Batch-Scale Synthesis of Nanoparticle-Agminated Three-Dimensional Porous Cu@Cu2O Microspheres for Highly Selective Electrocatalysis of Nitrate to Ammonia

Minghang Jiang; Qiang Zhu; Xinmei Song

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Batch-Scale Synthesis of Nanoparticle-Agminated Three-Dimensional Porous Cu@Cu2O Microspheres for Highly Selective Electrocatalysis of Nitrate to Ammonia

机译：Batch-Scale Synthesis of Nanoparticle-Agminated Three-Dimensional Porous Cu@Cu2O Microspheres for Highly Selective Electrocatalysis of Nitrate to Ammonia

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The electrochemical nitrate reduction reaction(NITRR),which converts nitrate to ammonia,is promising for artificial ammonia synthesis at mild conditions.However,the lack of favorable electro-catalysts has hampered its large-scale applications.Herein,we report the batch-scale synthesis of three-dimensional(3D)porous Cu@Cu2O microspheres(Cu@Cu2O MSs)composed of fine Cu@Cu2O nano-particles(NPs)using a convenient electric explosion method with outstanding activity and stability for the electrochemical reduction of nitrate to ammonia.Density functional theory(DFT)calculations revealed that the Cu2O(111)facets could facilitate the formation of *NO3H and *NO2H intermediates and suppress the hydrogen evolution reaction(HER),resulting in high selectivity for the NITRR.Moreover,the 3D porous structure of Cu@Cu2O MSs facilitates electrolyte penetration and increases the localized concentration of reactive species for the NITRR As expected,the obtained Cu@Cu2O MSs exhibited an ultrahigh NH3 production rate of 327.6 mmol·h~(-1)·g~(-1)_(cat)(which is superior to that of the Haber-Bosch process with a typical NH3 yield<200 mmol·h~(-1)·g~(-1)_(cat),a maximum Faradaic efficiency of 80.57%,and remarkable stability for the NITRR under ambient conditions.Quantitative ~(15)N isotope labeling experiments indicated that the synthesized ammonia originated from the electrochemical reduction of nitrate.Achieving the batch-scale and low-cost production of high-performance Cu@Cu2O MSs electrocatalysts using the electric explosion method is promising for the large-scale realization of selective electrochemical reduction of nitrate toward artificial ammonia synthesis.

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《Environmental Science & Technology: ES&T》 |2022年第14期|10299-10307|共9页
作者
Minghang Jiang; Qiang Zhu; Xinmei Song;
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作者单位

MOE Key Laboratory of Mesoscopic Chemistry,MOE Key Laboratory of High Performance Polymer Materials and Technology,Jiangsu Key Laboratory of Advanced Organic Materials,School of Chemistry and Chemical Engineering Nanjing University,Nanjing Jiangsu 210023,;

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收录信息美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
原文格式 PDF
正文语种英语
中图分类环境科学、安全科学;
关键词
electrochemical ammonia synthesis; electric explosion method; mass production; 3D porous Cu@Cu2O microspheres; nanoparticle agglomeration;

Batch-Scale Synthesis of Nanoparticle-Agminated Three-Dimensional Porous Cu@Cu2O Microspheres for Highly Selective Electrocatalysis of Nitrate to Ammonia

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