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Hierarchical Cobalt Phosphide Hollow Nanocages toward Electrocatalytic Ammonia Synthesis under Ambient Pressure and Room Temperature
Small Methods ( IF 12.4 ) Pub Date : 2018-08-23 , DOI: 10.1002/smtd.201800204
Wenhan Guo 1 , Zibin Liang 1 , Junliang Zhao 2 , Bingjun Zhu 1 , Kunting Cai 1 , Ruqiang Zou 1 , Qiang Xu 3, 4
Affiliation  

Electrochemical nitrogen reduction reaction (NRR) under room temperature and ambient pressure is a promising energy‐ and environmental‐friendly method for ammonia synthesis, which currently highly relies on the energy‐consuming Haber‐Bosch process with enormous CO2 emissions. This study reports the synthesis of a noble‐metal‐free CoP hollow nanocage (CoP HNC) catalyst from a metal‐organic framework precursor through a layered‐double‐hydroxide intermediate, and the use as the cathode for electrochemical NRR. The 3D hierarchical nanoparticle–nanosheet–nanocage structure provides rich surface active sites for nitrogen adsorption and reduction. When applied for NRR, CoP HNC exhibits exciting performance with high Faraday efficiency at low overpotentials (7.36% at 0 V vs reversible hydrogen electrode [RHE]), and the ammonia yield rate increases exponentially at more negative potential, reaching 10.78 µg h−1 at −0.4 V (vs RHE) with good selectivity (no hydrazine produced) under ambient conditions. This noble‐metal‐free electrocatalyst with promising performance demonstrates the unique potential of transition metal and their compounds in the field of NRR, providing new perspectives to rational catalyst design and mechanism study.

中文翻译:

常压常温下磷化钴空心纳米笼对电催化合成氨的影响

室温和环境压力下的电化学氮还原反应(NRR)是一种有前途的能源和环境友好型合成氨的方法,目前该方法高度依赖具有大量CO 2的耗能的Haber-Bosch工艺排放。这项研究报告了从金属有机骨架前体通过层状双氢氧化物中间体合成无贵金属的CoP空心纳米笼(CoP HNC)催化剂,并将其用作电化学NRR的阴极。3D分层的纳米颗粒-纳米片-纳米结构为氮的吸附和还原提供了丰富的表面活性位。当用于NRR时,CoP HNC表现出令人兴奋的性能,在低过电势下(法拉第效率为06%,相对于可逆氢电极[RHE]在0 V时为7.36%),并且法拉第效率很高,并且氨的产率在更多的负电势下呈指数增长,达到10.78 µg h -1在−0.4 V(vs RHE)下,在环境条件下具有良好的选择性(不产生肼)。这种性能优异的无贵金属电催化剂证明了过渡金属及其化合物在NRR领域的独特潜力,为合理的催化剂设计和机理研究提供了新的视角。
更新日期:2018-08-23
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