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Ionic liquids screening for lignin dissolution: COSMO-RS simulations and experimental characterization
No full textAs the second most abundant terrestrial polymer, lignin has emerged as a major sustainable source for the production of fuels, chemicals, and materials. However, efficient screening of solvents for lignin dissolving faces great challenges. In this work, COSMO-RS was used to screen 3886 ionic liquids (ILs) composed of 58 cations and 67 anions, to find out the most effective ones for lignin dissolving by considering the critical items of logarithmic infinite dilution activity coefficient (ln gamma(infinity)) and sigma-profiles. The substantial improvement of lignin dissolution was achieved in [PMpyrr][OAc] IL by both simulations and experiments validations. Moreover, it was found that the anions dominate the dissolution process and the strongly polar anions exhibit better dissolution ability. Furthermore, the underlying mechanism originated from the hydrogen bond (H-bond) between ILs and lignin was also revealed and systemically analyzed from donor and acceptor ability, indicating that high lignin solubility is reached in the ILs with stronger ability to form H-bond acceptors. This work leads to possible ways toward developing more selective and efficient lignin dissolution methods based on solvent properties. (C) 2021 Elsevier B.V. All rights reserved
@Robust enhancing stability and fructose tolerance of sucrose phosphorylase by immobilization on Ni-NTA functionalized agarose microspheres for the biosynthesis of 2-alpha-glucosylglycerol
No full textSucrose phosphorylase (SPase) is a carbohydrate-active enzyme with outstanding potential for the biocatalytic conversion of sucrose and glycerol into 2-alpha-glucosylglycerol (2-alpha-GG) with attractive properties. However, poor stability, lack of appropriate immobilization strategy and serious inhibition of fructose by-products significantly restrict the industrial application of SPase. In this study, a new recombinant SPase from the Bifidobacterium Magian was specifically immobilized by agarose microspheres with Ni2+-nitrotriacetic acid for significantly enhancing its stability and fructose tolerance. Agarose immobilization greatly improved the stability of SPase. At 50 degrees C, the relative activity of the immobilized SPase (95%) was obviously greater than that of the free SPase (55%). Moreover, immobilized SPase exhibited excellent reusability and storage stability, retaining over 60% of its initial activity after 15 cycles, maintaining 70% relative activity after 15 days. It was first found that SPase immobilized by agamse still hold 98% activity even under 0.6 M fructose. Based on Raman spectrum analysis, agarose immobilization significantly enhanced the beta-sheet structures of SPase, which helped to maintain its efficient catalytic performance under extreme environment and high inhibitor concentration. Immobilized SPase based on agamse would have a brilliant future in the production of 2-alpha-GG
Pickering interfacial biocatalysis with enhanced diffusion processes for CO2 mineralization
No full textUtilization of carbon dioxide (CO2) has become a crucial and anticipated solution to address environmental and ecological issues. Enzymes such as carbonic anhydrase (CA) can efficiently convert CO2 into various platform chemicals under ambient conditions, which offers a promising way for CO2 utilization. Herein, we constructed a Pickering interfacial biocatalytic system (PIBS) stabilized by CA-embedded MOFs (ZIF-8 and ZIF-L) for CO2 mineralization. Through structure engineering of MOFs and incorporation of Pickering emulsion, the internal and external diffusion processes of CO2 during the enzymatic mineralization were greatly intensified. When CO2 was ventilated at a flow rate of 50 mL min(-1) for 1 h, the pH value of PIBS dropped from similar to 8.00 to similar to 6.50, while the average pH value of free system only dropped to similar to 7.15, indicating that the initial reaction rate of CO2 mineralization of PIBS is nearly twice that of the free system. After the 8th cycle reaction, PIBS can still produce more than 9.8 mg of CaCO3 in 5 min, realizing efficient and continuous mineralization of CO2. (c) 2022, Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. All rights reserved
High molecular weight chitosan oligosaccharide exhibited antifungal activity by misleading cell wall organization via targeting PHR transglucosidases
No full textThe fungal cell wall is an ideal target for the design of antifungal drugs. In this study we used an analog of cell wall polymer, a highly deacetylated high molecular-weight chitosan oligosaccharide (HCOS), to test its effect against pathogenic Candida strains. Results showed that HCOS was successfully incorporated into the dynamic cell wall organization process and exhibited an apparent antifungal activity against both plankton and mature fungal biofilm, by impairing the cell wall integrity. Unexpectedly, mechanistic studies suggested that HCOS exerts its activity by interfering with family members of PHR beta-(1,3)-glucanosyl transferases and affecting the connection and assembly of cell wall polysaccharides. Furthermore, HCOS showed great synergistic activity with different fungicides against Candida cells, especially those in biofilm. These findings indicated HCOS has a great potential as an antifungal drug or drug synergist and proposed a novel antifungal strategy with structure-specific oligosaccharides mimicking cell wall polysaccharide fragments
