化学•材料最新文献

{"title":"Polystyrene Nanoplastics Regulate Silicon Cycling and Biosilica Deposition in Marine Synechococcus","authors":"Meng-Xin Xu, Mei-Yan Liu, Rong-Xiang Xing, Yue Wang, Xiao-Yu Liu, Jian-Lu Duan, Xiao-Dong Sun, Xiao-Han Zhang, Ming-Gang Zheng, Zi-Shan Diao, Jia-Xin Liu, Guang-Shuo Yao, Xian-Zheng Yuan, Fan-Ping Zhu","doi":"10.1021/acs.est.5c09315","DOIUrl":"https://doi.org/10.1021/acs.est.5c09315","url":null,"abstract":"Nanoplastics are emerging pollutants with the potential to disrupt the microbial physiology and biogeochemical cycles in marine ecosystems. However, their influence on silicon cycling in cyanobacteria remains poorly understood. Here, we investigate how amine-modified polystyrene nanoplastics (PS-NH₂) regulate silicon transport and biosilica deposition in Synechococcus sp. CC9311, a key contributor to oceanic primary production. At an environmentally relevant concentration (0.1 μg/mL), PS-NH₂ primarily modified the cell surface microenvironment, which significantly increased the level of extracellular biosilica deposition. In contrast, higher PS-NH₂ concentrations (0.5–2.0 μg/mL) induced oxidative stress and membrane damage, leading to a shift toward enhanced intracellular silicon accumulation. Notably, at 2.0 μg/mL, the oxidative damage was the most severe, resulting in the most significant intracellular silicon accumulation compared to 0.5 and 1.0 μg/mL. Transcriptomic analysis revealed that PS-NH₂ exposure downregulated genes involved in energy metabolism and photosynthesis while upregulating stress response pathways, suggesting that silicon accumulation may serve as a protective mechanism against PS-NH₂-induced cellular stress. These findings provide novel insights into the interplay between nanoplastics and microbial silicon metabolism, highlighting a previously unknown pathway by which plastic pollution could influence silicon biogeochemistry in marine ecosystems.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"50 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-09-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145009126","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":"The Arch from the Stones: Understanding Protein Folding Energy Landscapes via Bioinspired Collective Variables","authors":"Valerio Rizzi, Margaux Héritier, Nicola Piasentin, Simone Aureli, Francesco Luigi Gervasio","doi":"10.1021/acs.jpclett.5c02079","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c02079","url":null,"abstract":"Protein folding remains a formidable challenge despite significant advances, particularly in sequence-to-structure prediction. Accurately capturing thermodynamics and intermediates via simulations demands overcoming time scale limitations, making effective collective variable (CV) design for enhanced sampling crucial. Here, we introduce a strategy to automatically construct complementary, bioinspired CVs. These uniquely capture local hydrogen bonding─explicitly distinguishing protein–protein from protein–water interactions─and side-chain packing, taking into account both native and non-native contacts to enhance state resolution. Using these CVs in combination with advanced enhanced sampling methods, we simulate the folding of Chignolin and TRP-cage, validating our approach against extensive unbiased simulations. Our results accurately resolve complex free-energy landscapes, reveal critical intermediates such as the dry molten globule, and demonstrate agreement with reference data. This interpretable and portable strategy underscores the critical role of microscopic details in protein folding, opening up a promising avenue for studying larger and more-complex biomolecular systems.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"14 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2025-09-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145009138","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":"Noncompetitive Inhibition of DNA Polymerase β by a Nonnative Nucleotide.","authors":"A Hasan Howlader,Xuanhe Jiang,Zehui Zhou,Marc M Greenberg","doi":"10.1021/acs.joc.5c01529","DOIUrl":"https://doi.org/10.1021/acs.joc.5c01529","url":null,"abstract":"Base excision repair (BER) is a DNA repair pathway responsible for protecting the genome against modified nucleotides. DNA polymerase β (Pol β) participates in this process by removing the remnants of a damaged nucleotide and filling in the resulting gap. Pol β is overexpressed in some cancers and is synthetic lethal in cells deficient in BRCA1/2, providing additional impetus for identifying inhibitors of this enzyme. We report noncovalent Pol β inhibitors that are nonnative nucleotides. The inhibitors were identified via a combination of structural and biochemical analysis, as well as serendipity, from an initial library of covalent inhibitor candidates in which diversity was introduced sequentially at the C3'- and C5-positions of pyrimidine nucleotides. The molecules are among the most potent Pol β inhibitors (Ki ≤ 70 nM) of the enzyme's