化学•材料最新文献

{"title":"Chemist: A Domain-Specific Language by Chemists for Chemists.","authors":"Jonathan M Waldrop, Wibe de Jong, Edward F Valeev, Theresa L Windus, Ryan M Richard","doi":"10.1021/acs.jpca.5c02993","DOIUrl":"https://doi.org/10.1021/acs.jpca.5c02993","url":null,"abstract":"<p><p>Managing the complexity of quantum chemistry (QC) software is key to ensuring it remains accessible, maintainable, and reusable. Noticeably missing from the QC ecosystem are modules targeting bottleneck routines. Here we argue that this is likely due to the difficulty in defining interfaces for such modules. To that end, we introduce the open-source, publicly available Chemist library https://github.com/NWChemEx/Chemist. Chemist is a domain-specific language targeting the QC domain. Chemist has been developed focusing on performance and user-friendliness. Using Chemist, QC tasks are defined using familiar domain concepts such as molecules, wave functions, and operators. The domain objects are hierarchical to ensure a systematic encapsulation of information. Key features of Chemist include: extensibility, the ability to alias existing data, and the ability to succinctly define many common QC tasks. The usefulness of Chemist is demonstrated by discussing the interface of NWChemEx's Fock build module and by showcasing a proof-of-concept self-consistent field algorithm containing uncertainty propagation.</p>","PeriodicalId":59,"journal":{"name":"The Journal of Physical Chemistry A","volume":" ","pages":""},"PeriodicalIF":2.8,"publicationDate":"2025-08-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144858701","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":"Structural Impacts of the Addition of Succinic Acid to Cationic Ammonium Bisulfate Clusters.","authors":"Annapoorani Hariharan, Nanna Myllys, Christopher J Johnson","doi":"10.1021/acs.jpca.5c04153","DOIUrl":"https://doi.org/10.1021/acs.jpca.5c04153","url":null,"abstract":"<p><p>The process by which atmospheric trace vapors cluster and grow into climatically relevant sizes is called new particle formation (NPF). While sulfuric acid and ammonia are the most abundant acid and base in the atmosphere, these two vapors alone cannot adequately explain observed NPF rates, and organic acids have been studied as a third vapor that could stabilize new particles or drive NPF on their own. We used infrared spectroscopy and mass spectrometry to characterize the structure of clusters composed of succinic acid (SuA), ammonia and sulfuric acid. We show that the structures of ammonium-bisulfate clusters are largely retained upon binding of up to two SuA molecules. Computed structures show significant COOH-COOH hydrogen bonding. These observations suggest that, even at these small sizes, these clusters feature incipient inorganic-organic phase separation. We also find that, despite the fact that the inorganic portion of these clusters feature more hydrogen bond donors than acceptors, there are few free carboxylic acid OH groups, suggesting that the cluster surface is relatively nonpolar and depleted in binding sites for further vapors. Increasing SuA content is correlated to spectral broadening, suggesting that organic-enriched new particles are likely to be more fluxional than inorganic ones.</p>","PeriodicalId":59,"journal":{"name":"The Journal of Physical Chemistry A","volume":" ","pages":""},"PeriodicalIF":2.8,"publicationDate":"2025-08-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144858702","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":"Cooperative Ice Binding of Engineered Antifreeze Protein Produces Superior Activity.","authors":"Yitzhar Shalom, Fredy Zypman, Ran Drori","doi":"10.1021/acs.jpcb.5c03982","DOIUrl":"https://doi.org/10.1021/acs.jpcb.5c03982","url":null,"abstract":"<p><p>Antifreeze proteins (AFPs) bind irreversibly to ice surfaces and prevent ice crystal growth at temperatures of up to 10 °C below the melting point. The remarkable ability of AFPs to adsorb onto the ice surface and stop further growth is not fully understood, and their structural diversity hinders efforts to find a universal ice-binding motif. Multivalent AFP assemblies have achieved better ice growth inhibition compared to the corresponding monomers, yet the mechanism of these improved inhibitors is poorly understood. The innovative approach of this study is to test the effect of multivalency on the AFP's adsorption rates to ice in addition to testing AFP activity. A monomer, dimer, and multimer (12-subunits) of type III AFP were tested for thermal hysteresis (TH) activity, and their adsorption rates were measured using fluorescence microscopy. To fit the experimental data, we developed a revised Langmuir