化学•材料最新文献

{"title":"Activation of Chlorite with Sunlight for the Efficient Disinfection of Antibiotic-Resistant Bacteria: the Overlooked Contribution of Cytomembrane-Bound Chlorite.","authors":"Yutao Shen,Fuyang Liu,Jialiang Liang,Zhengmao Li,Yanghui Hou,Jingfeng Wu,Yong Ting,Renjie Guo,Yong Liu,Peng Han,Meiping Tong","doi":"10.1021/acs.est.5c02180","DOIUrl":"https://doi.org/10.1021/acs.est.5c02180","url":null,"abstract":"Current antibiotic-resistant bacteria (ARB) disinfection techniques commonly rely on large dosages of oxidants, resulting in the presence of considerable amounts of residuals and toxic disinfection byproducts (DBPs) in water. Herein, we propose a highly effective ARB disinfection approach via activating an ultralow concentration (10 μM) of chlorite (ClO2-) by naturally abundant sunlight to generate various reactive species (i.e., HO•, Cl•, ClO•, and ClO2) with negligible generation of halogenated DBPs. Combining in situ characterization with theoretical calculations, we reveal that, in addition to the photolysis of ClO2- in the bulk solution, ClO2- ions electrostatically adsorbed on the positive local sites of lipids can boost light absorption and facilitate the in situ generation of reactive species upon sunlight irradiation, enabling more efficient attacks toward cell membranes and the intracellular antioxidant enzyme system. The intracellular antibiotic resistance genes (ARGs) are then released and further degraded, inhibiting horizontal ARG transfer. This approach can also achieve excellent ARB disinfection performance in real water matrices (e.g., lake and river water) in 1 L tanks and 500 mL plastic bottles with natural sunlight irradiation. Overall, this work presents an efficient, safe, and sustainable method to inactivate ARB with deep insights into disinfection mechanisms at the subcellular level.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"12 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-09-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145003219","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Deciphering the Microstructures and Electronic Properties of the YVO₄:Re (Re = Pr, Nd, and Tm) Crystals: A Theoretical Insight.","authors":"Yue Xu, Wenhao Ji, Meng Ju, Mingmin Zhong, Yang Xiao, Weiguo Sun, Yuanyuan Jin, Chuanzhao Zhang","doi":"10.1021/acs.jpca.5c01554","DOIUrl":"https://doi.org/10.1021/acs.jpca.5c01554","url":null,"abstract":"<p><p>Rare-earth ion (Pr³⁺, Nd³⁺, and Tm³⁺)-doped yttrium vanadate (YVO₄) crystals have aroused great research interest owing to their excellent laser performances. However, the microstructures, which underlie the optical properties of these crystals, are still unclear. In this paper, the stable crystal structures of the YVO₄:Re (Re = Pr, Nd, and Tm) systems are predicted by using the crystal structure analysis by the particle swarm optimization (CALYPSO) structure search method. The unique tetragonal structures with the <i>P</i>4̅<i>m</i>2 (no. 115) space group for the YVO₄:Re crystals are identified for the first time. It is found that the rare-earth ions (Pr³⁺, Nd³⁺, and Tm³⁺) can accurately occupy the Y³⁺ sites and successfully fuse into the YVO₄ host crystals. The simulated X-ray diffraction (XRD) patterns of the YVO₄ and YVO₄:Re (Re = Pr, Nd, and Tm) are consistent with the experimental measurements, demonstrating the possibility and rationality of the predicted structures. Furthermore, we are motivated to clarify the electronic properties of the pure YVO₄ and YVO₄:Re (Re = Pr, Nd, and Tm) crystals based on density functional theory (DFT). The calculated electronic band structures of YVO₄:Re (Re = Pr, Nd, and Tm) indicate reductions in the band gaps. With the increase in f-electrons, the energies of the f-electrons in the conduction bands decrease slightly. The calculated electron localization functions (ELF) of YVO₄:Re (Re = Pr, Nd, and Tm) show that the bonding characteristics of Y-O, Pr-O, Nd-O, and Tm-O are all ionic. These theoretical results could provide important information for further research on the rare-earth-doped laser materials.