APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
·
IF 21.1
Lizhang Chen,Xuan Wang,Tingyu Lu,Huan Pang,Songtao Zhang,Lin Xu,Gaixiu Yang,Qixing Zhou,Yawen Tang
As one of the most competitive alternatives to precious Pt-based electrocatalysts towards the oxygen reduction reaction (ORR), Fe-N-C single atom catalysts (SACs) are still eagerly anticipated to undergo further performance enhancement to advance their practical applications in diverse renewable energy systems. The regulation of energy level of Fe site through the manipulation of d-orbital splitting manner provides a novel route to improve the intrinsic activity, yet still in its infancy. We herein present a Fe d-orbital splitting modulation strategy via crafting atomically dispersed Fe-N 5 moieties with axial N ligand anchored on “lotus root”-like N-doped multichannel carbon nanofibers (abbreviated as FeN 5 @NMCNFs hereafter). Symmetrical experimental and theoretical findings reveal that near-range coordinated effect of axial N ligand results in the deformation of local symmetry, deep valence band spin-polarization of d orbitals and downshifted d-band center of Fe center site, endowing the optimized adsorption energetics of ORR intermediates and reduced reaction energy barrier. Accordingly, the as-developed FeN 5 @NMCNFs deliver Pt-competitive ORR activity and extraordinary long-term durability in KOH electrolyte with a halfwave potential of 0.87 V, exceeding a majority of recently reported non-precious SACs. Furthermore, when incorporated into liquid and flexible all-solid-state Zn air batteries (ZABs), the FeN 5 @NMCNFs||RuO 2 -assembled ZABs demonstrate superior electrochemical performance to the state-of-the-art Pt/C||RuO 2 counterpart. This work offers a new perspective for the performance optimization of SACs via the manipulation of the local coordination manner and the precise spin-polarization regulation strategy.
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Environmental Science-Nano
·
2025
·
IF 5.1
Lu Wang,Siyuan Zhang,Jukun Xiong,Meicheng Wen
Formaldehyde (HCHO), a prevalent indoor volatile organic compound, poses significant health risks to humans even at very low concentrations. As a result, its efficient degradation at room temperature is of utmost importance. However, the detailed mechanism for catalytic oxidation of formaldehyde remains unclear, particularly regarding the role of water vapor, which has been subject to considerable debate. In this study, we synthesized Pt-supported TiO2 glass fiber catalysts (Pt/TiO2 GF) via NaBH4 reduction to investigate the reaction pathways and clarify the influence of water vapor on the oxidation process. The reaction mechanism and intermediates were systematically studied at room temperature using in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), kinetic isotope effect (KIE) analysis, and density functional theory (DFT) calculations. Results revealed a clear reaction pathway of HCHO → DOM → HCOO− → CO2, with formate C–H bond cleavage (HCOO−* + O* → CO2 + OH*) identified as the rate-determining step. Both experimental KIE results and theoretical calculations confirmed that water vapor substantially reduces the activation barrier for this step, significantly promoting formate decomposition and subsequent CO2 formation. This work provides critical insights into the role of water in enhancing formaldehyde oxidation and offers theoretical support for developing efficient catalysts suitable for humid environments.
