ACS Synthetic Biology
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2024
·
IF 3.7
Tianfu Wu,Yihan Chen,Wanqing Wei,Wei Song,Jing Wu,Jian Wen,Guipeng Hu,Xiaomin Li,Cong Gao,Xiulai Chen,Liming Liu
Aromatic d-amino acids (d-AAs) play a pivotal role as important chiral building blocks and key intermediates in fine chemical and drug synthesis. Meso-diaminopimelate dehydrogenase (DAPDH) serves as an excellent biocatalyst in the synthesis of d-AAs and their derivatives. However, its strict substrate specificity and the lack of efficient engineering methods have hindered its widespread application. Therefore, this study aims to elucidate the catalytic mechanism underlying DAPDH from Proteus vulgaris (PvDAPDH) through the examination of its crystallographic structure, computational simulations of potential energies and molecular dynamics simulations, and site-directed mutagenesis. Mechanism-guided computational design showed that the optimal mutant PvDAPDH-M3 increased specific activity and catalytic efficiency (kcat/Km) for aromatic keto acids up to 124-fold and 92.4-fold, respectively, compared to that of the wild type. Additionally, it expanded the substrate scope to 10 aromatic keto acid substrates. Finally, six high-value-added aromatic d-AAs and their derivatives were synthesized using a one-pot three-enzyme cascade reaction, exhibiting a good conversion rate ranging from 32 to 84% and excellent stereoselectivity (enantiomeric excess >99%). These findings provide a potential synthetic pathway for the green industrial production of aromatic d-AAs.
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ANALYTICAL CHEMISTRY
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2025
·
IF 6.7
Mubalake Rehemaitijiang,Gaosheng Li,Rongchao Zhu,Baiyi Zu,Xincun Dou,Zhi Su,Zhenzhen Cai
The rational design of the D-π-A chemodosimeter with a significant Stokes shift is of great importance for enhancing the visualization of optical sensing signals. Here, three D-π-A fluorescent chemodosimeters with 2-(3-cyano-4,5,5-trimethylfuran-2(5H)-ylidene) malononitrile (TCF) as the electron-withdrawing group are synthesized by precisely modulating the electron-releasing strength. By decreasing the ability of electron release, the electrophilicity of the recognition site is increased by 1.449 kcal/mol, the Stokes shift of the chemodosimeter is improved to 201 nm, and the sensing mode changes from fluorescence quenching to ratiometric fluorescence and finally to fluorescence on. Furthermore, the three D-π-A fluorescent chemodosimeters display superior sensing performance toward ClO–, including low limits of detection (LOD, 37.0, 5.1, and 1.0 nM), rapid response (<5 s), and great selectivity in the presence of 16 kinds of interferents. Moreover, the practicality of the chemodosimeters is further validated by a portable triple-standard quantitative array detection platform, which can quantitatively detect ClO– solutions. The proposed design and modulation strategy for chemodosimeters can provide a new pathway for the sensitive and visualized identification of oxidants and other hazardous chemicals.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
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IF 9.7
Xing Zhang,Peng Deng,Mengyang Zheng,Yanling Hao,Xiu Gong,Fuzhong Gong,Jing-Chang Li
Anion redox reactions in layered cathode materials have attracted significant attention due to their remarkable potential to enhance the capacity and energy density of lithium-ion batteries. However, in conventional sulfide-based cathodes such as Li x TiS 2 , anionic redox is only partially reversible at high voltages and suffers from rapid capacity fading. These challenges primarily originate from the intrinsic electronic band structure of Li x TiS 2 , where the Ti 3+ /Ti 4+ redox couple lies far above the S 3 p band, suppressing ligand-to-metal charge transfer during Li + (de)intercalation. To overcome this limitation, we introduce a bandgap-engineering strategy via partial substitution of Ti 3+ with Cr 3+ , effectively narrowing the d- p bandgap and activating sustainable sulfur redox chemistry. The Cr-substituted compound, Li 0.80 Cr 0.67 Ti 0.33 S 2 , exhibits sustainable sulfur redox activity, thereby achieving a higher capacity of 223.0 mA h g −1 and nearly doubling the energy density of pristine Li 0.80 TiS 2 . Furthermore, Li 0.80 Cr 0.67 Ti 0.33 S 2 preserves its layered framework throughout the whole (de)lithiation process, indicating effective suppression of structural collapse during sulfur redox. Therefore, it demonstrates outstanding rate performance (77.5% capacity retention at 5.0C) and excellent long-term cycling stability (80% retention after 330 cycles), significantly outperforming its undoped counterpart. These findings highlight the critical role of ligand-metal d- p orbital overlap in enabling and stabilizing sustainable sulfur redox, providing valuable insights for the design of high-performance cathodes for next-generation lithium-ion batteries.
