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表面Ru-H双复合物-接种TiO₂纳米混合物用于高效的光催化CO₂甲化

Pu Zhang¹, Xiaoyu Sui¹, Ying Wang¹

¹State Key Lab of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou 350116, P. R. China.

Journal of the American Chemical Society

|March 2, 2023

概括

新型二氧化 (TiO2) 纳米混合物与化 (Ru-H) 二氧化复合物有效地使用可见光将二氧化碳 (CO2) 转化为甲 (CH4). 这种关键的光催化过程的选择性和活性显著提升.

科学领域:

材料科学
催化剂
摄影化学

背景情况:

开发高效的二氧化碳 (CO2) 转化光催化剂对于可持续的能源解决方案至关重要.
二氧化 (TiO2) 是一个广泛研究的光催化剂,但其在二氧化碳甲化中的效率需要改进.
用有机金属复合物的TiO2表面修饰提供了增强光催化活性的有希望的途径.

研究的目的:

合成新的Ru-H双复合体-移植的TiO2纳米混合物用于光催化CO2转化.
研究合成后配体交换对光催化剂的选择性和活性的影响.
在开发的纳米混合物上阐明二氧化碳甲化机制.

主要方法:

通过表面有机金属化学制备TiO2纳米混合物.
使用4,4'-二甲基-2'-二氨酸 (4,4'-bpy) 的合成后连接物交换.
在可见光照射下使用H2作为减光剂的光催化CO2转化为CH4.
使用秒瞬态红外吸收光谱和光谱分析进行表征.

主要成果:

在连接物交换后,对CH4的选择性达到93.4%.
与未交换的催化剂相比,增强了CO2甲化活性的4.4倍.
获得了241.2μL·g-1·h-1的高CH4生产率.
从Ru复合体向TiO2进行快速热电子注入,形成电荷分离状态,寿命为50.0n.
确定了表面氧气空缺的二氧化碳−基的形成作为关键步骤.

结论:

新型Ru-H双复合体移植的TiO2纳米混合体是有效的二氧化碳转化为CH4的光催化剂.
连接物交换是优化选择性和活动的关键策略.
该机制涉及向TiO2和CO2基形成的电子注入,然后插入Ru-H键.

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