APPLIED CATALYSIS B-ENVIRONMENTAL
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2026
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IF 21.1
Meng Li,Liyao Zeng,Peitong Cen,Ziyin Xia,Jiaqian Zhang,Lei Huang,Jia Yan,Shaoqi Zhou,Ce-Hui Mo,Xiangkang Zeng,Hongguo Zhang
This work introduces an innovative stacked iron mesh electrode configuration to achieve accelerated degradation of perfluorooctanoic acid (PFOA) by synergistically coupling electrochemical oxidation with peroxymonosulfate (PMS) activation. The system was systematically evaluated through electrochemical measurements, free radical quenching, and electron paramagnetic resonance spectroscopy, complemented by density functional theory calculations. The optimized triple-layer Fe electrode demonstrated outstanding performance, attaining nearly complete PFOA removal (100 %) within 12 min and a high kinetic rate constant of 0.218 min –1 . DFT analysis revealed that the Fe mesh possessed the strongest PMS adsorption energy (–2.68 eV) and the shortest Fe–O bond length (2.24 Å), confirming its superior activation capability. Mechanistic studies confirm the effectiveness of the electron transfer coupled with the hydroxyl radicals in defluorination and decarbonization during PFOA degradation. In addition, the system exhibited high cycle stability and strong tolerance to various background ion under continuous operations in the amplification experiment. The system also exhibited superior performance and low leaching of metal ions in treating various organic pollutants of practical wastewater (fluoride wastewater and landfill leachate). These findings present an effective and practical strategy for the remediation of persistent per- and polyfluoroalkyl substances in contaminated water sources.
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Nature Communications
·
2026
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IF 15.7
Zhang Xinyi,Wang Liangjie,Wei Jian,Guo Zhuang,Liu Xinyao,Duan Lijie,Zhao Huazhang,Song Yonghui
Oxygen vacancies (O v ) on metal oxide surfaces exhibit high catalytic activity for activating peroxymonosulfate (PMS) in wastewater decontamination, yet their in-situ regeneration remains a significant challenge. This study successfully achieves in-situ real-time regeneration of O v on CuO surfaces through simple alkali etching without interrupting the contaminant removal process. The surface hydroxyl groups introduced by alkali treatment significantly reduce the formation energy of O v on CuO surfaces from 1.60 eV to 0.38 eV. Both experimental results and density functional theory calculations reveal that the high activity of CuO relies on the synergy of surface hydroxyl groups and O v . This synergy increases the antibonding states below the Fermi level and the electron spin density of Cu near O v , thereby promoting electron transfer from CuO to PMS. As a result, by just adding an equimolar amount of alkali relative to PMS in CuO/PMS system, the degradation rate constant of sulfamethoxazole (SMX) greatly increases by 42 times. The primary reactive oxygen species in this system are sulfate radicals and hydroxyl radicals. Furthermore, OH - /CuO/PMS system exhibits a long-term stability (> 300 h) for SMX removal in a real water matrix. This work provides a highly executable method to in-situ real-time regenerate O v on CuO surfaces, representing significant progress in the critical yet underappreciated field of catalyst regeneration.
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PubMed
高影响因子
FOOD CHEMISTRY
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2026
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IF 9.8
Xinge Ju,Guantong Liu,Xin Sun,Haiyang Lv,Zhanye Yang,Shutong Zhang,Yuan Tian,Bing Zhao
This work developed a dual-mode sensor based on aptamer regulation of silver core-cuprous oxide shell (Ag@Cu 2 O) nanozyme activity for kanamycin detection. The synthesized Ag@Cu 2 O nanoparticles served as both a surface-enhanced Raman scattering activity (SERS) substrate and a peroxidase-like catalytic activity. The aptamer adsorbed on the Ag@Cu 2 O surface enhanced the nanozyme activity through electrostatic interactions with positively charged 3,3′,5,5′-tetramethylbenzidine (TMB). This promoted the oxidation of TMB to blue oxidized 3,3′,5,5′-tetramethylbenzidine (ox-TMB) by hydrogen peroxide (H 2 O 2 ). Upon kanamycin binding, the colorimetric absorbance and SERS intensity decreased. The SERS mode achieved a linear range of 0.01–1 μM and the limit of detection (LOD) of 1.78 nM. The colorimetric mode provided a linear range of 0.1–1 μM and a LOD of 47.7 nM. Good recoveries (92.48–102.57%) and low relative standard deviations (RSD < 5.0%) were achieved in spiked honey and mutton samples. This dual-mode design offered potential for food safety monitoring of kanamycin residues.
