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 CO2 Electroreduction in Wide Potential Windows
邵碧珠 1董慧君 1龚云南 1梅剑华 1蔡锋石 1刘金彪 2钟地长 1鲁统部1
作者信息
- 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
- 折叠
摘要
电催化二氧化碳(CO2)还原被认为是将CO2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CO2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CO2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CO2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CO2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CO2电还原催化剂的方法.
Abstract
The electrocatalytic carbon dioxide(CO2)reduction has gained recognition as an outstanding approach for transforming CO2 into renewable energy products.To accomplish this reduction reaction,the development of efficient electrocatalysts is required.Nickel-based electrocatalysts have been extensively investigated for CO2 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 CO2 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 CO2 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Key words
Nickel nanoparticle/Electrocatalyst/CO2 reduction/Metal-organic framework/Thermal treatment引用本文复制引用
基金项目
国家重点研发计划(2022YFA1502902)
国家自然科学基金(22271218)
国家自然科学基金(22071182)
国家自然科学基金(22001043)
国家自然科学基金(21931007)
天津市自然科学基金(20JCYBJC00380)
出版年
2024
国家科技期刊平台
NSTL
万方数据