化学•材料最新文献

{"title":"One-Pot Three-Component Coupling of Arylhydrazines with Aryl Aldehydes to Access the Triarylmethane Scaffold.","authors":"Dong Wang,Mingxia Liu,Shuo Zhang,Yunjiao Wang,Xiaokun Zhai,Yilin Xu,Jin Wang","doi":"10.1021/acs.joc.5c00082","DOIUrl":"https://doi.org/10.1021/acs.joc.5c00082","url":null,"abstract":"We herein report a one-pot, three-component coupling of arylhydrazine HCl salts with aryl aldehydes to synthesize a triarylmethane scaffold. This reaction proceeds under simple, mild, and practical conditions without the need for an additional Bro̷nsted or Lewis acid additive, accommodating a broad substrate scope with good to excellent yields. Furthermore, this methodology can be scaled up and allows access to a diverse range of triarylmethane derivatives. Mechanistic studies suggest that the in situ formed hydrazone intermediate is essential for the high efficiency and selectivity of this transformation.","PeriodicalId":57,"journal":{"name":"Journal of Organic Chemistry","volume":"68 1","pages":""},"PeriodicalIF":4.354,"publicationDate":"2025-05-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143921109","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":"Theory of Nonadiabatic Tunneling Splitting","authors":"Leonardo Raso, Michele Ceotto, Eli Pollak","doi":"10.1021/acs.jpclett.5c00443","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00443","url":null,"abstract":"Estimating tunneling splittings is a long-standing quantum mechanical challenge for theoretical methods. Sometimes splittings are so small, i.e., within a fraction of a wavenumber, pushing the limits of experimental detection and computational precision. Currently, most computational methods are able, at best, to obtain only ground-state tunneling splittings, either for symmetric or asymmetric potentials. In this Letter, we introduce a unified theoretical approach, based on a two-state approximation that can be equally applied to symmetric and asymmetric diabatic potential crossing and for excited states, providing reliable estimates even for states near the energy crossing. The method opens the door to analytic approximations for the tunneling splitting of model potential systems. It provides a framework for the introduction of vibrational perturbation theory to the estimation of nonadiabatic tunneling splittings. It also provides new insight into the semiclassical theory, leading to an instanton based steepest descent expression applicable also to excited states. Numerical tests on model systems are promising, providing the groundwork for implementation to future multidimensional applications.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"48 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2025-05-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143921154","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":"Advancements in coupling strategies for urban microclimate and building energy models","authors":"Ye Lu ,&nbsp;Sidra bibi","doi":"10.1016/j.rser.2025.115790","DOIUrl":"10.1016/j.rser.2025.115790","url":null,"abstract":"<div><div>Urban microclimates within metropolitan landscapes exhibit pronounced deviations from their rural counterparts, exerting a substantial influence on building energy performance. The precise representation of these microclimatic variations is paramount for enhancing the fidelity of building energy simulations. This study presents a meticulous and up-to-date review of contemporary advancements in coupling strategies that integrate urban microclimate modeling with building energy models (BEMs). While significant research has been dedicated to these domains in isolation, a critical gap remains in systematically assessing the methodologies employed to interlink them. This review elucidates the principal coupling techniques, categorizing them into unidirectional and bidirectional frameworks, and critically evaluates their relative merits. Findings underscore that bidirectional coupling, despite its computational intensity, yields superior accuracy in capturing the dynamic interplay between urban microclimates and building energy performance. Conversely, unidirectional coupling, though computationally efficient, lacks dynamic reciprocity, thereby introducing potential discrepancies in energy demand estimations. Notably, the incorporation of microclimatic effects through coupling mechanisms consistently results in a discernible reduction in cooling loads and a concomitant increase in heating demands. Moreover, this study highlights prevailing challenges, including computational overhead, data synchronization complexities, and the absence of standardized integration protocols. By providing a structured classification of coupling methodologies, delineating their intrinsic advantages and limitations, and proposing avenues for future research, this review serves as a foundational reference for advancing the seamless integration of urban microclimate dynamics within BEMs.