</p>","PeriodicalId":59,"journal":{"name":"The Journal of Physical Chemistry A","volume":" ","pages":""},"PeriodicalIF":2.8,"publicationDate":"2025-09-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145005618","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Intelligent Self-Healing Polymeric Systems for Functional and Durable Coatings.","authors":"Sudipta Paul, Ankit Kumar Kaushik, Amul Jain, Sanjib Banerjee","doi":"10.1002/asia.70290","DOIUrl":"https://doi.org/10.1002/asia.70290","url":null,"abstract":"<p><p>Self-healing polymeric coatings represent a transformative class of smart materials capable of autonomously or stimuli-responsively repairing mechanical or environmental damage, thereby significantly extending the operational lifespan of protected substrates. This review systematically elucidates the underlying mechanisms and chemistries enabling self-healing behavior, encompassing both extrinsic strategies such as microcapsules, microvascular networks, and corrosion inhibitor reservoirs and intrinsic approaches based on dynamic covalent (e.g., disulfide exchange, Diels-Alder, imine, transesterification/vitrimer networks) and supramolecular interactions (e.g., hydrogen bonding, metal-ligand coordination, ionic, and host-guest systems). Emphasis is placed on recent advances in external stimuli-responsive systems triggered by heat, light, moisture, pH, electricity, or magnetic fields. The performance of these coatings under extreme conditions, including corrosive media, marine environments, thermal cycling, mechanical fatigue, and high-voltage fields, is critically evaluated. Furthermore, this review highlights industrial translation through commercial exemplars (e.g., NANOMYTE® MEND, BASF Elastocoat, Baydur HC, FEYNLAB), scalable fabrication routes (spray coating, dip-coating, UV-curing, and 3D/4D printing), and alignment with sustainability goals. Challenges such as multifunctional integration, interfacial adhesion, regulatory compliance, and the need for standardized evaluation metrics are discussed. Finally, future directions in predictive molecular design and high-throughput screening are outlined to accelerate the development of next-generation self-healing coatings (SHC) across diverse Asian industrial sectors.</p>","PeriodicalId":145,"journal":{"name":"Chemistry - An Asian Journal","volume":" ","pages":"e70290"},"PeriodicalIF":3.3,"publicationDate":"2025-09-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144999351","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Enantio- and Diastereoselective Synthesis of Tricyclic Lactones Bearing Three Quaternary Stereocenters.","authors":"Yasuaki Furuya,Kazunobu Igawa,Seiji Shirakawa","doi":"10.1021/acs.joc.5c01607","DOIUrl":"https://doi.org/10.1021/acs.joc.5c01607","url":null,"abstract":"An efficient method for the enantio- and diastereoselective synthesis of tricyclic γ-butyrolactones bearing three quaternary stereocenters has been developed through transformations of achiral alkenoic acid substrates. The target optically active tricyclic lactones were obtained as single diastereomers with good enantioselectivities through a sequence of catalytic asymmetric bromolactonization, azidation, and subsequent 1,3-dipolar cycloaddition. The origin of the complete diastereoselectivity observed in the formation of the tricyclic γ-butyrolactone products was elucidated in this study.","PeriodicalId":57,"journal":{"name":"Journal of Organic Chemistry","volume":"40 1","pages":""},"PeriodicalIF":4.354,"publicationDate":"2025-09-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145003262","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Dual Modulation of Barrier Width and Height in van der Waals Ferroelectric Tunnel Junctions.","authors":"Yingying Zheng,Haiyan Yu,Xuefei Li,Shuoguo Yuan","doi":"10.1021/acs.jpclett.5c02145","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c02145","url":null,"abstract":"Two-dimensional ferroelectric tunnel junctions (2D FTJs) have attracted extensive attention in recent years, which mainly change the height of the tunnel barrier via manipulation of the ferroelectric polarization. However, it is very challenging to realize the high tunneling electroresistance (TER) of FTJs based on the barrier height. Here, we report the 2D FTJs using a unique structure with semiconducting MoS2/α-In2Se3/monolayer graphene, where ferroelectric polarization of α-In2Se3 shifts the barrier height by 1.05 eV. More importantly, the MoS2 dynamically tunes the barrier width, overcoming traditional barrier height limitations and enhancing TER by an order of magnitude. The dual modulation of barrier width and height yields a giant TER of more than 1 × 109 at room temperature. In addition, the FTJs possess excellent retention time for up to 10 years. This study exhibits that the constructed 2D FTJs have unprecedented applications in achieving high-performance memory, electronic, optoelectronic, and neuromorphic computing devices.