2-巯基苯并咪唑改性TEPA-MCM-41烟气碳捕集吸附剂的抗氧化降解机理,The Canadian Journal of Chemical Engineering

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2-巯基苯并咪唑改性TEPA-MCM-41烟气碳捕集吸附剂的抗氧化降解机理
The Canadian Journal of Chemical Engineering ( IF 1.6 ) Pub Date : 2023-03-07 , DOI: 10.1002/cjce.24894
Ruotong Wang ₁ , Tuo Guo ₁ , Xiaoju Xiang ₁ , Yinmei Yin ₁ , Qingjie Guo _{1,

2} , Yanxia Wang ₃

Affiliation

固体胺吸附剂可以有效地吸附CO ₂，但一个显着的问题是胺基团被氧化。在这项研究中，四乙烯五胺浸渍的 MCM-41 吸附剂（TEPA-MCM-41）用含硫抗氧化剂 2-巯基苯并咪唑（称为抗氧化剂 MB）和 tns-(2.4-二叔丁基)-亚磷酸酯（分别定义为抗氧化剂168)。通过原位漫反射红外傅里叶变换（in situ DRIFT）光谱和高效液相色谱/质谱（HPLC/mass）分析了8% MB–50% TEPA-MCM-41的抗氧化降解机制。_{50% TEPA-MCM-41在15% CO 2} /85% N ₂条件下CO ₂吸附量为4.30 mmol/g_{，但在95% N 2} /5% O ₂一定条件下，100℃氧化42 h后下降至1.38 mmol/g 。8% MB–50% TEPA-MCM-41 的CO ₂容量从 3.90 降低至 2.86 mmol/g。_{5% O 2} /15% CO ₂ /80% N ₂下30次吸附循环后，8% MB–50% TEPA-MCM-41 的容量也仅下降了 16.8%，而 50% TEPA-MCM-41 则下降了 63.2%。8%MB–50%TEPA-MCM-41具有优异的抗氧化稳定性的原因是MB清除了胺氧化产生的自由基并分解了自由基反应产生的氢过氧化物。氢过氧化物分解成醇（非自由基产物），最终氧化成磺酸化合物。MB 改性抑制了固体胺吸附剂的氧化降解，可用于生产抗氧化高效吸附剂。

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Antioxidative degradation mechanism of 2-mercaptobenzimidazole modified TEPA-MCM-41 adsorbents for carbon capture from flue gas

Solid amine adsorbents can efficiently adsorb CO₂, but a significant problem is that amine groups are oxidized. In this research, tetraethylenepentamine-impregnated MCM-41 adsorbents (TEPA-MCM-41) were functionally modified with sulphur-containing antioxidant 2-mercaptobenzimidazole (described as antioxidant MB) and tns-(2.4-di-tert-butyl)-phosphite (defined as antioxidant 168), respectively. The antioxidative degradation mechanism of 8% MB–50% TEPA-MCM-41 was analyzed by in situ diffuse reflectance infrared Fourier transform (in situ DRIFT) spectrum and high-performance liquid chromatography/mass spectrometry (HPLC/mass). The CO₂ adsorption capacity of 50% TEPA-MCM-41 was 4.30 mmol/g under 15% CO₂/85% N₂, but decreased to 1.38 mmol/g after oxidation at 100°C for 42 h under 95% N₂/5% O₂ certain condition. The CO₂ capacity of 8% MB–50% TEPA-MCM-41 reduced from 3.90 to 2.86 mmol/g. After 30 adsorption cycles under 5% O₂/15% CO₂/80% N₂, the capacity of 8% MB–50% TEPA-MCM-41 also only decreased by 16.8%, while 50% TEPA-MCM-41 decreased by 63.2%. The reason for the excellent antioxidant stability of 8% MB–50% TEPA-MCM-41 is that MB scavenged free radicals from amine oxidation and decomposed the hydroperoxides produced by free radical reactions. The hydroperoxides were decomposed into alcohols (non-radical products), which were eventually oxidized to sulphonic compounds. The MB modification inhibited the oxidative degradation of solid amine adsorbents guided for the production of antioxidant-efficient adsorbents.

更新日期：2023-03-07

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