JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
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IF 9.7
Hui Su,Furong Ye,Siyi Zhang,Changcun Han,Jipeng Dong,Zhixin Dai,Xinguo Ma,Lei Ge
The sluggish anodic oxygen evolution reaction (OER) kinetics remains a critical bottleneck for sustainable hydrogen production via water electrolysis. Guided by Density Functional Theory (DFT) calculations, we engineered Fe-CoS 2 /Ni 3 S 4 dual-site catalysts where Co 3+ and Fe 3+ centers synergistically optimize p-d orbital hybridization to enhance OER kinetics. Operando analyses reveal Co 3+ as primary active sites facilitating rate-limiting OOH* → O 2 desorption with Gibbs free energy (ΔG) reduced by 0.94 eV, while Fe-induced electron delocalization lowers intermediate coupling barriers. Notably, the catalyst facilitates dynamic reconstruction, generating metastable Co 3+ species with optimized eg orbital occupancy (t 2 g 5 eg 1 configuration) and strengthened p-d hybridization via Fe-mediated charge transfer. This electronic synergy enables ultralow overpotentials of 156 mV (hydrogen evolution reaction HER) and 230 mV (OER) at 50 mA cm −2 , with a cell voltage of 1.48 V for overall water splitting at 10 mA cm −2 . The dual-site architecture simultaneously suppresses metal dissolution (<12 % after 20 h) while maintaining 89.2 % initial activity. This work establishes a dual-regulation strategy: atomic-level orbital engineering for OER intermediate optimization and dynamic surface reconstruction for HER-active phase stabilization, offering a paradigm for designing robust bifunctional electrocatalysts.
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JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
·
2025
·
IF 6.2
Hulin Qiu,Wenzhong Gong,Huilin Huang,Heng Guo,Zhizeng Gao,Lan Liu,Xinjian Yin
meso-Diaminopimelate dehydrogenase (DAPDH) holds considerable promise for D-amino acid synthesis but is limited by its low catalytic efficiency toward non-natural substrates. To address this, we present a Rosetta-driven evolution framework that enables the rapid tuning of DAPDH substrate specificity. This approach leverages Rosetta design to guide the construction of a smart-small mutant library, facilitating evolution in just one or two rounds with minimal screening (100–1,000 transformants), thus offering superior efficiency and cost-effectiveness. Using this strategy, the activities of two DAPDHs toward model substrates─benzoylformic acid (1b) and 3-indolepyruvic acid (10b)─were enhanced from undetectable levels to 29.5 and 5.1 U/mg, respectively. The activity toward 1b was nearly ten times higher than the best-reported mutant. The evolved DAPDHs displayed an expanded substrate spectrum and high catalytic performance, enabling the efficient synthesis of structurally diverse bulky D-amino acids at both analytical and preparative scales. The highest concentration of 1b achieved was 0.5 M (100 mL scale), with a space-time yield of 128.46 g/L/day. This study underscores the power of Rosetta-based evolution in accelerating enzyme engineering, offering a versatile and efficient platform for optimizing DAPDHs and other industrially significant enzymes.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2022
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IF 6.371
Yining Ma,Dandan Zhu,Huaijuan Zhou,Yue Tang,Chenchen Hu,Xinyu Meng,Xiaodong Jin,Tongxiang Xu,Xun Cao
Vanadium dioxide (VO 2 ) material has been deemed as a potential anode candidate for aqueous lithium-ion batteries. Among its diversified polymorphs, the latest discovered VO 2 (D) receives the fewest reports on its application in energy storage. Herein, we successfully utilized a template-free solvothermal method to prepare VO 2 (D) submicron-spherical hierarchical structures, constructed with colibacillus-like nanorods . The VO 2 (D) submicron-spheres were applied as an active anode material into the aqueous lithium-ion battery, which exhibited suitable working potential. Furthermore, VO 2 (D)-based full cell with LiMn 2 O 4 as the cathode demonstrated high discharge capacity, good rate capability, and excellent cycling stability. The structural evolution, valence states of the VO 2 (D) electrode, and impedance variation of the full cell during cycling were investigated. The work reveals the potential of VO 2 (D) as a novel anode material for aqueous lithium-ion batteries.
研究领域:
材料科学
·
能源存储
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ChemistrySelect
·
2022
·Vol. 7
·期 36
·e202202508
·
IF 2.307
Meifeng Wang,Liyin Zhang,Yiqun Li,Liuqun Gu
Graphical An unprecedent “mixing and stand” anomerization of D-glucose pentaacetate in solid state was discovered after simple premixing in solvent and then removal of solvent, and the reaction proceeded continuously to full conversion without stirring or mechanomixing. Gram scale reaction was demonstrated and a new mechanism was also proposed. Anomerization of glycosides was rarely performed under basic condition. Here, an imidazole promoted anomerization of β-D-glucose pentaacetate in solid state at room temperature was discovered. This unprecedent anomerization occurred after simple premixing and reaction proceeded continuously in solid state to full conversion without stirring or mechanomixing. Full conversion of all β-forms in the mixture (α:β=2.2 : 1) into α-forms only was demonstrated at 1 gram scale. A proposed mechanism involved with inter/intramolecular acyl transfer promoted by imidazoles in a concerted manner may promote the discovery of more new transformations in solid state.
