化学•材料最新文献

{"title":"Ammonia borane-promoted surface reconstruction of copper oxide catalysts for efficient catalytic hydrogen production from hydrolysis","authors":"Chenyang Wang,&nbsp;Yuchun Wang,&nbsp;Yiyan Bai,&nbsp;Wei Zhang,&nbsp;Zhaorong Liu","doi":"10.1016/j.apcata.2025.120283","DOIUrl":"10.1016/j.apcata.2025.120283","url":null,"abstract":"<div><div>During hydrogen production by hydrolysis of ammonia borane (AB), transition metal oxides act as active sites in the catalyst and can help to achieve rapid and large-scale release of hydrogen, but its catalytic mechanism is still under discussion. We developed a Cu₂O/CuO catalyst with precisely controlled valence states and identified the fundamental source of the catalytic activity of oxides. The successive changes in the Cu valence state content of Cu₂O/CuO resulted in a volcano-like trend of the catalyst activity, with the optimal hydrogen production rate from hydrolysis reaching 378.01 mL·g⁻¹·min⁻¹. The characterization of the catalysts after combined use revealed that AB prompted the catalyst surface to reconstruct during the catalytic process, forming a Cu/Cu₂O heterostructure. This study established, for the first time, the structure-activity relationship between the valence state of copper and its catalytic activity, providing a theoretical basis for the construction of copper-based catalysts for AB hydrolysis.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"699 ","pages":"Article 120283"},"PeriodicalIF":4.7,"publicationDate":"2025-04-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143826337","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":"Characterisation of strain localisation and crack evolution of Cf/SiC-SiC composites by SEM-DIC method","authors":"Kunjie Wang,&nbsp;Chenghai Xu,&nbsp;Bo Gao,&nbsp;Songhe Meng","doi":"10.1016/j.compositesa.2025.108936","DOIUrl":"10.1016/j.compositesa.2025.108936","url":null,"abstract":"<div><div>In thermo-mechanical-oxidative coupling service environments, stress-induced microscale damage in ceramic matrix composites (CMCs) governs diffusion kinetics of oxidising media, accelerating degradation of mechanical properties. Therefore, the quantification of microscale damage is a core issue in revealing damage mechanisms. In this study, a low-cost, highly uniform submicron speckle pattern was prepared on the surface of silicon carbide-coated carbon fibre-reinforced silicon carbide matrix (C_f/SiC-SiC) composites and the strain localisation and crack evolution were accurately characterised using scanning electron microscopy combined with digital image correlation. For the first time, this study completely tracked and quantified the dynamic damage evolution process of C_f/SiC-SiC composites at the microscale, including key mechanisms such as strain localisation, interfacial debonding, matrix cracking, fibre slip, and macroscopic failure, further verifying the key contribution of interfacial slip to composite toughening. The experimental results revealed the interaction dynamics of the multicrack system. Further research found that the initial crack widths of the SiC coating follow a log-normal distribution, while the evolution of crack density under tensile load exhibits a strain threshold effect. The crack opening displacement (COD) of the coating has a ‘stress memory’ effect. These findings contribute to deeper understanding of the synergistic effect of stress and oxidation and provide a new perspective for studying the microscale and mesoscale damage behaviour of CMCs.</div></div>","PeriodicalId":282,"journal":{"name":"Composites Part A: Applied Science and Manufacturing","volume":"194 ","pages":"Article 108936"},"PeriodicalIF":8.1,"publicationDate":"2025-04-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143817128","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Toilet Bowl Cleaning Tablets as Sources of Chlorine, Bromine, and Disinfection Byproducts in Wastewater","authors":"Vincent T. DiPietri, Zolani S. Grady, Alexis N. Frost, Shannon E. Stitzel, John D. Sivey","doi":"10.1021/acs.est.4c12026","DOIUrl":"https://doi.org/10.1021/acs.est.4c12026","url":null,"abstract":"Commercial toilet bowl cleaning tablets were examined in laboratory systems to characterize their release of active halogens and their potential to form trihalomethanes (THMs) when combined with synthetic sewage. Active halogens (e.g., HOCl, HOBr, and reactive halamines) were quantified via derivatization with 1,3,5-trimethoxybenzene prior to analysis by liquid chromatography. The effects of several variables on halogen release profiles were examined, including pH, ionic strength, temperature, tank solution volume, flushing frequency, and tablet brand. Changes in pH resulted in modest or no appreciable changes in halogen release profiles. Release of active halogens increased as ionic strength decreased and as temperature increased. Tank volume, flushing frequency, and tablet brand had pronounced impacts on halogen release profiles. Maximum measured active chlorine and bromine concentrations in toilet tank water were 189 mg/L as Cl₂ and 164 mg/L as Cl₂, respectively. Active halogens persisted in toilet bowl water for &gt;24 h. When toilet-tablet-treated water was combined with synthetic sewage, THMs formed at up to 219 ppb with bromine incorporation factors up to 2.86. Active halogens and highly brominated THMs released into wastewater from toilet tablets could have implications for downstream microbial ecology, septic system performance, and overall water quality.