五重孪晶铜纳米线@聚吡咯制备及其电催化硝酸盐还原制氨  

Preparation of five-fold twinned copper nanowires@polypyrrole and their electrocatalytic conversion of nitrate to ammonia

作　　者：严孝清 赵瑛 张宇哲 欧鸿辉 黄起中 胡华贵 杨贵东 YAN Xiaoqing;ZHAO Ying;ZHANG Yuzhe;OU Honghui;HUANG Qizhong;HU Huagui;YANG Guidong(School of Chemical Engineering and Technology,Xi’an Jiaotong University,Xi’an 710049,Shaanxi,China;China Energy Yulin Chemical Company,Yulin 719000,Shaanxi,China)

机构地区：[1]西安交通大学化学工程与技术学院,陕西西安710049 [2]国能榆林化工有限公司,陕西榆林719000

出　　处：《化工学报》2024年第4期1519-1532,共14页CIESC Journal

基　　金：国家重点研发计划重点专项(2020YFA0710000);国家自然科学基金项目(22108214,U22A20391);中国博士后科学基金站前特助(2021TQ0262);陕西省重点研发计划项目(2024GX-YBXM-461);中央高校基本科研业务费专项资金(xzy012022068);陕西省高校科协青年人才托举计划项目(20210605)。

摘　　要：合理设计高活性、高选择性、高稳定性、低成本纳米结构催化剂是电催化硝酸根还原制氨的一个重大挑战。采用水热法耦合原位还原法制备了厚度可控的聚吡咯包裹五重孪晶铜纳米线催化剂,实现了低偏压下产氨活性、法拉第效率的提高以及对抗腐蚀能力的大幅提升。偏压为-0.4 V(可逆氢电极)时T-CuNW-10样品合成氨活性达到13.83 mg·mg^(-1)·h^(-1),偏压-0.7 V(可逆氢电极)时达到23.24 mg·mg^(-1)·h^(-1);中间产物亚硝酸根与产物氨二者加和的法拉第效率(FE)接近100%;腐蚀电流降低至3.14 mA·cm^(-2)。最终实现催化剂高效稳定硝酸根还原制氨性能的提升,可为开发设计工业应用催化剂提供思路参考。Reasonable design of nanostructured catalysts with high activity,selectivity,stability,and low cost is a significant challenge for achieving efficient electrocatalytic reduction of nitrate to ammonia.In this study,we successfully prepared a five-fold twinned copper nanowires@polypyrrole(T-CuNW@ppy)by hydrothermal coupled in-situ reduction method,which achieved ammonia production activity under low bias voltage,improved Faradaic efficiency,and significantly improved corrosion resistance.At a bias of-0.4 V(vs RHE),the T-CuNW-10 exhibited an impressive ammonia synthesis activity of 13.83 mg·mg^(-1)·h^(-1);while at a bias of-0.7 V(vs RHE)it reached 23.24 mg·mg^(-1)·h^(-1).Furthermore,the Faradaic efficiency of NO-2 and NH3 is a close to 100%.Additionally,the corrosion current is reduced to 3.14 mA·cm^(-2).Overall,our findings demonstrate that this catalyst not only exhibits high efficiency and stability in nitrate reduction performance but also provides valuable insights for the development and design of industrial application-oriented catalysts.

关 键 词：聚吡咯 五重孪晶铜 纳米材料 硝酸根 电化学合成氨 催化剂 

分 类 号：TQ131.2[化学工程—无机化工] TQ441