polymerase and lyase activities. Kinetic analyses reveal that the molecules inhibit Pol β noncompetitively. Fluorescence anisotropy and kinetic experiments reveal that the more potent inhibitor binds in the lyase domain and does not prevent DNA binding. Neither the more potent noncompetitive inhibitor nor a neutral protide exhibits cytotoxic synergism with the DNA damaging agent methyl methanesulfonate in HeLa cells. Cell permeability experiments suggest that micromolar levels of the more potent noncompetitive inhibitor and corresponding protide are taken up by HeLa cells following 24 h incubation (25 μM). However, based upon a comparison with other molecules, it is possible that they are membrane bound. The molecules identified could be useful tools in biochemical studies and provide a starting point for creating new Pol β inhibitors that function in cells.","PeriodicalId":57,"journal":{"name":"Journal of Organic Chemistry","volume":"13 1","pages":""},"PeriodicalIF":4.354,"publicationDate":"2025-09-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145007121","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":"Catalytic C-N Bond-Forming Processes from Inorganic Ammonium Salts.","authors":"Lan Tian,Hao-Ran Zhang,Yu-Long Li,Yu-Feng Ren,Wei Shu","doi":"10.1021/acs.joc.5c01676","DOIUrl":"https://doi.org/10.1021/acs.joc.5c01676","url":null,"abstract":"Catalytic C-N coupling reactions are among the most important bond-forming events in synthetic chemistry. Ammonium salts are economic and easily available inorganic compounds, serving as ideal nitrogen sources for nitrogen-containing organic compounds. The use of ammonium salts highlights the synthesis of N-containing organic compounds from inorganic compounds. Therefore, it is of great significance to develop catalytic methods for the C-N reaction from ammonium salts. This JOCSynopsis focuses on the representative processes of catalytic C-N bond formation from ammonium salts.","PeriodicalId":57,"journal":{"name":"Journal of Organic Chemistry","volume":"31 1","pages":""},"PeriodicalIF":4.354,"publicationDate":"2025-09-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145008843","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":"Review of renewable energy-based products application for battery thermal management","authors":"Farbod Esmaeilion ,&nbsp;Siamak Hoseinzadeh ,&nbsp;Safiye Shafiei ,&nbsp;Ebrahim Pilali ,&nbsp;Alireza Taklifi ,&nbsp;M. Soltani ,&nbsp;Davide Astiaso Garcia","doi":"10.1016/j.rser.2025.116247","DOIUrl":"10.1016/j.rser.2025.116247","url":null,"abstract":"<div><div>Battery overheating can have detrimental effects on battery performance, safety, longevity, and environmental sustainability. Implementing effective thermal management strategies and safety measures to prevent overheating and ensure the safe and reliable operation of batteries in numerous applications is decisive. Reduced battery lifespan, safety hazards, performance degradation, loss of functionality, environmental impacts, and costs of replacement or repair are the detrimental impacts of battery operation in electric cars, renewable energy storage facilities, consumer appliances, and grid-scale energy storage systems. Renewable energy-based products can be effectively utilized for Battery Thermal Management Systems (BTMS) in several ways, confirming the ideal performance, longevity, and protection of batteries. The analysis demonstrates that renewable-integrated BTMS reduced peak battery temperatures by up to 15 °C, significantly lowering the risk of thermal runaway and extending battery lifespan. Solar-powered ventilation systems decreased cooling energy consumption by nearly 70 % compared with conventional methods, while biomass-driven PCMs maintained battery temperatures below 60 °C under high C-rate discharges. By integrating renewable energy-based products for BTMS, such as solar-powered ventilation systems, geothermal cooling technologies, wind-powered ventilation/cooling systems, hydroelectric facilities, and biomass energy-driven systems, the integration of renewable energy-based products enables maintainable and systematic operation of battery systems while dropping dependence on non-renewable energy resources and diminishing environmental influence. Geothermal-PVT hybrid systems improved overall energy efficiency by 53 % and decreased total energy consumption by 25.7 %, whereas hydrogen-based cooling stabilized battery temperatures below 30.5 °C with thermal gradients under 7 °C. Hybrid RES–BTMS configurations reduced the levelized cost of energy to 0.094 USD/kWh and lowered greenhouse gas emissions by up to 3.5 million kg CO₂ annually, indicating substantial environmental and economic benefits. The identified trend provides a practical pathway to attain the required specifications for environmentally benign, economic, and efficient performance. The proposed concept of renewable-energy-based BTMS enables electricity, material, and fuel production as a solution for future operations in the BTMS. A comprehensive examination of the concept has been presented in the review.