subjects: 119/118; 140/131; 140/146; 147/135; 147/143; 639/301/299; 639/638/77/886; Ammonia; Catalysis; Catalysts; Catalytic activity; Chemical reduction; Copper; Depletion; Electrocatalysts; Electrochemistry; Electrolytes; Electrons; Haber Bosch process; Heavy metals; Humanities and Social Sciences; Hydrogen evolution reactions; multidisciplinary; Nanoparticles; Nitrogenation; Science; Science (multidisciplinary); Selectivity; Substitution reactions
• ISSN: 2041-1723; 2041-1723
• DOI: 10.1038/s41467-019-12312-4

Production of ammonia is currently realized by the Haber–Bosch process, while electrochemical N 2 fixation under ambient conditions is recognized as a promising green substitution in the near future. A lack of efficient electrocatalysts remains the primary hurdle for the initiation of potential electrocatalytic synthesis of ammonia. For cheaper metals, such as copper, limited progress has been made to date. In this work, we boost the N 2 reduction reaction catalytic activity of Cu nanoparticles, which originally exhibited negligible N 2 reduction reaction activity, via a local electron depletion effect. The electron-deficient Cu nanoparticles are brought in a Schottky rectifying contact with a polyimide support which retards the hydrogen evolution reaction process in basic electrolytes and facilitates the electrochemical N 2 reduction reaction process under ambient aqueous conditions. This strategy of inducing electron deficiency provides new insight into the rational design of inexpensive N 2 reduction reaction catalysts with high selectivity and activity. Electrocatalytic nitrogen reduction is promising for ammonia production, but electrocatalysts are limited by low efficiency and high cost. Here, the authors report electron-deficient copper nanoparticles, induced by rectifying contact with polyimide, for selective reduction of nitrogen to ammonia.