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1.
Science ; 376(6597): 1105-1110, 2022 06 03.
Artigo em Inglês | MEDLINE | ID: mdl-35653467

RESUMO

The design of materials and their manufacture into membranes that can handle industrial conditions and separate complex nonaqueous mixtures are challenging. We report a versatile strategy to fabricate polytriazole membranes with 10-nanometer-thin selective layers containing subnanometer channels for the separation of hydrocarbons. The process involves the use of the classical nonsolvent-induced phase separation method and thermal cross-linking. The membrane selectivity can be tuned to the lower end of the typical nanofiltration range (200 to 1000 gram mole-1). The polytriazole membrane can enrich up to 80 to 95% of the hydrocarbon content with less than 10 carbon atoms (140 gram mole-1). These membranes preferentially separate paraffin over aromatic components, making them suitable for integration in hybrid distillation systems for crude oil fractionation.

2.
Mater Horiz ; 8(5): 1518-1527, 2021 May 01.
Artigo em Inglês | MEDLINE | ID: mdl-34846460

RESUMO

Metal- and halide-free, solid-state water vapor sorbents are highly desirable for water-sorption-based applications, because most of the solid sorbents suffer from low water sorption capacity caused by their rigid porosity, while the liquid sorbents are limited by their fluidity and strong corrosivity, which is caused by the halide ions. Herein, we report a novel type of highly efficient and benign polymeric sorbent, which contains no metal or halide, and has an expandable solid state when wet. A group of sorbents are synthesized by polymerizing and crosslinking the metal-free quaternary ammonium monomers followed by an ion-exchange process to replace chloride anions with benign-anions, including acetate, oxalate, and citrate. They show significantly reduced corrosivity and improved water sorption capacity. Importantly, the water sorption capacity of the acetate paired hydrogel is among the best of the literature reported hygroscopic polymers in their pure form, even though the hydrogel is crosslinked. The hydrogel-based sorbents are further used for water-sorption-driven cooling and atmospheric water harvesting applications, which show improved coefficient of performance (COP) and high freshwater production rate, respectively. The results of this work would inspire more research interest in developing better water sorbents and potentially broaden the application horizon of water-sorption-based processes towards the water-energy nexus.

3.
Adv Mater ; 32(25): e2000732, 2020 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-32410270

RESUMO

Most reported carbonaceous anodes of potassium-ion batteries (PIBs) have limited capacities. One approach to improve the performance of carbon anodes is edge-nitrogen doping, which effectively enhances the K-ion adsorption energy. It remains challenging to achieve high edge-nitrogen doping due to the difficulty in controlling the nitrogen dopant configuration. Herein, a new synthesis strategy is proposed to prepare carbon anodes with ultrahigh edge-nitrogen doping for high-performance PIBs. Specifically, self-assembled supermolecule precursors derived from pyromellitic acid and melamine are directly pyrolyzed. During the pyrolysis process, the amidation and imidization reactions between pyromellitic acid and melamine before carbonization enable the successful carbonization of pyromellitic acid-melamine supermolecule. The obtained 3D nitrogen-doped turbostratic carbon (3D-NTC) possesses a 3D framework composed of carbon nanosheets, turbostratic crystalline structure, and an ultrahigh edge-nitrogen-doping level up to 16.8 at% (73.7% of total 22.8 at% nitrogen doping). These features endow 3D-NTCs with remarkable performances as PIB anodes. The 3D-NTC anode displays a high capacity of 473 mAh g-1 , robust rate capability, and a long cycle life of 500 cycles with a high capacity retention of 93.1%. This new strategy will boost the development of carbon anodes for rechargeable alkali-metal-ion batteries.

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