化学•材料最新文献

{"title":"A Tribute to Alec M. Wodtke","authors":"Hua Guo, Gerard Meijer, Xueming Yang","doi":"10.1021/acs.jpcc.5c01321","DOIUrl":"https://doi.org/10.1021/acs.jpcc.5c01321","url":null,"abstract":"Published as part of <i>The Journal of Physical Chemistry C</i> special issue “Alec Wodtke Festschrift”. <named-content content-type=\"bio-pic\" type=\"simple\"><img alt=\"\" src=\"/cms/10.1021/acs.jpcc.5c01321/asset/images/medium/jp5c01321_0001.gif\"/></named-content> It is our great pleasure to present this Festschrift of the <i>Journal of Physical Chemistry</i> to Alec Wodtke - and our community - on the occasion of Alec’s 65th birthday. In his inspiring autobiography penned for this Festschrift, he notes that “Science - like creative art - can be part of a life worth living” - a message to entice the young generation to choose a life in science. In writing his autobiography, Alec did not abide by the rules that this journal has set for this, but he held on to his original version without changing a single word. This is characteristic of Alec and consistent with how we know and appreciate him. In a presentation that Alec gave just over ten years ago in Berlin as part of a ceremony in which he was anointed as Alexander von Humboldt Professor, he touched upon questions of curiosity and the joy of learning, of scientific originality and intellectual leadership. He explained that he saw his views on these matters aptly expressed in the poem by Robert Frost, entitled “The Road Not Taken”, which he then recited in full. The poem’s last three lines read: <i>Two roads diverged in a wood, and I - I took the one less traveled by, And that has made all the difference.</i> Throughout his career, Alec has made a difference by tackling a variety of important scientific problems in physical chemistry and chemical physics, for which he often specifically designed new instrumentation as well as exploited novel detection and analysis schemes, i.e., by taking roads less traveled or not traveled at all. Alec has always stressed, and demonstrated by example, the importance of doing science that takes us in new directions, and he recognized early on and demonstrated repeatedly the enormous value of experiment and theory working together. He has been critical - and rightfully so - about the trend of “chasing the numbers”, as this encourages scientists to mainly work in popular fields, where many others are active already, and he has mused about the citation impact of a scientist who is swimming against the stream. Nevertheless, let us mention one number: Alec has coauthored about 300 scientific papers that have appeared in the most respected journals in our field as well as in the highest-profile interdisciplinary journals. Apart from his papers, he is well-known for his lucid scientific lectures, typically showing novel, high-quality experimental results that define the state-of-the-art in the field and that challenge the current theory. What sets him apart from many other experimentalists is the impressive set of diverse topics that he has covered over the years, some of which we will mention below. As a PhD student of Yuan T. Lee at UC Berkeley, working alongside Dan Neu","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"47 18 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2025-04-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143766980","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":"Excitation Induced Mechanical Softening and Plastic Deformation in SiO2 and Al2O3","authors":"T. Thuy Hoang, Junhyeok Bang","doi":"10.1021/acs.jpcc.5c00352","DOIUrl":"https://doi.org/10.1021/acs.jpcc.5c00352","url":null,"abstract":"Precise shaping of glass oxides is vital for microelectronics, but it traditionally requires high-temperature processes that can damage components. Recent experiments revealed low-temperature but electron-beam-induced superplastic deformation in amorphous silica, hinting at a nonthermal mechanism, though the role of electronic excitation remains unclear. In this work, we investigated the nonthermal effects of electronic excitation on the mechanical and electronic properties of α-SiO₂, α-Al₂O₃, κ-Al₂O₃, and amorphous SiO₂. While the glass oxides exhibit strong covalent or ionic bonding in the electronic ground state, characterized by high elastic constants and phonon frequencies, both properties significantly decrease under electronic excitation. Based on the results, we found that the superplastic deformation under electron beam irradiation is primarily driven by a bond-switching mechanism. This study provides theoretical insights into the mechanisms underlying superplastic deformation and offers a foundation for developing precise nanoscale shaping techniques for oxide materials.