JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
·
IF 9.4
Xiaofei Zhou,Guijuan Wei,Chang Liu,Qian Zhao,Hui Gao,Wenbo Wang,Xixia Zhao,Xin Zhao,Honglei Chen
The production of hydrogen through seawater electrolysis has recently garnered increasing concern. However, hydrogen evolution reaction (HER) by alkaline seawater electrocatalysis is severely impeded by the slow H 2 O adsorption and H* binding kinetics at industrial current densities . Herein, a face-centered cubic/hexagonal close packed (fcc/hcp) NiRu alloy heterojunction was fabricated on Ni foam (N doped NiRu-inf/NF) by a low-temperature nitrogen plasma activation. Simultaneously, nitrogen atoms are introduced into the alloy to facilitate d-p hybridization. When N doped NiRu-inf/NF is integrated into a dual-electrode cell for urea-assisted seawater electrolysis, it achieves 100 mA cm −2 with an ultra-low voltage of 1.36 V and excellent stability. Density functional theory (DFT) verifies that the robust d-p hybridization among Ni, Ru and N exhibits more energy level matching for H 2 O molecule adsorption at the Ru sites, while simultaneously reducing the interaction between H* and Ni sites in N -doped NiRu-inf.
研究领域:
材料科学
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电化学
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能源材料
·
催化
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APPLIED AND ENVIRONMENTAL MICROBIOLOGY
·
2022
·Vol. 88
·期 9
·
IF 5.005
Dong-Xu Jia,Fan Wang,Rui Zhao,Bo-Di Gu,Chen Peng,Li-Qun Jin,Zhi-Qiang Liu,Yu-Guo Zheng
d-Alanine belongs to nonessential amino acids that have diverse applications in the fields of food and health care. (R)-transaminase [(R)-TA]-catalyzed asymmetric amination of pyruvate is a feasible alternative for the synthesis of d-alanine, but low catalytic efficiency and thermostability limit enzymatic utilization. In this work, several potential (R)-TAs were discovered using NCBI database mining synchronously with enzymatic structure-function analysis, among which Capronia epimyces TA (CeTA) showed the highest activity for amination of pyruvate using (R)-α-methylbenzylamine as the donor. Furthermore, enzymatic residues surrounding a large catalysis pocket were subjected to saturation and combinatorial mutagenesis, and positive mutant F113T showed dramatic improvement in activity and thermostability. Molecular modeling indicated that the substitution of phenylalanine with threonine afforded alleviation of steric hindrance in the pocket and induced formation of additional hydrogen bonds with neighboring residues. Finally, using recombinant cells containing F113T as a biocatalyst, the conversion yield of amination of 100 mM pyruvate to d-alanine achieved up to 95.2%, which seemed to be the highest level in the literature regarding synthesis of d-alanine using TAs. The inherent characteristics rendered CeTA F113T a promising platform for efficient preparation of d-alanine operating with high productivity.IMPORTANCE d-Alanine is an important compound with many valuable applications. Its asymmetric synthesis employing (R)-ω-TA is considered an attractive choice. According to the stereoselectivity, ω-TAs have either (R)- or (S)-enantiopreference. There has been a variety of literature regarding screening, characterizing, and molecular modification of (S)-ω-TAs; in contrast, the research about (R)-ω-TA has lagged behind. In this work, we identify several (R)-ω-TAs and succeeded in creating mutant F113T, which showed not only better efficiency toward pyruvate but also higher thermostability compared with the original enzyme. The obtained original enzymes and positive mutants displayed important application value for pushing symmetric synthesis of d-alanine to a higher level.
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ACS Applied Electronic Materials
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2022
·
IF 4.494
Zhang Chen,Xiaotian Sun,Zizheng Wang,Yong Zhu,Chuanxiang Cao,Jiadong Zhou,Yanfeng Gao
Porous carbon was fabricated for broadband microwave absorption application, which was obtained from facile KOH activated carbon microspheres prepared from hydrothermal d-fructose. It is found that micropores (diameter < 2 nm) in the porous carbon played an important role in broadband and high microwave absorption properties. The prepared samples can achieve a wide bandwidth (the widest is 7.9 GHz, from 10.1 to 18 GHz), high dielectric loss (−60.0 dB as the best), and low thickness sensitivity (the bandwidth maintains 70% of the maximum within a film thickness fluctuation of up to 1.02 mm). Our findings offered an invaluable insight into designing and synthesizing highly microwave-absorbing materials through the micro/nanostructure.