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"100 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-04-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143814084","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":"Design Rules for Selecting Suitable Weakly Solvating Electrolytes for Lithium Metal Batteries","authors":"Da Zhu, Yu Ou, Yingchun Xia, Li Sheng, Jianlong Wang, Yaping Tang, Kai Liu, Xiangming He, Hong Xu","doi":"10.1021/acs.jpclett.5c00627","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00627","url":null,"abstract":"Weakly solvating electrolyte (WSE) is a promising and convenient strategy to regulate Li⁺ solvation structures and promote the formation of an anion-driven and robust solid electrolyte interface layer. Here, we outline a reasonable workflow to realize high-throughput calculations of the binding energy of Li⁺-solvent in a stable conformation and molecular polarity index (MPI) of solvents to replace the value of donor number and dielectric constants, which are difficult to obtain experimentally. Twenty-six common solvent molecules are used to verify the workflow. Based on the output (binding energy and MPI value), we construct a descriptor (named <i>W</i>_s) that is suitable to screen WSE and verify it in 6 typical solvent systems through experiments, molecular dynamic (MD) simulations, and survival probability function. This work demonstrates a universal and useful strategy to distinguish potential solvents for the WSE system and can also be developed for other battery systems in the future.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"39 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2025-04-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143814133","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 Unexploring Optoelectronic Features in Organic Trans-Dimensional Materials of Gridofluorenes at the Nanoscale","authors":"Yongxia Wang, Lizhu Dong, Shuangyi Li, Yang Feng, Xinyao Ge, Xinxin Han, Chao Liu, Ying Wei, Xiaogang Cheng, Linghai Xie, Wei Huang","doi":"10.1021/acs.jpclett.4c03432","DOIUrl":"https://doi.org/10.1021/acs.jpclett.4c03432","url":null,"abstract":"Organic grido-architectures offer not only state-of-the-art models for exploring the complex relationships of multicarrier coherence among excitons, charges, photons, electrons, and phonons but also organic high-dimensional nanomaterials for flexible electronics and organic intelligence. Herein, we initiate the fundamental progress and perspective on gridofluorene-based zero-, one-, two-, and three-dimensional nanomolecules and their optoelectronic features. From the future point of view, the sterically trans-dimensional and hierarchically cross-scale effects of these covalent frameworks and nanostructures are discussed on their photophysical, electrical, mechanical and thermal properties. Organic multiscale systems, with the feature of synergistically molecule-programmable integration of diverse functionalities, open a bright door to flexible electronics, intelligent molecules, devices, systems, and even organobots as well as artificially intelligent and robotic chemists (AiRCs).","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"6 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2025-04-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143814334","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":"Computer-based tools for assessment of small-scale hydropower resources and project feasibility: a review","authors":"Petras Punys","doi":"10.1016/j.rser.2025.115717","DOIUrl":"10.1016/j.rser.2025.115717","url":null,"abstract":"<div><div>This article analyses and compares computer-based tools designed for small hydropower (SHP) potential assessment, site planning, and design, focusing on the initial assessment phase of project evaluation. The review draws from various sources, including open-access publications, research papers and projects, data repositories, and web resources. This paper presents more than 40 software tools currently in use, their main features, comparative analysis, and research studies using them, including a brief reminder of historic software tools. These tools can provide simple initial estimates or be sophisticated software considering unconventional (in-conduit) hydro. They are categorised into four groups: i) Hydraulic turbine selection (4 software), ii) Site feasibility assessment (18), iii) Environmental flow assessment (5), iv) Web-based hydropower atlases (9), and v) Multicriteria analysis (3).</div><div>The review highlights that while there are numerous tools for site assessment, the development of new tools for turbine selection, particularly for innovative hydro turbines, has declined. It also notes the increasing adoption of digital platforms and web-based mapping for hydropower, driven by advancements in GIS, which aid in identifying feasible hydro sites. Special tools for applying multicriteria analysis to evaluate conflicting and other aspects of hydropower development are also discussed. The paper emphasises the importance of user feedback in improving these tools. It critically reviews the available tools, summarises best practices, and provides guidelines for their further application and enhancement in hydropower resource assessment and project site feasibility evaluation. This review aims to assist SHP designers and practitioners in selecting the most suitable software.