研究领域:
有机化学
·
糖化学
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BIOORGANIC CHEMISTRY
·
2026
·
IF 4.7
Shaojie Zhang,Tanggan Wang,Meifeng Li,Qian Zhang,Hongju Liu
Scutellaria barbata D. Don has been used in traditional Chinese medicine for its heat-clearing and detoxifying effects to treat colitis. Polysaccharides are the key bioactive constituents of S. barbata . In this study, a heteropolysaccharide (SBP80) was extracted from S. barbata using water extraction methods. In vivo studies in mice demonstrated that SBP80 exhibited significant therapeutic effects on ulcerative colitis (UC). Specifically, SBP80 improved body weight and disease activity index (DAI) scores in UC mice, restored colon length, alleviated inflammatory cell infiltration in colonic tissues, and suppressed the levels of inflammatory cytokines and oxidative stress factors. Further purification of SBP80 yielded two polysaccharides, SBP80–1 (7.2 kDa) and SBP80–2 (292.3 kDa). Structural analysis revealed that both SBP80–1 and SBP80–2 were primarily composed of mannose, rhamnose, glucuronic acid, glucose, and galactose, with minor amounts of xylose, arabinose, and fucose. In addition, SBP80–2 contained higher amounts of glucuronic acid and xylose compared to SBP80–1. Methylation analysis further showed that the proportion of terminal residues and 1,6-linked residues in SBP80–2 was higher, while SBP80–1 exhibited more 1,4-linked residues. In vivo zebrafish experiments demonstrated that both SBP80–1 and SBP80–2 inhibited intestinal shortening and neutrophil infiltration in zebrafish with UC. They also reduced nitric oxide (NO) and reactive oxygen species (ROS) levels. Moreover, SBP80–2 exhibited superior anti-UC activity, which may be attributed to its structural characteristics. In conclusion, our findings indicate that S. barbata polysaccharides (SBP80–1 and SBP80–2) may be promising natural agents for the treatment of UC.
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International Journal of Environmental Research and Public Health
·
2022
·Vol. 19
·期 5
·
IF 4.614
Arcadia Del Rio,Narcisa Muresu,Giovanni Sotgiu,Laura Saderi,Illari Sechi,Andrea Cossu,Manuela Usai,Alessandra Palmieri,Bianca Maria Are,Giovanna Deiana
Background:Carbapenem-resistantKlebsiella pneumoniae(CR-Kp) is endemic globally, causing severe infections in hospitalized patients. Surveillance programs help monitor and promptly identify the emergence of new clones. We reported the rapid spread of a novel clone ofK. pneumoniaeco-harbouring class A and D carbapenemases in colonized patients, and the potential risk factors involved in the development of infections.Methods:Rectal swabs were used for microbiological analyses and detection of the most common carbapenemase encoding genes by real-time PCR (i.e., blaKPC, blaOXA-48, blaNDM, blaVIM, and blaIMP). All strains co-harbouring KPC and OXA-48 genes were evaluated. For each patient, the following variables were collected: age, sex, length and ward of stay, device use, and outcome. Clonality of CR-Kp was assessed by preliminary pulsed field gel electrophoresis (PFGE), followed by multi-locus sequence typing (MLST) analyses.Results:A total of 127 isolates ofK. pneumoniaeco-harbouring KPC and OXA-48 were collected between September 2019 and December 2020. The median age (IQR) of patients was 70 (61–77). More than 40% of patients were admitted to intensive care unit (ICU). Around 25% of patients developed an invasive infection, the majority of which were respiratory tract infections (17/31; 54.8%). ICU stay and invasive infection increased the risk of mortality (OR: 5.39, 95% CI: 2.42–12.00; OR 6.12, 95% CI: 2.55–14.69, respectively;p-value ≤ 0.001). The antibiotic susceptibility test showed a resistance profile for almost all antibiotics considered. Monoclonal origin was confirmed by PFGE and MLST showing a similar restriction pattern and belonging to ST-512.Conclusions:We report the spread and the marked antibiotic resistance profiles ofK. pneumoniaestrains co-producing KPC and OXA-48. Further study could clarify the roles of clinical and microbiological variables in the development of invasive infection and increasing risk of mortality, in colonized patients.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
·
2019
·
IF 2.931
Xiaojuan Zhou,Chunli Xu,Yan Jin,Baoxin Li
Chiral recognition of enantiomers is fundamentally important. In this work, an effective and simple chiral sensing strategy for discrimination of leucine (Leu) enantiomers was constructed. In this chiral sensing, cube-shaped gold nanoparticles (AuNCs) as colorimetric probes are used to recognize Leu enantiomers . L-Leu can induce rapidly the aggregation of AuNCs, leading to change of AuNCs solution from red to colorless, while D-Leu cannot induce the color change. This distinct color changes allow naked-eye to distinguish chiral isomers of Leu. The chiral sensing was applied to measure the enantiometric excess of L-Leu in the whole range (from −100% to 100%). This chiral analysis can be performed by naked eye or simple ultraviolet-visible spectrometer. In addition, the mechanism of chiral recognition has been studied with circular dichroism (CD) spectra, UV–vis absorption spectra and zeta potential . In this method, the chiral recognition is due to the intrinsic chirality of AuNCs, and the AuNCs don't need any chiral labeling or modification. This chiral sensing method is simple, cheap, rapid and easy to operate. Furthermore, this work provides one experimental evidence for intrinsic chirality of nanoparticles , and helps people understand the chirality of nanostructures .