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PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
·
2025
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IF 7.8
Jinyu Shi,Xiunan Cai,Zhongqiu Luo,Chaochao Lai,Cuirong Yan,Qian Long,Shiyu Liu,Xintao Zhou
Green iron-based materials suffer from severe alkaline deactivation and limited photoactivity, restricting synergistic pollutant remediation. Herein, a bioinspired microenvironment engineering strategy to convert copper slag into amorphous SiO 2 -stabilized Mn-doped ferrous oxalate hollow tubus (MnFeOx@SiO 2 ). In the complex, amorphous SiO 2 neutralizes external alkalinity, while Si−OH dissociation maintains an weak-acidic microenvironment, preventing hydrolysis deactivation and ensuring robust photo-Fenton cycles. Experimental and DFT studies reveal that silicate-derived silica gel synergizes with glycerol to direct MnFeOx axial growth, forming channeled hollow tubes that enhance light harvesting and mass transfer. Concurrently, Mn doping builds Fe−O−Mn interfaces optimizing Fe d -band centers via d-d hybridization, accelerating charge separation. The catalyst showed exceptional performance under wide pH range (pH 2 −9), achieving 96.4 % methyl orange degradation and 98.2 % Cr(VI) reduction within 5 min. It exhibits 22.1/10.0-fold activity enhancement over FeC 2 O 4 under alkaline conditions and > 85.1 %/85.4 % stability after ten cycles. This work pioneers waste-derived catalysts for pH-universal water purification.
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INTERNATIONAL IMMUNOPHARMACOLOGY
·
2017
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IF 2.956
Zhixin Peng,Xiaobao Gong,You Yang,Ligua Huang,Qingyan Zhang,Peng Zhang,Rongzhen Wan,Baoshun Zhang
Quercetin is regarded as a potential hepatoprotective agent in the treatment of acute liver injury. However, the underlying mechanism of how quercetin to protect against lipopolysaccharides/ d -galactosamine (LPS/ d -GalN) induced acute liver injury remains unclear. To investigate the mechanism, the antioxidative, anti-inflammatory and antiapoptotic responses were performed. The results showed that quercetin pretreatment improved the survival rate and substantially reduced the liver histopathological changes in mice. It also alleviated the hepatic damage and reduced the productions of oxidative markers induced by LPS/ d -GalN. In addition, quercetin pretreatment significantly diminished the production of inflammatory cytokines, including TNF-α, IL-6 and IL-1β, and inhibited the activation of the NF-κB and MAPK signaling pathways as well as the expression of apoptotic-related proteins induced by LPS/ d -GalN. We found that the potential mechanism of this quercetin-induced protection is mainly mediated through its powerful antioxidative capacity, inhibition of hepatocyte apoptosis and suppression of inflammatory cytokines through the IKK/NF-κB and MAPK signaling pathways. Thus, quercetin shows a promising therapeutic effect on acute liver injury in mice.
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高影响因子
BIOSENSORS & BIOELECTRONICS
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2021
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IF 10.618
Shuju Zhao,Nianzu Liu,Wenqi Wang,Zhenying Xu,Yumin Wu,Xiliang Luo
The development of antifouling biosensors capable of detecting biomarkers at low concentrations in complex bio-fluids with many interference components is of great importance in the diagnosis and treatment of diseases. Certain zwitterionic peptides composed of natural L-amino acids have been used for the construction of low fouling biosensors and demonstrated excellent antifouling performances, but they are prone to enzymatic degradation in biological media, such as serum that contains a variety of enzymes . In this work, a novel antifouling peptide with the sequence of cppPPEKEKEkek was designed, and three unnatural D-amino acids were set at both ends of the peptide to enhance its tolerance to enzymatic degradation. An electrochemical biosensor was constructed by coupling the antifouling peptide with a conducting polymer polyaniline (PANI) to achieve accurate detection of alpha-fetoprotein (AFP) in clinical samples. Owing to the presence of the designed peptide with partial D-amino acids (pD-peptide), the biosensing interface showed significantly high antifouling performance and enhanced stability in human serum. Meanwhile, the pD-peptide based biosensor exhibited high sensitivity toward the target AFP, with the linear range from 0.1 fg mL −1 to 1.0 ng mL −1 and the limit of detection of 0.03 fg mL −1 (S/N = 3). This strategy of enhancing the stability (tolerance to enzymolysis) of antifouling peptides in biological samples provided an effective way to develop antifouling biosensors for practical applications.