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Advanced Healthcare Materials
·
2026
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IF 9.6
Meichan Wu,Puze Li,Xin Xin,Cheng Song,Xiangliang Yang,Qingxia Xu,Yan Liu,Yong Shen,Guoping Wang,Jun Hu
The activation and infiltration of cytotoxic T lymphocytes (CTLs) are the key of tumor immunotherapy. However, the suppressive tumor immune microenvironment usually inhibits the function of CTLs. Tumor-associated macrophages (TAMs) play an important role in remodeling the tumor immune microenvironment. In this work, probiotic Escherichia coli Nissle 1917 (EcN) is used as a bioreactor to achieve intracellular synthesis of copper selenide nanoparticles (Cu 2-x Se NPs), giving Cu 2-x Se@EcN, which effectively repolarize macrophages from pro-tumor M2 phenotype to anti-tumor M1 phenotype mainly through activating MAPK signaling pathway. The synthesized Cu 2-x Se NPs exhibited excellent photothermal performance, inducing hyperthermia-sensitized Fenton-like reaction to catalyze the generation of hydroxyl radical from H 2 O 2 , then resulted in immunogenic death effect of tumor cells and the repolarization of M2 macrophages. Combined with surface-expressed pathogen-associated molecular patterns (PAMPs) of bacteria, Cu 2-x Se@EcN synergistically promoted DCs maturation and TAMs reprogramming, eventually promoting the infiltration and activation of T cells. Therefore, the bacteria-inorganic hybrid nanomaterials showed satisfied effect in inhibiting tumor growth and recurrence.
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CHEMICAL ENGINEERING JOURNAL
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2026
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IF 13.2
Yilin Wu,Jichao Zhang,Jing Su,Yutong Wu,Shaohai Fu
Existing separation technologies struggle to separate nanosized oil droplets from highly stabilized emulsions to address the water supply shortage, exhibiting an inherent shortcoming of poor permeability and severe oil fouling. Herein, we presented a microscale channel of ceramic membranes with a piezoelectric semiconductor microsphere skin constructed of hydrophobic nanodomains and rich oxygen vacancies. The sprinkled hydrophobic nanodomains acted as “oil capturing tentacles”, facilitating the efficient coalescence of oil droplets and preventing the formation of oil cake layer. The obtained membranes with microchannels could efficiently separate 16 types of oil-in-water nano/submicrometer-emulsions, achieving an ultrahigh permeation flux of up to 6550 L·m −2 ·h −1 with the separation efficiency exceeding 99.85%. Additionally, oily foulants on the membrane undergo degradation by piezotronic effect-enhanced photocatalysts, where piezoelectric-induced band bending drives highly efficient separation of photogenerated carriers, markedly boosting oil degradation with a nearly 99.5% flux recovery of the membrane. This research pioneers new pathways to advance membrane separation and environmental remediation for real-world applications.
