在ZnZrO催化剂上的不对称位置,以促进CO2化中的形式形成和转化
Zhendong Feng1,2, Chizhou Tang1,2, Pengfei Zhang1
1State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China.
Journal of the American Chemical Society
|June 1, 2023
概括
甲酸盐是二氧化碳化成甲醇的关键中间体. 这项研究表明,ZnZr催化剂上的不对称Zn-O-Zr位点有助于酸盐的形成和转化,从而增强甲醇的产生.
科学领域:
- 催化剂
- 表面化学
- 材料科学
背景情况:
- 在二氧化碳化成甲醇中的甲酸盐的作用仍在争论中,对其反应途径的直接证据有限.
- 酸盐经常被观察到,但其作为甲醇合成的反应中间体的确切作用尚未确定.
研究的目的:
- 通过ZnZrO固体溶液催化剂对二氧化碳化过程中形成和转化形式的研究.
- 阐明反应机制,并确定负责甲醇生产的活性部位.
主要方法:
- 在现场/操作中扩散反射红外里叶变换光谱-质谱 (DRIFTS-MS) 实时反应监测.
- 密度函数理论 (DFT) 计算以了解反应途径和中间稳定.
- 使用具有定义不对称活性位点的ZnZrO固体溶液催化剂.
主要成果:
- 由二氧化碳吸附形成的二氧化碳酸在不对称的Zn-O-Zr位点上形成.
- Zn位点激活H2,而Zr位点稳定反应中间体,促进酸盐的形成和转化.
- 不对称的Zn-O-Zr位点对于酸盐生成及其随后的转化至关重要.
结论:
- 在甲醇形成中,ZnZrO催化剂的优异性能归因于不对称的Zn和Zr位点.
- 这些不对称的位点促进了H2的异质裂变,通过形式中间体促进了反应途径.
- 该研究提供了关于二氧化碳化成甲醇对ZnZrO催化剂的形式物质反应的确证据.
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