Zhiwei Ma, Xianrong Zheng, Liping Chang, Ruiyuan He, Weiren Bao
{"title":"半焦载体负载ZnO吸附剂对热煤气的脱硫动力学研究","authors":"Zhiwei Ma, Xianrong Zheng, Liping Chang, Ruiyuan He, Weiren Bao","doi":"10.1016/S1003-9953(11)60404-0","DOIUrl":null,"url":null,"abstract":"<div><p>Zn-based sorbent (Z20SC) prepared through semi-coke support in 20 wt% zinc nitrate solution by high-pressure impregnation presents an excellent desulfurization capacity in hot coal gas, in which H<sub>2</sub>S can not be nearly detected in the outlet gas before 20 h breakthrough time. The effects of the main operational conditions and the particle size of Z20SC sorbent on its desulfurization performances sorbent were investigated in a fixed-bed reactor and the desulfurization kinetics of Z20SC sorbent removing H<sub>2</sub>S from hot coal gas was calculated based on experimental data. Results showed that the conversion of Z20SC sorbent desulfurization reaction increased with the decrease of the particle size of the sorbent and the increases of gas volumetric flow rate, reaction temperature and H<sub>2</sub>S content in inlet gas. Z20SC sorbent obtained from hydrothermal synthesis by high-pressure impregnation possessed much larger surface area and pore volume than semi-coke support, and they were significantly reduced after the desulfurization reaction. The equivalent grain model was reasonably used to analyze experimental data, in which <em>k</em><sub>s</sub> = 4.382×10<sup>−3</sup> exp(−8.270×10<sup>3</sup>/<em>R</em><sub>g</sub><em>T</em>) and <em>D</em><sub>ep</sub> = 1.262×10<sup>−4</sup>exp(−1.522×10<sup>4</sup>/<em>R</em><sub>g</sub><em>T</em>). It suggests that the desulfurization reaction of the Z20SC sorbent is mainly controlled by the chemical reaction in the initial stage and later by the diffusion through the reacted sorbent layer.</p></div>","PeriodicalId":56116,"journal":{"name":"Journal of Natural Gas Chemistry","volume":"21 5","pages":"Pages 556-562"},"PeriodicalIF":0.0000,"publicationDate":"2012-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1016/S1003-9953(11)60404-0","citationCount":"10","resultStr":"{\"title\":\"Desulfurization kinetics of ZnO sorbent loaded on semi-coke support for hot coal gas\",\"authors\":\"Zhiwei Ma, Xianrong Zheng, Liping Chang, Ruiyuan He, Weiren Bao\",\"doi\":\"10.1016/S1003-9953(11)60404-0\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>Zn-based sorbent (Z20SC) prepared through semi-coke support in 20 wt% zinc nitrate solution by high-pressure impregnation presents an excellent desulfurization capacity in hot coal gas, in which H<sub>2</sub>S can not be nearly detected in the outlet gas before 20 h breakthrough time. The effects of the main operational conditions and the particle size of Z20SC sorbent on its desulfurization performances sorbent were investigated in a fixed-bed reactor and the desulfurization kinetics of Z20SC sorbent removing H<sub>2</sub>S from hot coal gas was calculated based on experimental data. Results showed that the conversion of Z20SC sorbent desulfurization reaction increased with the decrease of the particle size of the sorbent and the increases of gas volumetric flow rate, reaction temperature and H<sub>2</sub>S content in inlet gas. Z20SC sorbent obtained from hydrothermal synthesis by high-pressure impregnation possessed much larger surface area and pore volume than semi-coke support, and they were significantly reduced after the desulfurization reaction. The equivalent grain model was reasonably used to analyze experimental data, in which <em>k</em><sub>s</sub> = 4.382×10<sup>−3</sup> exp(−8.270×10<sup>3</sup>/<em>R</em><sub>g</sub><em>T</em>) and <em>D</em><sub>ep</sub> = 1.262×10<sup>−4</sup>exp(−1.522×10<sup>4</sup>/<em>R</em><sub>g</sub><em>T</em>). It suggests that the desulfurization reaction of the Z20SC sorbent is mainly controlled by the chemical reaction in the initial stage and later by the diffusion through the reacted sorbent layer.</p></div>\",\"PeriodicalId\":56116,\"journal\":{\"name\":\"Journal of Natural Gas Chemistry\",\"volume\":\"21 5\",\"pages\":\"Pages 556-562\"},\"PeriodicalIF\":0.0000,\"publicationDate\":\"2012-09-01\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"https://sci-hub-pdf.com/10.1016/S1003-9953(11)60404-0\",\"citationCount\":\"10\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Natural Gas Chemistry\",\"FirstCategoryId\":\"1085\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S1003995311604040\",\"RegionNum\":0,\"RegionCategory\":null,\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"\",\"JCRName\":\"\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Natural Gas Chemistry","FirstCategoryId":"1085","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S1003995311604040","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"","JCRName":"","Score":null,"Total":0}
引用次数: 10
摘要
在20% wt%硝酸锌溶液中高压浸渍半焦载体制备的锌基吸附剂(Z20SC)在热煤气中具有良好的脱硫能力,在突破时间20h之前,出口煤气中几乎检测不到H2S。在固定床反应器上研究了Z20SC吸附剂的主要操作条件和粒径对其脱硫性能的影响,并根据实验数据计算了Z20SC吸附剂去除热煤气中H2S的脱硫动力学。结果表明:Z20SC吸附剂脱硫反应的转化率随着吸附剂粒径的减小、气体体积流量、反应温度和入口气体H2S含量的升高而提高;高压浸渍水热合成的Z20SC吸附剂比半焦载体具有更大的比表面积和孔隙体积,且经过脱硫反应后明显减少。合理采用等效颗粒模型对实验数据进行分析,其中ks = 4.382×10−3 exp(−8.270×103/RgT), Dep = 1.262×10−4exp(−1.522×104/RgT)。说明Z20SC吸附剂的脱硫反应主要由初始阶段的化学反应控制,后期通过反应吸附层的扩散控制。
Desulfurization kinetics of ZnO sorbent loaded on semi-coke support for hot coal gas
Zn-based sorbent (Z20SC) prepared through semi-coke support in 20 wt% zinc nitrate solution by high-pressure impregnation presents an excellent desulfurization capacity in hot coal gas, in which H2S can not be nearly detected in the outlet gas before 20 h breakthrough time. The effects of the main operational conditions and the particle size of Z20SC sorbent on its desulfurization performances sorbent were investigated in a fixed-bed reactor and the desulfurization kinetics of Z20SC sorbent removing H2S from hot coal gas was calculated based on experimental data. Results showed that the conversion of Z20SC sorbent desulfurization reaction increased with the decrease of the particle size of the sorbent and the increases of gas volumetric flow rate, reaction temperature and H2S content in inlet gas. Z20SC sorbent obtained from hydrothermal synthesis by high-pressure impregnation possessed much larger surface area and pore volume than semi-coke support, and they were significantly reduced after the desulfurization reaction. The equivalent grain model was reasonably used to analyze experimental data, in which ks = 4.382×10−3 exp(−8.270×103/RgT) and Dep = 1.262×10−4exp(−1.522×104/RgT). It suggests that the desulfurization reaction of the Z20SC sorbent is mainly controlled by the chemical reaction in the initial stage and later by the diffusion through the reacted sorbent layer.