化学•材料最新文献

{"title":"Diverse Effects of SO2-Induced Pt–O–SO3 on the Catalytic Oxidation of C3H6 and C3H8","authors":"Baojian Zhang, Yuan Yang, Juan Zheng, Dijierui Zhang, Wei Chen, Weidong Yuan, Xiaoping Chen, Rui Liu, Bosheng Chen, Liangwei Li, Limin Shi, Jinlong Wang, Zhu Luo, Yanbing Guo","doi":"10.1021/acs.est.4c04946","DOIUrl":"https://doi.org/10.1021/acs.est.4c04946","url":null,"abstract":"The effects of sulfur dioxide (SO₂) in the catalytic purification of short-chain hydrocarbons are still controversial, and the exact role of SO₂ on adsorption and reaction pathways during the catalytic oxidation of different volatile organic compounds (VOCs) remains unclear. Herein, a three-dimensional ordered macroporous Ce_0.8Zr_0.2O₂ supported Pt nanoparticle monolithic catalyst (Pt/OM CZO) was synthesized to investigate these effects. Our findings uncover the diverse effects of SO₂: Upon SO₂ treatment, the coupling between the S 3p and Pt 5d orbitals promotes the Pt–O–SO₃ structure in situ formed on the catalyst surface. The propene (C₃H₆) molecule readily binds with the oxygen atom in Pt–O–SO₃, resulting in the accumulation of acetone and carbon deposition, thereby hindering C₃H₆ oxidation. Conversely, a cleaved oxygen atom within the Pt–O–SO₃ structure enhances propane (C₃H₈) adsorption and activates the C–H bond, facilitating C₃H₈ oxidation. These insights are pivotal for advancing the frontier of sulfur-tolerant catalysts, addressing both economic and environmental challenges.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":9.028,"publicationDate":"2024-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142321631","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":"Natural Organic Matter Enhances Natural Transformation of Extracellular Antibiotic Resistance Genes in Sunlit Water","authors":"Qian-He Liu, Li Yuan, Zheng-Hao Li, Kenneth Mei Yee Leung, Guo-Ping Sheng","doi":"10.1021/acs.est.4c08211","DOIUrl":"https://doi.org/10.1021/acs.est.4c08211","url":null,"abstract":"Antibiotic resistance genes (ARGs) as emerging environmental contaminants exacerbate the risk of spreading antibiotic resistance. Natural organic matter (NOM) is ubiquitous in aquatic environments and plays a crucial role in biogeochemical cycles. However, its impact on the dissemination of extracellular antibiotic resistance genes (eARGs) under sunlight exposure remains elusive. This study reveals that environmentally relevant levels of NOM (0.1–20 mg/L) can significantly enhance the natural transformation frequency of the model bacterium <i>Acinetobacter baylyi</i> ADP1 by up to 7.6-fold under simulated sunlight. Similarly, this enhancement was consistently observed in natural water and wastewater systems. Further mechanism analysis revealed that reactive oxygen species (ROS) generated by NOM under sunlight irradiation, primarily singlet oxygen and hydroxyl radicals, play a crucial role in this process. These ROS induce intracellular oxidative stress and elevated cellular membrane permeability, thereby indirectly boosting ATP production and enhancing cell competence of extracellular DNA uptake and integration. Our findings highlight a previously underestimated role of natural factors in the dissemination of eARGs within aquatic ecosystems and deepen our understanding of the complex interplay between NOM, sunlight, and microbes in environmental water bodies. This underscores the importance of developing comprehensive strategies to mitigate the spread of antibiotic resistance in aquatic environments.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":9.028,"publicationDate":"2024-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142321633","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":"Conformation-Dictated Aggregation Photophysics in Isoindigo-Based Copolymers","authors":"Eninges Asmare, Nika Bekri, Leonato Tambua Nchinda, Fekadu G. Hone, Wendimagegn Mammo, Tjaart P. J. Krüger, Newayemedhin A. Tegegne","doi":"10.1021/acs.jpcc.4c04825","DOIUrl":"https://doi.org/10.1021/acs.jpcc.4c04825","url":null,"abstract":"The aggregation of polymer chains directly influences the morphology of thin films used in optoelectronic devices. Therefore, understanding the relationship between the backbone conformation and aggregation of conjugated polymers is essential for ensuring optimal electronic performance. In this work, we study the effect of the backbone conformation on the aggregation photophysics of isoindigo-based copolymers, namely, bithiophene-isoindigo (<b>P2TI</b>) and thienothiophene-spaced bithiophene-isoindigo (<b>P2TITT</b>). The latter was systematically tuned by inserting thieno[3,2-<i>b</i>]thiophene (<b>TT</b>) into the former. Modification of the backbone by inserting <b>TT</b> was found to affect the planarity due to reduced steric hindrance between the donor and acceptor units. This reduced steric hindrance was further evidenced by the difference in the oscillator strength of the first excited-state transition, identified as an intramolecular charge transfer transition in time-dependent density functional theory (TD/DFT) calculations. Temperature-dependent photoluminescence (PL) of the two polymers was well reproduced using two Franck–Condon progressions, indicating the formation of both H- and J-type aggregates. This was supported by the presence of two emission lifetimes obtained from time-resolved fluorescence measurements. The evolution of the first two vibronic peaks with temperature clearly showed a stronger interchain interaction in <b>P2TITT</b>.