</div></div>","PeriodicalId":418,"journal":{"name":"Renewable and Sustainable Energy Reviews","volume":"218 ","pages":"Article 115790"},"PeriodicalIF":16.3,"publicationDate":"2025-05-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143916129","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":"Direct Electrosynthesis and Separation Platform for Chlorine from Saline Water","authors":"Jianan Gao, Qingquan Ma, Yihan Zhang, Shan Xue, Guangyu Guo, Bingcai Pan, Han-Qing Yu, Wen Zhang","doi":"10.1021/acs.est.5c02676","DOIUrl":"https://doi.org/10.1021/acs.est.5c02676","url":null,"abstract":"Electrosynthesis of chlorine (Cl₂) from seawater and natural and industrial brines emerges as a transformative approach for wastewater valorization while achieving water purification. However, the effective separation of chlorine from complex saline mixtures and the mitigation of environmental impacts from chlorine derivatives are two critical challenges to tackle. Here, we report a scalable electrosynthesis platform capable of producing and separating chlorine directly at a single three-phase interface, achieving up to 97% selectivity and nearly 100% separation efficiency. Employing a three-stacked modular electrolyzer, we successfully generated sodium hypochlorite solutions at concentrations of 0.53 and 5.1 wt % from real reverse osmosis retentate and seawater. The treated brine discharge met the stringent environmental standards for chlorine-based contaminants. Compared to ion exchange and electrodialysis, this upcycling and separation process has the potential to advance decentralized chlor-alkali production and nonpotable water generation. Additionally, it can be seamlessly integrated with direct or indirect electrochemical impure water splitting, eliminating low-value oxygen production, reducing the need for alkali additives, and addressing safety concerns such as hydrogen/oxygen crossover.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"13 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-05-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143920940","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":"Construction of 3-Nitro-1H-pyrazole-5-yl-Bridged/Fused 4,5-Diamino-4H-1,2,4-triazoles Achieving High-Energy Insensitive Energetic Materials.","authors":"Lingfeng Xie,Chenchen Lin,Pingping Yi,Xiaoyi Yi,Piao He,Tingwei Wang,Jianguo Zhang","doi":"10.1021/acs.joc.4c02633","DOIUrl":"https://doi.org/10.1021/acs.joc.4c02633","url":null,"abstract":"Aminotriazole is a privileged structural motif in the design of various thermostable and insensitive energetic materials. A series of 3-nitro-1H-pyrazole-5-yl-bridged/fused 4,5-diamino-4H-1,2,4-triazoles was prepared via the cycloaddition of carboxyl pyrazole as a raw material. These newly synthesized compounds and their corresponding salts were fully characterized by chemical analysis (single-crystal X-ray diffraction, infrared, NMR, and mass spectroscopy) as well as experimental tests (thermostability and sensitivities). Their detonation properties (detonation velocity, detonation pressure, etc.) were determined with the EXPLO5 program on the basis of crystal density and calculated heat of formation with the Gaussian 09 suite. These pyrazole-triazoles show very high thermostabilities (Td > 320 °C) and low mechanical sensitivities (IS ≥ 25 J, FS ≥ 288 N) due to intermolecular hydrogen bonding interactions in polycyclic triazoles. In particular, tricyclic 3a displays an ultrahigh decomposition temperature of 371 °C, surpassing that of 2,2',4,4',6,6'-hexanitrostilbene (HNS) and can be used as a candidate for heat-resistant explosives. Dinitroamino compounds 2 (PCJ = 38.58 GPa, Vdet = 9268 m s-1) and 2d (PCJ = 36.15 GPa, Vdet = 8913 m s-1) were found to show excellent detonation performance, with 2 being comparable to 1,3,4,7-tetranitro-1,3,5,7-tetrazocane (HMX). Furthermore, compound 1 exhibits desirable detonation properties (PCJ = 34.74 GPa, Vdet = 9284 m s-1), high thermostability (333 °C), and low sensitivities (IS > 40 J, FS > 360 N), making it a promising HMX replacement. This study supports the superiority of utilizing the polycyclic pyrazole-triazole system in the development of new high-energy insensitive energetic materials.","PeriodicalId":57,"journal":{"name":"Journal of Organic Chemistry","volume":"110 1","pages":""},"PeriodicalIF":4.354,"publicationDate":"2025-05-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143921112","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":"Multifunctional BODIPY-Structured n-Type Conjugated Polymer for Simultaneous Interface Energetic Modification and Defect Passivation to Boost Efficiency and Stability of Inverted Perovskite Solar Cells","authors":"Shuang Lian, Mengyu Liu, Helong Zhu, Yanjie Wu, Anudari Dolgormaa, Yichi Zhang, Hongmei Zhan, Jun Liu, Lixiang Wang, Chuanjiang Qin","doi":"10.1021/acs.jpclett.5c00521","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00521","url":null,"abstract":"The performance of inverted perovskite solar cells (PSCs) is hindered by non-radiative recombination within the perovskite and charge recombination at the