adsorption model. As expected, the monomer achieved the lowest TH activity, and its adsorption rate was slowest, followed by the dimer, which achieved slightly higher TH activity. The multimer was the most active, and its adsorption rate was found to be 11-fold higher than that of the monomer. The newly developed model identifies cooperativity effects in the multimer but not in the monomer and dimer. The rate at which the ice surface is covered by multimeric AFPs increases with continuous binding, suggesting cooperative ice binding. These results suggest a mechanism for the AFP multimer binding. After the binding of its first subunit to ice, subsequent binding of a second subunit becomes faster, which in turn facilitates the binding of a third subunit. Thus, cooperative ice binding is key to the superior inhibition of ice growth.</p>","PeriodicalId":60,"journal":{"name":"The Journal of Physical Chemistry B","volume":" ","pages":""},"PeriodicalIF":2.9,"publicationDate":"2025-08-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144858704","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":"Photochemical Chain Scissions Enhance Polyethylene Glycol Biodegradability: from Probabilistic Modeling to Experimental Demonstration.","authors":"Kevin Kleemann, Madalina Jaggi, Stefano M Bernasconi, Robert Alexander Schmitz, Andreas Künkel, Carsten Simon, Kristopher McNeill, Glauco Battagliarin, Michael Sander","doi":"10.1021/acs.est.5c03567","DOIUrl":"https://doi.org/10.1021/acs.est.5c03567","url":null,"abstract":"<p><p>Polyethylene glycols (PEGs), a major class of water-soluble polymers (WSPs), are widely used in diverse applications, from which PEGs may be released into the environment. This work investigates the effect of PEG reaction with photochemically produced hydroxyl radicals (^•OH), an important environmental oxidant, on the molecular weight (MW) distribution of PEGs and their subsequent biodegradation in soil and sediment. Monte Carlo simulations demonstrated a pronounced decrease in the PEG MW after only a few ^•OH-reaction-induced chain scissions on initial PEG molecules. The simulation results were validated by experimentally reacting ¹³C-labeled PEGs (<math><msub><mover><mi>M</mi><mo>¯</mo></mover><mi>n</mi></msub></math> = 6380 ± 400 Da) with photochemically produced ^•OH to three extents and by analyzing the formed low MW PEG reaction products. Incubation of unreacted and ^•OH-reacted PEGs in both a sediment and a soil over 150 days demonstrated increasing rates and extents of PEG biodegradation into ¹³CO₂ with increasing ^•OH-reaction extent and thus increasing amounts of low MW PEG products. This work underscores the importance of considering WSP MW distributions and dynamics caused by biotic or abiotic chain scission reactions when advancing a detailed understanding of WSP fate and biodegradability in natural and engineered receiving environments.</p>","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":" ","pages":""},"PeriodicalIF":11.3,"publicationDate":"2025-08-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144853982","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":"tert-BuONO-Promoted Nitrosation of 4-Nitroisoxazole-Based Enamines: Synthesis of 5-Cyanoisoxazoles and Their Application","authors":"Nadezhda E. Astakhova, Dmitry A. Vasilenko, Maria S. Kuzmina, Aleksandr K. Pupeza, Yuri K. Grishin, Victor A. Tafeenko, Elena B. Averina","doi":"10.1021/acs.joc.5c01207","DOIUrl":"https://doi.org/10.1021/acs.joc.5c01207","url":null,"abstract":"An efficient approach to previously unknown 5-cyano-4-nitroisoxazoles has been developed using nitrosation of 4-nitroisoxazole-based enamines with tert-butyl nitrite (TBN) followed by a BF₃- or TFAA-mediated unusual C═C bond cleavage reaction. This two-step one-pot process is applicable to a broad range of substrates and provides the desired products in mild reaction conditions in moderate to high yields. The dichotomy of reactivity in the S_<i>N</i>Ar reaction of the resulting 5-cyano-4-nitroisoxazoles has been demonstrated by the cyano-group substitution with N-nucleophiles and the nitro-group substitution with thiophenols and rationalized with DFT-calculations.","PeriodicalId":57,"journal":{"name":"Journal of Organic Chemistry","volume":"52 1","pages":""},"PeriodicalIF":4.354,"publicationDate":"2025-08-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144840271","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 on the development and challenges of clean energy sources for ships","authors":"Longxiang Feng ,&nbsp;Yuwei Sun ,&nbsp;Xujing Tang ,&nbsp;Chengqing Yuan ,&nbsp;Huabing Yin ,&nbsp;Wenjun Luo","doi":"10.1016/j.rser.2025.116181","DOIUrl":"10.1016/j.rser.2025.116181","url":null,"abstract":"<div><div>The