JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2025
·
IF 14.3
Yanhui Cao,Junhao Zeng,Xuerong Zheng,Yuan Liu,Junda Lu,Jinfeng Zhang,Yang Wang,Yida Deng,Wenbin Hu
Oxygen reduction reaction (ORR) in neutral electrolyte is urgently needed in various areas, such as metal-air batteries. However, the N-coordinated transition-metal single-atom electrocatalysts confront sluggish catalytic kinetics due to the inappropriate electronic structure and the as-resulted unreasonable adsorption strength towards oxygen-containing intermediates. In this work, we develop a strategy to tune the Fe d-orbital spin state by introducing inert Si atom into the first coordination sphere of Fe-N 4 moieties. The experimental and theoretical results suggest that Si atom generates the coordination field distortion of Fe and induces the Fe d-orbital spin state transforming from low to medium spin state. The optimized spin-electron filled state (t 2g 4 e g 1 ) of Fe sites weakens the adsorption strength to intermediates and reduces the energy barrier of *OH desorption. Consequently, Fe-Si/NC catalyst exhibits superior ORR performance compared with that of Fe-NC and commercial Pt/C, showing a more positive half-wave potential of 0.751 V (vs. RHE) in 0.1 mol/L phosphate buffered saline. In addition, Fe-Si/NC-based neutral zinc-air batteries show a maximum power density of 108.9 mW cm −2 and long-term stability for more than 200 h. This work represents the possibility of constructing distorted coordination configurations of single-atom catalysts to modulate electronic structure and enhance ORR activity in neutral electrolyte.
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Bioactive Materials
·
2025
·
IF 20.3
Qi Zhang,Zhe Zheng,Yiting Zhao,Qing Wu,Chu Wu,Xiuli Wang,Xia Wang,Qigang Wang,Peiru Wang
The transformation of O 2 is primarily facilitated by the catalytic action of redox enzymes, which play a pivotal role in sustaining cellular energy metabolism and redox balance. Bioinspired by O 2 distribution and ROS regulation related to cascade biocatalytic process, a D-peptide NapG D F D F D Y engineered hydrogel has been constructed with encapsulated dual-enzyme superoxide (SOD) and chloroperoxidase (CPO) cascade catalytic circuit and co-assembled photosensitizer of 5-aminolevulinic acid molecules (ALA). Multimodal oxygen modulation has been conducted by the concurrent oxygen generation via SOD-catalyzed ⋅O 2 − dismutation and oxygen consumption for 1 O 2 production by CPO and ALA, achieving self-sustaining enzymatic dynamic therapy (EDT)-photodynamic therapy (PDT) (EDT-PDT) synergy. The endogenous cascade-amplified EDT not only enhances the 1 O 2 efficacy in exogenous PDT therapy, but the intermediate O 2 can also alleviate local neuropathic pain caused by hypoxia for safe PDT treatment. This work pioneers enzyme-mediated dynamic control of tumor redox homeostasis, establishing a new therapeutic axis between biocatalytic amplification and photodynamic processes.
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ADVANCED MATERIALS
·
2025
·
IF 26.8
Miaomiao He,Qiancun Wang,Zhijie Lin,Dan Sun,Guangfu Yin,Yi Deng,Weizhong Yang
Pathogenic infections pose a persistent threat to global public health, necessitating innovative antibacterial strategies with well-defined disinfection pathway. The antibacterial efficiency is confined in the contradiction between reactants adsorption and intermediates desorption. Here, the FeMoS 4 /MXene bio-heterojunction enzyme (FM BioHJzyme) is proposed and constructed. Under the inspiration of near-infrared light (NIR), the heterostructures between the FeMoS 4 and MXene facilitates efficient electron-hole separation with localized electron accumulation at FeMoS 4 sites. Crucially, the electronic push-pull effect induced by Mo polarizes oxygen-containing reactants (H 2 O 2 , H 2 O, O2) toward Fe active centers, enabling sequential electron capture for reactive oxygen species (ROS) generation. The results also reveal an enhancement in electron density at Fe sites compared to FeS/MXene controls, which is accompanied by a downshift in the Fe d-band center that reduces intermediates adsorption energy. The therapeutic efficacy is systematically evaluated using an S. aureus -infected full-thickness skin defect model. The bi-modulated FM BioHJzyme exhibits favorable antibacterial efficiency under NIR irradiation, while subsequent wound healing is facilitated through collagen deposition and angiogenesis in the following absence of NIR irradiation. This work offers a deep insight into the intricate mechanism-performance relationship of BioHJzyme platform in catalytic anti-bacterial application and proposes a sustainable approach of mechanism-guided materials design.