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BIOCHEMICAL AND BIOPHYSICAL RESEARCH COMMUNICATIONS
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2021
·
IF 3.575
Yongxin Li,Hua Huang,Xinshuai Zhang
1-Deoxy-D-sorbitol, the 1-deoxy analogue of D-sorbitol, has been detected in human urine as well as in natural herbs and spices. Although there are sporadic reports about 1-deoxy-D-sorbitol dehydrogenase, the complete catabolic pathway of 1-deoxy-D-sorbitol remains unsolved. Informed by the promiscuous activities of fructose-6-phosphate aldolase (FSA) which is involved in the sorbitol (glucitol) utilization ( gut ) operon and guided by the large scale bioinformatics analysis, we predicted and then experimentally verified the gut operon encoded by Bacillus licheniformis ATCC14580 is responsible for the catabolism of both D-sorbitol and 1-deoxy-D-sorbitol by in vitro activity assays of pathway enzymes , in vivo growth phenotypes, and transcriptomic studies. Moreover, the phylogenetic distribution analysis suggests that the D-sorbitol and 1-deoxy-D-sorbitol catabolic gene cluster is mostly conserved in members of Firmicutes phylum.
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Scientific Reports
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2021
·Vol. 11
·期 1
·1-9
·
IF 4.38
Dong Wenjing,Song Erqun,Song Yang
The acute liver injury (ALI) and hepatic fibrosis caused by the co-treatment of lipopolysaccharide (LPS)/ d -galactosamine (D-GalN) have been extensively studied. However, whether LPS/D-GalN are genotoxic has been left unknown. In this study, male mice were divided into eight groups with eight animals in each group. For acute challenge of LPS/D-GalN, the mice in each group received a combination of LPS/D-GalN via intraperitoneal injection at the dose of 25 μg/kg/250 mg/kg, 25 μg/kg/500 mg/kg, or 50 μg/kg/500 mg/kg body weight. An additional group for chronic administration of test compounds was conducted by i.p. injection of LPS/D-GalN (10 μg/kg/100 mg/kg) every other day for 8 weeks. Saline solution (0.9%) and cyclophosphamide (CTX) (50 mg/kg body weight) given by i.p. injection was used as the negative and positive control, respectively. The results of single cell gel electrophoresis (SCGE) assay indicated that acute exposure of the mice to LPS/D-GalN caused severe DNA damage in hepatic cells, but not in the brain, sperm or bone marrow cells, which evidenced the genotoxicity of LPS/D-GalN administrated in combination. Interestingly, the chronic administration of LPS/D-GalN triggered significant genotoxic effects not only in hepatic but also in brain cells, with negative results in sperm and bone marrow cells. Histopathological examination in the liver and brain tissues revealed changes consistent with the SCGE results. The present study indicates genotoxic potential of LPS/D-GalN co-administered in mice, which may serve as an in vivo experimental model for relevant genotoxic study.