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":null,"pages":null},"PeriodicalIF":4.126,"publicationDate":"2024-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142321406","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":"Hiroaki Misawa Festschrift: Frontiers in Photochemistry","authors":"Kosei Ueno, Hong-Bo Sun, Paul Mulvaney, Stephan Link, Johan Hofkens","doi":"10.1021/acs.jpcc.4c05538","DOIUrl":"https://doi.org/10.1021/acs.jpcc.4c05538","url":null,"abstract":"Published as part of &lt;i&gt;The Journal of Physical Chemistry C&lt;/i&gt; special issue “Hiroaki Misawa Festschrift”. &lt;named-content content-type=\"bio-pic\" type=\"simple\"&gt;&lt;img alt=\"\" src=\"/cms/10.1021/acs.jpcc.4c05538/asset/images/medium/jp4c05538_0001.gif\"/&gt;&lt;/named-content&gt; This Festschrift is dedicated to Hiroaki Misawa, Extraordinary Professor at the Research Institute for Electronic Science, Hokkaido University, concurrently serving as Professor Emeritus at Hokkaido University, and Specially Appointed Professor at Okayama University, as well as Lifetime Chair Professor at National Yang Ming Chiao Tung University in Taiwan. The collection of articles featured herein is contributed by many of his colleagues, collaborators, friends, and students. It is presented in recognition of Misawa’s numerous outstanding scientific accomplishments, with a special emphasis on his contributions to photochemistry in general and plasmonic chemistry in particular. We honor his significant impact on these fields. Hiroaki Misawa was born and raised in Tokyo, Japan. He earned his B. Eng. degree in Industrial Chemistry from Tokyo Metropolitan University in 1979 under the supervision of Professor Mitsuhiko Hida. During this time, he conducted research on the photochromism of 1-(2-naphthoxy) anthraquinone derivatives under the guidance of Professor Haruo Inoue, who served as a research associate in Professor Hida’s laboratory. After graduating from Tokyo Metropolitan University, he spent five years as a graduate student in the Organic Physical Chemistry Laboratory at the Department of Chemistry, University of Tsukuba, led by the renowned organic photochemist Professor Katsumi Tokumaru. He conducted research on singlet-sensitized decomposition of dibenzoyl peroxide during his Master’s program and on photocatalytic reactions including hydrogen evolution using titanium dioxide (TiO&lt;sub&gt;2&lt;/sub&gt;) and dye sensitizers such as Eosin Y during both his Ph.D. programs under the supervision of Professor Tokumaru. He received his Ph.D. in Chemistry from the University of Tsukuba in 1984. After obtaining his doctoral degree, he embarked on a postdoctoral research journey under the supervision of Professor Richard A. Caldwell in the Department of Chemistry at the University of Texas at Dallas for almost two years. Here, he delved deep into the photophysical aspects of photoisomerization. His contributions included research that revealed significant isotope effects by combining spectroscopic measurements such as time-resolved absorption spectroscopy in the photoisomerization of &lt;i&gt;trans&lt;/i&gt;-1-phenylcyclohexene. His experience in research life in the United States was notably different from that in Japan, bringing him a fresh perspective. At the time, while benzene was still commonly used as a solvent in organic synthesis in Japan, its use required special permits and notifications in the United States. This highlighted his pioneering role in ensuring safety standards within university laborator","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":null,"pages":null},"PeriodicalIF":4.126,"publicationDate":"2024-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142321451","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":"The Challenging Conformational Landscape of Cysteamine···H2O Revealed by the Strong Interplay of Rotational Spectroscopy and Quantum Chemical Calculations","authors":"Wentao Song, Assimo Maris, Charlotte N. Cummings, Luca Evangelisti, Nicholas R. Walker, Sonia Melandri","doi":"10.1021/acs.jpclett.4c02353","DOIUrl":"https://doi.org/10.1021/acs.jpclett.4c02353","url":null,"abstract":"A 1:1 molecular complex of cysteamine with water is shown to adopt a cage-like structure where cysteamine accepts a relatively strong hydrogen bond from water while also engaging in two additional weaker interactions (SH···O_w and CH···O_w). Experimental and theoretical approaches confirm this conformer as the global minimum on the potential energy surface. Fitting of key structural parameters to experimentally determined moments of inertia yields consistent and accurate results for rotational and ¹⁴N nuclear quadrupole coupling constants which are shown to be challenging to calculate using <i>ab