incorporation of clean energy sources into ship power systems has accelerated rapidly in recent years, primarily due to environmental concerns and stringent emission regulations. This paper first examines the following aspects of alternative marine fuels: their properties, emission reduction potential, risk assessments, implementation challenges with corresponding solutions, future prospects, and applications. Subsequently, current technical solutions and applications are analyzed for integrating batteries, supercapacitors, photovoltaic (PV) systems, and wind power into ship power systems. Next, the fundamental operational principles of shipboard DC microgrids—including technical configurations, structural topologies, and system characteristics—are reviewed, along with core technologies for new energy vessels, such as design selection, energy management, operational control, and multi-objective optimization with integrated algorithms. Finally, the future development trajectory of shipboard DC microgrids is assessed through analysis of their historical evolution, technical features, and practical applications in hybrid vessels. Collectively, these findings provide critical insights for ship operators and policymakers seeking to balance eco-friendliness with cost-effectiveness regarding alternative marine fuels. Furthermore, multi-energy integrated power systems are identified as pivotal technologies for achieving sustainable maritime operations that harmonize environmental protection and economic viability.</div></div>","PeriodicalId":418,"journal":{"name":"Renewable and Sustainable Energy Reviews","volume":"225 ","pages":"Article 116181"},"PeriodicalIF":16.3,"publicationDate":"2025-08-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144828950","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":"Anti-PD-L1 immobilization on Fe₃O₄ nanocluster-coated AuNR through terpyridine–gadolinium coordination for multimodal imaging and synergistic tumor therapy","authors":"Yue Chen,&nbsp;Yufei Xu,&nbsp;Sihan A,&nbsp;Binbin Shen,&nbsp;Shengwang Zhou","doi":"10.1016/j.colsurfb.2025.115047","DOIUrl":"10.1016/j.colsurfb.2025.115047","url":null,"abstract":"<div><div>Functionalized nanoparticles offer a versatile nanomedicine platform for engineering stimulus-responsive, theranostic drug delivery systems to enhance tumor diagnosis and treatment. Herein, we present the development of a stimulus-responsive Fe₃O₄@AuNR nanotherapeutic platform functionalized with anti-PD-L1, which enables antibody and dual drug loading, tumor-specific controlled release, image-guided combination therapy, and synergistic enhancement of antitumor efficacy. As a biomarker of senescence and tumor progression, β-galactosidase enables 5-FUR-β-Gal prodrug activation, contributing to targeted therapeutic strategies for ovarian cancer. The anti-PD-L1-functionalized Fe₃O₄@AuNR drug delivery system combines chemotherapy, targeted therapy, and photothermal therapy, while simultaneously enabling fluorescence imaging and MRI of tumor tissues, thus providing a synergistic theranostic platform with promising clinical applicability.</div></div>","PeriodicalId":279,"journal":{"name":"Colloids and Surfaces B: Biointerfaces","volume":"256 ","pages":"Article 115047"},"PeriodicalIF":5.6,"publicationDate":"2025-08-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144852445","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"医学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Triple-Enhanced Absorption Anisotropy in Arrayed Core-Shell Nanowire Design.","authors":"Zimin Liu,Huayi Tang,Weili Liu,Shuai Yang,Han Bao,Jiayi Li,Jing Li,Jijun Qiu,Jiao Xu,Yiming Yang","doi":"10.1021/acs.jpclett.5c01926","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c01926","url":null,"abstract":"One-dimensional semiconductor nanowires (NWs) are natural polarization photodetectors, thanks to their optical absorption anisotropy and efficient electrical transport channels. However, ultrathin NWs beyond practical fabrication capabilities are often required to achieve the desired polarization sensitivity. Here, we demonstrate a configuration of planar arrayed core-shell NW architectures with substantially enhanced absorption dichroism for linearly polarized light. The high polarization ratio originates from synergistic effect of three rational designs: a NW core consisting of indirect-bandgap semiconductor as light-trapping cavity, a thin shell of photosensitive material as light absorber, and arrayed photonic structure for optical interference. By employing all-inorganic halide perovskites, these NW arrays exhibit a dichroic ratio up to 110.5 without the need for ultrathin NWs. The core-shell NW architecture is experimentally feasible and offers insights into design of high-sensitivity polarization photodetectors using optical resonance.