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APPLIED SURFACE SCIENCE
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2026
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IF 6.6
Taotao Lv,Mengran Lou,Chunmei Xu,Yang Wang,Ruiying Wang,Hongtao Liu,Rui Liu,Xia Kong
The Cu/Fe-N@PCFs catalyst is prepared by electrospinning and pyrolysis. • Cu active species synergize with Fe-N@PCFs to boost the catalytic performance. • Cu/Fe-N@PCFs shows excellent ORR/OER activity with a low ΔE of 0.73 V. • Flexible Cu/Fe-N@PCFs achieves high peak power densities in ZAB and FZAB. The key to advancing Zn-air batteries (ZABs) and flexible Zn-air batteries (FZABs) lies in creating electrocatalysts with flexibility, porosity, high efficiency, and stability. Herein, Cu/Fe-N@PCFs is prepared by electrospinning and pyrolysis. Fe-ZIF-8 serves as a carbon and nitrogen source dispersing Fe sites, and promotes the formation of microporous structures during pyrolysis together with NaCl. Cu species are introduced onto the surface of Fe-N@PCFs to interact with Fe-N x sites and alleviate the Fenton-like effect, synergistically enhancing the bifunctional oxygen electrocatalytic performance toward oxygen reduction reaction (ORR) and oxygen evolution reaction (OER). The fibrous structure improves the peak power density of ZAB and FZAB. The Cu/Fe-N@PCFs exhibits an ORR half-wave potential (E 1/2 ) of 0.865 V (vs. 0.838 V for Pt/C) and an OER overpotential of 370 mV (vs. 305 mV for RuO 2 ) at 10 mA cm −2 . The ZAB achieves a peak power density of 278.2 mW cm −2 (vs. 145.5 mW cm −2 for Pt/C + RuO 2 ) and durability of 190 h. The self-supporting Cu/Fe-N@PCFs is assembled as FZAB, delivering a peak power density of 82.4 mW cm −2 (vs. 16.4 mW cm −2 for Pt/C + RuO 2 ) and durability of 17 h. This study provides significant perspectives on constructing flexible catalysts, potentially advancing the development of ZABs and FZABs. Download: Download high-res image (266KB) Download: Download full-size image
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INORGANIC CHEMISTRY COMMUNICATIONS
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2026
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IF 5.9
Jujiao Zhao,Yixuan Li,Xianghe Dong,Xiaoxia Bai,Hao Tang,Jia Zeng,Haoxuan Wei,Quanfeng Wang,Youzhou He
Designing low-cost heterogeneous catalysts that simultaneously offer accessible pore channels, abundant surface defects, and efficient interfacial electron transfer is important for peroxymonosulfate (PMS)-based antibiotic oxidation. In this work, porous copper ferrite-based catalysts were synthesized through a solvent-free grinding-calcination strategy using glucose, citric acid, and oxalic acid as reactive soft templates. The oxalic-acid-derived catalyst (O-CFO) showed a CuFe 2 O 4 /Fe 2 O 3 composite structure with a macroporous architecture and the highest oxygen-vacancy content, achieving a tetracycline (TC) removal efficiency of 92.4% within 60 min and an apparent rate constant of 0.073 min −1 , outperforming glucose- and citric acid-derived samples. The O-CFO/PMS system maintained efficient TC degradation over a broad pH range of 3.2–9.1 and was tolerant of common coexisting constituents and real water matrices. Quenching and electrochemical results suggest that 1 O 2 , •OH, SO 4 •- , and surface-mediated electron-transfer pathways jointly contribute to TC oxidation. This study demonstrates a scalable soft-template route for constructing porous oxygen-defective CuFe-based catalysts for PMS-driven antibiotic abatement.
