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Selective Photothermal Reduction of CO2 to CO over Ni-Nanoparticle/N-Doped CeO2 Nanocomposite Catalysts
ACS Applied Nano Materials ( IF 5.9 ) Pub Date : 2021-09-23 , DOI: 10.1021/acsanm.1c01991
Zewei Jia 1, 2 , Shangbo Ning 1, 2 , Yuxin Tong 1, 2 , Xin Chen 1, 2 , Huilin Hu 1, 2 , Lequan Liu 1, 2 , Jinhua Ye 1, 2, 3 , Defa Wang 1, 2
Affiliation  

Photothermal reverse water gas shift reaction is one of the promising methods to palliate global energy and environmental issues. Searching for catalysts with high activity and CO selectivity for CO2 conversion has been attracting extensive attention. In this work, Ni nanoparticle-loaded N-doped CeO2 (Ni/N-CeO2) composite catalysts were synthesized using a three-step method. Under light irradiation, the optimal Ni/N5.0-CeO2 exhibited a CO yield rate of 20.9 mmol·gcat–1·h–1 with almost 100% of CO selectivity via photothermal CO2 reduction. As a comparison, Ni/CeO2, without nitrogen doping, showed a high CH4 selectivity. The strong light absorption of Ni/N5.0-CeO2 mainly by loading of Ni nanoparticles and the enhanced adsorption/activation of CO2 molecules due to increased oxygen vacancies in N5.0-CeO2 by N-doping were supposed to account for the excellent catalytic performances. The doping of nitrogen was of particular importance for the formation of N–H bonds, which could modulate the reaction pathway for promoting the reduction of CO2 toward CO while suppressing the undesirable CO2 methanation process.

中文翻译:

在 Ni 纳米颗粒/N 掺杂 CeO2 纳米复合催化剂上选择性光热还原 CO2 为 CO

光热逆水煤气变换反应是缓解全球能源和环境问题的一种很有前景的方法。寻找具有高活性和CO选择性的CO 2转化催化剂已引起广泛关注。在这项工作中,使用三步法合成了负载Ni 纳米颗粒的N 掺杂CeO 2 (Ni/N-CeO 2 ) 复合催化剂。在光照射下,最佳的Ni/N 5.0 -CeO 2表现出20.9 mmol·g cat –1 ·h –1的CO 产率,通过光热CO 2还原几乎100%的CO 选择性。作为比较,Ni/CeO 2在没有氮掺杂的情况下,显示出高 CH 4选择性。Ni/N 5.0 -CeO 2 的强光吸收主要是由于 Ni 纳米颗粒的负载以及N 掺杂导致 N 5.0 -CeO 2 中氧空位增加导致CO 2分子的吸附/活化增强催化性能。氮的掺杂对于 N-H 键的形成特别重要,它可以调节反应途径,促进 CO 2还原为 CO ,同时抑制不需要的 CO 2甲烷化过程。
更新日期:2021-10-22
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