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JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
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2021
·
IF 5.279
Jiping Li,Jing Zhang,Langqiu Chen,Guochao Zhang,Jingyi Liao
Hydrophilic alkyl polyglycosides (APGs) and alkyl glycosides (AGs) with anomeric pure are a class of important substitutes for petroleum-based surfactants. Improving their water solubility should make such hydrophilic glycosurfactants have more excellent potential application value. To solve the inherent problem of poor water solubility of traditional alkyl β-d-glucopyranoside (5), a series of alkyltetra(oxyethyl) β-d-glucopyranosides (4a–4g, n = 7–18) were successfully synthesized by introducing tetra(oxyethylene) fragments to carry out the structural modification. The relationship between the related structure and the physicochemical properties was further investigated, including their hydrophilic–lipophilic balance (HLB), water-solubility, foaming performance, emulsification, hygroscopicity, surface activity, and thermotropic/lyotropic liquid crystal phase behavior. The results showed that the water solubility gradually decreased as the alkyl chain length increased due to the gradual decrease of their HLB number. Octadecyltetra(oxyethyl) β-d-glucopyranoside (4g, n = 18) was found to be insoluble in water at 25 °C. Taken together, long-chain alkyl glycosides had good foaming properties and excellent emulsifying properties. Among them, dodecyltetra(oxyethyl) β-d-glucopyranoside (4d, n = 12) had the best foaming performance. In the rapeseed oil/water system, cetyltetra(oxyethyl) β-d-glucopyranoside (4f, n = 16) had the best emulsifying ability. With the increase of the alkyl chain length, the critical micelle concentration (Ccmc), γcmc, Γmax, and hygroscopicity of this series of glycosides showed a downward trend. Differential scanning calorimetry (DSC) and polarizing optical microscopy (POM) showed that the thermal stability increased with the increase of the alkyl chain length, and alkyltetra(oxyethyl) β-d-glucopyranosides (4d–4g, n = 12–18) had the corresponding melting points and clearing points. Alkyltetra(oxyethyl) β-d-glucopyranosides (4b–4g, n = 8–18) formed a smectic phase with a typical fan-shaped and focal conic texture during the cooling process. In the water contact experiments, it was found that glycosides (4b–4g, n = 8–18) at high concentrations transformed into various lyotropic liquid crystal including hexagonal phase, bicontinuous cubic phase, and lamellar phase phases. Therefore, such green nonionic glycosurfactants alkyltetra(oxyethyl) β-d-glucopyranosides should have potential practical application prospects.
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PROCESS BIOCHEMISTRY
·
2024
·
IF 3.7
Puhong Yi,Yue Xu,Hanlin Liu,Yuhua Hao,Mengdan Liu,Zhiqiang Liu,Yaping Xue,Liqun Jin,Yuguo Zheng
2-oxo-4-[(hydroxy)(methyl)phosphinoyl]butyric acid (PPO) is a valuable prochiral keto acid for the asymmetric synthesis of the important herbicide L-phosphinothricin (L-PPT). Developing an efficient biocatalytic pathway to meet the increasing demand for PPO is highly attractive. In this study, a robust D-amino acid aminotransferase from Cytobacillus firmus ( Cf DAAT) was screened, which exhibited excellent tolerability to D,L-PPT and showed remarkable specific activity and affinity toward pyruvate (61.9 U/mg, Km = 7.4 mM). A designed co-substrate regeneration system was then introduced to shift the reaction equilibrium forward by coupling with D-amino acid oxidase (DAAO) and catalase (CAT). An efficient whole-cell biocatalyst was obtained by fine-tuning RBS intensity to coordinate the co-expression of the three enzymes. Moreover, the optimum conditions to promote overall conversion efficiency were identified by response surface methodology. Consequently, with only a catalytic amount of pyruvate (3.33 mol%) added in a 1 L reaction system, 200 mM D-PPT (400 mM D,L-PPT) was completely converted in 10 h, resulting in a PPO productivity of 3.33 g⋅L −1 ⋅h −1 , and a notable conversion rate of >99% at 300 mM D-PPT in 16 h. It demonstrated a considerable catalytic level and provided a competitive route for industrial PPO production from D,L-PPT.
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Soft Matter
·
2011
·Vol. 7
·期 14
·6451-6456
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IF 4.457
Shengtong Sun,Peiyi Wu
Near infrared spectroscopy in combination with two-dimensional correlation spectroscopy (2Dcos) and perturbation correlation moving window (PCMW) technique is employed to illustrate the gelation microdynamic mechanism of hydrogelator N-octyl-D-gluconamide (8-GA), which can rapidly self-agglomerate into helical bilayer micellar fibers upon cooling from spherical micelles. Boltzmann fitting and PCMW easily determined the gelation temperature to be ca. 72 °C and the transition temperature range to be 70–75 °C. Moreover, band shifting and splitting phenomena can be observed for CH-related overtones, indicating the formation of much ordered and tight hydrophobic core from octyl tails. On the other hand, 2Dcos was used to discern the sequential orders during the gelation process and concluded that all the group motions have a continuous transfer from the octyl tail to the chiral carbohydrate head followed by the final immobilization of the solvent, which meanwhile, is actually a continuous dehydration process from the hydrophobic core to the outer hydrophilic chiral head. The driving force of the gelation process in microdynamics can only be the dehydration process of hydrophobic octyl chains, but with final helical superstructures being stabilized by amide-associated hydrogen bonding and the “chiral bilayer effect” of carbohydrate heads.
