DICP OpenIR
Role of Oxygen Vacancies on Oxygen Evolution Reaction Activity: beta-Ga2O3 as a Case Study
Liu, Taifeng1; Feng, Zhaochi2; Li, Qiuye1; Yang, Jianjun1; Li, Can2; Dupuis, Michel2,3
Corresponding AuthorLiu, Taifeng(tfliu@vip.henu.edu.cn) ; Dupuis, Michel(mdupuis2@buffalo.edu)
Source PublicationCHEMISTRY OF MATERIALS
2018-11-13
ISSN0897-4756
DOI10.1021/acs.chemmater.8b03015
Volume30Issue:21Pages:7714-7726
Funding ProjectNational Natural Science Foundation of China[21703054] ; University at Buffalo
Funding OrganizationNational Natural Science Foundation of China ; National Natural Science Foundation of China ; University at Buffalo ; University at Buffalo ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; University at Buffalo ; University at Buffalo ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; University at Buffalo ; University at Buffalo ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; University at Buffalo ; University at Buffalo
WOS SubjectChemistry, Physical ; Materials Science, Multidisciplinary
WOS Research AreaChemistry ; Materials Science
WOS KeywordTOTAL-ENERGY CALCULATIONS ; WATER OXIDATION ; PHOTOCATALYST ; PEROVSKITE ; SURFACES ; ELECTROCATALYSTS ; ELECTROLYSIS ; PERFORMANCE ; ADSORPTION ; HYDROGEN
AbstractNeutral oxygen vacancies (Ov's) in semiconductor oxides give rise to excess electrons that have the potential to affect the binding of adsorbates to the surface through surface-to-adsorbate charge transfer, and, as a result, to alter the overpotential (OP) of reactions on oxygen-deficient materials compared to stoichiometric materials. We report a systematic computational investigation of the effects of Ov's on the oxygen evolution reaction (OER) overpotential for beta-Ga2O3, a d(10) semiconductor that has been shown to exhibit high activity for water splitting. We investigated 18 beta-Ga2O3 surfaces/slabs, with and without Ov's and observed a clear dependence of OER activity on Ov's. A general finding emerged that the excess electrons associated with Ov's are found to participate in charge transfer to OER intermediates, making their bonds to the surface more ionic and stronger, depending on the amount of charge transfer. The OER reaction step free energies are significantly affected and the ensuing overpotentials are altered. The amount of charge transfer varies with the types of intermediates (OH*, dangling O*, surface-bound peroxo O*, and dangling OOH*), their open valencies, and their electronegativity. The work function and the position of the gap states of the excess electrons in the band gap are found to be useful descriptors of whether and how much Ov-induced charge transfer may occur and affect the overpotential. However, it was also found that the chemical environment of the O atom where the vacancy was created, may have a negating effect on the general observation. Specifically some Ov structures underwent a strong relaxation to form Ga-Ga bonds, trapping the vacancy electrons, and preventing them to engage in charge transfer. Oxygen vacancies are common defects in photocatalyst materials so that our investigation can provide guiding principles for designing efficient photocatalysts.
Language英语
Funding OrganizationNational Natural Science Foundation of China ; National Natural Science Foundation of China ; University at Buffalo ; University at Buffalo ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; University at Buffalo ; University at Buffalo ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; University at Buffalo ; University at Buffalo ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; University at Buffalo ; University at Buffalo
WOS IDWOS:000450696100038
PublisherAMER CHEMICAL SOC
Citation statistics
Cited Times:3[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://cas-ir.dicp.ac.cn/handle/321008/166615
Collection中国科学院大连化学物理研究所
Corresponding AuthorLiu, Taifeng; Dupuis, Michel
Affiliation1.Henan Univ, Natl & Local Joint Engn Res Ctr Appl Technol Hybr, Collaborat Innovat Ctr Nano Funct Mat & Applicat, Kaifeng 475004, Peoples R China
2.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian Natl Lab Clean Energy, Zhongshan Rd 457, Dalian 116023, Peoples R China
3.SUNY Buffalo, Dept Chem & Biol Engn, Buffalo, NY 14260 USA
Recommended Citation
GB/T 7714
Liu, Taifeng,Feng, Zhaochi,Li, Qiuye,et al. Role of Oxygen Vacancies on Oxygen Evolution Reaction Activity: beta-Ga2O3 as a Case Study[J]. CHEMISTRY OF MATERIALS,2018,30(21):7714-7726.
APA Liu, Taifeng,Feng, Zhaochi,Li, Qiuye,Yang, Jianjun,Li, Can,&Dupuis, Michel.(2018).Role of Oxygen Vacancies on Oxygen Evolution Reaction Activity: beta-Ga2O3 as a Case Study.CHEMISTRY OF MATERIALS,30(21),7714-7726.
MLA Liu, Taifeng,et al."Role of Oxygen Vacancies on Oxygen Evolution Reaction Activity: beta-Ga2O3 as a Case Study".CHEMISTRY OF MATERIALS 30.21(2018):7714-7726.
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