</div></div>","PeriodicalId":418,"journal":{"name":"Renewable and Sustainable Energy Reviews","volume":"226 ","pages":"Article 116247"},"PeriodicalIF":16.3,"publicationDate":"2025-09-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145007630","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"A CuBi2O4/TiO2 p–n Heterojunction for Enhancing the Barrier Protection of a Nickel-Based Layer on the Magnesium Alloy","authors":"Yu Wen, Yanghua Teng, Yue Liu, Xiaoqiang Fan, Liang Wu, Zhi-Hui Xie","doi":"10.1021/acs.jpclett.5c02258","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c02258","url":null,"abstract":"Herein, CuBi₂O₄ microspheres were first deposited on TiO₂ nanotube arrays to develop a p–n CuBi₂O₄/TiO₂ heterojunction by a facile hydrothermal protocol. The variations in the photoinduced open-circuit potential, photocurrent, and electrochemical parameters of the nickel-plated magnesium alloy (Mg/Ni) demonstrated the remarkably strengthened photoelectrochemical efficiency and photocathodic protection (PCP) capability caused by the CuBi₂O₄ modification. This enhancement is attributed to establishing a built-in electric field and intensified light absorption in a broadened wavelength spectrum, confirmed by the valence band XPS and ultraviolet–visible spectra. The as-prepared photoanode showed an unprecedentedly high photocurrent density compared with that of current heterojunctions based on CuBi₂O₄ and TiO₂ semiconductors. The heterojunction continuously provided PCP to the Mg/Ni couple and suppressed the galvanic corrosion between the Mg and nickel–phosphorus alloy. This study proposed a new strategy for constructing a heterojunction with a novel morphology and considerably enhanced photoelectrochemical performance.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"40 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2025-09-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145007157","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":"ssDNA and ssRNA Promote Phase Condensation of SAMHD1.","authors":"Brandon E Smith, Ankita Pohnerkar, Benjamin Orris, Shridhar Bhat, Matthew Egleston, James T Stivers","doi":"10.1021/acs.biochem.5c00422","DOIUrl":"https://doi.org/10.1021/acs.biochem.5c00422","url":null,"abstract":"<p><p>SAMHD1 (SAM domain and HD domain-containing protein 1) is a deoxynucleoside triphosphate triphosphohydrolase (dNTPase) with functions in viral restriction, R-loop resolution, DNA repair, telomere maintenance, ssRNA homeostasis, and regulation of self-nucleic acids. As a dNTPase, SAMHD1 functions as an allosterically activated tetramer, where binding of GTP to the A1 activator site of each monomer initiates dNTP-dependent tetramerization. cEM structures reveal that the nucleic-acid-related functions of SAMHD1 involve binding of guanine residues to the A1 site, leading to oligomeric forms that appear as beads-on-a-string on single-stranded RNA and DNA. SAMHD1's cellular activities and known protein interactions involve liquid-liquid phase separation (LLPS), although there are no reports that SAMHD1 itself exhibits phase separation properties. The protein phase separation prediction algorithm MolPhase indicated an overall phase separation probability score of 0.65 and suggested that the amino terminal SAM domain and the disordered carboxyl terminus (CT) may promote phase separation. Although no phase separation behavior was observed in physiological buffer, in the presence of 9% PEG 2000 and ssDNA or ssRNA, SAMHD1 condensed into liquid-like droplets. These droplets were disrupted by deletion of the SAM or CT domains, showed fusion behavior, and were rapidly disrupted by the addition of A1 site ligands GTP, dGTP, and small-molecule inhibitors. We also observed that SAMHD1-ssDNA condensates within the nuclei of human cells in microinjection experiments, supporting a biological relevance for such complexes. LLPS by SAMHD1 could serve a regulatory role in cells and provide a new therapeutic target for the treatment of cancer and viral infections.</p>","PeriodicalId":28,"journal":{"name":"Biochemistry Biochemistry","volume":" ","pages":""},"PeriodicalIF":3.0,"publicationDate":"2025-09-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145005676","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":"Microplastic Diversity as a Potential Driver of Soil Denitrification Shifts.","authors":"Tian-Gui Cai,Da Lin,Bang Ni,Tian-Lun Zhang,Yi-Fei Wang,Dong Zhu","doi":"10.1021/acs.est.5c04981","DOIUrl":"https://doi.org/10.1021/acs.est.5c04981","url":null,"abstract":"Microplastics (MPs) are raising significant global concerns due to their environmental impacts. While most studies have focused on the effects of individual MP types, MPs in natural environments typically coexist as multiple types, and their combined effects remain poorly understood. In this study, we conducted a microcosm experiment with four levels of MP diversity (0, 1, 3, and 5 types) to investigate the effects