低碳化学与化工2025,Vol.50Issue(11):138-149,12.DOI:10.12434/j.issn.2097-2547.20250029
铜铝水滑石电催化还原硝酸盐合成氨性能研究
Performance study of ammonia synthesis via electrocatalytic nitrate reduction catalyzed by copper-aluminum layered double hydroxide
摘要
Abstract
Compared with the traditional ammonia synthesis process(Haber Bosch method),electrocatalytic nitrate reduction to ammonia offers advantages such as renewable energy input,mild reaction conditions and no secondary pollution.However,this reaction still faces challenges including insufficient catalytic activity,low product selectivity and poor stability.Copper-aluminum layered double hydroxides(CuxAl-LDH)with different ratios of Cu to Al(n(Cu)/n(Al)=x=1.5,2 or 3)were synthesized by hydrothermal method.Their structures were characterized,and their electrochemical performances were evaluated.The effects of Cu/Al ratio,initial NO-3-N mass concentration in the electrolyte,applied potential and illumination on the efficiency of electrocatalytic nitrate reduction to ammonia were systematically investigated.The results show that the Cu2Al-LDH electrode achieves a Faradaic efficiency of 98.2%and an ammonia yield of 822.3 μg/(h·cm2)at-0.6 V vs.RHE with an initial NO-3-N mass concentration of 500 mg/L.Upon light illumination,the Cu1.5Al-LDH electrode exhibits enhanced catalytic performance under the same conditions,achieving a theoretical Faradaic efficiency of 150.5%and an ammonia yield of 1149.1 μg/(h·cm2).Furthermore,both Cu2Al-LDH and Cu1.5Al-LDH electrodes display excellent stability under electrocatalytic and photo-assisted electrocatalytic conditions,respectively,maintaining high Faradaic efficiency after continuous operation for ten hours.These results indicate that copper-aluminum layered double hydroxides show promising performance for the electrocatalytic reduction of nitrate to ammonia and hold great potential for green ammonia synthesis.关键词
硝酸盐还原/合成氨/电催化储能/铜铝水滑石Key words
nitrate reduction/ammonia synthesis/electrocatalytic energy storage/copper-aluminum layered double hydroxide分类
化学工程引用本文复制引用
宇文晨,张泰境,吉欢欢..铜铝水滑石电催化还原硝酸盐合成氨性能研究[J].低碳化学与化工,2025,50(11):138-149,12.基金项目
河北农业大学引进人才科研专项(YJ201921). (YJ201921)