Guangping Lei,Guojun Xi,Zihan Liu,Qibin Li,Huiyuan Cheng,Hantao Liu
Efficient capture and separation of CO 2 from flue gas and natural gas are highly promising to reduce carbon emissions and promote fuel calorific value. Here, a novel adsorbent (FeTPPs@Cu-BTC) for CO 2 separation was synthesized by encapsulating 5, 10, 15, 20-tetrakis (4-sulfonatophenyl) porphyrinato iron (III) chloride (FeTPPs) into the cages of Cu-BTC through an in-situ packaging strategy. Such strategy efficiently overcomes the shortcoming of pore clogging and leaching induced by incorporating guest molecules through the wet impregnation method. Meanwhile, more tunable micropores and extra affinity sites for CO 2 adsorption were created after encapsulation of FeTPPs, which preferably enhanced the CO 2 uptakes of FeTPPs@Cu-BTC under low pressures and promoted the separation performances for CO 2 /N 2 (15:85, v/v) and CO 2 /CH 4 (50:50, v/v) mixtures. The corresponding selectivity of FeTPPs@Cu-BTC calculated by ideal adsorbed solution theory (IAST) respectively increase to 57.7 and 14.0 from 36.0 and 10.8 of the pristine Cu-BTC at 273 K and 100 kPa, which also exceeds most reported adsorbents. Grand Canonical Monte Carlo (GCMC) simulations further elucidated that extra interaction with CO 2 and ‘sieve effect’ for N 2 or CH 4 after FeTPPs encapsulation immediately boost CO 2 uptakes and separation performance of FeTPPs@Cu-BTC. This study provides a new design idea for the development of new adsorbent materials.
Bin Xiao,Junhao Xiao,Sisi Liu,Xiaoying Xiao,Shengping Dai,Yan Sui,Jinming Wu,Huixian Ye
Human calcitonin (hCT) is an endogenous polypeptide commonly employed in treating bone resorption-related illnesses, but its clinical application is limited due to its high aggregation tendency. Metalloporphyrins are effective in suppressing amyloid fibrillation, positioning them as potential drug candidates for amyloidogenic disorders like Alzheimer's and type 2 diabetes. In this work, we investigated the effects of Fe(III) meso-tetra(4-sulfonatophenyl)porphine chloride (FeTPPS), a highly efficient ONOO− decomposition catalyst, on hCT aggregation. Our findings reveal that FeTPPS effectively precludes hCT fibrillation by stabilizing the monomers and delaying the structural transition from α-helix bundles to β-sheet-rich aggregates. The macrocyclic ring of FeTPPS plays a significant role in disrupting hCT self-associations. Among various porphyrin analogs, those with an iron center and negatively charged peripheral substituents exhibit a stronger inhibitory effect on hCT aggregation. Spectroscopic analyses and computational simulations indicate that FeTPPS binds to hCT's core aggregation region via complexation with His20 in a 1 : 1 molar ratio. Hydrophobic interaction, hydrogen bonding, and π–π stacking with the residues involving Tyr12, Phe19, and Ala26 also contribute to the interactions. Collectively, our study provides a promising approach for developing novel hCT drug formulations and offers theoretical guidance for designing metalloporphyrin-based inhibitors for various amyloidosis conditions.
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