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Experimental and theoretical insights into an enhanced CO2 methanation mechanism over a Ru-based catalyst
Applied Catalysis B: Environment and Energy ( IF 20.2 ) Pub Date : 2022-08-28 , DOI: 10.1016/j.apcatb.2022.121903
Yangyang Li , Zhisong Liu , Zhiqiang Rao , Feng Yu , Wentao Bao , Ying Tang , Huanhuan Zhao , Jie Zhang , Zijun Wang , Jiangbing Li , Zeai Huang , Ying Zhou , Yongsheng Li , Bin Dai

Converting excessive CO2 emissions from industrial operation into methane (CH4) is critical for the remediation of global warming. However, this reaction requires a high temperature to overcome the high thermodynamic stability of CO2. The development of efficient catalysts for the CO2 methanation reaction at low temperature remains challenging. Here we report that when a TiO2 photothermal catalyst is loaded with Ru nanoparticles, the CO2 to CH4 conversion efficiency is markedly enhanced under light illumination. In fact, the CO2 performance was enhanced fourfold and twofold from those of the traditional thermal catalytic reaction at 200 °C and 250 °C, respectively. In-situ DRIFTS analysis revealed that light irradiation accelerates the transition of bicarbonate to formates via light-induced charge carriers. Moreover, theoretical calculations revealed that photo-induced electron transfer effectively promotes H2 dissociation and CO2 activation on the Ru atoms. This work provides new theoretical insights into CO2 activation and methanation under light illumination.



中文翻译:

对基于钌催化剂的增强 CO2 甲烷化机理的实验和理论见解

将工业运营产生的过量 CO 2排放转化为甲烷 (CH 4 ) 对于全球变暖的治理至关重要。然而,该反应需要高温来克服CO 2的高热力学稳定性。开发用于低温CO 2甲烷化反应的高效催化剂仍然具有挑战性。在这里,我们报道了当负载有Ru纳米粒子的TiO 2光热催化剂时,CO 2到CH 4的转化效率在光照下显着提高。事实上,CO 2在 200 °C 和 250 °C 下,性能分别比传统的热催化反应提高了四倍和两倍。原位 DRIFTS 分析表明,光照射通过光诱导的电荷载流子加速了碳酸氢盐向甲酸盐的转变。此外,理论计算表明,光诱导电子转移有效地促进了Ru原子上的H 2解离和CO 2活化。这项工作为光照下的CO 2活化和甲烷化提供了新的理论见解。

更新日期:2022-08-30
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