Efficient Hydrogen Peroxide (H2O2) Synthesis by CaSnO3 via Two-Electron Water Oxidation Reaction
Kang T1; Li B1; Hao QL1; Gao WJ1; Bin F(宾峰)4; Hui KN2; Fu D3; Dou BJ1
刊名ACS SUSTAINABLE CHEMISTRY & ENGINEERING
2020-10-05
卷号8期号:39页码:15005-15012
关键词CaSnO3 nanoparticles in situ H2O2 generation two-electron water oxidation reaction DFT vacancy oxygen calcination
ISSN号2168-0485
DOI10.1021/acssuschemeng.0c05449
通讯作者Fu, Dong(fudongimu@yahoo.com) ; Dou, Baojuan(bjdou@tust.edu.cn)
英文摘要Electrochemical in situ hydrogen peroxide (H2O2) generation from a two-electron water oxidation reaction (2e-WOR) is a challenge, not only on catalyst selection but also on electrode making. Herein, the H2O2 electrocatalyst CaSnO3 nanoparticles were prepared by low-cost glucose as an agent and characterized by X-ray diffraction (XRD), thermogravimetric and differential scanning calorimetry (TG-DSC), Fourier transform infrared spectra (FT-IR), scanning electron microscopy (SEM), transmission electron microscopy (TEM), and X-ray photoelectron spectroscopy (XPS). The active sites for the OH- adsorption on the surface CaSnO3 (121) was identified by density functional theory (DFT) calculation, and the corresponding reaction mechanism of H2O2 formation was proposed. The CaSnO3 nanoparticles can be formed from 650 to 850 degrees C, and the particle sizes are in the range of 27.2-37.3 nm. The mechanism of catalyst formation is that species of Ca and Sn reacted with oxygen to generate CaO and SnO2 during low-temperature calcination and CaSnO3 generated during high-temperature calcination. The active sites are the coordination-unsaturated Sn ions, which easily adsorb the negative-charge OH- from the solution, forming an OH* intermediate, and two adsorbed OH* can combine to generate a neutral H2O2 molecule. The H2O2 generation rate over CaSnO3 was calcinated at 850 degrees C is 347.7 mu mol.min(-1).g(-1) at 2.6 V versus Ag/AgCl under dark conditions. The work opens an in situ H2O2 generation route, direct water oxidation, with wide application prospects.
分类号一类
资助项目National Nature Science Foundation of China[51776216] ; Tianjin Weiming Technology Co. Ltd. ; Tianjin University of Science and Technology[1900030001]
WOS关键词WASTEWATERS ; ELECTRODES ; OXYGEN
WOS研究方向Chemistry ; Science & Technology - Other Topics ; Engineering
语种英语
WOS记录号WOS:000579967200039
资助机构National Nature Science Foundation of China ; Tianjin Weiming Technology Co. Ltd. ; Tianjin University of Science and Technology
其他责任者Fu, Dong ; Dou, Baojuan
内容类型期刊论文
源URL[http://dspace.imech.ac.cn/handle/311007/85351]  
专题力学研究所_高温气体动力学国家重点实验室
作者单位1.Tianjin Univ Sci & Technol, Tianjin Key Lab Brine Chem Engn & Resource Ecouti, Coll Chem Engn & Mat Sci, Tianjin 300457, Peoples R China;
2.Univ Macau, Inst Appl Phys & Mat Engn, Taipa 999078, Macau, Peoples R China;
3.Tianjin Weiming Technol Co Ltd, Tianjin 300384, Peoples R China
4.Chinese Acad Sci, Inst Mech, State Key Lab High Temp Gas Dynam, Beijing 100190, Peoples R China;
推荐引用方式
GB/T 7714
Kang T,Li B,Hao QL,et al. Efficient Hydrogen Peroxide (H2O2) Synthesis by CaSnO3 via Two-Electron Water Oxidation Reaction[J]. ACS SUSTAINABLE CHEMISTRY & ENGINEERING,2020,8(39):15005-15012.
APA Kang T.,Li B.,Hao QL.,Gao WJ.,宾峰.,...&Dou BJ.(2020).Efficient Hydrogen Peroxide (H2O2) Synthesis by CaSnO3 via Two-Electron Water Oxidation Reaction.ACS SUSTAINABLE CHEMISTRY & ENGINEERING,8(39),15005-15012.
MLA Kang T,et al."Efficient Hydrogen Peroxide (H2O2) Synthesis by CaSnO3 via Two-Electron Water Oxidation Reaction".ACS SUSTAINABLE CHEMISTRY & ENGINEERING 8.39(2020):15005-15012.
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