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ACS Nano
·
2025
·
IF 16
Xuyu Li,Qingfu Zhao,Xiaolin Feng,Pinyuan Cui,Jingjing Yu,Binyong Liang,Chao Liu,Ye Wang,Yiting Wu,Ruiqi Wang,Bo Hu,Yihan Lin,Lichong Zhu,Xuan Zhu,Ban Luo,Xiangliang Yang,Jun Hu
Immunoradiotherapy (iRT) has emerged as a promising strategy for liver hepatocellular carcinoma (LIHC) treatment to synergistically activate both localized antitumor immunity and systemic immune responses. However, radiation will aggravate LIHC hypoxia, resulting in an adenosine metabolism level elevation, which promotes the differentiation of T cells into terminally exhausted phenotypes and weakens the efficacy of immunotherapy. To overcome this challenge, we engineered a nanocatalytic probiotic-based radiation-metabolic modulator, in which Escherichia coli Nissle 1917 (EcN) was programmed to in situ synthesize gold–palladium bimetallic nanocatalysts (EcNcGP) via biodirected mineralization. Guided by lattice mismatch and interfacial strain engineering, engineered EcN orchestrates the epitaxial assembly of Au atoms on Pd nanoclusters, yielding a precisely strain-tuned heterostructure with a modulated d-band electronic structure. This architectural design optimizes oxygen intermediate adsorption–desorption kinetics and significantly enhances the catalytic efficiency. This design enables EcNcGP to exhibit robust catalase- and peroxidase-like activities, which effectively catalyze intratumoral H2O2 into O2 and hydroxyl radicals, intensifying radiation damage and alleviating tumor hypoxia to inhibit adenosine metabolism by downregulating the expression of ectonucleoside triphosphate diphosphate hydrolase 1 (CD39) and ecto-5′-nucleotidase (CD73). By blocking the binding of adenosine (ADO)–adenosine receptor A2A (ADORA2A) to inhibit the following cyclic adenosine monophosphate (cAMP)–protein kinase A (PKA)–phosphorylation of cAMP response element binding (pCREB) signaling transduction, radiation-induced T-cell exhaustion could be inhibited. Compared to stereotactic body radiotherapy (SBRT), the combination of EcNcGP with SBRT increased CD8+ T-cell infiltration by 99.8% and reduced PD-1hi-exhausted T cells by 63.9%. Integration with anti-PD-L1 therapy (αPD-L1) achieved complete tumor regression in 60% of the treated mice-bearing orthotopic hepatocellular carcinoma. These findings establish a paradigm-shifting strategy for reprogramming tumor-immune metabolic checkpoints using strain-engineered nanocatalytic probiotics, thereby enhancing iRT and overcoming radioresistance.
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Nanoscale
·
2016
·Vol. 8
·期 18
·9764-9770
·
IF 7.76
Tengfei Long,Yanjia Guo,Min Lin,Mengke Yuan,Zhongde Liu,Chengzhi Huang
Despite a significant surge in the number of investigations into both optically active Au and Ag nanostructures, there is currently only limited knowledge about optically active Cu nanoclusters (CuNCs) and their potential applications. Here, we have succeeded in preparing a pair of optically active red-emitting CuNCs on the basis of complexation and redox reaction between copper(II) and penicillamine (Pen) enantiomers, in which Pen serves as both a reducing agent and a stabilizing ligand. Significantly, the CuNCs feature unique aggregation induced emission (AIE) characteristics and therefore can serve as pH stimuli-responsive functional materials. Impressively, the ligand chirality plays a dramatic role for the creation of brightly emissive CuNCs, attributed to the conformation of racemic Pen being unfavorable for the electrostatic interaction, and thus suppressing the formation of cluster aggregates. In addition, the clusters display potential toward cytoplasmic staining and labelling due to the high photoluminescence (PL) quantum yields (QYs) and remarkable cellular uptake, in spite that no chirality-dependent effects in autophagy and subcellular localization are observed in the application of chiral cluster enantiomer-based cell imaging.