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Nutrients
·
2022
·Vol. 14
·期 13
·2591
·
IF 6.706
Cuicui Zhang,Hai Niu,Chengyu Wan,Xiuxian Yu,Guang Xin,Yuda Zhu,Zeliang Wei,Fan Li,Yilan Wang,Kun Zhang,Shiyi Li,Yuman Dong,Yangying Li,Wen Huang
Acute pancreatitis (AP) is one of the most common causes of hospitalization for gastrointestinal diseases, with high morbidity and mortality. Endoplasmic reticulum stress (ERS) and Gasdermin D (GSDMD) mediate AP, but little is known about their mutual influence on AP. Diosgenin has excellent anti-inflammatory and antioxidant effects. This study investigated whether Diosgenin derivative D (Drug D) inhibits L-arginine-induced acute pancreatitis through meditating GSDMD in the endoplasmic reticulum (ER). Our studies were conducted in a mouse model of L-arginine-induced AP as well as in an in vitro model on mouse pancreatic acinar cells. The GSDMD accumulation in ER was found in this study, which caused ERS of acinar cells. GSDMD inhibitor Disulfiram (DSF) notably decreased the expression of GSDMD in ER and TXNIP/HIF-1α signaling. The molecular docking study indicated that there was a potential interaction between Drug D and GSDMD. Our results showed that Drug D significantly inhibited necrosis of acinar cells dose-dependently, and we also found that Drug D alleviated pancreatic necrosis and systemic inflammation by inhibiting the GSDMD accumulation in the ER of acinar cells via the TXNIP/HIF-1α pathway. Furthermore, the level of p-IRE1α (a marker of ERS) was also down-regulated by Drug D in a dose-dependent manner in AP. We also found that Drug D alleviated TXNIP up-regulation and oxidative stress in AP. Moreover, our results revealed that GSDMD-/-mitigated AP by inhibiting TXNIP/HIF-1α. Therefore, Drug D, which is extracted from Dioscorea zingiberensis, may inhibit L-arginine-induced AP by meditating GSDMD in the ER by the TXNIP /HIF-1α pathway.Keywords:acute pancreatitis;L-arginine;Gasdermin D;endoplasmic reticulum stress;TXNIP
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EUROPEAN POLYMER JOURNAL
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2022
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IF 5.546
Zengfang Huang,Chaoyue Zhou,Yang Yu,Siyi Wang,Rao Fu,Xiaobo Liu,Liucheng Mao,Jinying Yuan,Lei Tao,Yen Wei
In recent years, fluorescent materials with aggregation-induced emission (AIE) have been receiving widespread attention in diverse fields due to their unique characteristics. In this work, a novel AIE fluorescent dye TTPA with electron acceptor–donor (A-D) structure were fabricated through Suzuki coupling and Knoevenagel condensation reaction using benzothiazole (BTA) and 4-(1,2,2-triphenylvinyl) benzaldehyde (TPB) as main components, and its maximum emission wavelength was about at 524 nm, otherwise, on the basis of the quantum calculations, the energy difference ΔE between HOMO and LUMO of TPB and TTPA were about 3.63 eV and 2.81 eV, respectively. The obtained TTPA dye with AIE feature could emit fluorescence in THF owing to the electron A-D structure and intramolecular charge transfer (ICT) effect. Subsequently, the amphiphilic fluorescent copolymers PEG-PA were synthesized through the RAFT polymerization of TTPA and PEGMA with various feeding ratios. The molecular weight (M W ) and molecular weight distribution (Ð) of PEG-PA1 were about 1.8 × 10 4 and 1.30, respectively. According to the 1 H NMR spectra, the molar proportion of TTPA in PEG-PA increased from 18.5 % to 26.6 % when the proportion of TTPA in the reactants increased from 20.0 % to 25.0 %. Moreover, the as-prepared PEG-PA copolymers would self-assemble into nanoparticles with 150–200 nm diameter in a water solution due to their amphiphilic property, which exhibited the prospective bioimaging application with many advantages such as hypotoxicity, good biocompatibility, and excellent cells penetration.