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"58 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758339","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":"Active Learning for the Discovery of Binary Intermetallic Compounds as Advanced Interconnects","authors":"Guoxiang Cui, Zikang Guo, Xiangyu Ren, Yuhang Jiang, Xinyu Jin, Yunwen Wu, Shenghong Ju","doi":"10.1021/acs.jpclett.5c00386","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00386","url":null,"abstract":"The scaling of advanced integrated circuits has posed significant challenges for traditional Cu interconnects, including increased resistivity and reduced electromigration lifetime. Materials with high cohesive energy and low ρ₀ × λ values are emerging as promising alternatives. In this work, active learning coupling density functional theory (DFT) computation is employed to accelerate the discovery of binary intermetallic compounds for interconnect materials. Following five active learning iterations, 100 compounds are screened out. Among them, the proportion of promising materials reaches an impressive 76%, in sharp contrast to a paltry 4.9% under traditional random screening. Moreover, this research adopts an interpretable machine learning method to provide further physical insights. The Shapley additive explanations (SHAP) analysis revealed that binary intermetallic compounds featuring small cell volumes and similar Mendeleev numbers tend to possess low ρ₀ × λ values. Several promising intermetallic candidates were also identified, including VMo, IrRh₃, PtRh₃, NbRu, and CrIr₃, as potential alternatives to traditional Cu interconnects in future technology nodes. The findings in the study highlight the immense potential of machine learning techniques to accelerate the discovery of novel high-performance interconnect materials.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"22 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758340","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":"Three-Component Synthesis of Oxazolidinones via Phosphine-Catalyzed Fixation of Carbon Dioxide and Mechanistic Investigation in Mass Spectrometry","authors":"Wangyu Li, Shiwen Zhou, He Tang, Fengjian Chu, Hongru Feng, Yuanjiang Pan","doi":"10.1021/acs.joc.4c03034","DOIUrl":"https://doi.org/10.1021/acs.joc.4c03034","url":null,"abstract":"A phosphine-catalyzed three-component cyclization reaction between anilines, carbon dioxide, and chloroalkanes was developed for the synthesis of oxazolidinones. This strategy not only proceeds under ambient CO₂ pressure and metal-free condition but also shows a broad substrate scope, including aromatic amines, aliphatic amines, chiral amino acid esters, and bioactive molecules, providing an efficient and environmentally benign route to synthesize pharmaceutically relevant <i>N</i>-aryl-oxazolidinones. Mechanistic investigations utilizing mass spectrometry (MS) indicate the involvement of multiple phosphine intermediates in this process, thereby elucidating the underlying mechanism. Moreover, the relationships between these phosphine intermediates and Tolman cone angles or the solvent effect of phosphines were examined through mass spectrometry.","PeriodicalId":57,"journal":{"name":"Journal of Organic Chemistry","volume":"25 1","pages":""},"PeriodicalIF":4.354,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758474","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":"Numerical Calculations of Electric Response Properties Using the Bubbles and Cube Framework.","authors":"Eelis Solala, Wen-Hua Xu, Pauli Parkkinen, Dage Sundholm","doi":"10.1021/acs.jpca.5c00849","DOIUrl":"https://doi.org/10.1021/acs.jpca.5c00849","url":null,"abstract":"<p><p>We have developed a fully numerical method for calculating the response of the Hartree-Fock orbitals to an external electric field. The Hartree-Fock orbitals are optimized using Green's function methods by iterative numerical integration of the convolution with the Helmholtz kernel. The orbital response is obtained analogously by iterative numerical integration of the convolution with the Helmholtz kernel of the Sternheimer equation. The orbitals are expanded in atom-centered functions (bubbles), consisting of numerical radial functions multiplied by spherical harmonics. The remainder, i.e., the difference between the bubble expansion and the exact orbitals, is expanded in numerical tensorial local basis functions on a three-dimensional grid (cube). The methods have been tested by calculating polarizabilities for He, H₂, and NH₃, which are compared to the literature values.