化学•材料最新文献

{"title":"All-Season Passive Thermal Management Film with Multifunctionality for Efficient Radiative Cooling and Solar Heating","authors":"Tingni Wu, Kai Yin, Yuchun He, Lingxiao Wang, Haonan Yu, Yin Huang, Ji-An Duan, Christopher J. Arnusch","doi":"10.1021/acs.jpclett.5c00436","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00436","url":null,"abstract":"Thermal radiation management is an important aspect of thermal engineering and plays a crucial role in various industrial and environmental applications. However, either cooling or heating devices alone can exacerbate all-season consumption during hot summers or cold winters. We have designed a dual-mode thermal management device that can switch modes by a pull-out method, with femtosecond laser-induced graphene (LIG) on the surface of a polyimide membrane as the heating surface and a SiO₂ hollow microsphere coating as the cooling surface. Due to the multi-interface reflection between SiO₂ hollow microspheres and air, high reflectivity (93%) and 97% thermal infrared emissivity can be obtained. Under a solar irradiation intensity of 75 J/cm², a temperature decrease of 6.3 °C can be realized. On the other hand, LIG can achieve an ultra-ambient temperature increase of 35 °C due to its excellent solar light absorption characteristics (ε ≈ 97%) and high thermal conductivity. Temperature regulation can be achieved by switching heating and cooling modes, which shows great promise in agriculture and for food and goods preservation. Also, this design is expected to offer a new approach to energy efficient cooling and heating in architecture.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"18 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2025-04-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143775884","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":"Similar Oxygen Sensitivities of Different Steps of Denitrification in Estuarine Waters","authors":"Weiyi Tang, Samantha G. Fortin, Naomi Intrator, Jenna A. Lee, Moriah A. Kunes, Amal Jayakumar, Shannon J. Haynes, Sergey Oleynik, Daniel M. Sigman, Bess B. Ward","doi":"10.1021/acs.est.5c02248","DOIUrl":"https://doi.org/10.1021/acs.est.5c02248","url":null,"abstract":"Hypoxia is observed and projected to expand in many aquatic environments, largely due to excess anthropogenic nutrient inputs and climate change, thus influencing biogeochemical processes. Denitrification, generally an anaerobic process, removes bioavailable nitrogen and produces nitrous oxide (N₂O). However, limited observations of the effect of oxygen on denitrification restrict our ability to estimate changes in the amount of bioavailable nitrogen and N₂O emissions under anthropogenic perturbations and climate change. Here, we show that all denitrification steps increased, while the N₂O production yield from denitrification decreased with decreasing oxygen in Chesapeake Bay – the largest estuary in the United States. The different steps of denitrification responded similarly to oxygen changes in Chesapeake Bay, unlike open ocean oxygen minimum zones, with implications for the accumulation or depletion of denitrification intermediates such as nitrite and N₂O. Our observations also suggest that current model parametrizations of denitrification in Chesapeake Bay likely overestimate denitrification and nitrogen removal in the presence of oxygen, which would bias the evaluation of nutrient cycling, ecosystem productivity, and the extent of hypoxia. Overall, our newly derived oxygen sensitivities of denitrification could be used to improve model parametrizations of denitrification and constrain the nitrogen budget and N₂O emissions in estuarine and coastal environments experiencing hypoxia.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"61 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-04-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143776088","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":"Carrier Recombination and Surface Band Bending in GaAs/InGaAs Core–Shell Nanowires with Reverse Type-I Band Alignment","authors":"Puning Wang, Bingheng Meng, Yubin Kang, Huan Liu, Xiaobing Hou, Jilong Tang, Qun Hao, Zhipeng Wei, Rui Chen","doi":"10.1021/acs.jpcc.5c01213","DOIUrl":"https://doi.org/10.1021/acs.jpcc.5c01213","url":null,"abstract":"GaAs/In<i>_<i>x</i></i>Ga_1<i>-x</i>As core–shell nanowires (NWs) with reverse type-I band alignment have attracted significant interest in optoelectronics due to their unique optical properties. However, the detailed characterizations of carrier recombination in