Liu Huimin, Lang Xiuyao, Zhu Chao, Timoshenko Janis, Rüscher Martina, Bai Lichen, Guijarro Néstor, Yin Haibo, Peng Yue, Li Junhua, Liu Zheng, Wang Weichao, Cuenya Beatriz Roldan, Luo Jingshan
Institute of Photoelectronic Thin Film Devices and Technology, Solar Energy Research Center, Key Laboratory of Photoelectronic Thin Film Devices and Technology of Tianjin, Ministry of Education Engineering Research Center of Thin Film Photoelectronic Technology, Renewable Energy Conversion and Storage Center, Nankai University, Tianjin, 300350, China.
School of Materials Science and Engineering, Nanyang Technological University, Singapore, 639798, Singapore.
Angew Chem Int Ed Engl. 2022 Jun 7;61(23):e202202556. doi: 10.1002/anie.202202556. Epub 2022 Apr 5.
The electrochemical nitrate reduction reaction (NITRR) provides a promising solution for restoring the imbalance in the global nitrogen cycle while enabling a sustainable and decentralized route to source ammonia. Here, we demonstrate a novel electrocatalyst for NITRR consisting of Rh clusters and single-atoms dispersed onto Cu nanowires (NWs), which delivers a partial current density of 162 mA cm for NH production and a Faradaic efficiency (FE) of 93 % at -0.2 V vs. RHE. The highest ammonia yield rate reached a record value of 1.27 mmol h cm . Detailed investigations by electron paramagnetic resonance, in situ infrared spectroscopy, differential electrochemical mass spectrometry and density functional theory modeling suggest that the high activity originates from the synergistic catalytic cooperation between Rh and Cu sites, whereby adsorbed hydrogen on Rh site transfers to vicinal *NO intermediate species adsorbed on Cu promoting the hydrogenation and ammonia formation.
电化学硝酸盐还原反应（NITRR）为恢复全球氮循环的失衡提供了一个有前景的解决方案，同时为氨的可持续生产和分散式生产提供了一条途径。在此，我们展示了一种用于NITRR的新型电催化剂，它由负载在铜纳米线（NWs）上的铑簇和单原子组成，在相对于可逆氢电极（RHE）为-0.2 V时，该催化剂对于氨的生成提供了162 mA cm的分电流密度和93%的法拉第效率（FE）。最高氨产率达到了创纪录的1.27 mmol h cm 。通过电子顺磁共振、原位红外光谱、差分电化学质谱和密度泛函理论建模进行的详细研究表明，高活性源于铑和铜位点之间的协同催化作用，即铑位点上吸附的氢转移到相邻的吸附在铜上的*NO中间物种上，促进了氢化和氨的形成。