</p>","PeriodicalId":59,"journal":{"name":"The Journal of Physical Chemistry A","volume":" ","pages":""},"PeriodicalIF":2.7,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143762601","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":"Hydrogen technology for maritime applications: A review of challenges, opportunities, and lessons from the port authority of New York and New Jersey","authors":"Veronika Semchukova,&nbsp;Kevin Topolski,&nbsp;Zainul Abdin","doi":"10.1016/j.rser.2025.115641","DOIUrl":"10.1016/j.rser.2025.115641","url":null,"abstract":"<div><div>The maritime industry faces increasing demand for energy security, operational efficiency, and environmental performance improvements. Hydrogen technology, considered a potential energy carrier, is being explored for port operations, including cargo-handling equipment, heavy-duty vehicles, and stationary power systems. This review evaluates the feasibility, challenges, and potential benefits of hydrogen integration within port infrastructure, using the Port Authority of New York and New Jersey as a representative case study. Drawing on case studies, technical reports, and policy analyses, this study examines the infrastructural, regulatory, and operational factors influencing large-scale deployment, emphasizing supply chain development, storage requirements, and refueling infrastructure. By situating hydrogen within broader maritime energy transition efforts, this review provides an evidence-based assessment of its role in port operations and energy diversification strategies. The findings outline key barriers to adoption and emphasize the need for coordinated efforts among stakeholders to determine hydrogen's role alongside other emerging energy technologies.</div></div>","PeriodicalId":418,"journal":{"name":"Renewable and Sustainable Energy Reviews","volume":"216 ","pages":"Article 115641"},"PeriodicalIF":16.3,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143759700","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":"Incorporation and Distribution of Polycyclic Aromatic Hydrocarbons in Experimental Sea-Ice","authors":"Katarzyna Polcwiartek, Gary A. Stern, Feiyue Wang","doi":"10.1021/acs.est.4c13839","DOIUrl":"https://doi.org/10.1021/acs.est.4c13839","url":null,"abstract":"Rapid melting of sea-ice makes the Arctic more accessible for marine shipping and other industrial activities, increasing the risk of oil spills in the Arctic Ocean. Polycyclic aromatic hydrocarbons (PAHs) are among the most toxic substances in petroleum oil, yet their behavior in sea-ice-covered waters remains poorly studied. Here, we report an outdoor microcosm study to examine the partitioning behavior of four PAHs (naphthalene, phenanthrene, pyrene, and benzo(a)pyrene) across the seawater-sea-ice-atmosphere interface in the presence of particulate humic acid as a surrogate for particulate organic carbon (POC). We show that the higher the molecular weight of the PAH, the higher its concentration in sea-ice and the POC fraction. The POC-aqueous phase (seawater or bulk sea-ice) partition coefficients, <i>K</i>_d, are reasonably well explained by temperature and salinity for all four PAHs in seawater and for phenanthrene and pyrene in sea-ice. Relationships of <i>K</i>_d with temperature and salinity in sea-ice and freezing seawater are complex and nonunidirectional, most likely due to the dynamic nature of sea-ice and seawater under such temperatures. This suggests that conventional equilibrium-based approaches developed for open-water conditions need to be revisited when describing the behavior of PAHs in ice-covered waters.