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- 2019
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Tidskriftsartikel (refereegranskat)
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- Bjelic, Sinisa, et al.
(författare)
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Exploration of Alternate Catalytic Mechanisms and Optimization Strategies for Retroaldolase Design
- 2014
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Ingår i: Journal of Molecular Biology. - : Elsevier BV. - 0022-2836 .- 1089-8638. ; 426:1, s. 256-271
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Tidskriftsartikel (refereegranskat)abstract
- Designed retroaldolases have utilized a nucleophilic lysine to promote carbon-carbon bond cleavage of β-hydroxy-ketones via a covalent Schiff base intermediate. Previous computational designs have incorporated a water molecule to facilitate formation and breakdown of the carbinolamine intermediate to give the Schiff base and to function as a general acid/base. Here we investigate an alternative active-site design in which the catalytic water molecule was replaced by the side chain of a glutamic acid. Five out of seven designs expressed solubly and exhibited catalytic efficiencies similar to previously designed retroaldolases for the conversion of 4-hydroxy-4-(6-methoxy-2-naphthyl)-2-butanone to 6-methoxy-2-naphthaldehyde and acetone. After one round of site-directed saturation mutagenesis, improved variants of the two best designs, RA114 and RA117, exhibited among the highest kcat (>10(-3)s(-1)) and kcat/KM (11-25M(-1)s(-1)) values observed for retroaldolase designs prior to comprehensive directed evolution. In both cases, the >10(5)-fold rate accelerations that were achieved are within 1-3 orders of magnitude of the rate enhancements reported for the best catalysts for related reactions, including catalytic antibodies (kcat/kuncat=10(6) to 10(8)) and an extensively evolved computational design (kcat/kuncat>10(7)). The catalytic sites, revealed by X-ray structures of optimized versions of the two active designs, are in close agreement with the design models except for the catalytic lysine in RA114. We further improved the variants by computational remodeling of the loops and yeast display selection for reactivity of the catalytic lysine with a diketone probe, obtaining an additional order of magnitude enhancement in activity with both approaches.
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- Liu, Yi, et al.
(författare)
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Porous, robust, thermally stable, and flame retardant nanocellulose/polyimide separators for safe lithium-ion batteries
- 2023
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Ingår i: Journal of Materials Chemistry A. - : Royal Society of Chemistry (RSC). - 2050-7488 .- 2050-7496. ; 11:43, s. 23360-23369
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Tidskriftsartikel (refereegranskat)abstract
- The safety of lithium-ion batteries (LIBs) is paramount for all users. One effective way to improve safety is incorporating heat-resistant polyimide (PI) separators, which can increase the thermal stability of batteries and minimize the risk of thermal runaway. However, preparing PI separators with both an ideal pore structure and adequate mechanical properties remains as a challenge. Here, we introduced decabromodiphenyl ethane (DBDPE) and cellulose nanofibers (CNFs) into PI and produced a hybrid separator with an outstanding pore structure and excellent mechanical properties. Aided with DBDPE, the separators attain a well-defined and uniform pore size (20 nm), while demonstrating high porosities (78%) through phase inversion processes. Owing to the addition of CNFs, the mechanical properties of the separators were significantly improved, with a tensile strength of 25.4 MPa and an elastic modulus of 550.1 MPa. Moreover, the separators demonstrate high ion conductivity (0.45 mS cm-1), excellent thermal-dimensional stability (up to 200 degrees C), remarkable flame retardancy, and outstanding electrolyte wettability. At room temperature, the batteries with the separators demonstrate comparable performance with those of polypropylene (PP) separators. However, when subjected to thermal shock treatments, the batteries with the separators outperform those with PP, showcasing their superior performance. The work introduces a novel strategy for designing high-performance separators, thereby paving the way for advancements in the fabrication of LIBs with enhanced safety features. A porous, robust, and thermally stable hybrid separator was developed to solve the dilemma between desired pore structures and mechanical properties in polyimide separators by introducing decabromodiphenyl ethane and cellulose nanofibers.
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