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ACTA PHYSICO-CHIMICA SINICA
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2026
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IF 13.5
Baogang Fu,Nan Su,Jianmin Luo,Yun Wang,Bo Hu,Liang Cheng,Hongjun Dong,Chunmei Li
SCN-AP with a D-π-A network was synthesized via sulfur doping and pyridine grafting. • SCN-AP achieves integrated design of 1 O 2 generation and kinetic matching of ORR/WOR. • SCN-AP boosts ·O 2 - / 1 O 2 generation, with a H 2 O 2 yield of 1030 μmol g -1 within 2 h. • Antibacterial assays verify the photoactivated antibacterial potential of SCN-AP. • In-situ XPS and DRIFTS characterize photogenerated electron flow and reaction intermediates. Photocatalytic H 2 O 2 synthesis is commonly dominated by the oxygen reduction reaction (ORR), whereas simultaneously enabling water oxidation reaction (WOR) and directional charge separation through band-structure regulation remains challenging. Herein, sulfur doping and pyridine modification were integrated to construct an intramolecular donor- π -acceptor (D- π -A) network within the carbon nitride framework. The resulting electronic polarization promotes directional separation of photogenerated charge carriers and optimizes the band structure to thermodynamically enable both ORR and WOR pathways. Consequently, the as-synthesized SCN-AP photocatalyst achieves an H 2 O 2 yield of 1030 μmol g -1 within 2 h in pure water, 3.73 times that of pristine PCN, and exhibits effective antibacterial activity against clinically relevant pathogens including Acinetobacter beijerinckii and Klebsiella variicola . The in-situ electron paramagnetic resonance (EPR) spectroscopy and in-situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) collectively support the coexistence of ORR and WOR pathways. The ORR serves as the predominant route and involves a ·O 2 - -mediated stepwise reduction pathway together with a 1 O 2 -associated pathway, while WOR provides a complementary hole-driven contribution to H 2 O 2 formation. This work demonstrates a feasible band-engineering strategy for constructing polymeric photocatalysts with directional charge transfer and dual-pathway H 2 O 2 photosynthesis. This work demonstrates a D-π-A-mediated electronic polarization strategy that directs charge migration in carbon nitride, enabling dual-pathway H 2 O 2 photosynthesis through coupled ORR and WOR processes. Download: Download high-res image (411KB) Download: Download full-size image
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ACS Applied Materials & Interfaces
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2026
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IF 7.8
Hu Ruiling,Zhang Yujie,Gao Chengzhi,Wei Hang,Hong Xianjian,Wei Xiaodan,Qiang Tinghui,Guo Zhongshang,Huang Li,Lei Xiaoyun,Zhao Caibin,Ji Xiaohui,Han Hao,Guo Shaobo
The treatment of wounds caused by drug-resistant bacteria is a significant challenge in clinical medicine. Silver (Ag) nanoparticles have attracted considerable attention due to their ability to inhibit drug-resistant bacteria. Nevertheless, the propensity of Ag nanoparticles to aggregate as well as their elevated toxicity have restricted their practical application. To address this issue, this study involved the design of a core–shell-type ZnO@ZIF-8/Ag nanocomposite material that combines high antibacterial activity with excellent biocompatibility. The mean diameter of the Ag nanoparticles in this material was approximately 2.4 nm, and they were highly dispersed. Within the wound microenvironment, antibacterial factors, such as hydroxyl radicals ( · OH), singlet oxygen ( 1 O 2 ), Zn 2+ , and Ag + , were generated. The material induced bacterial death by altering the structure of the cell wall of drug-resistant bacteria, thereby inhibiting respiration, lysing phospholipid layers, and causing cellular content leakage. The introduction of zinc oxide (ZnO) significantly reduced the toxicity of the Ag nanoparticles and regulated macrophage polarization, which inhibited the secretion of tumor necrosis factor-α (TNF-α) and interleukin-6 (IL-6) by M1-type macrophages (M1) while concomitantly promoting the secretion of interleukin-10 (IL-10) and vascular endothelial growth factor by M2-type macrophages (M2). The expression of platelet-endothelial cell adhesion molecule-1 (CD31), type I collagen/fibronectin (COL-I/FN), and proliferating cell nuclear antigen (PCNA) was significantly promoted, which significantly enhanced wound healing in infected wounds. This study thus offers a strategy for developing therapies against drug-resistant bacterial infections with the potential for clinical application.
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Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 5
·124602
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IF 7.5
Yunyi Wang,Ru Yang,Xiang Li,Haiping Wang,Ting Wu,Guigan Fang
Photocatalytic cleavage of lignin C–C bonds using graphitic carbon nitride (g-C 3 N 4 ) offers a sustainable route to aromatic monomers; however, its practical efficiency is critically constrained by the generation yield of superoxide radicals. Herein, we address this constraint through a simple yet effective design: replacing the edge amino groups of g-C 3 N 4 with benzene rings to construct a benzene–g-C 3 N 4 copolymer. DFT calculations suggest that the introduced benzene ring contributes an empty low-lying orbital that may serve as a temporary electron trap. This effect, together with in-situ XPS evidence for photo-induced charge redistribution, is consistent with the formation of an S-scheme charge transfer pathway and the observed suppression of picosecond-scale electron–hole recombination. The benzene ring is proposed to function as a π–π adsorption anchor, selectively binding the lignin C β carbocation in close proximity to the C–N = C sites where superoxide radicals are generated. This directed adsorption overcomes the mass-transfer limitation of superoxide radical typically encountered under chemisorption conditions, thereby enabling spontaneous and diffusion-free oxidation of the C β site. This benzene–g-C 3 N 4 copolymer exhibits a 134% higher reaction efficiency than g-C 3 N 4 in C–C bond photocleavage, while also demonstrating excellent cleavage performance on industrial lignin. Collectively, this work offers an effective approach to overcoming kinetic limitations in photocatalysis.
