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The activity enhancement of photocatalytic water splitting by F- pre-occupation on Pt(100) and Pt(111) co-catalyst facets
Wang, M(王萌)1,2,3; Liu, HX(刘红霞)1,2,3; Ma, JT(马建泰)3; Lu, Gongxuan1
2020
Source PublicationAPPLIED CATALYSIS B-ENVIRONMENTAL   Impact Factor & Quartile
ISSN0926-3373
EISSN1873-3883
Volume266
page numbers12
AbstractThe 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.
© 2020 Elsevier B.V.
KeywordTuning the adsorption sites Pt facets Fluorine ions occupation Overall water splitting
PublisherELSEVIER
DOI10.1016/j.apcatb.2020.118647
Indexed BySCIE ; EI
Language英语
Funding ProjectNational Basic Research Program of China (973 Program)[] ; National Natural Science Foundation of China[] ; National Basic Research Program of China (973 Program)[2018YFB1502000] ; National Natural Science Foundation of China[21433007]
WOS Research AreaChemistry ; Engineering
WOS SubjectChemistry, Physical ; Engineering, Environmental ; Engineering, Chemical
WOS IDWOS:000517665200029
PublisherElsevier B.V.
EI Accession Number20200408070273
EI KeywordsCatalysts ; Chemical bonds ; Cyclic voltammetry ; Density functional theory ; Electronegativity ; Employment ; Fluorine ; Hydrogen ; Ions ; Molecules ; Oxygen ; Photocatalytic activity ; Tuning
EI Classification NumberPhysical Chemistry:801.4 ; Electrochemistry:801.4.1 ; Chemical Operations:802.3 ; Chemical Products Generally:804 ; Atomic and Molecular Physics:931.3
Original Document TypeJournal article (JA)
Citation statistics
Cited Times:27[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttps://ir.lzu.edu.cn/handle/262010/417171
Collection生命科学学院
化学化工学院
管理学院
Corresponding AuthorLu, Gongxuan
Affiliation
1.State Key Laboratory for Oxo Synthesis and Selective Oxidation, Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences, Lanzhou; 730000, China
2.University of Chinese Academy of Sciences, Beijing; 100049, China
3.College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou; 730000, China
First Author AffilicationCollege of Chemistry and Chemical Engineering
Recommended Citation
GB/T 7714
Wang, Meng,Liu, Hongxia,Ma, Jiantai,et al. The activity enhancement of photocatalytic water splitting by F- pre-occupation on Pt(100) and Pt(111) co-catalyst facets[J]. APPLIED CATALYSIS B-ENVIRONMENTAL,2020,266.
APA Wang, Meng,Liu, Hongxia,Ma, Jiantai,&Lu, Gongxuan.(2020).The activity enhancement of photocatalytic water splitting by F- pre-occupation on Pt(100) and Pt(111) co-catalyst facets.APPLIED CATALYSIS B-ENVIRONMENTAL,266.
MLA Wang, Meng,et al."The activity enhancement of photocatalytic water splitting by F- pre-occupation on Pt(100) and Pt(111) co-catalyst facets".APPLIED CATALYSIS B-ENVIRONMENTAL 266(2020).
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