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"64 1","pages":"9577-9582"},"PeriodicalIF":6.475,"publicationDate":"2025-09-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144996005","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Reactive Evolution of HMML from Gas Phase Formation to Interface Transformation on Sulfuric Acid Aerosols: A Multiscale Computational Study.","authors":"Xihong Liu, Baozhong Zhang, Xiaohui Ma, Yahui Shi, Kunjie Hou, Junting Qiu, Xiangli Shi, Shengjie Qi, Jiayao Yang","doi":"10.1021/acs.jpca.5c04295","DOIUrl":"https://doi.org/10.1021/acs.jpca.5c04295","url":null,"abstract":"<p><p>Hydroxymethyl-methyl-α-lactone (HMML) is a key epoxide precursor in forming tracer compounds 2-methylglyceric acid (2-MG) or 2-methylglyceric acid sulfate (2-MGOS) from isoprene under high-NOx conditions. Despite its importance, the formation and transformation of HMML─particularly under acidic aerosol conditions─are still poorly understood, limiting comprehensive knowledge of secondary organic aerosol (SOA) formation. In this study, quantum chemical calculations, Born-Oppenheimer molecular dynamics (BOMD), and metadynamics (MTD) simulations are employed to investigate both the formation of HMML from methacryloyl peroxynitrate (MPAN) and its interfacial transformation mechanisms on sulfuric acid aerosols. Results show that OH radicals preferentially add to the <i>β</i>-carbon of MPAN, generating HMML via a concerted process involving C-O bond formation and O-O bond cleavage. At acidic aerosol interfaces, HMML stably adsorbs through hydrogen bonding and can convert to 2-MG or 2-MGOS through one-step or two-step pathways, depending on the local solvation environment. High sulfuric acid concentration (59 wt. %) promotes direct nucleophilic addition by interfacial HSO₄^-/SO₄^2- ions, favoring 2-MGOS formation, while lower concentration (30 wt. %) favors an H₂O-mediated 2-MG pathway. These findings underscore the decisive influence of aerosol interfacial microenvironments on HMML transformation pathways, product distribution, and their broader role in SOA formation and atmospheric multiphase chemistry.</p>","PeriodicalId":59,"journal":{"name":"The Journal of Physical Chemistry A","volume":" ","pages":""},"PeriodicalIF":2.8,"publicationDate":"2025-09-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144999190","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Efficient Urea Oxidation on MnCO₃/Ni(OH)₂ Nanoflower Arrays Via Interfacial Coupling.","authors":"Nan Lu, Hao Guo, Fozia Sultana, Jie Zhang, Xiaoqing Yan, Renhong Li","doi":"10.1002/asia.202500828","DOIUrl":"https://doi.org/10.1002/asia.202500828","url":null,"abstract":"<p><p>The electrochemical urea oxidation reaction (UOR) presents an energy-efficient alternative to the sluggish oxygen evolution reaction (OER), operating at a substantially lower thermodynamic potential and thereby reducing the energy input for hydrogen production by approximately 70%. Simultaneously, UOR facilitates wastewater remediation, offering dual environmental and energy benefits. In this work, we report a MnCO₃/Ni(OH)₂ heterostructured nanoflower array directly grown on conductive carbon cloth that exhibits outstanding UOR catalytic activity and stability. The catalyst achieves remarkably low overpotentials of 90 mV at 10 mA·cm^-2 and 167 mV at 200 mA·cm^-2, along with excellent long-term durability under continuous operation. Comprehensive characterization and mechanistic analysis reveal that the enhanced performance originates from interfacial electronic redistribution at the MnCO₃/Ni(OH)₂ junction. This electronic interaction promotes the stabilization of highly-valent Ni active species and improves electrode wettability, thereby facilitating efficient charge transfer and mass transport. This study underscores the critical role of heterointerface engineering and compositional modulation in developing robust and high-performance UOR electrocatalysts, providing valuable insights for their practical deployment in sustainable hydrogen generation and environmental remediation.</p>","PeriodicalId":145,"journal":{"name":"Chemistry - An Asian Journal","volume":" ","pages":"e00828"},"PeriodicalIF":3.3,"publicationDate":"2025-09-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144999272","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Structural Elements of Dwarf Open Reading Frame Required for Activation of the Sarco-Endoplasmic Reticulum Calcium Pump.","authors":"M'Lynn E Fisher, Justin R Gregory, Stan T J Aanhane, M Joanne Lemieux, Howard S Young","doi":"10.1021/acs.biochem.5c00305","DOIUrl":"https://doi.org/10.1021/acs.biochem.5c00305","url":null,"abstract":"<p><p>The sarco-endoplasmic reticulum calcium pump (SERCA) is a P-type ATPase that plays a critical role in intracellular calcium signaling. SERCA maintains the calcium gradient between the cytosol and the sarco-endoplasmic reticulum, which is essential for a variety of physiological events including the muscle contraction-relaxation cycle. In cardiac muscle, SERCA is regulated by transmembrane peptides phospholamban (PLN) and dwarf open reading frame (DWORF). These peptides encode the opposing functions of SERCA inhibition by PLN and SERCA activation by DWORF, though the underlying mechanisms remain unclear. Herein, we investigated structural elements of