烷基硫醇修饰纳米多孔电催化剂及其合成氨性能研究  

Alkyl mercaptan modified nanoporous electrocatalyst and its performance in ammonia synthesis

作　　者：顾先涛 刘怡瑢 陈晓春 郭兴旺 周仲康 计巧珍 吴妍 高宇祥 张更 朱胜利[5] GU Xiantao;LIU Yirong;CHEN Xiaochun;GUO Xingwang;ZHOU Zhongkang;JI Qiaozhen;WU Yan;GAO Yuxiang;ZHANG Geng;ZHU Shengli(State Grid Anhui Electric Power Co.,Ltd.Electric Power Research Institute,Hefei 230601,China;School of Materials Science and Engineering,Lanzhou Jiaotong University,Lanzhou 730070,China;Anhui Xinli Electric Power Technology Consulting Co.,Ltd.,Hefei 230601,China;State Grid Anhui Extra High Voltage Company,Hefei 230000,China;School of Materials Science and Engineering,Tianjin University,Tianjin 300350,China)

机构地区：[1]国网安徽省电力有限公司电力科学研究院,合肥230601 [2]兰州交通大学材料科学与工程学院,兰州730070 [3]安徽新力电业科技咨询有限责任公司,合肥230601 [4]国网安徽省电力有限公司超高压分公司,合肥230022 [5]天津大学材料科学与工程学院,天津300350

出　　处：《功能材料》2025年第1期1139-1146,共8页Journal of Functional Materials

基　　金：国网安徽省电力有限公司科技项目(B31205230008)。

摘　　要：电催化氮还原(electrocatalytic nitrogen reduction reaction,ENRR)合成氨作为一种新兴的人工固氮工艺,具有反应条件温和、可再生能源适配性强等特点。但电催化氮还原反应电位与析氢反应(hydrogen evolution reaction,HER)电位接近,造成氮还原反应选择性降低。通过正十八-烷基硫醇对纳米多孔FeNbMoP电催化剂进行疏水修饰,增加氮气分子与催化剂表面活性位点的接触,抑制析氢反应,提高氨产率及法拉第效率。修饰后的ENRR催化剂合成氨产率为15.45μg/(h·cm^(2)),法拉第效率为6.28%,性能较未修饰的FeNbMoP催化剂提升明显。该方法有望为氮还原催化剂的理性设计提供新的思路。Electrocatalytic nitrogen reduction reaction(ENRR)has been regarded as an emerging artificial nitrogen fixation process,due to the mild reaction conditions and strong adaptability to renewable energy.However,the applied potential of the ENRR is close to that of the hydrogen evolution reaction(HER),resulting in a decrease in the selectivity of the nitrogen reduction reaction.In this paper,the hydrophobic modification of the nanoporous FeNbMoP electrocatalyst was carried out by coating n-octadecyl mercaptan,which inhibits the HER,increases the contact between nitrogen molecules and the active site on the catalyst,thereby the ammonia yield and Faraday efficiency is improved.The ammonia yield of the modified ENRR catalyst is 15.45μg/(h·cm^(2))with the Faraday efficiency of 6.28%,which shows a significant improvement in performance compared with the unmodified FeNbMoP catalyst.This method may provide a new insight for the rational design of nitrogen reduction catalysts.

关 键 词：电催化氮还原 正十八-烷基硫醇 表面改性 纳米多孔材料 

分 类 号：TQ225.2[化学工程—有机化工]