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Published on: December 6, 2021
Constructing Ru@C3 N4 /Cu Tandem Electrocatalyst with Dual-Active Sites for Enhanced Nitrate Electroreduction to
Yinan Zheng1, MingXin Qin2, Xin Yu1
1Key Lab of Synthetic and Natural Functional Molecule Chemistry of Ministry of Education, The College of Chemistry and Materials Science, Northwest University, Xi'an, 710069, P. R. China.
Abstract:
Electroreduction of nitrate to ammonia reaction (NO3 - RR) is considered as a promising carbon-free energy technique, which can eliminate nitrate from waste-water also produce value-added ammonia. However, it remains a challenge for achieving satisfied ammonia selectivity and Faraday efficiency (FE) due to the complex multiple-electron reduction process. Herein, a novel Tandem electrocatalyst that Ru dispersed on the porous graphitized C3 N4 (g-C3 N4 ) encapsulated with self-supported Cu nanowires (denoted as Ru@C3 N4 /Cu) for NO3 - RR is presented. As expected, a high ammonia yield of 0.249 mmol h-1 cm-2 at -0.9 V and high FENH3 of 91.3% at -0.8 V versus RHE can be obtained, while achieving excellent nitrate conversion (96.1%) and ammonia selectivity (91.4%) in neutral solution. In addition, density functional theory (DFT) calculations further demonstrate that the superior NO3 - RR performance is mainly resulted from the synergistic effect between the Ru and Cu dual-active sites, which can significantly enhance the adsorption of NO3 - and facilitate hydrogenation, as well as suppress the hydrogen evolution reaction, thus lead to highly improved NO3 - RR performances. This novel design strategy would pave a feasible avenue for the development of advanced NO3 - RR electrocatalysts.
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