摘要
一氧化氮电还原反应将工业废气转化为有价值的氨,表现出极具潜力的应用前景.在本工作中,我们合成了具有高比表面积和丰富缺陷的氧化铜纳米片催化剂,在流动池中氨法拉第效率达到92.1%,在-0.2 V vs.RHE时,一氧化氮电还原电流密度和氨的生产速率分别达到1.1 A cm^(-2)和7356μmol cm^(-2)h^(-1).在电流密度超过400 m A cm-2时,氨法拉第效率在50小时保持在80%以上.准原位X射线光电子能谱和原位X射线吸收光谱结果表明氧化铜纳米片在一氧化氮电还原过程中被电化学还原成单质铜.与铜纳米颗粒相比,氧化铜纳米片展现出较高的电化学表面积和一氧化氮电还原的内在活性.
The removal of nitric oxide(NO)is deemed essential due to its environmental detrimental effects,and electrocatalytic NO reduction reaction(NORR)for ammonia synthesis presents a sustainable approach.In this work,we synthesized copper oxide(CuO)nanosheet catalyst with a high specific surface area and abundant defects.This catalyst ex-hibited a remarkable 92.1%ammonia Faradaic efficiency(FE)in a flow cell,accompanied by a current density of 1.1 A cm^(-2) and an ammonia production rate of 7356μmol cm^(-2) h^(-1) at-0.26 V vs.reversible hydrogen electrode.The FE of ammonia remained above 80%during stability test for 50 h at a current density of more than 400 mA cm^(-2).Quasi in situ X-ray pho-toelectron spectroscopy and in situ X-ray absorption spec-troscopy revealed that the CuO nanosheets were electrochemically reduced to monomeric copper during NORR.Compared with Cu nanoparticles,the CuO nanosheets showed a high electrochemical surface area and high intrinsic activity for NORR.
作者
邵加奇
魏鹏飞
王硕
宋延鹏
付云凡
李荣坦
张小敏
汪国雄
包信和
Jiaqi Shao;Pengfei Wei;Shuo Wang;Yanpeng Song;Yunfan Fu;Rongtan Li;Xiaomin Zhang;Guoxiong Wang;Xinhe Bao(State Key Laboratory of Catalysis,Dalian National Laboratory for Clean Energy,iChEM(Collaborative Innovation Center of Chemistry for Energy Materials),Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian 116023,China;University of Chinese Academy of Sciences,Beijing 100049,China)
基金
supported by the National Key R&D Program of China (2023YFA1508002)
the National Natural Science Foundation of China (22125205 and 92015302)
the Fundamental Research Funds for the Central Universities (20720220008)
Dalian National Laboratory for Clean Energy (DNL201923)
the Photon Science Center for Carbon Neutrality。
