Electrochemical Reduction of N2 into NH3 by Donor–Acceptor Couples of Ni and Au Nanoparticles with a 67.8% Faradaic Efficiency

• DOI: 10.1021/jacs.9b07963
• Publication Date: 2019-09-15T17:26:30Z
• Authors: Zhong-Hua Xue; Shi-Nan Zhang; Yun-Xiao Lin; Hui Su; Guang-Yao Zhai; Jing-Tan Han; Qiu-Ying Yu; Xin-Hao Li; Markus Antonietti; Jie-Sheng Chen
• Keywords: 7. Clean energy; 01 natural sciences; 0104 chemical sciences

The traditional NH3 production method (Haber-Bosch process) is currently complemented by electrochemical synthesis at ambient conditions, but the rather low selectivity (as indicated by the Faradaic efficiency) for the electrochemical reduction of molecular N2 into NH3 impedes the progress. Here, we present a powerful method to significantly boost the Faradaic efficiency of Au electrocatalysts to 67.8% for the nitrogen reduction reaction (NRR) by increasing their electron density through the construction of inorganic donor-acceptor couples of Ni and Au nanoparticles. The unique role of the electron-rich Au centers in facilitating the fixation and activation of N2 was also investigated via theoretical simulation methods and then confirmed by experimental results. The highly coupled Au and Ni nanoparticles supported on nitrogen-doped carbon are stable for reuse and long-term performance of the NRR, making the electrochemical process more sustainable for practical application.