金属有机框架衍生镍纳米颗粒在宽电位窗口内高效电催化二氧化碳还原  

Metal-Organic Framework-Derived Nickel Nanoparticles for Efficient CO_(2) Electroreduction in Wide Potential Windows

作　　者：邵碧珠 董慧君 龚云南 梅剑华 蔡锋石 刘金彪[2] 钟地长 鲁统部 Bizhu Shao;Huijun Dong;Yunnan Gong;Jianhua Mei;Fengshi Cai;Jinbiao Liu;Dichang Zhong(Tongbu Lu 11 Institute for New Energy Materials and Low Carbon Technologies,School of Materials Science and Engineering,Tianjin University of Technology,Tianjin 300384,China;School of Chemistry and Chemical Engineering,Tianjin University of Technology,Tianjin 300384,China)

机构地区：[1]天津理工大学新能源材料与低碳技术研究院,材料科学与工程学院,天津300384 [2]天津理工大学化学化工学院,天津300384

出　　处：《物理化学学报》2024年第4期193-198,共6页Acta Physico-Chimica Sinica

基　　金：国家重点研发计划(2022YFA1502902);国家自然科学基金(22271218,22071182,22001043,21931007);天津市自然科学基金(20JCYBJC00380)资助项目。

摘　　要：电催化二氧化碳(CO_(2))还原被认为是将CO_(2)转化为可再生能源产品的一种有前途的方法。开发性能优异的电催化剂高效完成这一重要反应是关键。镍基催化剂广泛应用于电催化CO_(2)还原研究,但是,镍纳米颗粒经常表现较差的催化性能。在本文中,通过在氮气气氛中高温热解镍基金属有机骨架(MOF)、尿素和炭黑混合物,获得了镍纳米颗粒负载于多孔碳氮中的催化材料(NiNPs-NC)。有趣的是,NiNPs-NC在H型和流动相电池中都表现出优异的CO_(2)电还原性能。在H型电解池和-0.67–-1.07 V vs.RHE(可逆氢电极)电位窗口内,NiNPs-NC催化CO_(2)还原为CO的法拉第效率大于90%,其中,在-0.87 V vs.RHE时,CO的法拉第效率约为100%。在流动相电解池和-0.50–-0.70 V vs.RHE电位窗口内,NiNPs-NC催化CO_(2)还原为CO的选择性大于95%。电化学阻抗谱图和塔菲尔斜率表征显示,NiNPs-NC的高催化活性归因于其在催化过程中的快速电荷转移。本文提供了一种制备高效CO_(2)电还原催化剂的方法。The electrocatalytic carbon dioxide(CO_(2))reduction has gained recognition as an outstanding approach for transforming CO_(2) into renewable energy products.To accomplish this reduction reaction,the development of efficient electrocatalysts is required.Nickel-based electrocatalysts have been extensively investigated for CO_(2) reduction;however,nickel nanoparticles(NiNPs)have demonstrated limited catalytic performance.In this study,NiNPs implanted in N-doped porous carbon(NiNPs-NC)were prepared by thermal treatment of nickel metal-organic framework,urea,and carbon black under an N2 atmosphere.The NiNPs-NC exhibited high catalytic performance for the electroreduction of CO_(2) to CO in both H-type and flow cells.In the H-type cell,the CO faradaic efficiencies(FEs)of NiNPs-NC exceeded 90%in the potential window from-0.67 to-1.07 V vs.reversible hydrogen electrode(RHE),reaching a maximum CO FE of approximately 100%at-0.87 V vs.RHE.In the flow cell,the CO selectivities of NiNPs-NC exceeded 95%in the potential window from-0.50 to-0.70 V vs.RHE.The fast charge transfer,as demonstrated by electrochemical impedance spectroscopy and Tafel slope,can be attributed to the high catalytic activity of NiNPs-NC.This study provides a simple method to develop highly efficient catalysts for electrocatalytic CO_(2) reduction.

关 键 词：镍纳米颗粒 电催化剂 二氧化碳还原 金属有机框架 热处理 

分 类 号：O643[理学—物理化学]