研究领域:
纳米技术
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分析化学
·
手性传感
·
材料科学
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APPLIED BIOCHEMISTRY AND BIOTECHNOLOGY
·
2026
·
IF 3.5
Long Neng-Bing,Zhu Hong-Lin,Li Tian-Hua,Zhang Rui-Feng
A large-sized 3D microflow support was prepared by chemical liquid deposition of an epoxy-based porous polymer within a 3D melamine sponge. This novel support demonstrated advantages over traditional microfluidic reactors in terms of easier scalability, simplified enzyme loading, and superior multiphase dispersion. The resultant composite sponge was utilized as a microflow support for the immobilization of phospholipase D (PLD) through an adsorption and cross-linking method. Under optimal immobilization conditions, the loading capacity and specific activity of the immobilized PLD were 50.2 mg/g support and 14.5 U/mg protein, respectively. The PLD-immobilized microflow supports were positioned in a columnar reactor, where a biphasic transesterification reaction was conducted in a continuous circulation mode powered by two pumps. The PLD-catalyzed reaction yielded phosphatidylserine (PS) with high yields and reaction ratios. Under optimized conditions, the PS yield reached as high as 93.1% within 4 h at 45 °C, by using free PLD the PS yield reached only 61.5% within 12 h. After 10 cycles, the immobilized PLD retained 76% of its original activity.
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2023
·
IF 3.8
Hui Jiang,Zijian Zhao,Ning Yu,Yi Qin,Zhengwei Luo,Wenhua Geng,Jianliang Zhu
Using N -methyl-D-glucosamine (NMDG) as the functional monomer , glycidyl methacrylate (GMA) as the connecting monomer, functionalized Fe 3 O 4 nano-particles (NPs) as the support, three adsorbents were prepared including direct polymer GMA-NMDG, magnetic GMA-NMDG polymer (MGN), and boron magnetic ion-imprinted polymer (BMIIP). Based upon the optimization of synthesis conditions, the prepared adsorbents and intermediate products were characterized using Fourier transform infrared spectroscopy, thermogravimetric analysis, scanning electron microscope, energy dispersive spectroscopy, X-ray diffraction, vibrating sample magnetometer, and Brunauer–Emmett–Teller to investigate the synthesis process, the morphological structure and the functional properties of the materials. The optimum performances of GMA-NMDG, MGN and BMIIP were obtained in the initial neutral solution (pH of 6.5). Moreover, GMA-NMDG and MGN reached the maximum adsorption capacity at 120 min, whereas BMIIP reached adsorption saturation at 60 min. The pseudo-second-order kinetic model was more suitable for the adsorption of boron using the adsorbents. The maximum adsorption capacity of GMA-NMDG was found to be 43.4 mg·g −1 , while those of MGN and BMIIP were 32.5 and 28.3 mg·g −1 , respectively. The Langmuir isotherm model was more appropriate to describe the adsorption process . The adsorbents maintained satisfactory adsorption performance within a certain temperature range. Competing ions had little effect on the adsorption of boron, and would be adsorbed simultaneously, due to which, the effect of co-adsorption can be considered. The adsorption capacity of GMA-NMDG was high, while the adsorption selectivity of BMIIP was much better. Furthermore, BMIIP showed good adsorption after five cycles of adsorption and desorption. The comparison of adsorbents showed that GMA-NMDG had the highest adsorption capacity and was suitable for co-adsorption. MGN had a high adsorption capacity, good comprehensive performance and magnetic properties. BMIIP had better adsorption rate, adsorption selectivity and recyclability. Through the optimization of synthesis conditions, the adsorption capacity of the traditional monomer NMDG polymer was increased, and the magnetism was given to facilitate rapid recovery. Combined with the ion imprinting technology, it showed higher boron adsorption selectivity in the presence of competitive ions.
