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Wide-ph-range adaptable ammonia electrosynthesis from nitrate on Cu-pd interfaces

Science China Chemistry 2023年第3期66卷 913-922页

作者： Yongtao Wang peng Zhang Xiaoyun Lin Gong Zhang hui Gao Qingzhen Wang Zhi-Jian Zhao Tuo Wang Jinlong Gong Key Laboratory for Green Chemical Technology of Ministry of Education School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China Collaborative Innovation Center of Chemical Science and Engineering Tianjin 300072China haihe Laboratory of Sustainable Chemical Transformations Tianjin 300192China Joint School of National University of Singapore and Tianjin University International Campus of Tianjin UniversityBinhai New CityFuzhou 350207China

Ammonia production via electrochemical nitrate reduction is essential for environmental protection and the emerging hydrogen economy. Complex nitrate wastewater with a wide ph range calls for flexible catalysts with high selectivity. A high Faradaic efficiency(FE) of Nh3 cannot be obtained under strong acid or alkaline conditions due to the uncontrollable adsorption energy and coverage of hydrogen species(h*) on active sites. This article describes the design and fabrication of a copper-palladium(Cu-pd) alloy nanocrystal catalyst that inhibits h2 and nitrite generation in electrolytes with different nitrate concentrations and varied ph. The interfacial sites of Cu-pd alloys could enhance the adsorption energy and coverage of h* while increasing the reaction rate constant of NO_(2)*-to-NO*, which achieves a rapid conversion of NO_(2)* along with a decreased FE of NO_(2)-. Under ambient conditions, optimal FE(Nh3) is close to 100% at a wide ph range, with the solar-to-chemical conversion efficiency approaching 4.29%. The combination of thermodynamics and kinetics investigations would offer new insights into the reduction mechanism of NO_(2)* for further development of nitrate reduction.

关键词： nitrate reduction ammonia synthesis Cu-pd interfaces reaction kinetics break p h limitation

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