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ADVANCED FUNCTIONAL MATERIALS
·
2025
·
IF 19
Yutong Tong,Butian Chen,Chong Liu,Ruoyu Wang,Dewen Wang,Tianran Zhang,Xiaobai Ma,Limei Sun,Jinbo Yang,Wenyun Yang,Xiangfeng Liu
Halide solid electrolytes (SEs) show great potential in all-solid-state batteries (ASSBs) because of their high ionic conductivity and high oxidative stability. But the long-term cycling stability remains a major concern due to the cathode/halide interface side reactions, especially under high current density. Herein, a s-p-d orbital hybridization strategy is proposed via introducing Zr 4+ and F − into Li 3 InCl 6 (LIC-ZrF 4 ) to regulate the electron localization structure around the central In 3+ . The electron transfer between the cation and Cl is alleviated by the enlarged bandgap (4.485–4.894 eV) with ZrF 4 introduction, and more electrons aggregate around In 3+ after s-p-d hybridization among Zr, In, and Cl. This effectively prevents LIC-ZrF 4 from being attacked by O atoms in LiNi 0 . 8 Co 0 . 1 Mn 0 . 1 (NCM811) and significantly suppresses the interface side reactions. The in situ formed LiF-containing layer further enhances the interface stability. The assembled ASSB (NCM811/LIC-ZrF 4 /LPSC/Li-In) exhibits a state-of-the-art capacity retention (96.7%@500cycles@1C; 80.7%@1600 cycles@2C). Furthermore, the ionic conductivity of LIC-ZrF 4 is also enhanced from 0.6 to 1.5 mS cm −1 while the electronic conductivity is decreased from 3.66 × 10 −8 to 8.39 × 10 −9 S cm −1 . This work highlights the crucial role of s-p-d hybridization on the electron localization regulation and the interface stability, and presents some distinct insights into developing high-performance halides-based ASSBs.
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ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Jinhuan Liang,Xiaoqi Wu,Jingwen Ma,Jin Huang,Jiaxin Wu,Rongrong Zhong,Zehua Zou,Yanjun Hou,Qingxiang Wang,Xuan Zheng
Constructing efficient and durable bifunctional electrocatalysts for overall water splitting (OWS) under industrial current densities remains a critical challenge. Herein, we report a crystalline–amorphous (C–A) Schottky junction catalyst, NiFe(OH)x/Fe7S8/IF, featuring a nanosphere-assembled hierarchical architecture synthesized via a two-step in situ growth strategy. The hybrid integration of conductive Fe7S8 nanorods and amorphous NiFe(OH)x nanosheets generates a robust C–A heterointerface. Mechanistic investigations reveal that the built-in electric field (BIEF) at the Schottky interface not only narrows the band gap of NiFe (oxy)hydroxide to improve charge transport, but also modulates the adsorption behavior of reaction intermediates by tuning the d/p-band center proximity (Δεd–p) of surface reaction sites. First-principles calculations demonstrate that Δεd–p serves as a reliable electronic descriptor for optimizing HER and OER pathways of NiFe (oxy)hydroxide-Fe7S8 heterointerface via balancing H adsorption and weakening OOH binding, respectively. Benefiting from these unique electronic regulations, the resulting catalyst exhibits exceptional bifunctional electrocatalytic performance, requiring overpotentials of only 359 mV for the hydrogen evolution reaction (HER) at 1 A cm–2 and 380 mV for the oxygen evolution reaction (OER) at 500 mA cm–2. When integrated into a two-electrode electrolyzer, the NiFe(OH)x/Fe7S8/IF couple achieves a low cell voltage of 1.42 V at 10 mA cm–2 and sustains 1 A cm–2 over 300 h with minimal current density decay. This work sheds light on a generalizable interfacial design strategy and introduces Δεd–p as a conceptual framework for the rational design of cost-effective, high-performance water-splitting electrocatalysts.
