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1.
J Am Chem Soc ; 146(31): 21721-21728, 2024 Aug 07.
Artigo em Inglês | MEDLINE | ID: mdl-39051979

RESUMO

A battery is composed of two electrodes that depend on and interact with each other. However, galvanostatic charging-discharging measurement, the most widely used method for battery evaluation, cannot simultaneously reflect performance metrics [capacity, Coulombic efficiency (CE), and cycling stability] of both electrodes because the result is generally governed by the lower-capacity electrode of the cell, namely the limiting reagent of the battery reaction. In studying stoichiometric Li-S cells operating under application-relevant high-mass-loading and lean-electrolyte conditions, we take advantage of the two-stage discharging behavior of sulfur to construct a simple framework that allows us to analyze both electrodes simultaneously. The cell capacity and its decay are anode performance descriptors, whereas the first plateau capacity and cell CE are cathode performance descriptors. Our analysis within this frame identifies Li stripping/plating and polysulfide shuttling to be the limiting factors for the cycling performance of the stoichiometric Li-S cell. Using our newly developed framework, we examine various previously reported strategies to mitigate these bottleneck problems and find modifying the separator with a reduced graphene oxide layer to be an effective means, which improves the capacity retention rate of the cell to 99.7% per cycle.

2.
Angew Chem Int Ed Engl ; 62(30): e202305251, 2023 Jul 24.
Artigo em Inglês | MEDLINE | ID: mdl-37235523

RESUMO

Photothermal CO2 reduction is one of the most promising routes to efficiently utilize solar energy for fuel production at high rates. However, this reaction is currently limited by underdeveloped catalysts with low photothermal conversion efficiency, insufficient exposure of active sites, low active material loading, and high material cost. Herein, we report a potassium-modified carbon-supported cobalt (K+ -Co-C) catalyst mimicking the structure of a lotus pod that addresses these challenges. As a result of the designed lotus-pod structure which features an efficient photothermal C substrate with hierarchical pores, an intimate Co/C interface with covalent bonding, and exposed Co catalytic sites with optimized CO binding strength, the K+ -Co-C catalyst shows a record-high photothermal CO2 hydrogenation rate of 758 mmol gcat -1 h-1 (2871 mmol gCo -1 h-1 ) with a 99.8 % selectivity for CO, three orders of magnitude higher than typical photochemical CO2 reduction reactions. We further demonstrate with this catalyst effective CO2 conversion under natural sunlight one hour before sunset during the winter season, putting forward an important step towards practical solar fuel production.

3.
Small ; 16(28): e2000040, 2020 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-32519511

RESUMO

Structures comprising high capacity active material are highly desirable in the development of advanced electrodes for energy storage devices. However, the structure degradation of such material still remains a challenge. The construction of amorphous and crystalline heterostructure appears to be a novel and effectual strategy to figure out the problem, owing to the distinct properties of the amorphous protective layer. Herein, crystalline-Co3 O4 @amorphous-TiO2 core-shell nanoarrays directly grown on the carbon cloth substrate are rationally designed to construct the free-standing electrode. In the unique structure, the 3D porous nanoarrays provide increased availability of electrochemical active sites, and the array with a unique heterostructure of crystalline Co3 O4 core and amorphous TiO2 shell exhibits intriguing synergistic properties. Besides, the amorphous TiO2 protective layer shows elastic behavior to mitigate the volume effect of Co3 O4 . Benefiting from these structural advantages, the as-prepared free-standing electrode exhibits superior lithium storage properties, including high coulombic efficiency, outstanding cyclic stability, and rate capability. Pouch cells with high flexibility are also fabricated and show remarkable electrochemical performances, holding great potential for flexible electronic devices in the future.

