2024年1月常州大学低碳清洁能源与安全高效燃烧科研团队孙运兰教授课题组王佳欣老师在Geoenergy Science and Engineering期刊发表了题为“Effects of surface functionalizing and pore structure on dissolved mercury adsorption in gasoline by covalent sulphur-doped templated carbons: Experimental and theoretical insights”的研究论文。
凝析油,又被称为天然汽油,其中的溶解态汞不仅降低了油品质量,而且会腐蚀加工设备,引发催化剂中毒和环境污染等问题。然而,目前的脱汞吸附剂存在对凝析油中溶解态汞吸附能力弱和选择性差问题,这难以满足绿色生产加工需求。因此本工作采用浸渍-热解(IP)法制备了共价硫掺杂模板碳(TCs),用于脱除凝析油中溶解的离子汞(Hg2+)和有机汞(Hgorg)。TCs对Hg2+和Hgorg的最大吸附量分别为1904 μg/g和299 μg/g。TCs的汞选择性吸附与其物理化学结构密切相关。50%-TC样品含有较多的含硫官能团(S=O和C-S)和微孔,相比于Hgorg对Hg2+吸附效果更好,而100%-TC样品含有较多的含氧官能团(C-O)和介孔,对Hgorg表现出更好的吸附选择性。在实验方法的基础上,本工作还利用分子动力学(MD)模拟揭示了对Hg2+和Hgorg的吸附机理。结果表明,孔径分别为2.03 nm和2.98 nm的TCs样品更容易吸附Hg2+和Hgorg,这与吸附实验结果较为一致。最终,TCs样品在5次再生循环后对汞吸附能力下降不到28.5%。上述研究结果为制备高选择性脱汞吸附剂提供了新的思路。
该论文第一作者王佳欣博士是常州大学低碳清洁能源与安全高效燃烧课题组讲师,该成果为华北电力大学和常州大学合作成果,常州大学是第一作者和通讯作者单位,华北电力大学是第二通讯单位。
英文摘要:
Mercury pollutants dissolved in gasoline would damage the processing equipment and corrosion the pipeline, which required to be removed. However, the adsorption capacity and selectivity of current adsorbents on mercury pollutants in gasoline make it difficult to meet the demand for green ecological production. In this work, the covalent sulphur-doped templated carbons (TCs) were prepared by the impregnation-pyrolysis (IP) method to remove dissolved ionic mercury (Hg2+) and organic mercury (Hgorg) in gasoline. The maximum adsorption capacities of TCs on Hg2+ and Hgorg were 1904 μg/g and 299 μg/g, respectively. The adsorption selectively of TCs was closely related to their physical and chemical structure. The 50%-TC with more sulphur-containing functional groups (S=O and C-S) and micropores showed an adsorption preference for Hg2+. However, 100%-TC dominated by more mesopores coupled with oxygen-containing functional groups (C-O) exhibited better adsorption selectivity for Hgorg. Apart from experimental methods, molecular dynamics (MD) simulation was used to reveal the adsorption mechanism. The results showed that Hg2+ and Hgorg were easily adsorbed by TC samples with pore sizes of 2.03 nm and 2.98 nm, respectively, which was consistent with the adsorption experiment. In the end, the mercury adsorption capacity of TCs decreased by less than 28.5% after five regeneration cycles. The above-discussed results cast a new light on the preparation of highly selective mercury removal adsorbents.
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原文链接:https://doi.org/10.1016/j.geoen.2023.212629
(撰稿:王佳欣 审核:朱宝忠)