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Efficient Removal of Thallium from Flue Gas Using Manganese-Based MOF Catalysts by Gas–Solid Phase Catalytic Oxidation and Adsorption
Industrial & Engineering Chemistry Research ( IF 3.8 ) Pub Date : 2020-06-26 , DOI: 10.1021/acs.iecr.0c01676 Qiang Ma 1, 2 , Lijuan Jia 3 , Xueqian Wang 1 , Ping Ning 1 , Langlang Wang 1 , Lixia Xu 1 , Shu Sun 2 , Yixing Ma 1 , Yingjie Zhang 1 , Tao Lei 1 , Wei Liu 1 , Jiming Hao 4
Industrial & Engineering Chemistry Research ( IF 3.8 ) Pub Date : 2020-06-26 , DOI: 10.1021/acs.iecr.0c01676 Qiang Ma 1, 2 , Lijuan Jia 3 , Xueqian Wang 1 , Ping Ning 1 , Langlang Wang 1 , Lixia Xu 1 , Shu Sun 2 , Yixing Ma 1 , Yingjie Zhang 1 , Tao Lei 1 , Wei Liu 1 , Jiming Hao 4
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Thallium (Tl) is known to be extremely toxic. However, thallium pollution from smelting tail gas has long been neglected as an environmental issue. This study aims to develop a gaseous thallium control technology based on manganese-based metal–organic framework (MOF) catalysts, using a manganese centered paddle wheel structure as a support. Tl removal testing showed that these catalysts were effective at both adsorbing and oxidizing Tl(I), producing Tl(III), which is less harmful. Details of the catalytic oxidation mechanism were investigated, which demonstrated that Tl(I) loses electrons to Mn(III), Mn(IV), and O2, generating Tl2O3. Over 90% removal efficiency was maintained for 10 h by a MOF catalyst with 10% Mn loading, at 423 K with 10% O2 in the feed gas, which was determined to be the optimal level of O2. SO2 inhibited thallium removal in this system, while 10% CO2 had no significant effect. Regeneration through acid washing was found to be effective, with the catalyst maintaining thallium removal efficiency for five regeneration cycles. Molecular simulation of Tl removal is investigated, based on which the possible reaction path is found.
中文翻译：
固相催化氧化和吸附法基于锰的MOF催化剂有效去除烟道气中的T
hall（Tl）毒性极高。然而，长期以来，熔融尾气中的pollution污染一直被忽略为环境问题。这项研究旨在开发一种基于锰的金属-有机骨架（MOF）催化剂的气态control控制技术，该技术以锰为中心的桨轮结构为载体。Tl去除测试表明，这些催化剂在吸附和氧化Tl（I）方面均有效，产生的Tl（III）危害较小。研究了催化氧化机理的细节，结果表明Tl（I）失去电子，生成Mn（III），Mn（IV）和O 2，生成Tl 2 O 3。在423 K下使用10％O 2的Mn负载量为10％的MOF催化剂可保持90％以上的去除效率进料气中的O 2被确定为最佳水平的O 2。在该系统中，SO 2抑制了removal的去除，而10％CO 2则无明显作用。发现通过酸洗的再生是有效的，该催化剂在五个再生循环中保持除去removal的效率。研究了T1去除的分子模拟，基于其发现了可能的反应路径。
更新日期：2020-07-22
中文翻译：
固相催化氧化和吸附法基于锰的MOF催化剂有效去除烟道气中的T
hall（Tl）毒性极高。然而，长期以来，熔融尾气中的pollution污染一直被忽略为环境问题。这项研究旨在开发一种基于锰的金属-有机骨架（MOF）催化剂的气态control控制技术，该技术以锰为中心的桨轮结构为载体。Tl去除测试表明，这些催化剂在吸附和氧化Tl（I）方面均有效，产生的Tl（III）危害较小。研究了催化氧化机理的细节，结果表明Tl（I）失去电子，生成Mn（III），Mn（IV）和O 2，生成Tl 2 O 3。在423 K下使用10％O 2的Mn负载量为10％的MOF催化剂可保持90％以上的去除效率进料气中的O 2被确定为最佳水平的O 2。在该系统中，SO 2抑制了removal的去除，而10％CO 2则无明显作用。发现通过酸洗的再生是有效的，该催化剂在五个再生循环中保持除去removal的效率。研究了T1去除的分子模拟，基于其发现了可能的反应路径。
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