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EUROPEAN JOURNAL OF PHARMACEUTICS AND BIOPHARMACEUTICS
·
2024
·
IF 4.4
Lixin Liu,Yuning Wang,Jiuyi Sun,Yunan Zhang,Xiangyu Zhang,Lili Wu,Yingli Liu,Xuan Zhang,Yidi Xia,Qiumei Zhang,Ning Gao
To improve the solubility of the fluoroquinolone drug fleroxacin (FL), based on the previous experience of our research group in synthesizing co-crystals/salts of quinolone drugs to improve the physicochemical properties of drugs, Fleroxacin-D-tartaric acid dihydrate salt (FL-D-TT, C 17 H 19 F 3 N 3 O 3 ·C 4 H 5 O 6 ·2(H 2 O)), was synthesized for the first time using fleroxacin and D/L-tartaric acid (D/L-TT). Structural characterization of FL-D-TT was carried out using single-crystal X-ray diffraction, infrared spectral analysis (FT-IR) and powder X-ray diffraction (PXRD). Molecular electrostatic potential analysis showed that D-tartaric acid interacted more readily with FL than L-tartaric acid. The solubility of FL-D-TT (9.71 mg/mL, 1.82 mg/mL) was significantly higher compared to FL (0.39 mg/mL, 0.71 mg/mL) in water and buffer solution at pH 7.4. This may be attributed to the formation of charge-assisted hydrogen bonds (CAHBs) between FL and D-TT that facilitates the dissociation of FL cations in the dissolution medium, leading to an increase in FL solubility. This also led to some improvement in the in vitro antimicrobial activity of FL-D-TT against E. coli , S. typhi , and S. aureus. In addition, the hygroscopic stability of FL has been improved. Surprisingly, FL-D-TT had better photostability than FL, which could be attributed to the introduction of D-TT to make the photosensitizing moiety of FL more stable, which led to the improvement of the photostability of FL.
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Materials
·
2018
·Vol. 11
·期 10
·2063
·
IF 2.467
Xuejing Song,Lingqian Kong,Hongmei Du,Xiangyu Li,Hanlin Feng,Jinsheng Zhao,Yu Xie
Pyrazine derivatives quinoxaline and pyridopyrazine were selected as the acceptors, and benzocarbazole was used as the donor to synthesize four different D–A–D compounds. The results showed that 2,3-bis(decyloxy)pyridine[3,4-b]pyrazine (DPP) exhibited stronger electron-withdrawing ability than that of 2,3-bis(decyloxy)quinoxaline (DPx), because DPP possesses one more nitrogen (N) atom, resulting in a red-shift of the intramolecular charge transfer (ICT) absorption bands and fluorescent emission spectra for compounds with DPP as the acceptor compared with those that use DPx as the acceptor. The band-gap energy (Eg) of the four D–A–D compounds were 2.82 eV, 2.70 eV, 2.48 eV, and 2.62 eV, respectively, for BPC-2DPx, BPC-3DPx, BPC-2DPP, and BPC-3DPP. The solvatochromic effect was insignificant when the four compounds were in the ground state, which became significant in an excited state. With increasing solvent polarity, a 30–43 nm red shift was observed in the emissive spectra of the compounds. The thermal decomposition temperatures of the four compounds between 436 and 453 °C had very high thermal stability. Resistor-type memory devices based on BPC-2DPx and BPC-2DPP were fabricated in a simple sandwich configuration, Al/BPC-2DPx/ITO or Al/BPC-2DPP/ITO. The two devices showed a binary non-volatile flash memory, with lower threshold voltages and better repeatability.Keywords:pyrazine;quinoxaline;benzocarbazole;donor-acceptor-donor;photoelectric properties;electromemory
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