Appending Polyamines on Metal–Organic Frameworks as an Efficient Strategy for Selective Removal of H2S under Humid Conditions

Guillaume Esser, Robin Crits, Gabriella Barozzino-Consiglio, Ayoub Daouli, Guillaume Maurin, Yaroslav Filinchuk*, Sophie Hermans* and Timothy Steenhaut*, 
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Abstract

Removal of highly toxic and corrosive hydrogen sulfide from gas flows is of paramount importance for controlling the environment and in several industrial processes. This contribution reports a straightforward strategy to engineer sorbents for efficient hydrogen sulfide removal under humid conditions by functionalizing the open metal sites of metal–organic frameworks (MOFs) with polyamines. MIL-101(Cr) MOFs were successfully modified with ethylenediamine and tris(2-aminoethyl)amine, and the resulting materials were characterized using X-ray diffraction, FTIR, NMR, nitrogen sorption, and thermogravimetric analysis (TGA), confirming the functionalization. Although the functionalized MOFs exhibited a greater affinity for water compared to the unmodified MIL-101(Cr), they efficiently removed H2S under humid conditions without framework degradation, whereas the pristine material did not. This was demonstrated by TGA-MS and elemental analysis and confirmed by density functional theory calculations. The developed approach offers a promising pathway for the design of advanced sorbents tailored for H2S removal in industrial and environmental applications.

在金属有机框架上添加多胺作为在潮湿条件下选择性去除 H2S 的有效策略
去除气流中的剧毒和腐蚀性硫化氢对于控制环境和若干工业流程至关重要。这篇论文报告了一种简单直接的策略,即用多胺对金属有机框架(MOFs)的开放金属位点进行功能化,从而设计出可在潮湿条件下高效去除硫化氢的吸附剂。研究人员成功地用乙二胺和三(2-氨基乙基)胺修饰了 MIL-101(Cr)MOFs,并使用 X 射线衍射、傅立叶变换红外光谱、核磁共振、氮吸附和热重分析 (TGA) 对所得到的材料进行了表征,从而证实了功能化。虽然与未改性的 MIL-101(Cr)相比,功能化的 MOFs 对水的亲和力更大,但在潮湿条件下,它们能有效地去除 H2S 而不发生框架降解,而原始材料则不能。TGA-MS 和元素分析证明了这一点,密度泛函理论计算也证实了这一点。所开发的方法为在工业和环境应用中设计专门用于去除 H2S 的先进吸附剂提供了一条前景广阔的途径。
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期刊介绍: ACS Applied Engineering Materials is an international and interdisciplinary forum devoted to original research covering all aspects of engineered materials complementing the ACS Applied Materials portfolio. Papers that describe theory simulation modeling or machine learning assisted design of materials and that provide new insights into engineering applications are welcomed. The journal also considers experimental research that includes novel methods of preparing characterizing and evaluating new materials designed for timely applications. With its focus on innovative applications ACS Applied Engineering Materials also complements and expands the scope of existing ACS publications that focus on materials science discovery including Biomacromolecules Chemistry of Materials Crystal Growth & Design Industrial & Engineering Chemistry Research Inorganic Chemistry Langmuir and Macromolecules.The scope of ACS Applied Engineering Materials includes high quality research of an applied nature that integrates knowledge in materials science engineering physics mechanics and chemistry.
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