Affiliation:
1. Institute for Energy Research Jiangsu University 212013 Zhenjiang China
2. Department of Chemistry Tsinghua University 100084 Beijing China
3. Department of Chemical Engineering Columbia University 10027 New York USA
4. The Sanya Science and Education Innovation Park Wuhan University of Technology 572000 Sanya China
Abstract
AbstractElectrochemical nitrate reduction method (NitRR) is a low‐carbon, environmentally friendly, and efficient method for synthesizing ammonia, which has received widespread attention in recent years. Copper‐based catalysts have a leading edge in nitrate reduction due to their good adsorption of *NO3. However, the formation of active hydrogen (*H) on Cu surfaces is difficult and insufficient, resulting in a large amount of the by‐product NO2−. In this work, Pd single atoms suspended on the interlayer unsaturated bonds of CuO atoms formed due to dislocations (Pd−CuO) were prepared by low temperature treatment, and the Pd single atoms located on the dislocations were subjected to shear stress and the dynamic effect of support formation to promote the conversion of nitrate into ammonia. The catalysis had an ammonia yield of 4.2 mol. gcat−1. h−1, and a Faraday efficiency of 90 % for ammonia production at −0.5 V vs. RHE. Electrochemical in situ characterization and theoretical calculations indicate that the dynamic effects of Pd single atoms and carriers under shear stress obviously promote the production of active hydrogen, reduce the reaction energy barrier of the decision‐making step for nitrate conversion to ammonia, further promote ammonia generation.