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JOURNAL OF MOLECULAR STRUCTURE
·
2025
·
IF 4.7
Xinru Dong,Yang Li,Xuejun Zhang,Nan Liu,Peng Gao
A donor–acceptor (D–A) covalent organic framework (CoPcPA-COF) was constructed from a metal phthalocyanine donor and a polycarboxylic acid acceptor unit. Molecular structure modulation endowed the material with exceptional visible-light absorption (bandgap: 1.34 eV) and a strong photoelectronic response. In photocatalytic tetracycline degradation, CoPcPA-COF achieved 91.1% removal within 60 min and maintained stable performance in various real water matrices, demonstrating excellent environmental adaptability. Density functional theory (DFT) analysis revealed pronounced spatial charge separation (CT ratio: 88.97%), a high exciton binding energy (4.314 eV), and a ligand-to-metal charge transfer tendency. Density of states (DOS) calculations indicated a theoretical bandgap of 0.5 eV, corroborating its broad-spectrum light response and favorable electronic structure. This work provides a theoretical foundation for the development of visible-light-driven COF photocatalysts and offers a promising strategy for efficient remediation of antibiotic contamination in water.
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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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APPLIED THERMAL ENGINEERING
·
2024
·
IF 6.1
Zhao-ran Li,Gao-ning Liang,Yu-dong Ding,Qiang Liao,Xun Zhu,Min Cheng
As an important intermediary between the green energy and human society, the lithium-ion battery has promising prospects in the new energy vehicles, energy storage, and green development fields. However, lithium-ion batteries can generate a large amount of heat during operation. In addition, excess temperature or big temperature difference of the surface of the lithium-ion battery can reduce its performance, which also results in reducing its operational life and even triggers incidents such as fires and explosions. Therefore, studying efficient thermal management methods for lithium-ion batteries is crucial for increasing their application range. This paper proposes a novel thermal management method by combining 3-D finned tubes with PCM. The thermal management system maintains a battery operating temperature less than 45 °C and a maximum temperature difference less than 2.4 °C. The influence of different fin structure parameters on the melting dynamics of PCM and the heat transfer performance is then discussed. The obtained results show that under each solid–liquid ratio of PCM, the heat transfer performance increases with the increases of the fin height, while it initially decreases and then increases with the increase of the width and axial spacing. Moreover, the heat transfer performance of the 3-D finned tube with different PCM liquid–solid ratios is investigated. The obtained results demonstrate that for constant fin parameters, the heat transfer reaches its highest performance for a PCM liquid–solid ratio greater than 2:2. The findings of this study lay a foundation for the design of efficient thermal management systems incorporating PCM applications.
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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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ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Yuelong Xu,He Wang,Changrui Xing,Jianhao Zhang,Wenjing Yan
Bacterial infection has always posed a severe threat to public health. Gold nanoparticles (Au NPs) exhibit exceptional biocompatibility and hold immense potential in biomedical applications. However, their antibacterial effectiveness is currently unsatisfactory. Herein, a chiral antibacterial agent with high stability was prepared by the modification of Au NPs with d-cysteine with the assistance of polyethylene glycol (PEG). The as-synthesized d-cysteine/PEG-Au NPs (D/P-Au NPs) exhibited a stronger (99.5–99.9%) and more stable (at least 14 days) antibacterial performance against Gram-negative (Escherichia coli and Listeria monocytogenes) and Gram-positive (Salmonella enteritidis and Staphylococcus aureus) bacteria, compared with other groups. The analysis of the antibacterial mechanism revealed that the D/P-Au NPs mainly affected the assembly of ribosomes, the biosynthesis of amino acids and proteins, as well as the DNA replication and mismatch repair, ultimately leading to bacterial death, which is significantly different from the mechanism of reactive oxygen species-activated metallic antibacterial NPs. In particular, the D/P-Au NPs were shown to effectively accelerate the healing of S. aureus-infected wounds in mice to a rate comparable to or slightly higher than that of vancomycin. This work provides a novel approach to effectively design chiral antibacterial agents for bacterial infection treatment.
