铜掺杂氮化碳电催化硝酸盐产氨性能研究  

Study on Performance of Copper Doped Carbon Nitride Electrocatalyzing Nitrate to Produce Ammonia

作　　者：韩晶 廖润华 邓文强 梁博宇 周雨晴 任帅 洪燕 Jing Han;Runhua Liao;Wenqiang Deng;Boyu Liang;Yuqing Zhou;Shuai Ren;Yan Hong(School of Materials Science and Engineering,Jingdezhen Ceramic University,Jingdezhen 333403,Jiangxi,China)

机构地区：[1]景德镇陶瓷大学材料科学与工程学院,景德镇333403

出　　处：《化学学报》2024年第3期295-302,共8页Acta Chimica Sinica

基　　金：景德镇市级科技计划项目(Nos.20234NY006,20234SF009);景德镇陶瓷大学研究生创新创业项目(No.JYC202312);大学本科生创新项目(Nos.X202310408145,X202310408140)资助。

摘　　要：NH_(3)是硝酸盐还原产物之一,不仅在工业中需要大量应用,在清洁生产过程中也是一种非常有前途的能源载体,现有的哈伯-博施(Haber-Bosch)工艺生产NH_(3)会对大气环境造成危害,而电催化法由于便捷、安全且能够在常温和常压下催化合成NH_(3)成为最近研究的热点.本实验以3-氨基-1,2,4三唑为前驱体,利用热解法先合成C_(3)N_(5),再通过调控铜元素的比例在煅烧条件下合成Cu-C_(3)N_(5),合成一系列材料形貌、晶体构相、化学价态存在差异的C_3N_5基催化剂,并评价这些催化剂的电化学性能以及电催化硝酸盐还原产氨性能,通过在0.1 mol/L KOH+0.1 mol/L KNO_(3)混合电解液中进行1h电解实验后发现,氨气产量和法拉第效率可以达到0.541 mmol·h^(-1)·mg_(cat)^(-1)87.79%,远远高于C_3N_5,且该催化剂在循环试验和长时间实验中具有良好的活性和稳定性,表明在电催化硝酸盐领域中具有一定的研究价值.As the increasing demand for ammonia in other industries such as energy, the ammonia production now available can no longer meet the needs of industrial production, and the existing Haber-Bosch process for the production of NH_(3) will cause harm to the atmospheric environment. Therefore, there is an urgent need to find a new method that is compatible with or can replace the existing ammonia production process. Nitrate wastewater contains a large amount of nitrogen, and NH_(3) is one of the nitrate reduction products, the reduction of nitrate into ammonia can not only reduce the environmental pollution of nitrate nitrogen, but also alleviate the industrial demand for ammonia, nitrate wastewater treatment methods are generally physical, chemical and biological, but there are shortcomings of long cycle time and high cost. The electrocatalytic method is convenient, safe and can catalyze the synthesis of NH_(3) at room temperature and pressure, which makes the electrocatalytic synthesis of NH_(3) become a hot research topic in recent years. In this experiment, 3-amino-1,2,4-triazole was loaded into alumina crucible and used as the precursor to synthesize C_(3)N_(5) by pyrolysis method in Muffle furnace, and then Cu-C_(3)N_(5) was synthesized under calcination conditions by modulating the ratio of copper elements, which resulted in a series of C_(3)N_(5)-based catalysts with differences in material morphology, crystal conformation, and chemical valence state, including five catalysts of different proportions were synthesized. These catalysts were tested, then their electrochemical performance and electrocatalytic reduction of nitrate to produce ammonia performance were evaluated, and it was found that the ammonia yield and Faraday efficiency could reach 0.541 mmol•h^(−1)•mgcat^(−1) and 87.79% by 1 h electrolysis experiments in a mixed electrolyte solution of 0.1 mol/L KOH+0.1 mol/L KNO_(3), which are much higher than that of C_(3)N_(5),and the catalyst has good activity and stability in cyclic and long time ex

关 键 词：电催化还原 氨产率 法拉第效率 C_3N_5基催化剂 硝酸盐 

分 类 号：TQ113.2[化学工程—无机化工] O643.36[理学—物理化学]