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"183 1","pages":"8642-8648"},"PeriodicalIF":6.475,"publicationDate":"2025-08-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144851030","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":"Global Land Use Change Impacts on Soil Nitrogen Availability and Environmental Losses.","authors":"Jing Wang,Yves Uwiragiye,Miaomiao Cao,Meiqi Chen,Nyumah Fallah,Yuanyuan Huang,Yuanyuan Huang,Yi Cheng,Zucong Cai,Minggang Xu,Scott X Chang,Christoph Müller","doi":"10.1021/acs.est.5c03285","DOIUrl":"https://doi.org/10.1021/acs.est.5c03285","url":null,"abstract":"Anthropogenic activities, particularly land use change and management practices, alter the global nitrogen (N) cycle. As a central part of the global N cycle, soil N supply from net N mineralization (NNM) and net nitrification (NN) contributes to over 50% of crop N uptake. However, how global land use changes impact soil N supply and potential N loss remains elusive. By compiling a global data set of 1,782 paired observations from 185 publications, we show that land use conversion from natural to managed ecosystems significantly reduced NNM by 7.5% (-11.5, -2.8%) and increased NN by 150% (86, 194%), indicating decreasing N availability while increasing potential N loss through denitrification and nitrate leaching. In contrast, reversing managed to natural ecosystems significantly increased NNM by 20% (9.7, 25.4%) and decreased NN by 89% (-125, -46%), indicating increasing N availability while decreasing potential N loss. Structural equation modeling revealed that land use change induced changes in soil properties, including organic matter content, bulk density, microbial biomass and pH, and anthropogenic activities, including application of ammonium-based fertilizers and manure, were the most important factors regulating NNM and NN. The land use change effect was the strongest in tropical and subtropical regions, where NNM was negatively affected and NN positively affected by land use change. Our findings indicate that increasing soil organic matter content and enhancing soil structural development post land use change can boost soil N supply and reduce the risk for N loss.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"24 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-08-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144851055","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":"Global Decarbonization Enabled by a Novel Strategy of Biomineralization for Concrete Corrosion Inhibition.","authors":"Xiaohao Sun,Yong Wang,Jiadong Ren,Onyx W H Wai,Xiangdong Li","doi":"10.1021/acs.est.5c00261","DOIUrl":"https://doi.org/10.1021/acs.est.5c00261","url":null,"abstract":"With rapid urban population growth, predominantly in coastal regions, decarbonizing concrete structures in coastal cities is crucial. Extending the lifespan of concrete is highly efficient in achieving net-zero greenhouse gas (GHG) emissions by 2050. Biomineralization for concrete corrosion inhibition (BCCI) was previously proposed and demonstrated to effectively protect marine concrete in laboratory experiments, showing promise for decarbonization due to potentially increased lifespans. The potential of BCCI for decarbonization and sustainability warrants further investigation. Therefore, this study evaluated its impact on GHG emissions for insights into global decarbonization. Field corrosion experiments were conducted to ascertain its effectiveness as a valuable GHG calculation input, including biofilm community analysis and microstructure and macroscopic measurements of concrete. Results show that BCCI decreased the total/relative abundances of corrosive bacteria, inhibited sulfate and chloride diffusion, and enhanced carbon functions, irrespective of concrete type. Moreover, BCCI significantly reduced GHG emissions, particularly in 20 MPa concrete. BCCI demonstrated substantial GHG mitigation potential in China, Indonesia, and the USA, which enabled a competitive 37-65% reduction in global GHG from producing underwater concrete. In the long term, this strategy would yield more sustainable development benefits. Findings contribute to achieving global decarbonization and multiple sustainable development goals for concrete sectors and coastal infrastructures.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"79 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-08-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144851119","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}