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"37 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143766855","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":"Direct Photoactivation of Sulfinic Acids to Access Hydrosulfonylation and Arylsulfonylation of Alkenes","authors":"Yu-Xing Zhang, Xi-Rui Xia, Si-Yu Guo, Zhen-Xiao Lei, Hong Jiang, Wan-Min Cheng","doi":"10.1021/acs.joc.5c00399","DOIUrl":"https://doi.org/10.1021/acs.joc.5c00399","url":null,"abstract":"Simple and atom-economical hydrosulfonylation and arylsulfonylation of alkenes have been developed using sulfinic acid as both the sulfonyl group source and the hydrogen atom donor under light irradiation. These reactions feature catalyst-, oxidant-, and additive-free conditions, offering a highly practical approach for the synthesis of diversely functionalized sulfones. Preliminary mechanistic studies indicate that these reactions proceed via the photoactivation of sulfinic acid to generate a sulfonyl radical, followed by a radical chain process.","PeriodicalId":57,"journal":{"name":"Journal of Organic Chemistry","volume":"23 1","pages":""},"PeriodicalIF":4.354,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143766879","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":"TCF7l2 Regulates Fatty Acid Chain Elongase HACD3 during Lipid-Induced Stress.","authors":"Atanu Mondal, Sandhik Nandi, Vipin Singh, Arnab Chakraborty, Indrakshi Banerjee, Sabyasachi Sen, Shrikanth S Gadad, Siddhartha Roy, Siddhesh S Kamat, Chandrima Das","doi":"10.1021/acs.biochem.4c00491","DOIUrl":"https://doi.org/10.1021/acs.biochem.4c00491","url":null,"abstract":"<p><p>The transcriptional regulation of metabolic genes is crucial for maintaining metabolic homeostasis under cellular stress conditions. Transcription factor 7-like 2 (TCF7l2 or TCF4) is associated with type 2 diabetes (T2D) and functions as a transcription factor for various gluconeogenic genes. T2D often coexists with metabolic dysfunction-associated steatotic liver disease (MASLD) due to common underlying mechanisms and shared risk factors such as insulin resistance and obesity. This study demonstrates the transcriptional regulation of one of the important fatty acid chain elongases implicated in T2D, HACD3 (encoded by <i>PTPLAD1</i> gene), under palmitic acid (PA)-induced stress conditions. We observed that TCF7l2 is associated with histone H3K4me3-binder protein TCF19 and is corecruited to the promoter of <i>PTPLAD1</i>. Upon PA treatment, the TCF19-TCF7l2 complex dissociates from the lipid chain elongase gene due to the reduced level of H3K4me3 enrichment, leading to <i>PTPLAD1</i> activation. Remarkably, gene expression analysis from the PA-injected mice and NAFLD patients indicates an anticorrelation whereby reduced TCF7l2 expression enhances HACD3-mediated chain elongation and triglyceride production, thereby promoting the development of MASLD. Our findings delineate that the epigenetic mechanism of activation of lipid chain elongase genes mediated by TCF7l2 in concert with TCF19 has important implications in metabolic disorders.</p>","PeriodicalId":28,"journal":{"name":"Biochemistry Biochemistry","volume":" ","pages":""},"PeriodicalIF":2.9,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143762480","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":"Electron–Vibration Couplings Open New Channels for Energy Redistribution of Self-Assembled Monolayers on Plasmonic Nanoparticles","authors":"Quanbing Pei, Xiaoxuan Zheng, Junjun Tan, Yi Luo, Shuji Ye","doi":"10.1021/acs.jpclett.4c02930","DOIUrl":"https://doi.org/10.1021/acs.jpclett.4c02930","url":null,"abstract":"Unveiling how the interaction between self-assembled monolayers and plasmonic nanoparticles (PNPs) impacts molecular vibrational energy redistribution (VER) is crucial for optimizing plasmon-mediated chemical reactions (PMCRs). However, direct experimental evidence for molecule–PNP interactions opening new energy channels, such as up-pumping energy transfer and self-trapping of vibrational excitation, for VER has yet to be validated. Here, we demonstrate that electron–vibration coupling (EVC) induced by molecule–PNP interactions can open these new pathways for VER by utilizing femtosecond time-resolved sum-frequency generation vibrational spectroscopy. Using self-assembled 4-nitrothiophenol (4-NTP) monolayers on PNPs as a model, we observed that EVC opens a “forbidden” up-pumping energy transfer channel from 4-NTP nitro symmetric stretching (ν_NO2) to phenyl ring C═C stretching (ν_C═C) modes. The self-trapped state of excited ν_C═C modes is found, which originates from EVC-driven intermolecular coupling. These findings contribute to a better understanding of PMCR mechanisms and help guide the design of plasmonic catalysts with excellent performance.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"73 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758337","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}