在现场重建可扩展的无形基金属有机框架,用于CO2电还原以形成超宽潜在窗口
Ziyun Liu1, Xinxin Han1, Junhui Liu2
1School of Resources & Environment, Nanchang University, Nanchang 330031, People's Republic of China.
ACS applied materials & interfaces
|May 22, 2024
概括
可扩展的无形金属有机框架 (aMOF) 使用自下而上的方法生产,以实现高效的二氧化碳电催化减排 (CO2RR). 由此产生的催化剂实现了高格式选择性,证明了可行的批量规模战略.
科学领域:
- 材料科学 材料科学 材料科学
- 电化学 电化学 电化学
- 催化剂是一种催化剂.
背景情况:
- 无形金属有机框架 (aMOFs) 为电催化提供导电性和缺陷.
- 传统的"自上而下的"合成方法涉及恶劣的条件,限制了aMOF的应用.
- 为aMOFs开发可扩展和易于合成的合成路径对于广泛采用至关重要.
研究的目的:
- 开发一种可扩展的"自下而上的"合成,用于无形的基于In的MOF.
- 为了研究合成的aMOF的电催化性能,以减少二氧化碳.
- 为了阐明二氧化碳电催化还原过程中的活性位点和反应机制.
主要方法:
- 简单的"自下而上"合成使用连接体竞争.
- 在现场和现场表征 (例如,XRD,XPS,TEM).
- 在流电池中测试电化学CO2降解反应 (CO2RR).
- 密度函数理论 (DFT) 的计算.
主要成果:
- 通过简单的"自下而上"方法实现了aMIL-68(In) -NH2的可扩展生产.
- 在CO2RR过程中,催化剂转化为In/In2O3-活性位点,保留的氨基基团有助于CO2吸附.
- 高格式法拉第效率 (>90%) 在广泛的潜能范围内实现,超过现有催化剂.
- DFT的计算表明,氧气空缺通过促进HCOO*中间体的形成来增强电催化活性.
- 16克的批量生产表现出一致的性能,突出了可扩展性.
结论:
- 为无形MOF合成建立了一个简单且可扩展的"自下而上的"战略.
- 合成的aMOF,aMIL-68(In) -NH2,在二氧化碳电催化降解以形成中表现出色.
- 该研究提供了对活性部位和机制的洞察,为高效的电解CO2转化铺平了道路.
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