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Frontiers in Pharmacology
·
2022
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IF 5.988
Jinfu Peng,Guoping Yang,Zhijun Huang
This study aimed to determine the effect of vitamin D (VD) deficiency on the efficacy and pharmacokinetics of pravastatin and clarify whether the effects are mediated by Organic anion-transporting polypeptides (OATPs). Experiments were conducted in rats to explore the effect of VD deficiency on the pharmacodynamics and pharmacokinetics of pravastatin. In the pharmacodynamic study, rats were fed a VD-free or VD-supplement high-fat diet for 25–30 days, and plasma 25(OH)VD was dynamically monitored. The response of pravastatin (changes in blood lipids) on rats were then examined after 15 days of pravastatin treatment. In the pharmacokinetic study, rats were fed a VD-free or VD-supplement diet for 25–30 days. The pharmacokinetics of single oral dose pravastatin was then studied, and intestinal and hepatic Oatp1a1 and Oatp2b1 expression was determined using quantitative polymerase chain reaction (qPCR) and western blot. Furthermore, OATP1B1 and OATP2B1 expression in Huh7 cells with or without 1.25(OH) 2 D were assessed via qPCR and western blot. For the pharmacodynamic study, the decrease of total cholesterol and increase of high-density lipoprotein cholesterol in VD-deficient rats were smaller than in VD-sufficient rats, indicating that VD deficiency reduced the response of pravastatin in rats. For the pharmacokinetic study, the plasma exposure slightly increased, and liver exposure decreased in VD-deficient rats, but not significantly. VD deficiency decreased the Oatp1a1 and Oatp2b1 expression in the liver, but not in the small intestine. Similarly, OATP1B1 and OATP2B1 protein levels in Huh7 cells were reduced when 1.25(OH) 2 D was absent. In conclusion, VD deficiency can decrease the response of pravastatin in rats by reducing the liver pravastatin exposure and expression of hepatic OATPs, consistent with the extended hepatic clearance model theory.
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JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
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2018
·Vol. 94
·期 4
·1220-1229
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IF 2.587
Weide Xiong,Xianhai Zeng,Shih-Hsin Ho,Xueping Ling,Liang Shen,Chuanyi Yao,Yinghua Lu
BACKGROUND Phospholipase D (PLD) has great potential in the pharmaceutical and food industries for manufacturing bioactive phospholipids. Overproduction of PLD in Escherichia coli is difficult due to its high cytotoxicity which causes plasmid instability, short-term PLD synthesis, cell lysis and PLD leakage. To address this issue, integrated optimization of PLD production in upstream and downstream processing was performed. RESULTS Effective strategies in upstream processing include the use of plasmids containing the pSC101 par region in recA − E. coli , the use of moderately strong and tightly regulated promoter P BAD , optimization of codon usage and amino acid supplementation, maintaining the best cellular state by supplementing nutrition, and saturation induction at low temperature. Using these strategies, a large amount of PLD (1.2 × 10 5 U L −1 , 81.5 mg L −1 ) was obtained in the batch culture and PLD synthesis lasted 9 h. Additionally, cell lysis did not occur –99% of the recombinant PLD remained in the periplasm. Ultimately, the PLD was purified 327-fold by a four-step downstream process comprising extraction with 10 mmol L −1 Ethylenediaminetetraacetic acid and 0.05% (w/v) sodium deoxycholate, ammonium sulfate precipitation, anion exchange and Ni 2+ -affinity chromatography. CONCLUSION This study provides the basis for large-scale production of PLD in E. coli . © 2018 Society of Chemical Industry
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Journal of Energy Chemistry
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2025
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IF 14.9
Lina Hu,Zengyu Han,Ya Chen,Yaoda Liu,Lei Li,Jie Su,Zhengfei Dai,Dong-Shuang Wu
The development of pH‐robust electrocatalysts is highly desirable but challenging for the hydrogen evolution reaction (HER) in water electrolysis. Among the noble metal groups, ruthenium (Ru) holds the promise in balancing the cost and activity in HER, but it is restricted by the strong H adsorption and the sluggish Heyrovsky step. It appeals for a rational d -band manipulation to neutralize the hydrogen adsorption to promote the HER kinetics. Herein, we profiled a confined structure with RuCo alloy nanoparticles in N-doped carbon nanofiber (RuCo@NCNF) by a facile electrospinning-pyrolysis process for HER electrocatalysis. An electron transfer from Co to Ru is indicated in the RuCo@NCNF composite to enhance the electron-donating character of Ru active sites to couple the HER. Resultantly, the optimized Ru 1 Co 2.5 @NCNF catalyst stably exhibits the Pt-beyond HER activity in both alkaline (10 mV at 10 mA cm −2 ) and acidic electrolytes (23 mV at 10 mA cm −2 ), while delivering competitive HER performance in neutral electrolytes. Density functional theory (DFT) calculations also confirm that the Ru-Co electronic interactions can effectuate the d -band center downshift, moderating the adsorption energies of hydrogen (Δ G H* ) and H 2 O for efficient hydrogen production. This study provides a reference for the rational design of Ru-based pH-robust HER electrocatalyst through confined nanoalloy structures.