these NWs remain insufficiently explored. In this study, GaAs/In_0.3Ga_0.7As core–shell NWs were grown via molecular beam epitaxy, and their optical properties were investigated by optical spectroscopies. For GaAs/In_0.3Ga_0.7As core–shell NWs with an 80 nm core and a 30 nm shell, the bandgap of the InGaAs shell was found to be significantly reduced by approximately 0.93 eV due to compressive strain. Power-dependent photoluminescence measurement revealed a direct transition near the band edge in the shell as well as an indirect transition associated with surface states. With an increase in temperature, the Fermi level shifts closer to the valence band, leading to band bending and a reduction in the depletion region. When the temperature exceeds 180 K, the surface-trapped carriers overcome the potential barrier, resulting in an increase in the number of direct transitions. Our results demonstrate that GaAs/InGaAs core–shell NWs with reverse type-I band alignment exhibit a strong potential for efficient photogenerated carrier extraction and collection, making them promising candidates for a wide range of optoelectronic applications.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"58 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2025-04-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143782954","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":"Correction to “Mechanisms Underlying the Size-Dependent Neurotoxicity of Polystyrene Nanoplastics in Zebrafish”","authors":"Chao Wu, Hong-Jie Zhang, Hongxia Ma, Rong Ji, Ke Pan, Tongtao Yue, Ai-Jun Miao","doi":"10.1021/acs.est.5c03983","DOIUrl":"https://doi.org/10.1021/acs.est.5c03983","url":null,"abstract":"The correct first affiliation of Chao Wu is College of Physics and Optoelectronic Engineering, Shenzhen University, Shenzhen 518060, China. This article has not yet been cited by other publications.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"59 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-04-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143782927","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 Product Synthesis Enabled by Radical-Polar Crossover Reactions","authors":"Nicolas Müller, Thomas Magauer, Ondřej Kováč","doi":"10.1021/acs.joc.5c00306","DOIUrl":"https://doi.org/10.1021/acs.joc.5c00306","url":null,"abstract":"Radical-polar crossover (RPC) chemistry is an emerging field characterized by transformations that involve the coexistence of both radical and ionic species. Since the reactivities of radical and ionic intermediates are orthogonal, applying these two mechanisms in sequence provides significant advantages in the construction of complex molecular architectures. The concept of the RPC approach has become increasingly important in the total synthesis of natural products. This Synopsis presents several examples to showcase recent advancements in this area, including our research on the synthesis of <i>Ganoderma</i> meroterpenoids. In these selected cases, RPC reactions enhance the building of structural complexity and improve overall synthetic efficiency that cannot be achieved by standard synthetic methods.","PeriodicalId":57,"journal":{"name":"Journal of Organic Chemistry","volume":"216 1","pages":""},"PeriodicalIF":4.354,"publicationDate":"2025-04-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143775767","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":"Membrane Binding and Cholesterol Sensing Motif in <i>Mycoplasma genitalium</i> FtsZ: A Novel Mode of Membrane Recruitment for Bacterial FtsZ.","authors":"Soumyajit Dutta, Sakshi Poddar, Joyeeta Chakraborty, Ramanujam Srinivasan, Pananghat Gayathri","doi":"10.1021/acs.biochem.4c00543","DOIUrl":"https://doi.org/10.1021/acs.biochem.4c00543","url":null,"abstract":"<p><p>Cell division in bacteria is initiated by constriction of the Z-ring comprising two essential proteins, FtsZ and FtsA. Though the essential function of the Z-ring in bacterial division has been established, the precise roles of FtsZ and FtsA in the constriction process remain elusive. Due to the minimal number of components, FtsZ/FtsA in cell wall-less bacteria is an ideal model system for obtaining mechanistic insights into Z-ring constriction in the absence of a cell wall synthesis machinery. In this study, we undertook a comparative analysis of FtsZ and FtsA protein sequences from 113 mycoplasma species and the corresponding sequences in cell-walled bacteria. We report a phylogenetically distinct group of 12 species that possess a putative membrane binding amphipathic helix at either the N- or C-terminal extensions of the globular FtsZ domain. Importantly, these FtsZs lack conservation of the conserved C-terminal peptide sequence. We experimentally prove that the proposed C-terminal amphipathic helix in <i>Mycoplasma genitalium</i> (<i>M. genitalium</i>) FtsZ exhibits membrane binding. Additionally, we identify a potential cholesterol recognition motif within the C-terminal amphipathic helix region of <i>M. genitalium</i> FtsZ. Our study catalogues the functional variations of membrane attachment by the FtsZ and FtsA system in cell wall-less mycoplasmas and provides a new perspective to dissect the role of FtsZ and FtsA in cell division.