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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
8.4
)
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
- State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, Nanjing University, Nanjing 210023, PR China
- Key Laboratory of Mesoscopic Chemistry of MOE, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210023, PR China
- Jiangsu Key Laboratory of Vehicle Emissions Control, Center of Modern Analysis, Nanjing University, Nanjing 210093, PR China
- School of Chemistry and Chemical Engineering, Yancheng Institute of Technology, Yancheng 224051, PR China
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