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Nature Communications
·
2026
·
IF 18.1
Zuo Shulin,Lin Muke,Xu Guizhi,Huang Jiahao,Zhang Rumeng,Mei Ji,Fang Jingyun,Xia Dehua
Conventional catalytic ozonation of electron-rich sulfur-containing pollutants shows limited efficiency due to nonselective oxidation of hydroxyl radicals ( • OH) and sulfate-induced deactivation of active metal sites. Here, we synthesized a high-entropy spinel, (CuNiMnCo)Fe 2 O 4 , featuring sublattice-resolved electronic reconstruction that enables selective ozone activation and suppresses sulfur poisoning. The catalyst achieves 99% removal of methyl mercaptan (CH 3 SH), significantly outperforming 51% of CoFe 2 O 4 . Spectroscopic analyses and density functional theory calculations reveal that high-entropy doping induces lattice distortion and local coordination disorder, which strengthen A–O–B covalency and inter-site electronic communication. This structural perturbation further drives a sublattice-resolved electronic reconstruction, enriching Co/Mn sites while depleting Fe/Cu/Ni sites. This electronic differentiation promotes cooperative dual-end activation of O 3 on Fe–Co/Mn motifs and preferential CH 3 SH adsorption on Cu/Ni sites. Orbital modulation of Co t 2g and Fe e g states near the Fermi level balances interfacial charge transfer, favoring formation of a surface-bound *O 3 species over conventional O–O bond cleavage. The resulting spatially separated activation and oxidation sites enable CH 3 SH mineralization via an electron transfer process while suppressing • OH generation and minimizing sulfate accumulation. This spatially differentiated reaction environment ensures durable performance under humid conditions. These findings establish sublattice-engineered electronic asymmetry as a strategy for selective catalytic ozonation.
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Nature Communications
·
2026
·
IF 18.1
Liu Xu,Cao Miao,Jia Feiyue,Jia Hongbao,Li Zonglin,Guo Xueping,Zhang Junrong,Hua Weijie,Li Lina,Wu Qian,Zhao Hongying
Antibiotic-resistant bacteria (ARB) and their genes (ARGs) pose a significant risk to public health and the ecosystem. Conventional water disinfection efficiently eliminates pathogens, however, it requires intensive chemical consumption but inefficiently removes ARGs. Herein, we propose an on-demand electrochemical platform that simultaneously eliminate both ARB and ARGs with in-situ generated hydroxyl radicals (·OH) without additional chemical inputs. Single-atom copper catalysts with CuN 4 coordination structure (SA-CuN 4 /NC) are precisely tuned to directly convert oxygen into controllable ·OH via three-electron oxygen reduction reaction (3e⁻ ORR). Operando X-ray adsorption near-edge spectroscopy reveals a potential-driven self-reconstruction of single-atom Cu sites to optimize ·OH concentration. Specially, the preferentially adsorbed H + onto the adjacent N atoms promotes the breaking of Cu-N bonds to form stable Cu 2 -CuN 2 cluster as a genuine active site. As expected, the SA-CuN 4 /NC with moderate ·OH (~11.5 μM) exhibits ultra-fast degradation of E. coli HT115 , accomplishing an ~ 8 log removal within 1 min and a complete elimination of ARGs in 30 min. Excess ·OH (~47.9 μM) triggers bacterial aggregation which compromises bacterial inactivation. These findings demonstrate that 3e⁻ ORR is a sustainable and effective strategy to obtain fast and complete water disinfection, preventing environmental spread of ARGs.
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