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Metabolic Engineering Communications
·
2018
·
IF 0
Xiaojing Jia,Robert M. Kelly,Yejun Han
( R )-acetoin is a four-carbon platform compound used as the precursor for synthesizing novel optically active materials. Ethylene glycol (EG) is a large-volume two-carbon commodity chemical used as the anti-freezing agent and building-block molecule for various polymers. Currently established microbial fermentation processes for converting monosaccharides to either ( R )-acetoin or EG are plagued by the formation of undesirable by-products. We show here that a cell-free bioreaction scheme can generate enantiomerically pure acetoin and EG as co-products from biomass-derived D -xylose. The seven-step, ATP-free system included in situ cofactor regeneration and recruited enzymes from Escherichia coli W3110, Bacillus subtilis shaijiu 32 and Caulobacter crescentus CB 2. Optimized in vitro biocatalytic conditions generated 3.2 mM ( R )-acetoin with stereoisomeric purity of 99.5% from 10 mM D -xylose at 30 °C and pH 7.5 after 24 h, with an initial ( R )-acetoin productivity of 1.0 mM/h. Concomitantly, EG was produced at 5.5 mM, with an initial productivity of 1.7 mM/h. This in vitro biocatalytic platform illustrates the potential for production of multiple value-added biomolecules from biomass-based sugars with no ATP requirement.
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ACS Sensors
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2025
·
IF 9.1
Changle Pei,Muhammad Hamza Nadeem,Nan Li,Jun Fu,Nan Xu,You Wang,Adrian Carl Stevenson,Guang Li,Ruifen Hu
The complexity of in situ volatile organic compounds (VOCs) detection demands high selectivity and anti-interference capability of electronic noses (E-noses). Multivariant virtual sensor array (VSA) is a new generation of E-noses under research to overcome the insufficient VOCs selectivity limitation of existing electronic noses and alleviate the issue of sensor drifts. In this paper, a frequency-amplitude dual-parameter modulation strategy is presented on a wireless electrodeless quartz crystal microbalance with dissipation (WE-QCM-D) to realize the recognition and analysis of VOC mixtures and complex real-world analytes with a single multivariant VSA E-nose, by probing the gas dynamic sorption in a sensitive film at various scales of oscillating shear displacements and obtaining multiple partially independent responses to VOCs. Ten VOC analytes from alcohols, esters, and aromatic hydrocarbons were classified with accuracies of above 95% for both interclass and intraclass discriminations. Additionally, a discriminating accuracy of 95% has been achieved on VOC mixtures, and their component concentrations were predicted with coefficients of determination above 0.9. For practical testing, the system was exposed to the headspace VOCs of banana, pineapple, and mango under different concentrations. It recognized different fruits and identified the ripen state of bananas based on the detection of their volatiles. The dual-parameter modulated WE-QCM-D paves a promising multivariant way to realize online real-time VOCs monitoring with high performance on selectivity and quantitative analysis.
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Nano Energy
·
2020
·
IF 16.602
Zheng Zhou,Xiangxin Du,Zhao Zhang,Jikui Luo,Shaoyu Niu,Da Shen,Yuanyu Wang,Hui Yang,Qilong Zhang,Shurong Dong
Flexible piezoelectric nanogenerator (PENG) has been regarded as one of the promising solutions to harvesting mechanical energy, as a sustainable energy source for wearable devices , etc. Here, a universal strategy of carbon coating modulation is proposed to synthesis carbon coated 0-D piezoceramics nanoparticles (NPs). Owing to the good electric conductivity of carbon shell, the redistribution and accumulation of mobile charges in carbon layer gives rise to reinforcement of electric field, results in the much-enhanced piezoelectric effect. Polydimethylsiloxane (PDMS) composites with those 0-D piezoceramics NPs are used to fabricate PENGs. The peak power density of BT@C, PZT@C and KNN@C based PENGs reaches up to 45.4 μW/cm 2 , 59.8 μW/cm 2 and 9.9 μW/cm 2 , that are 20, 20.4 and 13.4 times larger than those of control PENGs incorporated with bare 0-D piezoceramic NPs, respectively. A theoretical model based on Lewis diffusion theory is constructed to reveal the mechanism of piezoelectric enhancement in the poling process. This research provides a new strategy for synthesis of high piezoelectric characteristic composites by embedding carbon coated 0-D piezoceramic NPs.