</div></div>","PeriodicalId":418,"journal":{"name":"Renewable and Sustainable Energy Reviews","volume":"216 ","pages":"Article 115717"},"PeriodicalIF":16.3,"publicationDate":"2025-04-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143816680","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":"Multiset Variational Quantum Dynamics Algorithm for Simulating Nonadiabatic Dynamics on Quantum Computers","authors":"Jingjing Li, Weitang Li, Xiaoxiao Xiao, Limin Liu, Zhendong Li, Jiajun Ren, Weihai Fang","doi":"10.1021/acs.jpclett.5c00739","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00739","url":null,"abstract":"Accelerating quantum dynamical simulations with quantum computing has received considerable attention but remains a significant challenge. In variational quantum algorithms for quantum dynamics, designing an expressive and shallow-depth parametrized quantum circuit (PQC) is a key difficulty. Here, we propose a multiset variational quantum dynamics algorithm (MS-VQD) tailored for nonadiabatic dynamics involving multiple electronic states. The MS-VQD employs multiple PQCs to represent the electronic–nuclear coupled wave function, with each circuit adapting to the motion of the nuclear wavepacket on a specific potential energy surface. By simulating excitation energy transfer dynamics in molecular aggregates described by the Frenkel–Holstein model, we demonstrate that the MS-VQD achieves the same accuracy as the traditional VQD while requiring significantly shallower PQCs. Notably, its advantage increases with the number of electronic states, making it suitable for simulating nonadiabatic quantum dynamics in complex molecular systems.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"17 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2025-04-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143820145","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":"Pd-Catalyzed Selective Arylative Cascade Cyclization of 1,6-Diynes and Dibenzoxaborins for Fused Naphthalene Derivatives","authors":"Muniganti Naveen Kumar, Shivunapuram Mahesh, Jagadeesh Babu Nanubolu, Maddi Sridhar Reddy","doi":"10.1021/acs.joc.5c00034","DOIUrl":"https://doi.org/10.1021/acs.joc.5c00034","url":null,"abstract":"A palladium-catalyzed new mode of cascade arylative cyclization of 1,6-diynes is disclosed using dibenzoxaborin as an arylating agent featuring transmetalation and selective migratory insertion as the key steps. This process enables the efficient construction of polysubstituted fused naphthalene skeletons via the formation of three new C–C bonds through dual regioselectivity in both arylation as well as C–H functionalization. Some control experiments and kinetic isotope effect (KIE) studies were conducted to elucidate the reaction mechanism, and some product diversifications were achieved to showcase the synthetic potential.","PeriodicalId":57,"journal":{"name":"Journal of Organic Chemistry","volume":"17 1","pages":""},"PeriodicalIF":4.354,"publicationDate":"2025-04-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143813956","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":"TCT-Mediated and Water-Controlled Synthesis of Benzofuran-3(2H)-ones Bearing a Quaternary Carbon Center via a Radical Process Using Dimethyl Sulfoxide as a Dual Synthon","authors":"Qing Chen, Zhao Du, Chuanqi Liu, Xiaoqian Wang, Wantong Yue, Yilei Wang, Zhihua Peng","doi":"10.1021/acs.joc.5c00201","DOIUrl":"https://doi.org/10.1021/acs.joc.5c00201","url":null,"abstract":"An efficient and attractive method for the synthesis of valuable benzofuran-3(2<i>H</i>)-one derivatives bearing a quaternary center in one step by employing dimethyl sulfoxide (DMSO) as a dual synthon under metal-free conditions has been developed. In this reaction, DMSO activated by cyanuric chloride (TCT) provides two different units (CH₃ and SMe) in the target molecules, and the construction of the quaternary carbon center in the benzofuran-3(2<i>H</i>)-ones can be controlled by the addition of water. Furthermore, the functional group compatibility and synthetic value were demonstrated by scope evaluation and gram-scale experiments. The mechanistic studies show that the reaction may proceed via a radical process.","PeriodicalId":57,"journal":{"name":"Journal of Organic Chemistry","volume":"183 1","pages":""},"PeriodicalIF":4.354,"publicationDate":"2025-04-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143813958","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":"Pt 5d Density of States in Pt3Mg–N–C Catalyst Governed by Ligand Effect","authors":"Jiabin Xu, Jiatang Chen, Yun-Mui Yiu, Jun Zhong, Yining Huang, Tsun-Kong Sham","doi":"10.1021/acs.jpclett.5c00201","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00201","url":null,"abstract":"In alloy systems, the strain and ligand effects are prevalent, but it is challenging to study the impact of either on the material structure independently. We conducted high-energy-resolution fluorescence detection (HERFD) X-ray absorption spectroscopy (XAS) and resonant X-ray emission spectroscopy (XES)/resonant inelastic X-ray scattering (RIXS) spectroscopy on a Pt₃Mg alloy-based carbon material (Pt₃Mg–N–C). By introducing a size-comparable atom, the strain effect is minimized, allowing the Pt d-density of states (d-DOS) to be primarily affected by the ligand effect. The experimental results reveal that Pt gains electrons in Pt₃Mg–N–C, exhibiting a more symmetric d-band shape and a downshift of the d-band center compared to Pt metal, which is further confirmed by density functional theory (DFT) calculations. The correlation between the Pt d-DOS and oxygen reduction reaction (ORR) activity is also discussed.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"99 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2025-04-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143820143","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}