of MP diversity on soil ecosystem functions using metagenomic sequencing. Our results revealed that increasing MP diversity significantly raised soil pH and organic carbon content while reducing available nitrogen. Notably, bacterial alpha diversity (Shannon and Invsimpson indices) increased significantly with higher MP diversity. Moreover, increasing MP diversity markedly shifted bacterial life-history strategies to adapt to the altered environment. Importantly, the abundance of nitrogen-related functional genes also increased with MP diversity. In particular, the abundance of denitrifying genes, predominantly driven by Rhodocyclaceae, was notably enhanced, resulting in a reduction of soil available nitrogen. Collectively, these findings offer valuable insights into the impact of MP diversity on soil function─especially within the nitrogen cycle─and have important implications for soil management strategies under MP stress.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"25 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-09-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145003218","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":"Strong Metal-Support Interactions in Catalytic Oxidation of VOCs: Mechanistic Insights, Support Engineering Strategies, and Emerging Catalyst Design Paradigms.","authors":"Ziyue Jiang,Yongtao Li,Ziyu Tang,Dingkun Yuan,Fawei Lin","doi":"10.1021/acs.est.5c09511","DOIUrl":"https://doi.org/10.1021/acs.est.5c09511","url":null,"abstract":"Volatile organic compounds (VOCs) significantly impact air quality as photochemical smog precursors and health hazards. Catalytic oxidation is a leading VOC abatement method but suffers from catalyst deactivation due to metal sintering and competitive adsorption in complex mixtures. Strong metal-support interactions (SMSIs) provide atomic level control of interfacial electronic and geometric structures. SMSI enables bidirectional charge transfer, d band center modulation, oxygen vacancy generation, and tunable encapsulation that together promote O2 activation, lower barriers, and impart thermal and chemical robustness. This review synthesizes mechanistic insights and recent progress in SMSI-enabled VOC oxidation, integrating in situ and operando probes with kinetics. Reactivity and selectivity across aromatics, alkanes, oxygenates, and chlorinated species are rationalized by SMSI-mediated tuning of adsorption and intermediate evolution. Practical levers include control of particle size and dispersion, core-shell architectures, metal loading, and support acidity or basicity. Emerging directions include single atom catalysts, high entropy alloys, and nonmetal supports. Key challenges concern the dynamic evolution of SMSI under realistic feeds and the scalable, reproducible synthesis of interfaces. Future developments combining in situ characterization with data-driven catalyst design hold promise for achieving durable, high-performance VOC abatement with reduced precious metal usage.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"16 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-09-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145003217","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":"Mechanistic and Kinetic Insights into Nitrogen Chemistry: NH₂-Mediated H-Abstraction and HCN Addition Pathways in NH₃/Ethanol Combustion.","authors":"Tong Yan, Pan Wang, Jianmin Liu, Jinsheng Zhang, Lidong Zhang","doi":"10.1021/acs.jpca.5c03451","DOIUrl":"https://doi.org/10.1021/acs.jpca.5c03451","url":null,"abstract":"<p><p>To elucidate possible mechanisms of nitrogen chemistry between ammonia (NH₃) and ethanol, the potential pathways of ethanol radicals (Wa, Wb, and Wc) following H-abstraction by NH₂ radicals were primarily investigated including HCN addition, H-transfer, and dissociation reactions by quantum chemical calculations. The rate constants were solved in the master equation based on RRKM and TST theory and fitted to the Arrhenius equation. The results demonstrate that H-abstraction from C₂H₅OH by NH₂ at the b-site is the most competitive, facilitating subsequent HCN addition. The HCN addition-entranced channel exhibits a negative temperature coefficient (NTC) behavior at 0.01 atm, and the onset of this effect is progressively delayed with pressure. The low-temperature reaction path of ethanol radicals with HCN is dominated by the initial adduct (WaHCN, WbHCN, and WcHCN) formation and subsequent isomerization. The multiple dissociation product channels become more competitive with temperature, especially the HCNH elimination. Findings from this study identify new growth pathways for NPAHs and OPAHs in the reaction of straight-chain molecules with HCN and provide comprehensive kinetic insights.</p>","PeriodicalId":59,"journal":{"name":"The Journal of Physical Chemistry A","volume":" ","pages":""},"PeriodicalIF":2.8,"publicationDate":"2025-09-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145008039","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}