DWORF expected to play a role in SERCA activation. We first measured SERCA activity in the absence and presence of DWORF variants targeting Leu¹² and Pro¹⁵. These residues were selected based on sequence alignment with PLN. Leu¹² and Pro¹⁵ of DWORF align with the essential residues Leu³¹ and Asn³⁴ of PLN, which are required for SERCA inhibition. We found that both residues are required for SERCA activation by DWORF and that substitution of Pro¹⁵ (to Ala, Asn, or Leu) resulted in potent inhibition of SERCA. We next investigated the roles of Gly²¹, Ile²³, and Gly²⁵ in SERCA activation and DWORF oligomerization. These residues are part of a common helix interaction motif, GxxxG (Gly²¹-Trp-Ile-Val-Gly²⁵) found in DWORF, which is unique among the regulins. The data suggest that the GxxxG motif does not play a role in DWORF oligomerization. Instead, this motif appears to interact with SERCA and provides a smooth interface that promotes activation and avoids inhibitory interactions with SERCA.</p>","PeriodicalId":28,"journal":{"name":"Biochemistry Biochemistry","volume":" ","pages":""},"PeriodicalIF":3.0,"publicationDate":"2025-09-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144999276","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"生物学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Free-Standing Soft Carbon Fibers with High Orientation for Na+ Storage to Achieve High Volumetric Capacity.","authors":"Peipei Ren,Xiaoxu Liu,Tianyi Ji,Tian Wang,Dawei Sheng,Yang Li,Hangtian Yin,Jianxin Ran,Hanmei Zhang,Jie Wang,Yongbin Wang,Ze Xiang Shen","doi":"10.1021/acs.jpclett.5c01423","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c01423","url":null,"abstract":"Noncrystalline carbon materials typically encounter challenges of low volumetric capacity, high discharge plateau, and poor rate capability when utilized as sodium-storage anode materials. The effect of the orientation of carbon layers in noncrystalline carbon materials on sodium storage behavior remains unclear. This study clarifies the sodium storage behavior of high-carbon layer orientation soft carbon fiber materials and reveals the desolvation process of their ordered carbon layer structures as well as pore structure filling and sodium deposition processes, which enhanced the sodium storage capacity. When employed as a sodium-storage anode material, it demonstrates a plateau capacity of 218.9 mAh g-1 and a volumetric capacity of 316.5 mAh cm-3 at 50 mA g-1. Remarkably, the material still exhibits a reversible capacity of 97.9 mAh g-1 at a rate of 2 A g-1. This study demonstrates the impact of carbon layer orientation on sodium storage behavior in carbon-based electrode materials and also provides a new insight for designing high-volumetric-capacity noncrystalline carbon materials.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"30 1","pages":"9590-9598"},"PeriodicalIF":6.475,"publicationDate":"2025-09-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144995992","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"The Liquid Crystal Monomer 3cH2B Affects the Visual System via Neural-Cell-Specific Retinoic Acid Disruption in the Optic Tectum.","authors":"Kai Wang,Lu He,Xiaoyu Liu,Minghui Fu,Mingxiao Li,Yanyang Xu,Jing Qiu,Shunlong Meng,Xiyan Mu","doi":"10.1021/acs.est.5c08283","DOIUrl":"https://doi.org/10.1021/acs.est.5c08283","url":null,"abstract":"As a newly recognized type of emerging contaminant, liquid crystal monomers (LCMs) are widely distributed in the environment and human consumptions and their effects on visual systems and the underlying mechanisms are yet to be elucidated. Therefore, this study investigated the visual-neuro influence of 3cH2B (a frequently detected LCM) under environmentally relevant concentrations in zebrafish. The findings revealed that 40 μg/L 3cH2B induced visual behaviors after 40 days of exposure, which was accompanied by decreased retinoic acid (RA) levels and retinal structural deformation in the eyes. Simultaneously, a decline in the number of synaptic vesicles and loss of neurons were observed in the central nervous system (CNS). In addition, downregulation of RA metabolism pathways was identified in inhibitory neurons of the CNS. Spatial transcriptomic analysis showed that 3cH2B exposure reduced both the proportion of inhibitory neurons and the expression of RA-related genes in the optic tectum of the midbrain. Furthermore, RA supplementation significantly alleviated the behavioral alterations and retinal damage induced by 3cH2B, highlighting the critical role of RA in regulating these effects.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"111 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-09-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145003220","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}