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TALANTA
·
2025
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IF 6.1
Xiang Li,Yuting Zhang,Mengyuan He,Jiarui Sun,Bowen Xiong,Gongke Wang
In this work, we present an ultrasensitive, specific, and high-signal-to-background ratio fluorescence split-aptasensor for D-vasopressin (D-VP) detection. This sensor is based on target-induced self-propelled 3D DNA walkers in conjunction with CRISPR-Cas12a technology. Two split probes (SDA 1 and SDA 2) were designed to undergo structural recombination and function as a walking chain (SDA) under the induction of D-VP. Simultaneously, an intact Mg 2+ -dependent DNAzyme domain was formed at the tail of SDA and subsequently activated. The activated Mg 2+ -dependent DNAzyme continuously propelled the 3D DNA walker, enabling the generation of signal strand DNA (activator DNA). The activator DNA can subsequently trigger the activation of the Cas12a protein, enabling it to cleave the FAM-ssDNA-BHQ1 substrate. This process leads to signal amplification and the specific detection of D-VP. Under optimal conditions, the designed split-aptasensor exhibits excellent linearity across a concentration range of 5 ng/mL to 1215 ng/mL, with a detection limit (LOD) as low as 0.22 ng/mL. This split-aptasensor were employed to identify D-VP in human serum and urine samples, yielding highly satisfactory results. This unique design acts as a proof of concept and illustrates considerable promise for the detection of a wide range of analytes.
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JOURNAL OF MOLECULAR LIQUIDS
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2024
·
IF 5.3
Chuxin Qi,Lifang Chen,Zhiwen Qi
The heterogeneous liquid–liquid O-glycosidation is a crucial step in pharmaceutical synthesis. Herein, a theoretical methodology based on COSMO-RS, quantum chemical calculations combined with Transformer-CNN model was used to screen ionic liquids (ILs) as phase transfer catalysts (PTCs) to intensify O-glycosidation between 4-nitrophenol and 2,3,4,6-tetra-O-acetyl-α-D-galactopyranosyl bromide. The anions of ILs were screened by the evaluation of ILs hydrophilicity via infinite dilution selectivity of ILs and the molecular descriptor HB_acc3 of the anion using COSMO-RS, a predictive model for thermodynamic properties. Additionally, the binding energy between the phenoxide anion and IL cation was used to assess reaction extent in the aqueous phase through quantum chemical calculation. The cations of ILs were evaluated by the infinite dilution selectivity of the combination between phenoxide anion and IL cations, and physical properties including viscosity and melting point were also predicted using an advanced Transformer-CNN model. The screened IL 1-octyl-3-methylimidazolium acetate and 1-hexyl-3-methylimidazolium acetate were demonstrated its superior catalytic activity for the aromatic O-glycosidation of not only 4-nitrophenol, but also various phenols and thiophenols. Moreover, the presence of PTCs enhances the likelihood of the reactant migrating into another phase. This behavior is validated by COSMO-RS calculated liquid–liquid equilibrium (LLE) and interaction energy analysis. The method provides great potential for screening and designing ILs as phase transfer catalysts for heterogeneous liquid–liquid reactions.
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CHINESE JOURNAL OF POLYMER SCIENCE
·
2022
·Vol. 41
·期 7
·1115-1122
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IF 3.815
Zhong Chan-Na,Liu Ya-Dong,Tang Juan,Chen Wei-Shuo,Li Shuang-Cheng,Shao Jun,Hou Hao-Qing
Blending of poly(levorotatory-lactic acid) (PLLA) and poly(dextrorotatory-lactic acid) (PDLA) produces the stereocomplex crystallites (PLA SC), which present higher melting temperature and mechanical properties than that of neat PLLA or PDLA. However, in the PLLA/PDLA blends with higher molecular weights, the phase separation occurs and the SC exhibits weak memory after melting, which lead to a small amount of SC together with a large amount of homochiral crystallites (HC) develop during crystallization from the melt. In this study, a small content of graphite oxide was blended with PLLA and PDLA to form ternary blends, and it was exciting to find that the formation of SC was enhanced gradually with the content of graphite oxide. The SC exclusively developed when 2 wt% graphite oxide was incorporated into the PLLA/PDLA, and the crystallinity with ∼50% was received even during fast cooling from the melt (−50 °C/min). The acceleration formation of SC was speculated due to the interaction between PLA molecular chains and the hydroxyl groups on the surface of graphite oxide and the obstruction of proliferation of graphite oxide.
