Crystal-Plane Effects of CeO2{110} and CeO2{100} on Photocatalytic CO2 Reduction: Synergistic Interactions of Oxygen Defects and Hydroxyl Groups,ACS Sustainable Chemistry & Engineering

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Crystal-Plane Effects of CeO2{110} and CeO2{100} on Photocatalytic CO2 Reduction: Synergistic Interactions of Oxygen Defects and Hydroxyl Groups
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2020-08-31 , DOI: 10.1021/acssuschemeng.0c04205
Chengzhang Zhu ₁ , Xiaoqian Wei _{2,

3} , Wanqin Li ₁ , Yu Pu _{2,

3} , Jingfang Sun _{2,

3} , Kunlin Tang ₁ , Haiqin Wan _{1,

3} , Chengyan Ge _{2,

4} , Weixin Zou _{1,

2,

3} , Lin Dong _{1,

2,

3}

Affiliation

For photocatalytic CO₂ reduction, the synergistic effect of Lewis acidity and basicity on CO₂ activation is worthy of study. On the basis of a large number of oxygen defects (Lewis acidity) and hydroxyl groups (Lewis basicity) on the CeO₂ surface, CeO₂{110} and CeO₂{100} crystal planes were developed to investigate the synergistic effect on photocatalytic CO₂ reduction. Compared with CeO₂{100}, the surface oxygen defects were prone to generate on CeO₂{110}, leading to available visible light absorption and faster photogenerated charge transfer. The experimental results and DFT calculations showed that the OH species on the CeO₂{110} surface were richer and provided more electron density, i.e., Lewis basicity. Furthermore, the possible adsorption intermediate was investigated and suggested that CeO₂{110} was more beneficial for the adsorption and activation of CO₂ reactant than CeO₂{100}, resulting in generation of carboxylate species and •CO₂^– radicals, instead of carbonate. Under the control of surface Lewis acidity and basicity, CeO₂{110} had superior photocatalytic performance of CO₂ reduction than the {100} plane.

中文翻译：

CeO ₂ {110}和CeO ₂ {100}的晶面效应对光催化CO ₂还原的影响：氧缺陷和羟基的协同相互作用

对于光催化还原CO ₂，路易斯酸度和碱性对CO ₂活化的协同作用值得研究。基于CeO ₂表面的大量氧缺陷（刘易斯酸度）和羟基（刘易斯碱度），开发了CeO ₂ {110}和CeO ₂ {100}晶面以研究其对光催化CO的协同作用。₂减少。利用CeO相比₂ {100}，该表面的氧缺陷是容易产生对CEO ₂ {110}，导致可用的可见光吸收和更快的光生电荷转移。实验结果和DFT计算表明CeO上的OH种类₂ {110}表面更丰富，并提供更多的电子密度，即路易斯碱性。此外，可能的吸附中间进行了研究，并建议的CeO ₂ {110}是对于CO的吸附和活化更有益₂反应物比的CeO ₂ {100}，导致产生羧酸酯物种和•CO的₂^-基团，而不是碳酸盐。在表面路易斯酸度和碱度的控制下，CeO ₂ {110}具有比{100}面更好的CO ₂还原光催化性能。

更新日期：2020-09-28

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