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ADVANCED MATERIALS
·
2022
·Vol. 35
·期 5
·2208034
·
IF 32.086
Kai Jia,Jun Ma,Junxiong Wang,Zheng Liang,Guanjun Ji,Zhihong Piao,Runhua Gao,Yanfei Zhu,Zhaofeng Zhuang,Guangmin Zhou,Hui-Ming Cheng
A large amount of spent LiFePO 4 (LFP) has been produced in recent years because it is one of the most widely used cathode materials for electric vehicles. The traditional hydrometallurgical and pyrometallurgical recycling methods are doubted because of the economic and environmental benefits; the direct regeneration method is considered a promising way to recycle spent LFP. However, the performance of regenerated LFP by direct recycling is not ideal due to the migration of Fe ions during cycling and irreversible phase transition caused by sluggish Li + diffusion. The key to addressing the challenge is to immobilize Fe atoms in the lattice and improve the Li + migration capability during cycling. In this work, spent LFP is regenerated by using environmentally friendly ethanol, and its cycling stability is promoted by elevating the d-band center of Fe atoms via construction of a heterogeneous interface between LFP and nitrogen-doped carbon. The Fe O bonding is strengthened and the migration of Fe ions during cycling is suppressed due to the elevated d-band center. The Li + diffusion kinetics in the regenerated LFP are improved, leading to an excellent reversibility of the phase transition. Therefore, the regenerated LFP exhibits an ultrastable cycling performance at a high rate of 10 C with ≈80% capacity retention after 1000 cycles.
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APPLIED CATALYSIS A-GENERAL
·
2022
·
IF 5.723
Chaofeng Chang,Yuhua Xie,Fang Luo,Shaowei Zhou,Zehui Yang
To economically realize proton electrolyte membrane water splitting technology, stable and high-performance oxygen evolution reaction (OER) electrocatalyst is significantly demanded. In this work, we invite tungsten atoms to metallic iridium (Ir) to weaken s-d hybridization of Ir-Ir bond due to the higher electronegativity accepting electron from Ir atoms; as a result, the adsorbed O* species become electrophilic favorable for the nucleophilic attack by H 2 O leading to 22 % decrement in energy barrier for the formation of OOH* species. Therefore, iridium-tungsten (IrW) electrocatalyst exhibits 3.7-fold higher turnover frequency (TOF) than metallic Ir at overpotential of 370 mV in acidic OER catalysis. Moreover, stable OER performance is recorded due to the high cohesive energy of tungsten atoms. Additionally, TOF of IrW electrocatalyst reaches 10.1 s −1 at overpotential of 100 mV in acidic hydrogen evolution reaction (HER) test, 7.6-time higher than Pt/C and metallic Ir. IrW electrocatalyst only needs 1.52 V to attain 10 mA cm −2 in acidic overall water splitting.
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Food & Function
·
2023
·Vol. 14
·期 6
·2684-2697
·
IF 6.1
Ran Wei,Zhucheng Su,Gerardo G. Mackenzie
Chlorogenic acid (CGA) and epigallocatechin-3-gallate (EGCG) are major polyphenolic constituents of coffee and green tea with beneficial health properties. In this study, we evaluated the gut protecting effect of CGA and EGCG, alone or in combination, on D-galactose-induced aging mice. CGA plus EGCG more effectively improved the cognition deficits and protected the gut barrier function, compared with the agents alone. Specifically, CGA plus EGCG prevented the D-galactose mediated reactive oxygen species accumulation by increasing the total antioxidant capacity, reducing the levels of malondialdehyde, and suppressing the activity of the antioxidant enzymes superoxide dismutase and catalase. In addition, supplementation of CGA and EGCG suppressed gut inflammation by reducing the levels of the proinflammatory cytokines TNFα, IFNγ, IL-1β and IL-6. Moreover, CGA and EGCG modulated the gut microbiome altered by D-galactose. For instance, CGA plus EGCG restored the Firmicutes/Bacteroidetes ratio of the aging mice to control levels. Furthermore, CGA plus EGCG decreased the abundance of Lactobacillaceae, Erysipelotrichaceae, and Deferribacteraceae, while increased the abundance of Lachnospiraceae, Muribaculaceae, and Rikenellaceae, at the family level. In conclusion, CGA in combination with EGCG ameliorated the gut alterations induced by aging, in part, through antioxidant and anti-inflammatory effects, along with its gut microbiota modulatory capacity.
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