Role of oxygen vacancies on oxygen evolution reaction activity: beta-ga2o3 as a case study
文献类型：期刊论文
| 作者 | Liu, Taifeng1; Feng, Zhaochi2; Li, Qiuye1; Yang, Jianjun1; Li, Can2; Dupuis, Michel2,3 |
| 刊名 | Chemistry of materials
 |
| 出版日期 | 2018-11-13 |
| 卷号 | 30期号:21页码:7714-7726 |
| ISSN号 | 0897-4756 |
| DOI | 10.1021/acs.chemmater.8b03015 |
| 通讯作者 | Liu, taifeng(tfliu@vip.henu.edu.cn) ; Dupuis, michel(mdupuis2@buffalo.edu) |
| 英文摘要 | Neutral 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. |
| WOS关键词 | TOTAL-ENERGY CALCULATIONS ; WATER OXIDATION ; PHOTOCATALYST ; PEROVSKITE ; SURFACES ; ELECTROCATALYSTS ; ELECTROLYSIS ; PERFORMANCE ; ADSORPTION ; HYDROGEN |
| WOS研究方向 | Chemistry ; Materials Science |
| WOS类目 | Chemistry, Physical ; Materials Science, Multidisciplinary |
| 语种 | 英语 |
| 出版者 | AMER CHEMICAL SOC |
| WOS记录号 | WOS:000450696100038 |
| URI标识 | http://www.irgrid.ac.cn/handle/1471x/2373064 |
| 专题 | 大连化学物理研究所 |
| 通讯作者 | Liu, Taifeng; Dupuis, Michel |
| 作者单位 | 1.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 |
| 推荐引用方式 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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来源：大连化学物理研究所
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