Flexible Dual Fe-based Catalyst: MIL-53(Fe) Loaded with Deep Eutectic Solvent for Discontinuous Selective Oxidation of H2S

Fengke Wang, Chaofan Li, Weizhen Kong, Shucan Qin, Qianqian Peng,Lihua Zang,Yunqian Ma, Yi Nie,Guihuan Yan

AEROSOL AND AIR QUALITY RESEARCH(2024)

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摘要
Deep eutectic solvent (DES) as the guest molecule and flexible Metal -organic framework (MOF) as the supporting material can be used to provide an efficient catalyst: flexible dual Fe -based DES@MOF, which can efficiently remove H2S in discontinuous removal process (100-180 degrees C). The materials were characterized by XRD SEM, FT-IR, BET, XPS, TG, CV and Py-FTIR. According to the result, MOF (MIL-53(Fe)) incorporating 30 wt% DES (ChCl/FeCl3) exhibited the best H2S removal performance at 180 degrees C, with the H2S removal capacity of 2527 mg mL-1(3744 mg g-1). And the H2S removal capacity reduced by 9% after two cycles of thermal regeneration. The process of desulfurization includes two stages: catalytic oxidation and adsorption, which are determined by the Fe3+ in DES and the structural characteristics, such as the aggregation of mesopores, respectively. For MIL-53(Fe), FeOOH as an intermediate and Lewis acid sites also played a catalytic role. Elemental sulfur was the predominant product with a small amount of sulfate. Both elemental sulfur and DES can induce the flexible deformation of MOF as the guest molecule to relieve the passivation of catalyst.
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关键词
Deep eutectic solvent,Metal-organic framework,Catalytic oxidation,H2S removal,Flexible deformation
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