initio</i> methods. Comprehensive analysis of the intermolecular interactions and a thorough comparison with the properties of aminoethanol–water is presented, utilizing independent gradient models based on Hirshfeld partition, quantum theory of atoms-in-molecules, and symmetry-adapted perturbation theory approaches. As expected, the OH group of aminoethanol is a stronger hydrogen bond donor than the SH group in cysteamine, while the CH···O_w interaction is a key determining factor of the conformational landscape in both cysteamine–water and aminoethanol–water complexes. The results show very clearly that the synergy between theoretical calculations and experimental results is not only desirable but mandatory to get the right answers in such complex conformational surfaces. The results are also clear benchmarks for the accuracy of different theoretical methods in assessing the structures and energy order of the conformations.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":null,"pages":null},"PeriodicalIF":6.475,"publicationDate":"2024-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142321448","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":"Topological Protection of Oxygen Redox in Li-Rich Cathodes","authors":"Zhefeng Chen, Wentao Zhang, Shunning Li, Feng Pan","doi":"10.1021/acs.jpclett.4c01929","DOIUrl":"https://doi.org/10.1021/acs.jpclett.4c01929","url":null,"abstract":"Lithium-rich layered oxides (LRLOs) are regarded as promising candidates for next-generation cathode materials because of their high energy density derived from anionic redox activity. Recent years have seen increasing efforts in promoting the cyclability of LRLO cathodes, at the core of which is the suppression of irreversible internal structural evolution during cycling. The present article aims to provide an informative perspective on the materials design strategies related to the issue of oxygen release. Emphasis is placed on the underlying chemistry of oxygen redox in LRLOs and the strategies based on material topology that can mitigate oxygen migration to the cathode surface. We speculate that these insights could guide researchers in developing high-capacity cathodes with intrinsically high reversibility of oxygen redox.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":null,"pages":null},"PeriodicalIF":6.475,"publicationDate":"2024-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142321876","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":"A comprehensive review on luminescent carbon dots and their polymer composites: Synthesis to applications","authors":"","doi":"10.1016/j.nanoso.2024.101339","DOIUrl":"10.1016/j.nanoso.2024.101339","url":null,"abstract":"<div><div>Due to their distinct versatility and application qualities, carbon dots (CDs) and their composite materials have become promising luminous materials in a variety of industries. We give a comprehensive summary of current progress in the synthesis, characterization, and uses of carbon dots and their composites in luminescence and other domains in this review. This review focuses on the types of carbon dots and characterization methods used to investigate different properties like luminescence, including time-resolved spectroscopy, UV-Vis spectroscopy, and fluorescence spectroscopy. Additionally, different techniques for creating carbon dots, such as top-down and bottom-up procedures, as well as how precursor materials, surface passivation, doping, and size management affect the luminous properties of carbon dots are all discussed. The next section focuses on formation of carbon dots/polymer composite materials. Additionally, we go over how to create and design these composites, emphasizing how to improve their usefulness, stability, and luminous qualities. Further, we provide a thorough overview of the uses for carbon dots and their composites in the area of luminescence, including those for LEDs, sensors, displays, and biomedicine. Carbon dots have many properties like low toxicity, photostability, biocompatibility, and tunable emission wavelengths, that make them desirable candidates for various applications. In addition, we emphasize the most recent debates and views in the area of carbon dots and their composites for luminous applications. A thorough understanding of the synthesis, characterization, and uses of carbon dots and carbon dots composite materials in luminescence and other domains is what this paper aims to accomplish. For those working in the fields of nanomaterials, optoelectronics, and photonics who want to exploit the potential of carbon dots and their composites for creating improved luminous materials and devices, it is a useful resource.