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高活性异质CuS/Mo_(6)S_(8)的构筑及其电催化硝酸根合成氨

Design and construction of heterostructured CuS/Mo_(6)S_(8) with rich active sites and its electrochemical reduction of nitrate for ammonia production
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摘要 电化学还原硝酸根合成氨(NO_(3)^(-)RR)不仅有助于水中硝态氮污染物的去除,而且有助于缓解社会对氨能源的需求,减少污染,降低能耗。催化剂在一定程度上决定了NO_(3)^(-)RR的性能,然而,已报道的NO_(3)^(-)RR催化剂大多存在氨产率低和稳定性差等问题,设计和制备高性能和稳定性的NO_(3)^(-)RR催化剂是该领域的一个关键。论文设计和构筑了CuS/Mo_(6)S_(8)异质结构电催化剂,系统研究了其物化特性和NO_(3)^(-)RR性能,探讨了相关构效关系。实验结果表明,CuS/Mo_(6)S_(8)的法拉第效率和NO_(3)^(-)转化率分别为92.12%和91.34%,优于CuS(81.11%和74.13%)和Mo_(6)S_(8)(84.27%和80.23%),且经过连续4个循环(共12 h)NO_(3)^(-)RR测试,CuS/Mo_(6)S_(8)的各项性能均无明显衰减,展现出了优异的稳定性。分析和对比发现,该异质催化剂具有强的界面作用,通过Cu和Mo之间的电子转移改变了CuS/Mo_(6)S_(8)的电子结构,进而提升了NO_(3)^(-)RR性能。该研究提供了一种高性能和稳定性的NO_(3)^(-)RR催化剂,也可借鉴到设计其他高效异质催化剂。 Electrochemical reduction of nitrate synthesis ammonia(NO_(3)^(-)RR)not only contributes to the removal of nitrate nitrogen pollutants in water,but also helps to alleviate the social demand for ammonia energy,reduce pollution and energy consumption.Catalysts determine the performance of NO_(3)^(-)RR to some extent.However,most reported NO_(3)^(-)RR catalysts have low ammonia yield and poor stability,so the preparation of high performance and stable NO_(3)^(-)RR catalysts becomes important in this field.CuS/Mo_(6)S_(8) heterogeneous electrocatalysts were prepared.The physicochemical properties and NO_(3)^(-)RR properties of CuS/Mo_(6)S_(8) heterogeneous electrocatalysts were system-atically studied,and the related structure-activity relationships were discussed.The experimental results show that the Faraday efficiency and NO_(3)^(-)conversion rate of CuS/Mo_(6)S_(8) were 92.12%and 91.34%,respectively,better than CuS(81.11%and 74.13%)and Mo_(6)S_(8)(84.27%and 80.23%),and that after four consecutive cycles(12 hours in total)of NO_(3)^(-)RR test,CuS/Mo_(6)S_(8) showed excellent stability with no obvious attenuation of various properties.The heterogeneous catalyst had a strong interfacial effect,which changed the electronic structure of CuS/Mo_(6)S_(8) through electron transfer between Cu and Mo,and thus improved NO_(3)^(-)RR performance.This study provides a high performance and stable NO_(3)^(-)RR catalyst,which can also be used for reference in the design of other highly efficient heterogeneous catalysts.
作者 谭子轩 杜沣 佟梦棋 郭春显 TAN Zixuan;DU Feng;TONG Mengqi;GUO Chunxian(School of Physical Science and Technology,SUST,Suzhou 215009,China;School of Materials Science and Engineering,SUST,Suzhou 215009,China)
出处 《苏州科技大学学报(自然科学版)》 CAS 2024年第1期36-42,60,共8页 Journal of Suzhou University of Science and Technology(Natural Science Edition)
基金 国家自然科学基金项目(21972102,22202144)。
关键词 电化学还原硝酸根合成氨 CuS/Mo_(6)S_(8)异质结构 界面作用 活性位点 催化效率 electrochemical reduction nitrate synthesis ammonia CuS/Mo_(6)S_(8) heterostructure interfacial action active site catalytic efficiency
作者简介 谭子轩(1998-),男,江苏宿迁人,硕士研究生,研究方向:凝聚态物理,E-mail:2011181002@post.usts.edu.cn;通信作者:郭春显(1983-),男,博士,教授,硕士生导师,E-mail:cxguo@usts.edu.cn。
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