The activity enhancement of photocatalytic water splitting by F- preoccupation on Pt(100) and Pt(111) co-catalyst facets. | |
Department | 羰基合成与选择氧化国家重点实验室(OSSO) |
Meng Wang1,2,3; Hongxia Liu1,2,3; Jiantai Ma3; Gongxuan Lu1 | |
The second department | 环境催化与氢能 |
2020-06 | |
Source Publication | Applied Catalysis B: Environmental |
Issue | 266Pages:118647 |
Abstract | The reversible hydrogen and oxygen recombination reaction in semiconductor dispersion highly impede the yield increase of photocatalytic water splitting to hydrogen and oxygen. In order to inhibit such reverse reaction, it is necessary to reduce the degree of hydrogen and oxygen adsorption and activiation over co-catalyst on semiconductor. It is known that partial occupation of Pt sites by halogen ions with high electronegativity can decrease the adsorption and activation degree of hydrogen and oxygen molecules over Pt/TiO2, by this way, hydrogen and oxygen recombination reaction can be significantly inhibited, and the overall water splitting activity can be remarkably enhanced. Nevertheless, the detail inhibition mechanism on the reverse recombination reaction by halogen ions occupation on different Pt sites is still unclear. In the present work, by comparing the fluorine ions occupation on different Pt facets, we found that the fluorine ions occupation could decrease the numbers of adsorption sites on Pt(100) and Pt(111) surface. On Pt(100) facet, a fluorine ion occupation affect the four adjacent adsorption sites for H2 and O2 molecules adsorption, while, on Pt(111) surface, a fluorine ion occupation could affect the six adjacent adsorption sites for H2 and O2 molecules adsorption. The difference of fluorine ions occupation on the Pt(100) and Pt(111) facets led to the different adsorption strength of hydrogen and oxygen molecules, which further induced the activiation difference of hydrogen and oxygen on Pt co-catalyst. The results of density functional theory (DFT) calculation indicated that the hydrogen and oxygen adsorption energies on F/Pt(100) were higher than that on F/Pt(111) surface. The H2/O2-TPD, cyclic voltammetry and in-situ XPS experimental results also verified that the hydrogen and oxygen adsorption on F/Pt(100) surface was stronger than that of F/Pt(111) surface. The hydrogen and oxygen recombination experimental results showed that the hydrogen and oxygen recombination rates over F/Pt(100) surface was higher than that of F/Pt(111) surface. Upon light irradiation, the F/Pt(100)/TiO2 photocatalyst exhibited lower activity for overall water splitting than F/Pt(111)/TiO2 photocatalyst. Results in this paper provide a new avenue to promote seimiconductor catalyst for over-all water splitting by tuning the adsorption sites of hydrogen and oxygen on co-catalyst surface. |
Indexed By | SCI ; EI |
If | 16.683 |
Language | 英语 |
compositor | 第一作者单位 |
Document Type | 期刊论文 |
Identifier | http://ir.licp.cn/handle/362003/26592 |
Collection | 羰基合成与选择氧化国家重点实验室(OSSO) |
Corresponding Author | Gongxuan Lu |
Affiliation | 1.State Key Laboratory for Oxo Synthesis and Selective Oxidation, Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences, Lanzhou 730000, China 2.College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou 730000, China 3.University of Chinese Academy of Sciences, Beijing 100049, China |
Recommended Citation GB/T 7714 | Meng Wang,Hongxia Liu,Jiantai Ma,et al. The activity enhancement of photocatalytic water splitting by F- preoccupation on Pt(100) and Pt(111) co-catalyst facets.[J]. Applied Catalysis B: Environmental,2020(266):118647. |
APA | Meng Wang,Hongxia Liu,Jiantai Ma,&Gongxuan Lu.(2020).The activity enhancement of photocatalytic water splitting by F- preoccupation on Pt(100) and Pt(111) co-catalyst facets..Applied Catalysis B: Environmental(266),118647. |
MLA | Meng Wang,et al."The activity enhancement of photocatalytic water splitting by F- preoccupation on Pt(100) and Pt(111) co-catalyst facets.".Applied Catalysis B: Environmental .266(2020):118647. |
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2020, 266,118647 App(4920KB) | 期刊论文 | 作者接受稿 | 开放获取 | CC BY-NC-SA | View Application Full Text |
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