</div></div>","PeriodicalId":397,"journal":{"name":"Nano-Structures & Nano-Objects","volume":null,"pages":null},"PeriodicalIF":5.45,"publicationDate":"2024-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142322093","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Towards robust and scalable dispatch modeling of long-duration energy storage","authors":"","doi":"10.1016/j.rser.2024.114940","DOIUrl":"10.1016/j.rser.2024.114940","url":null,"abstract":"<div><div>Energy storage technologies, including short-duration, long-duration, and seasonal storage, are seen as technologies that can facilitate the integration of larger shares of variable renewable energy, such as wind and solar photovoltaics, in power systems. However, despite recent advances in the techno-economic modeling of energy storage (particularly for short-duration applications), the operation and economics of long-duration energy storage are still incomplete in power systems modeling platforms. For instance, existing modeling approaches for long-duration storage are often based either on an oversimplified representation of power system operations or limited representation of storage technologies, e.g., evaluation of only a single application. This manuscript presents an overview of the challenges of modeling long-duration energy storage technologies in power system operations, as well as a discussion regarding the capabilities and limitations of existing approaches. Here two test power systems with high shares of both solar photovoltaics- and wind (70 %–90 % annual variable renewable energy shares) are used to assess long-duration energy storage dispatch approaches. Our results estimate that better dispatch modeling of long-duration energy storage could increase the associated operational value by 4 %–14 % and increase the standard capacity credit by 14 %–34 %. Thus, a better long-duration energy storage dispatch could represent significant cost saving opportunities for electric utilities and system operators. In addition, existing long-duration dispatch modeling approaches were tested in terms of both improved system value (e.g., based on production cost and standard capacity credit) and scalability (e.g., based on central processing unit time and peak memory usage). Both copper plate and nodal representations of the power system were considered. Although the end volume target dispatch approach, i.e., based on mid-term scheduling, showed promising performance in terms of both improved system value and scalability, there is a need for robust and scalable dispatch approaches for long-duration energy storage in transmission-constrained electric grids. Moreover, more research is required to better understand the optimal operation of long-duration storage considering extreme climate/weather events, reliability applications, and power system operational uncertainties.</div></div>","PeriodicalId":418,"journal":{"name":"Renewable and Sustainable Energy Reviews","volume":null,"pages":null},"PeriodicalIF":16.3,"publicationDate":"2024-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142323059","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":"VUV Activated Fe(VI) by Promoting the Generation of Intermediate Valent Iron and Hydroxyl Radicals","authors":"Lian Wu, Lu Wang, Yu-Lei Liu, Xiao-Na Zhao, Jun Ma","doi":"10.1021/acs.est.4c05343","DOIUrl":"https://doi.org/10.1021/acs.est.4c05343","url":null,"abstract":"In this study, vacuum ultraviolet (VUV) was first proposed to activate ferrate (Fe(VI)) for degrading micropollutants (e.g., carbamazepine (CBZ)). Results indicated that VUV/Fe(VI) could significantly facilitate the CBZ degradation, and the removal efficiencies of VUV/Fe(VI) were 30.9–83.4% higher than those of Fe(VI) at pH = 7.0–9.0. Correspondingly, the degradation rate constants of VUV/Fe(VI) were 2.3–36.0-fold faster than those of Fe(VI). Free radical quenching and probe experiments revealed that the dominant active species of VUV/Fe(VI) were ^•OH and Fe(V)/Fe(IV), whose contribution ratios were 43.3 to 48.6% and 48.2 to 46.6%, respectively, at pH = 7.0–9.0. VUV combined with Fe(VI) not only effectively mitigated the weak oxidizing ability of Fe(VI) under alkaline conditions (especially pH = 9.0) but also attenuated the deteriorating effect of background constituents on Fe(VI). In different real waters (tap water, river water, WWTPs effluent), VUV/Fe(VI) retained a remarkably enhanced effect on CBZ degradation compared to Fe(VI). Moreover, VUV/Fe(VI) exhibited outstanding performance in the debasement of CBZ and sulfamethoxazole (SMX), as well as six other micropollutants, displaying broad-spectrum capability in degrading micropollutants. Overall, this study developed a novel oxidation process that was efficient and energy-saving for the rapid removal of micropollutants.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":9.028,"publicationDate":"2024-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142321573","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":"Hiroaki Misawa Festschrift: Frontiers in Photochemistry","authors":"Kosei Ueno*,&nbsp;Hong-Bo Sun,&nbsp;Paul Mulvaney,&nbsp;Stephan Link and Johan Hofkens,&nbsp;","doi":"10.1021/acs.jpcc.4c0553810.1021/acs.jpcc.4c05538","DOIUrl":"https://doi.org/10.1021/acs.jpcc.4c05538https://doi.org/10.1021/acs.jpcc.4c05538","url":null,"abstract":"","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":null,"pages":null},"PeriodicalIF":3.3,"publicationDate":"2024-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142318180","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}