cathode interface. To address these issues, we propose a technique involving oriented crystallization control and interface energetic modification using a conjugated thienyl-fused BODIPY homopolymer named IP1. IP1 demonstrated effectiveness in both defect passivation and energy level adjustment. Simultaneously, IP1 acts as a “protective shield” anchored on the grain boundaries and surfaces of perovskite, enhancing the crystal structure and preventing degradation of perovskite. Based on the efficient synergy above, the IP1-modified device achieves a high power conversion efficiency (PCE) of 25.06%, representing the highest value among n-type polymer-incorporated PSCs. More importantly, the IP1-modified device maintains 95% of its initial PCE after operating at the maximum power point (MPP) of 1000 h. This work combines achievements of n-type conjugated polymer science and interface energetic modification to open a new door for efficient and stable PSCs.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"25 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2025-05-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143921146","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":"50 and 100 Years Ago in The Journal of Physical Chemistry – 2025 Edition","authors":"Joan-Emma Shea, T. Daniel Crawford, Barbara Kirchner, Cary Pint, Gregory V. Hartland","doi":"10.1021/acs.jpcc.5c02643","DOIUrl":"https://doi.org/10.1021/acs.jpcc.5c02643","url":null,"abstract":"In this series of editorials we look back at the work published in the Journal of Physical Chemistry 50 and 100 years ago. In 1925, &lt;i&gt;The Journal of Physical Chemistry&lt;/i&gt; published 153 articles, a 40% increase from the previous year and continuing the trend of journal growth in the 1920s. A large number of the papers dealt with the properties of colloids and emulsions, which was an important topic at the time and a major focus of the Journal’s editor-in-chief. The most prolific authors were N. R. Dhar from the University of Allahabad, India, and W. A. Patrick from Johns Hopkins University with eight papers each. Patrick pioneered a method to quickly and cheaply produce silica gel, which has a variety of uses, an important example being as the active agent in gas masks in World War I. His papers and correspondence have been archived by Johns Hopkins University. All of Patrick’s papers published &lt;i&gt;The Journal of Physical Chemistry&lt;/i&gt; in 1925 were studies of absorption of different species onto silica gel, except for a study of boiling points and conductivity of soap in alcohol solutions. (1) The soap study showed, not too surprisingly, that sodium oleate is dissociated in alcohol solutions at the boiling point. Dhar published on a wide range of topics including the viscosity of colloid solutions, (2) studies of corrosion of metals by nitric acid, (3) how the color of colloidal solutions changes with ion adsorption, (4) and photosynthesis in tropical light compared to artificial UV light. (5) Dhar was an extremely prolific scientist, and was an early leader of physical chemistry in India. The most cited papers in 1925 were studies of the performance of different types of adhesives by McBain and Hopkins (6) and how thin films affect water evaporation by E. K. Rideal (who later achieved fame for his work on surface catalysis). (7) A diagram of the apparatus used by McBain and Hopkins to measure the strength of adhesives is shown in Figure 1. (6) This paper was cited 14 times in 2024! Also in 1925 Kharasch and Sher presented a 33-page “preliminary communication” on determining the heat of combustion by counting the number of valence electrons─see Figure 1. (8) In their view of bonding, atoms have a series of orbits and two atoms can hold a pair of electrons at the points where the orbits intersect. Which orbit is used depends on the affinity of the atom for electrons. Although this is not the modern view, the differences between the calculated and measured heats of combustion were generally &lt;1%, which is outstanding. Also in 1925 Barker published a similar set of calculations based on Lewis structures; (9) however, the predicted combustion energies were less accurate. The Journal also published two papers on the stabilization of gold colloids (“Zsigmondy’s gold sols”) by surface active agents (10,11) and four papers on the properties of phosgene (dielectric constant, conductivity and solution density) by Germann and co-workers. (12−15) The work ","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"404 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2025-05-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143921150","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":"Mechanisms, technical optimization, and perspectives in the recycling and reprocessing of waste wind turbine blades: A review","authors":"Leilei Cheng ,&nbsp;Ruizhe Chen ,&nbsp;Jialiang Yang ,&nbsp;Xueru Chen ,&nbsp;Xinyu Yan ,&nbsp;Jing Gu ,&nbsp;Zejian Liu ,&nbsp;Haoran Yuan ,&nbsp;Yong