质子型固体电解质膜反应器电催化氧化H2S过程中对称电极失活机理与再生研究

项目名称： 质子型固体电解质膜反应器电催化氧化H2S过程中对称电极失活机理与再生研究

项目编号： No.21207064

项目类型： 青年科学基金项目

立项/批准年度： 2013

项目学科： 环境化学

项目作者： 谭文轶

作者单位： 南京工程学院

项目金额： 24万元

中文摘要： 本项目针对固体电解质膜反应器(SEMR)处理H2S时阳极易失活这一瓶颈问题，以调节阳极硫形态分布，获取易脱附的产物硫为思路，开展钙钛矿对称电极的失活机理与再生途径研究。根据半导体催化和晶体结构缺陷理论，制备Mn、Ti、V等过渡金属掺杂的La1-xSrxMO3钙钛矿对称电极，构建对称电极负载的质子型SEMR电催化氧化H2S。通过瞬态响应技术序贯切换反应物组成，结合原位Raman、XPS表征结果，揭示H2S在钙钛矿对称电极表面氧空位上的吸附机制，用表面泛函理论预测电极种类和成分对吸附活性位的调变规律；同时根据原位电化学测定，探寻稳态质子传导条件下电极失活原因，建立H2S电催化氧化动力学模型。通过互换阴阳极气体，探明O2和阴极产物水蒸汽对电极表面产物硫的脱附机制，探讨钙钛矿对称电极再生可行性。这将为H2S电催化氧化过程中阳极失活和耐硫电极设计提供理论依据，促进高效低耗处理H2S尾气的研发。

中文关键词： 硫化氢；固体电解质膜反应器；对称电极；原位；再生

英文摘要： Enlighted by the fact that the accommodation of sulfide species distribution on the anode to form renewable sulfides, the project focuses on deactivation mechanism and regeneration of symmetric electodes with perovskite structure, aiming to solve the key issue about the easily deactivated anode in solid eletrolyte membrane reactor (SEMR) degrading H2S. Based on the semi-conductor catalysis and crystal defect theory, the project plans to fabricate proton-conducting SEMR, which is coated by symmetric electrodes with perovskite structure, La1-xSrxMO3(M= Mn、Ti、V, etc) to electro-catalytically oxidize H2S. H2S adsorption on the oxygen vacancies of the symmetric electrodes will be investigated by sequential switch of reactants compositions in transient response method and by characterizations including in-situ Raman, XPS, etc. Density funtional theory will be applied to set up the model of active sites modification in adsorption. By the aid of in-situ electrochemical measurement, the causes to deactivation of symmetrical electrodes oxidizing H2S in an electro-catalytical way can be revealed and the kinetic models can also be proposed, in combination with steady proton transport in SEMR. Furthermore, after interconverting the fuel and oxidative gas, the desorption of renewable sulfur on the surface of electrodes will b

英文关键词： Hydrogen sulfide；Solid electrolyte membrane reactor；Symmetrical electrode；In-situ；Regeneration