首页|多酸基UiO-66的合成及其对硫化氢的脱除性能

多酸基UiO-66的合成及其对硫化氢的脱除性能

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硫化氢具有较强的毒性和腐蚀性,高效脱除硫化氢对于工业生产、环境治理等过程意义重大。该文基于钼基杂多酸(HPAs),以UiO-66为载体,一步水热合成HPAs@UiO-66,构建不同活性中心多酸基固相脱硫体系,考察杂多酸结构(Keggin、Dawson)、中心原子(P、Si)、取代原子(V、W)对脱硫的影响,并通过BET、FT-IR、XRD、SEM、TEM进行理化性质分析。结果表明,PMo12@UiO-66脱硫活性最高,且其脱硫能力在100 ℃时最佳,吸附量可达到17。18 mg/g,同时发现水分对其脱硫具有促进作用。与PMo12和UiO-66相比,PMo12@UiO-66表现出明显脱硫优势,其吸附量分别为PMo12和UiO-66的7。5和14。2倍,证明了 PMo12与UiO-66具有协同脱硫作用。XPS结果表明,PMo12与H2S之间发生了氧化还原反应,H2S在PMo12氧化作用下被转化成单质硫。研究表明PMo12的引入对UiO-66脱硫性能的强化作用最为显著,可为开发新型多酸基固相脱硫剂提供参考。
Heteropoly-Acid-Based Modified UiO-66:Its Synthesis and H2S Removal Performances
Hydrogen sulfide is characterized with strong toxicity and corrosivity,so it is important to efficiently minimize its pollution.In this laboratory experiment a series of HPAs@UiO-66 were prepared by one-step hydrothermal method with molybdenum-based heteropoly acid(HPAs)as active centers and UiO-66 as a carrier,and a multi-acid-based solid phase desulfurization system with various active centers was set up.The effects of Keggin and Dawson structures,the central atoms(P and Si),and the substitutional atoms(V and W)of HPAs on desulfurization performance were studied,and their physico-chemical properties were analyzed by BET,FT-IR,XRD,SEM,and TEM.As a result,it was showed that PMo12@UiO-66 had excellent desulfurization activity,its H2S removal ability was maximized at 100 ℃ with a absorbing capacity being able to reach 17.18 mg/g,and it was found the presence of water in the mixed gas can promote PMo12@UiO-66 to remove H2S.In comparison with PMo12 and UiO-66,PMo12@UiO-66 was far better in desulfurization,its H2S absorbing capacity was 7.5 and 14.2 times PMo12 and UiO-66,respectively,demonstrating the synergistic desulfurization effect of PMo12 and UiO-66.Analysis by use of XPS(X-ray photo-electron spectroscopy)showed that the redox reaction took place between PMo12 and H2S,during which H2S was converted into elemental sulfur due to the oxidizing action of PMo12.In conclusion,this study proved that the introduction of PMo12 had exhibited the most remarkable effect on enforcing the desulfurization performance of UiO-66,which could provide a reference for exploiting more novel HPA-based solid phase desulfurization agents.

heteropoly acidhydrogen sulfideheterogeneous desulfurizationmetal-organic frameworkresource conversion

李祥华、左强、李品、张艺柯、马双龙、王竞侦、高博强、黄岩

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河南省生态环境技术中心,河南 郑州 450004

河南省生态环境损害鉴定评估与土壤污染修复治理工程技术研究中心,河南 郑州 450004

河南农业大学资源与环境学院,河南 郑州 450046

杂多酸 硫化氢 非均相脱硫 金属有机框架 资源化转化

河南省自然科学基金河南省科技攻关项目河南省科技攻关项目河南农业大学拔尖人才项目

23230042037424210232018123210232007730500945

2024

环境科学与技术
湖北省环境科学研究院

环境科学与技术

CSTPCD北大核心
影响因子:0.943
ISSN:1003-6504
年,卷(期):2024.47(6)