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Foods
·
2025
·Vol. 14
·期 9
·1538
·
IF 5.1
Zepeng Li,Runmin Wang,Xiantai Lai,Wenyi Liao,Runfeng Liao,Zhuohong Wu,Guoyan Zhang,Xianghui Qi
D-tagatose is a functional sweetener with glucose-regulating and prebiotic properties, but its bioproduction from D-galactose faces many limitations, particularly the high production costs. In particular, the current biosynthesis of D-tagatose suffers from thermal instability and the substrate selectivity issues of L-arabinose isomerase (L-AI) required to convert D-galactose into D-tagatose. In this study, recombinantEscherichia coliBW25113/pQE-80L-araAF118M/F279Iexpressing double mutant L-AI was immobilized to enhance its stability and reusability. The optimal conditions for whole-cell catalysis were 60 °C, pH 6.5, 5 mM Mn2+, and 20 h, with a yield of 55.2 g/L of D-tagatose. Immobilization with 3% sodium alginate and 2% CaCl2retained 90% of the production efficiency displayed by free cells. Notably, the immobilized cells exhibited enhanced heat resistance (60–70 °C) and operational stability, retaining 76% activity after five cycles. The D-tagatose production was further increased to 129.43 g/L by increasing the substrate concentration to 250 g/L. Compared to free cells, immobilized cells retained 83.6% of the initial yield up to 10 batches. This study presents a cost-effective and sustainable method for the production of D-tagatose using optimized whole-cell catalysis through immobilization, which paves the way to solve industrial challenges such as thermal instability and low substrate efficiency.
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ANALYTICA CHIMICA ACTA
·
2025
·
IF 6
Juan Li,Ming-Chun Lai,Ya-Meng Zhong,Ya-Ling Chen,Na Wu,Wei Chen,Hua-Ping Peng
Monitoring D-amino acids concentrations has essential implications for gastric cancer diagnosis and treatment, especially in the non-invasive detection of gastric cancer. However, it remains a challenge to establish a high-performance detection method for D-amino acids. Here, a highly sensitive and selective d -alanine (D-Ala) ECL assay strategy via a turn-off-on split-type electrochemiluminescence (ECL) platform has been proposed. We found that hydrogen peroxide (H 2 O 2 ) could be used as an efficient etching agent to turn on the MnO 2 /gold nanocluster (AuNC)-based ECL nanoswitch platform. Based on abovementioned characteristics, we extended it to the D-amino acids assay since the enzymatic reaction between D-Ala and D-amino acid oxidase (DAAO) generates H 2 O 2 . Based on the abovementioned characteristics, this ECL sensing platform achieved a preferable linear-dependent curve in the detection range of 1.0 × 10 − 10 ∼1.0 × 10 − 3 mol L −1 , and realized the detection of D-Ala as low as 2.2 × 10 − 11 mol L −1 (S/N = 3). Furthermore, the proposed ECL biosensor showed excellent selectivity, stability, and reproducibility. Together with its powerful performance, this strategy could test D-Ala in saliva samples, which suggested that this ECL assay platform shows great prospect in disease diagnosis. We ascribe the high sensitivity and good anti-interference capability of the sensor to the combination of specific enzyme catalysis reaction, high-efficiency split-type AuNC probe-based ECL technique and the highly etching efficiency of H 2 O 2 to MnO 2 nanomaterials on electrode surface. In our perception, this H 2 O 2 mediated split-type ECL sensing platform provides a viable tool in ECL based bioananlysis. Therefore, our proposed approach not only provides a strategy for developing a high-performance platform for D-Ala detection, but also establishes a framework for the detailed design and development of ECL platform for other biological assays.
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