Chen","doi":"10.1016/j.rser.2025.115834","DOIUrl":"10.1016/j.rser.2025.115834","url":null,"abstract":"<div><div>Wind energy plays a key role in reducing carbon emissions in the power industry, but current recycling methods for waste wind turbine blades (WTBs) remain unsustainable. This paper reviews the principles, technologies, and potential applications of WTB recycling. It combines fundamental research with an engineering perspective to assess interdependencies across processing stages. Physical methods, such as cutting structural materials and grinding fillers, still face challenges in final waste disposal. Chemical methods, including pyrolysis with product upgrading, solvolysis, and selective deconstruction using liquid-phase catalysts, enable integrated recovery of organic and fiber products but face issues with heat and mass transfer. Moreover, chemical recycling processes must minimize energy consumption, costs, and emissions, while ensuring the separation of chemicals that meet market standards. Additionally, developing deconstruction-functionalization routes to produce higher-value chemicals is crucial. We explore fiber loss mechanisms, mainly due to wear at cutting points, high-temperature hotspots (pyrolysis-oxidation), and chemical reagent-induced leaching of fiber components. We also examine various applications for high-strength and degraded fibers, balancing the integrated recycling of high-value organic products and fibers. Beyond basic research, we discuss the potential of pilot-scale processing equipment and its scalability. In the short term, scalable, cost-effective, and environmentally friendly technologies are essential. In the long term, we recommend developing electrified composite manufacturing and recycling models using locally sourced renewable energy, along with designing new resins for controlled degradation and multi-field coupled deconstruction.</div></div>","PeriodicalId":418,"journal":{"name":"Renewable and Sustainable Energy Reviews","volume":"218 ","pages":"Article 115834"},"PeriodicalIF":16.3,"publicationDate":"2025-05-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143924790","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":"Accommodating more electric vehicles in old residential communities by enabling distributed vehicle-to-grid dispatching and coordinated system operation","authors":"Hang Yu ,&nbsp;Jiayang Tu ,&nbsp;Ziyun Shao ,&nbsp;Linni Jian","doi":"10.1016/j.rser.2025.115814","DOIUrl":"10.1016/j.rser.2025.115814","url":null,"abstract":"<div><div>Electric vehicles' (EVs') popularity in recent years not only reduces oil demands and gas emissions, but also effectively promotes the deployment of charging infrastructure. However, regarding old residential communities (ORCs), implementing widespread charging facilities may not be a wise choice due to scarce public areas, complex reconstruction, and significant costs. In this context, this paper proposes to utilize vehicle-to-grid (V2G) technology to support the shared DC fast charging for ORCs’ applications. Initially, the underlying reasons for difficult-to-charge issues in ORCs are unveiled and analyzed comprehensively. Then, a hierarchical management framework with operation strategies is designed based on a novel reconstructed charging station architecture. A new power electronic device called smart interlinking unit (SIU) is the critical component in this architecture. Then, an introduced distributed V2G dispatching strategy is to be executed by each local AC charger, considering the extra DC charging load and five typical charging scenarios. This paper also proposes a feeder coordination strategy, taking the efficiency feature of deployed transformers and power converters into account. For the real case studies, the developed V2G dispatching strategy is verified to achieve a prominent 45.7 % EV penetration level. In addition, the efficient problem-solving and lower peak-to-valley difference are to be realized. The feeder coordination strategy is demonstrated to achieve flexible power flow dispatching and overall optimization of operation efficiency effectively.</div></div>","PeriodicalId":418,"journal":{"name":"Renewable and Sustainable Energy Reviews","volume":"218 ","pages":"Article 115814"},"PeriodicalIF":16.3,"publicationDate":"2025-05-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143924801","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":"50 and 100 Years Ago in The Journal of Physical Chemistry – 2025 Edition","authors":"Joan-Emma Shea,&nbsp;T. Daniel Crawford,&nbsp;Barbara Kirchner,&nbsp;Cary Pint and Gregory V. Hartland*,&nbsp;","doi":"10.1021/acs.jpcb.5c0264210.1021/acs.jpcb.5c02642","DOIUrl":"https://doi.org/10.1021/acs.jpcb.5c02642https://doi.org/10.1021/acs.jpcb.5c02642","url":null,"abstract":"","PeriodicalId":60,"journal":{"name":"The Journal of Physical Chemistry B","volume":"129 18","pages":"4279–4281 4279–4281"},"PeriodicalIF":2.8,"publicationDate":"2025-05-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143917084","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}