4.
Adv Healthc Mater ; : e2402136, 2024 Aug 18.
Artigo em Inglês | MEDLINE | ID: mdl-39155413

RESUMO

High H2O2 levels are widely present at the infection sites or in the biofilm microenvironment. Herein, hemin with peroxidase-like catalytic activity and its substrate, 2,2'-azino-bis(3-ethylbenzothiazoline-6-sulfonic acid) (ABTS), are simultaneously introduced into a liposomal nanoparticle containing thermosensitive 2,2'-azobis[2-(2-imidazolin-2-yl) propane] dihydrochloride (AIBI)-loaded bovine serum albumin (BAG), rationally constructing an H2O2-activatable liposomal nanobomb (Lipo@BHA) for combating biofilm-associated bacterial infections with high performance. In the presence of H2O2, hemin can catalyze the conversion of ABTS into its oxidized form (ABTS·+) with strong near-infrared (NIR) absorption, which produces photonic hyperpyrexia to cause the decomposition of AIBI into oxygen-independent alkyl radicals (·R) and nitrogen (N2) microbubbles. The former not only directly damage bacterial cells but also significantly accelerates the oxidization of ABTS to ABTS·+ for augmenting photothermal-triggered generation of ·R. Interestingly, the released N2 can induce transient cavitation to rupture lysosomal nanoparticle and improve the biofilm permeability, thereby enhancing the antibiofilm effect of Lipo@BHA. The proposed Lipo@BHA exhibits satisfactory multi-mode combination antibacterial properties. Through endogenous H2O2-activated cascade reaction, Lipo@BHA achieves remarkable hypoxia-irrelevant ·R therapy of biofilm-associated wound infections with low cytotoxicity and good in vivo biosafety. Therefore, this work presents a versatile H2O2-activatable cascade ·R generation strategy for biofilm-specific therapeutic applications.

5.
Adv Mater ; 35(42): e2302771, 2023 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-37278254

RESUMO

Increasing sulfur mass loading and minimizing electrolyte amount remains a major challenge for the development of high-energy-density Li-S batteries, which needs to be tackled with combined efforts of materials development and mechanistic analysis. This work, following the same team's most recent identification of the potential-limiting step of Li-S batteries under lean electrolyte conditions, seeks to advance the understanding by extending it to a new catalyst and into the high-sulfur-mass-loading region. CeOx nanostructures are integrated into cotton-derived carbon to develop a multifunctional 3D network that can host a large amount of active material, facilitate electron transport, and catalyze the sulfur lithiation reaction. The resulting S/CeOx /C electrode can deliver a stable areal capacity of 9 mAh cm-2 with a high sulfur loading of 14 mg cm-2 at a low electrolyte/sulfur ratio of 5 µL mg-1 . This study discovers that Li||S/CeOx /C cells usually fail during charging at high current density, as a consequence of local short circuiting caused by electrochemically deposited Li dendrites penetrating through the separator, a previously overlooked failure pattern distinctive to cells operating under lean electrolyte conditions. This work highlights the importance of developing new material structures and analyzing failure mechanisms in the advancement of Li-S batteries.

6.
J Oleo Sci ; 71(7): 935-946, 2022 Jul 01.
Artigo em Inglês | MEDLINE | ID: mdl-35691837

RESUMO

Large quantities of oils and proteins are demanded per year while their production needs environmentally friendly (green), safe, low cost, efficient and sustainable methods. Hydration method for producing Pinus armandi seed kernel oil and defatted meal rich in proteins was therefore developed, which had the following optimal conditions: baking kernels at 130 °C for 10 min, grinding them to pass through a 80-mesh sieve, mixing the ground kernel (10.00 g) with 1.00 mL of 8% brine or water and agitating at room temperature for 30 min. This method recovered 96.71% edible oil with vitamin E and K, phytosterols, carotenoids and squalene concentrated and de-oiled meal containing 57.98% proteins and 4.17% oils with ascorbic acid, thiamine, riboflavin, niacin, pantothenic acid, pyridoxine, folate, total phenolic and flavonoids concentrated. It had higher recovery rate and other physicochemical indices of edible oil and was found to be more sustainable as compared with cold pressing, enzyme-assisted aqueous extraction and solvent extraction.


Assuntos
Pinus , Antioxidantes/análise , Fenóis , Óleos de Plantas , Sementes/química , Água
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