摘要
现代工业中,氨是主要的化工原料与农业化肥。工业上传统的Haber-Bosch法产氨工艺占主导地位,但其需要高温(400~500℃)来加速反应动力学,需要高压(10~30 MPa)来有利地改变反应平衡,同时还存在高碳排放的弊端。电催化氮还原反应(eNRR)是替代Haber-Bosch法的潜在途径,具有反应条件温和、环境友好等优势,但开发高性能的eNRR催化剂仍是挑战。本文通过电沉积法在三维铜泡沫基底上制备铜基催化剂,经退火处理后获得CoCu氧化物纳米阵列。利用X射线衍射(XRD)、扫描电子显微镜(SEM)、X射线光电子能谱(XPS)等技术表征了其结构和表面组成,结果表明纳米阵列表面为CuO/Co_(3)O_(4),衬底为金属Cu。该材料对eNRR具有良好的催化性能,在-0.3 V电位下氨产率达26.6μg·h^(-1)·cm^(-2) cat.,法拉第效率为4.99%。本研究为设计高性能eNRR催化剂提供了新策略。
In modern industry,ammonia is the main chemical raw material and agricultural fertilizer.the traditional Haber-Bosch ammonia production process is still dominant,but it requires high temperature(400-500℃)to accelerate the reaction kinetics,high pressure(10-30 Mpa)to change the equilibrium favorably,and has the disadvantages of high carbon emissions.Electrocatalytic nitrogen reduction reaction(eNRR)is a potential alternative to the Haber-Bosch method,which has the advantages of mild reaction conditions and environmental friendliness,but the development of high-performance eNRR catalysts is still a challenge.In this study,copper-based catalysts were prepared on three-dimensional copper foam substrates via electrodeposition,followed by annealing treatment to obtain CoCu oxide nanoarrays.The structure and surface composition were characterized using X-ray diffraction(XRD),scanning electron microscopy(SEM),and X-ray photoelectron spectroscopy(XPS).The results reveal that the nanoarray surface consists of CuO/Co_(3)O_(4) while the substrate remains metallic Cu.This material exhibits excellent catalytic performance for eNRR,achieving an ammonia yield rate of 26.6μg·h^(-1)·cm^(-2) cat.and a Faradaic efficiency of 4.99%at a potential of-0.3 V.This work offers a novel strategy for designing high-performance eNRR catalysts.
作者
聂锁府
姚辉超
王秀林
隋依言
伍思达
李杨宇
任森
熊艳
葛性波
NIE Suo-fu;YAO Hui-chao;WANG Xiu-ling;SUI Yi-yan;WU Si-da;LI Yang-yu;REN Sen;Xiong Yan;GE Xing-bo(CNOOC Key Laboratory of Liquefied Natural Gas and Low-Carbon Technology,Beijing 100028,China;CNOOC Gaa&Ponwcr Group,Rcacarch&Dcvclopmcnt Ccnter,Becijing 100028,China;College of Chemistry and Chemical Engineering,Southwest Petroleum University,Chengdu 610500,China)
出处
《化学研究与应用》
北大核心
2026年第2期390-397,共8页
Chemical Research and Application
基金
中国海洋石油集团有限公司液化天然气及低碳技术重点实验室开放基金项目(QDKJQZ-2024-65)资助。
关键词
电催化氮还原反应
非贵金属催化剂
CoCu
纳米阵列
电沉积
electrocatalytic nitrogen reduction reactions
non-precious metal catalysts
CoCu
nanoarrays
electrodeposition