Directing electrochemical reaction mechanism via interfacial control for better sulfur cathode
No full textThe "shuttle effect" in ether electrolyte or nucleophilic reaction in carbonate electrolyte are major obstacles to developing of lithium-sulfur (Li-S) batteries. Superficial sulfur on the outside of microporous carbon host can occur"shuttle effect" in ether electrolyte or nucleophilic reaction in carbonate electrolyte, which may affect the electrochemical reaction mechanism for lithium-sulfur batteries and need to be further clarified. Herein, we rationally designed microporous carbon and non-microporous carbon as the sulfur hosts, and manipulated the distribution of sulfur via interfacial control in cathode material, exhibiting diverse electrochemical behavior in carbonate electrolyte and ether electrolyte. The surface composition of the electrode was confirmed by ex-situ XPS and verified by in-situ XRD, which contributes to demonstrating the definite reaction mechanisms of lithium-sulfur batteries in the different electrolytes. The results show only the sulfur confined in microporous structure is active via "solid-solid" pathway, and the presence of sulfur on the outer surface of the cathode electrode has the negative effect on electrochemical performance in both electrolytes, which should be avoided in the fabrication of carbon/sulfur composites. Based on microporous carbon/sulfur composites, the lithiated GeS full cell was proposed and exhibited superior cycling performance and high Coulombic Efficiency
Support project for outstanding young talents in colleges and universities in Anhui Province[qxyq2021228]
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A novel strategy of lithium recycling from spent lithium-ion batteries using imidazolium ionic liquid
No full textIn light of the increasing demand for environmental protection and energy conservation, the recovery of highly valuable metals, such as Li, Co, and Ni, from spent lithium-ion batteries (LIBs) has attracted widespread attention. Most conventional recycling strategies, however, suffer from a lack of lithium recycling, although they display high efficiency in the recovery of Co and Ni. In this work, we report an efficient extraction process of lithium from the spent LIBs by using a functional imidazolium ionic liquid. The extraction efficiency can be reached to 92.5% after a three-stage extraction, while the extraction efficiency of Ni-Co-Mn is less than 4.0%. The new process shows a high selectivity of lithium ion. FTIR spectroscopy and ultraviolet are utilized to characterize the variations in the functional groups during extraction to reveal that the possible extraction mechanism is cation exchange. The results of this work provide an effective and sustainable strategy of lithium recycling from spent LIBs. (C) 2021 The Chemical Industry and Engineering Society of China, and Chemical Industry Press Co., Ltd. All rights reserved
Developing and Regenerating Cofactors for Sustainable Enzymatic CO2 Conversion
No full textEnzymatic CO2 conversion offers a promising strategy for alleviating global warming and promoting renewable energy exploitation, while the high cost of cofactors is a bottleneck for large-scale applications. To address the challenge, cofactor regeneration is usually coupled with the enzymatic reaction. Meanwhile, artificial cofactors have been developed to further improve conversion efficiency and decrease cost. In this review, the methods, such as enzymatic, chemical, electrochemical, and photochemical catalysis, developed for cofactor regeneration, together with those developed artificial cofactors, were summarized and compared to offer a solution for large-scale enzymatic CO2 conversion in a sustainable way
InOOH as an efficient bidirectional catalyst for accelerated polysulfides conversion to enable high-performance lithium-sulfur batteries
No full textLithium-sulfur (Li-S) batteries with the prominent advantages are greatly expected to be the attractive alternatives in the next-generation energy-storage systems. However, the practical success of Li-S batteries suffers from the shuttle effect and depressed redox kinetics of polysulfides. Herein, for the first time, InOOH nanoparticles are employed as a potent catalytic additive in sulfur electrode to overcome these issues. As demonstrated by the theoretical and experimental results, the strong interactions between the InOOH nanoparticles and sulfur species enable the effective adsorption of polysulfides. More significantly, InOOH nanoparticles not only effectively expedite the reduction of sulfur during the discharge process, but also dramatically accelerate the oxidation of Li2S during the charge process, presenting the marvelous bidirectional catalytic effects. Benefited from these distinctive superiorities, the cells with InOOH nanoparticles harvest an excellent capacity retention of 69.5% over 500 cycles at 2C and a commendable discharge capacity of 891 mAh g1under a high-sulfur loading of 5.0 mg cm2. The detailed investigations in this work provide a novel insight to ameliorate the Li-S electrochemistry by the bidirec-tional catalyst for high-performance Li-S batteries. (c) 2021 Elsevier Inc. All rights reserved