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Breaking the trade-off between selectivity and adsorption capacity for gas separation.

ABSTRACT: The trade-off between selectivity and adsorption capacity with porous materials is a major roadblock to reducing the energy footprint of gas separation technologies. To address this matter, we report herein a systematic crystal engineering study of C₂H₂ removal from CO₂ in a family of hybrid ultramicroporous materials (HUMs). The HUMs are composed of the same organic linker ligand, 4-(3,5-dimethyl-1H-pyrazol-4-yl)pyridine, pypz, three inorganic pillar ligands, and two metal cations, thereby affording six isostructural pcu topology HUMs. All six HUMs exhibited strong binding sites for C₂H₂ and weaker affinity for CO₂. The tuning of pore size and chemistry enabled by crystal engineering resulted in benchmark C₂H₂/CO₂ separation performance. Fixed-bed dynamic column breakthrough experiments for an equimolar (v/v = 1:1) C₂H₂/CO₂ binary gas mixture revealed that one sorbent, SIFSIX-21-Ni, was the first C₂H₂ selective sorbent that combines exceptional separation selectivity (27.7) with high adsorption capacity (4 mmol·g^-1).

SUBMITTER: Kumar N

PROVIDER: S-EPMC8600127 | biostudies-literature | 2021 Nov

REPOSITORIES: biostudies-literature

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Breaking the trade-off between selectivity and adsorption capacity for gas separation.

Kumar Naveen N Mukherjee Soumya S Harvey-Reid Nathan C NC Bezrukov Andrey A AA Tan Kui K Martins Vinicius V Vandichel Matthias M Pham Tony T van Wyk Lisa M LM Oyekan Kolade K Kumar Amrit A Forrest Katherine A KA Patil Komal M KM Barbour Leonard J LJ Space Brian B Huang Yining Y Kruger Paul E PE Zaworotko Michael J MJ

Chem 20211111 11

The trade-off between selectivity and adsorption capacity with porous materials is a major roadblock to reducing the energy footprint of gas separation technologies. To address this matter, we report herein a systematic crystal engineering study of C2H2 removal from CO2 in a family of hybrid ultramicroporous materials (HUMs). The HUMs are composed of the same organic linker ligand, 4-(3,5-dimethyl-1H-pyrazol-4-yl)pyridine, pypz, three inorganic pillar liga ...[more]

PMID: 34825106

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Project description:BackgroundPhotoimmunotherapy involves targeted delivery of photosensitizers via an antibody conjugate (i.e., photoimmunoconjugate, PIC) followed by light activation for selective tumor killing. The trade-off between PIC selectivity and PIC uptake is a major drawback limiting the efficacy of photoimmunotherapy. Despite ample evidence showing that photoimmunotherapy is most effective when combined with chemotherapy, the design of nanocarriers to co-deliver PICs and chemotherapy drugs remains an unmet need. To overcome these challenges, we developed a novel photoimmunoconjugate-nanoliposome (PIC-Nal) comprising of three clinically used agents: anti-epidermal growth factor receptor (anti-EGFR) monoclonal antibody cetuximab (Cet), benzoporphyrin derivative (BPD) photosensitizer, and irinotecan (IRI) chemotherapy.ResultsThe BPD photosensitizers were first tethered to Cet at a molar ratio of 6:1 using carbodiimide chemistry to form PICs. Conjugation of PICs onto nanoliposome irinotecan (Nal-IRI) was facilitated by copper-free click chemistry, which resulted in monodispersed PIC-Nal-IRI with an average size of 158.8 ± 15.6 nm. PIC-Nal-IRI is highly selective against EGFR-overexpressing epithelial ovarian cancer cells with 2- to 6-fold less accumulation in low EGFR expressing cells. Successful coupling of PIC onto Nal-IRI enhanced PIC uptake and photoimmunotherapy efficacy by up to 30% in OVCAR-5 cells. Furthermore, PIC-Nal-IRI synergistically reduced cancer viability via a unique three-way mechanism (i.e., EGFR downregulation, mitochondrial depolarization, and DNA damage).ConclusionIt is increasingly evident that the most effective therapies for cancer will involve combination treatments that target multiple non-overlapping pathways while minimizing side effects. Nanotechnology combined with photochemistry provides a unique opportunity to simultaneously deliver and activate multiple drugs that target all major regions of a cancer cell-plasma membrane, cytoplasm, and nucleus. PIC-Nal-IRI offers a promising strategy to overcome the selectivity-uptake trade-off, improve photoimmunotherapy efficacy, and enable multi-tier cancer targeting. Controllable drug compartmentalization, easy surface modification, and high clinical relevance collectively make PIC-Nal-IRI extremely valuable and merits further investigations in living animals.

Dataset Information

Breaking the trade-off between selectivity and adsorption capacity for gas separation.

Publications

Breaking the trade-off between selectivity and adsorption capacity for gas separation.

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