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JOURNAL OF MOLECULAR LIQUIDS
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2021
·
IF 6.165
Yannan Du,Hongjun Zang,Yimo Feng,Kai Wang,Yaxin Lv,Zhipeng Liu
This paper briefs the emerging strategies for the designing of catalytic systems, which direct conversion of chitin biomass monomer N -acetyl- d -glucosamine (NAG) to 3-acetylamino-5-acetylfuran was studied systemically. Twelve catalysts were investigated, and pyrazine hydrochloride ([Pyz]Cl) ionic liquid exhibited the good performance-achieving 3A5AF with yields of 36.94% from NAG . Further adding boric acid and CaCl 2 , treating at 190 °C for 60 min, the conversion rate of NAG is 100%, and the yield of 3A5AF can be increased to 69.54% in DMA. Furthermore, functional group changes before and after the reaction have been characterized by FTIR, HPLC-MS and 13 C NMR were applied to monitor the reaction process with [Pyz]Cl as the catalyst. The reactive intermediate was clearly detected by these techniques. Accordingly, a possible reaction pathway was proposed. The results of this experiment provide a mild and efficient reaction route for the degradation of biomass, and enrich the theoretical research of quaternary amine catalysts in the conversion of biomass waste into high value-added chemicals.
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DYES AND PIGMENTS
·
2023
·
IF 4.5
Peiyu Wu,Shengxiong Zhang,Wenjun Zhang,Weijie Song
Dual functional electrochromic (EC)/electrofluorochromic (EFC) materials play a pivotal role in wearable and smart electronic equipments. Developing new materials with high performance of EC/EFC properties is still a big challenge. Here a new D-A structure polymer PPDOTTPD based on thieno(3,4-c)pyrrole-(4,6)dione ( TPD ) was synthesized by Stille coupling, and the EC/EFC properties were investigated for the first time. PPDOTTPD film exhibits reversible color changes from purple neutral state to transparent colored state in the process of reversible redox. Photophysical and electrochemical studies revealed that the polymer has outstanding EC properties, including high optical contrast (52%), fast response time (0.5 s/0.7 s), high coloring efficiency (427.1 cm 2 C −1 ) and good stability. What's more, PPDOTTPD exhibited EFC phenomenon. PPDOTTPD film showed an intense red near-infrared fluorescence with a peak of 672 nm, which gradually doped with the increase of applied potential with a maximum contrast ratio of 12.9. The EC/EFC dual-functional device based on PPDOTTPD was also successfully fabricated, which exhibited high optical and fluorescence contrast. The fine dual-functional performance indicates TPD can be further explored as potential acceptors for synthesizing high performance D-A molecules for intelligent optical devices.
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JOURNAL OF COORDINATION CHEMISTRY
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2020
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IF 1.41
Kun Lu,Zihan Zhu,Lin Peng,Hai Fu,Xinlong Wang,Enbo Wang
An unusual metal-organic framework, {H[Ag(I)L][Mo(VI)4O13]}n (1) (L=(4-((1H-1,2,4-triazol-1-yl)methyl)phenyl)methanol)), has been obtained under ionothermal conditions. According to the single-crystal X-ray diffraction analysis, 1 is a new 3-D framework based on β-[Mo8O26]4− type polymolybdate anions with two kinds of channels (A and B) along the b-axes and c-axes in the framework. The neighboring inorganic Mo8-Ag chains are linked by the organic ligands through the Ag centers resulting in 2-D layers. These adjacent 2-D layers extend into a 3-D framework through Ag1 nodes and β-[Mo8O26]4− anions, respectively, resulting in a topological symbol (64 · 82)2(64 · 82). In addition, the gas adsorption, proton conduction and luminescent properties of 1 are also discussed in detail. Moreover, the electrochemical impedance spectroscopy (EIS) measurements show a conductivity (1.9 × 10−4 S cm−1 at 65 °C and 95% relative humidity (RH)), with an activation energy of 0.41 eV for 1. The mechanism of proton conduction for 1 is proved to be the vehicular mechanism.
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