</p>","PeriodicalId":28,"journal":{"name":"Biochemistry Biochemistry","volume":" ","pages":""},"PeriodicalIF":2.9,"publicationDate":"2025-04-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143784360","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":"High-Frequency Tails in Spectral Densities.","authors":"Roman Korol, Xinxian Chen, Ignacio Franco","doi":"10.1021/acs.jpca.5c00943","DOIUrl":"https://doi.org/10.1021/acs.jpca.5c00943","url":null,"abstract":"<p><p>Recent advances in numerically exact quantum dynamics methods have brought the dream of accurately modeling the dynamics of chemically complex open systems within reach. Path-integral-based methods, hierarchical equations of motion, and quantum analog simulators all require the spectral density (SD) of the environment to describe its effect on the system. Here, we focus on the decoherence dynamics of electronically excited species in solution in the common case where nonradiative electronic relaxation dominates and is much slower than electronic dephasing. We show that the computed relaxation rate is highly sensitive to the choice of SD representation─such as the Drude-Lorentz or Brownian modes─or strategy used to capture the main SD features, even when early-time dephasing dynamics remains robust. The key reason is that electronic relaxation is dominated by the resonant contribution from the high-frequency tails of the SD, which are orders of magnitude weaker than the main features of the SD and can vary significantly between strategies. This finding highlights an important, yet overlooked, numerical challenge: obtaining an accurate SD requires capturing its structure over several orders of magnitude to ensure correct decoherence dynamics at both early and late times. To address this, we provide a simple transformation that recovers the correct relaxation rates in quantum simulations constrained by algorithmic or physical limitations on the shape of the SD. Our findings enable a comparison of different numerically exact simulation methods and expand the capabilities of analog simulations of open quantum dynamics.</p>","PeriodicalId":59,"journal":{"name":"The Journal of Physical Chemistry A","volume":" ","pages":""},"PeriodicalIF":2.7,"publicationDate":"2025-04-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143784382","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":"Integrating sustainability across the lifecycle of electric vehicle batteries: Circular supply chain challenges, innovations, and global policy impacts","authors":"Aishwarya V.M. ,&nbsp;Banu Yetkin Ekren ,&nbsp;Tej Singh ,&nbsp;Vedant Singh","doi":"10.1016/j.rser.2025.115671","DOIUrl":"10.1016/j.rser.2025.115671","url":null,"abstract":"<div><div>This study investigates the integration of sustainability practices into the circular supply chain (SC) of electric vehicle (EV) batteries to address environmental and economic challenges. Using the Preferred Reporting Items for Systematic Reviews and Meta-Analyses (PRISMA) protocol, a systematic review of 147 articles (2009–2024) identifies key challenges, solutions, innovations, and policy measures shaping the EV battery SC. The research uncovers 10 major challenges, 31 sub-challenges, and 160 detailed challenges, highlighting issues related to SC resilience, environmental impact, and economic sustainability. In response, 40 main solutions and 174 complete solutions are mapped, leading to the identification of 102 detailed technologies, 24 sub-technologies, and 8 core technologies supporting circular economy principles. These technologies are analysed for their long-term industry impact, with comparisons within categories to highlight their advantages, disadvantages, and contributions to circular economy goals. Additionally, global policy analysis reveals regulatory advancements, with China and the UK leading efforts to improve recycling, material recovery, and sustainability governance. This study also compares EV battery policies across countries using indicators like policy coverage, enforcement intensity, and effectiveness, highlighting their impact on sustainability and resource efficiency. A conceptual framework is developed to integrate these challenges, solutions, and innovations into a sustainable EV battery SC. The study concludes with theoretical insights, industry recommendations, and policy implications, offering a structured pathway toward sustainable and resilient EV battery SCs.