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JOURNAL OF ENZYME INHIBITION AND MEDICINAL CHEMISTRY
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2026
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IF 5.3
Jiake Gao,Yujing Zhang,Rui Qu,Qianqian Xu,Zhenjuan Sun,Liya Cui,Chao Wang
Microtubules assembled from α/β-tubulin heterodimers are critical for cell division and well-established anticancer drug targets, making tubulin polymerization inhibitors a viable route for new chemotherapeutics. Guided by structural analysis of colchicine-site binders and tubulin-ligand computational simulations, we rationally designed and synthesized a series of 6-aryl-1-(3,4,5-trimethoxyphenyl)-1H-pyrazolo[3,4-d]pyrimidines as novel colchicine-binding site tubulin inhibitors. Derivative 9t displayed the strongest antiproliferative potency, with IC₅。 values of 0.065-0.096 μM across tested cancer lines. It exerted minimal toxicity to normal L929 fibroblasts, yielding a selectivity index over 300. Mechanistic assays confirmed 9t suppresses cell-free tubulin polymerization, destroys cellular microtubule architecture, induces persistent G₂/M cell cycle arrest, and activates cancer cell apoptosis. Overall, 9t serves as a promising dual-function tubulin inhibitor with both cytostatic and cytotoxic anticancer effects, meriting further preclinical investigation.
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Molecular Catalysis
·
2026
·
IF 4.3
Wenhui Li,Jiajia Chen,Jiaolong Fu,Zhi Chen,Xin Ju,Liangzhi Li
Design and fabrication of multifunctional charge-tunable hydrogel carriers. • Molecular docking reveals hydrogen bonding mechanisms in charge-assisted non-covalent immobilization. • PASP/PNIPAM-immobilized enzymes retain 89.7% initial activity after six cycles. • A novel biocatalytic pathway for D-xylose enables efficient rare sugar production. Immobilization of enzymatic cascades is an important tool for the efficient production of value added products, such as rare sugars from biomass monosaccharides. However, there is a lack of biocompatible and inexpensive immobilization carriers with high reusability in immobilizing multiple enzyme proteins currently. In this study, poly-N-isopropylacrylamide (PNIPAM) hydrogels were fabricated and employed to immobilize the enzymatic cascade of glucose isomerase (GI) and D-tagatose-3epimerase (DTE) for the conversion of D-xylose to rare sugar products, D-xylulose and D-ribulose. To attain stable protein attachment and high reusability, PNIPAM microspheres were further grafted by polyaspartic acid (PASP), polyethylene glycol (PEG), polylysine (PL), and anionic polyacrylamide (APAM), obtaining composite hydrogels with tailored surface charges to achieve effective non-covalent immobilization. The enzymatic cascades immobilized by modified PNIPAM hydrogels demonstrated improved thermal stability in the range of 40–70 °C with prolonged enzyme half-lives, and higher conversion of D-xylose. After 6 recycles, PASP/PNIPAM-GI-DTE retained 89.7% initial activity which was superior in enzyme immobilization by PNIPAM. Molecular simulation studies revealed that PASP/PNIPAM formed stable hydrogen bonds with GI and DTE, rationalizing its superior performance. This work proved charge aided immobilization of proteins as a feasible strategy for the production of biomass derived high value chemicals, and provided a practical protocol for industrial scale biomanufacturing. Download: Download high-res image (204KB) Download: Download full-size image
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