绿色电化学水分解法制备臭氧:机理研究（英文）

发布时间：2018-03-24 06:14

本文选题：臭氧析出反应　切入点：水分解　出处：《电化学》2017年02期

【摘要】：采用电催化剂通过水分解反应形成臭氧的绿色节能方法为常规耗能量大的冷电晕放电提供了非常具有吸引力的替代方法.在大量研究的用于电化学合成臭氧的电催化剂中,β-氧化铅(β-PbO_2)和氧化锡(SnO_2)基催化剂在室温下最有效.本工作通过密度泛函理论计算,研究了上述两种催化剂作用下臭氧的形成机制.两种催化剂β-PbO_2和镍/锑掺杂氧化锡(Ni/Sb-SnO_2)的(110)晶面最稳定,故作者特别关注β-PbO_2(110)和Ni/Sb-SnO_2(110)表面发生的最后两步反应,即氧气和臭氧的形成,模拟了可能的水分解机理.结果表明,在β-PbO_2催化剂的作用下,臭氧是遵循Eley-Rideal机理形成,与在Ni/Sb-SnO_2,表面臭氧的形成机理相反,后者是通过Langmuir-Hinshelwood机理形成.将β-PbO_2主要模拟为固-液相,Ni/Sb-SnO_2主要模拟为气相,计算得到吸附能(E_(ads))、吉布斯自由能(ΔG)和活化能(E_(act))等热力学参数值,并进行了分析与比较.这些结果为设计和研发新型的高电流效率电化学制臭氧用催化剂提供了依据.
[Abstract]:The green energy saving method of using electrocatalyst to form ozone through water decomposition provides a very attractive alternative to conventional cold corona discharge with large energy consumption. Among the catalysts, 尾 -PbO _ 2 (尾 -PbO _ 2)-based catalysts are most effective at room temperature. The formation mechanism of ozone under the action of the above two catalysts has been studied. The crystal plane of 尾 -PbO _ 2 and Ni / SB doped tin oxide (Nip / Sb-SnO _ 2) is the most stable. Therefore, the author pays special attention to the last two steps of the reaction on the surface of 尾 -PbO _ 2O _ 2 (10) and Ni / Sb-SnO _ 2110), that is, the formation of oxygen and ozone, The possible mechanism of water decomposition has been simulated. The results show that the formation of ozone follows the Eley-Rideal mechanism under the action of 尾 -PbO _ 2 catalyst, which is contrary to the formation mechanism of surface ozone in Ni- / Sb-SnO _ 2. The latter is formed by Langmuir-Hinshelwood mechanism. The main simulation of 尾 -PbO2 is that the solid-liquid phase Ni- / Sb-SnO2 is mainly simulated as gas phase, and the thermodynamic parameters such as adsorption energy, Gibbs free energy and activation energy are calculated. These results provide a basis for the design and development of new catalysts for electrochemical ozone production with high current efficiency.
【作者单位】：英国拉夫堡大学化学工程系;英国贝尔法斯特女王大学化学与化学工程学院;
【基金】：the Department of Education and Learning(DEL) of Northern Ireland Northern Ireland Water Limited Modern Water plc,UK EPSRC Loughborough University for their supports
【分类号】：TQ123.2

【相似文献】