</div></div>","PeriodicalId":418,"journal":{"name":"Renewable and Sustainable Energy Reviews","volume":"216 ","pages":"Article 115671"},"PeriodicalIF":16.3,"publicationDate":"2025-04-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143767896","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":"Unraveling the Primary Photochemistry of Pyruvic Acid: Direct Observation of Three Competing Channels","authors":"Lyra J. Sauer, H. Floyd Davis","doi":"10.1021/acs.jpclett.5c00323","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00323","url":null,"abstract":"The photodissociation of gaseous pyruvic acid at three representative wavelengths, 369.74, 354.45, and 322.50 nm, was studied under collision-free molecular beam conditions. Kinetic energy distributions of the neutral products were measured using tunable vacuum ultraviolet photoionization followed by mass spectrometric analysis. Decarboxylation (CO₂ elimination) was dominant for all three wavelengths, producing primarily ground state singlet methylhydroxycarbene, ¹CH₃COH, as well as a minor yield of electronically excited ³CH₃COH. Excitation at 369.74 and 354.45 nm produced ¹CH₃COH with internal energies lying below and above the calculated potential energy barriers for isomerization to vinyl alcohol (C₂H₃OH) and acetaldehyde (CH₃CHO). This suggests that the bimolecular chemistry of CH₃COH may be important in the atmosphere. At 322.5 nm, C–C bond fission producing HOCO + CH₃CO was also observed as a minor channel. While decarboxylation producing ¹CH₃COH + CO₂ on the singlet potential energy surface (PES) is clearly dominant, observation of ³CH₃COH + CO₂ and HOCO + CH₃CO confirms that the triplet PES also plays a role in pyruvic acid photochemistry in the actinic region.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"108 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2025-04-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143782885","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":"Phonon Anisotropy and Anharmonicity in Epitaxial Al2Mo3O12 Nanoflakes","authors":"Jindong Bai, Yuedong Wang, Baopeng Yang, Zhiyi Liu, Xiao Guo, Tao Xu, Fangyan Ang, Haipeng Xie, Fangping Ouyang, Jin Li, Han Huang","doi":"10.1021/acs.jpclett.5c00478","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00478","url":null,"abstract":"Aluminum molybdate (Al₂Mo₃O₁₂) exhibits superior properties for wide bandgap, chemical flexibility, negative thermal expansion, and good thermal stability. However, Al₂Mo₃O₁₂ prepared by traditional processes still suffered from inefficiency and poor quality so far. Here, we report on epitaxial growth of α-Al₂Mo₃O₁₂ nanoflake arrays with unidirectional domain orientations on c-sapphire via chemical vapor deposition. Optical microscopy, atomic force microscopy, scanning electron microscopy, energy dispersive spectroscopy, X-ray diffraction, high-resolution transmission electron microscopy, selected area electron diffraction, and Raman spectroscopy measurements reveal the high-quality of as-grown samples and the specific epitaxial relationship between α-Al₂Mo₃O₁₂ and c-sapphire: α-Al₂Mo₃O₁₂[021] || sapphire[112̅0] and α-Al₂Mo₃O₁₂[02̅1] || sapphire[11̅00]. Phonon polarizations of α-Al₂Mo₃O₁₂ exhibit a strong anisotropy ratio up to 3.13 for A_g modes, which can be used to identify the crystal orientation. The abnormal temperature dependence of MoO₄ symmetric stretching vibration phonon modes (SSVPMs) reveal giant anharmonic phonon–phonon interaction in α-Al₂Mo₃O₁₂. The ultralow thermal conductivity of α-Al₂Mo₃O₁₂ is predicted by the ultrashort phonon lifetime of ∼0.12 ps. Our findings provide insight into the thermal properties of α-Al₂Mo₃O₁₂ and are helpful for the application in polarization-sensitive optoelectronic detector and thermoelectric material.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"37 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2025-04-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143775885","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}