化学•材料最新文献

{"title":"Global Land Use Change Impacts on Soil Nitrogen Availability and Environmental Losses.","authors":"Jing Wang,Yves Uwiragiye,Miaomiao Cao,Meiqi Chen,Nyumah Fallah,Yuanyuan Huang,Yuanyuan Huang,Yi Cheng,Zucong Cai,Minggang Xu,Scott X Chang,Christoph Müller","doi":"10.1021/acs.est.5c03285","DOIUrl":"https://doi.org/10.1021/acs.est.5c03285","url":null,"abstract":"Anthropogenic activities, particularly land use change and management practices, alter the global nitrogen (N) cycle. As a central part of the global N cycle, soil N supply from net N mineralization (NNM) and net nitrification (NN) contributes to over 50% of crop N uptake. However, how global land use changes impact soil N supply and potential N loss remains elusive. By compiling a global data set of 1,782 paired observations from 185 publications, we show that land use conversion from natural to managed ecosystems significantly reduced NNM by 7.5% (-11.5, -2.8%) and increased NN by 150% (86, 194%), indicating decreasing N availability while increasing potential N loss through denitrification and nitrate leaching. In contrast, reversing managed to natural ecosystems significantly increased NNM by 20% (9.7, 25.4%) and decreased NN by 89% (-125, -46%), indicating increasing N availability while decreasing potential N loss. Structural equation modeling revealed that land use change induced changes in soil properties, including organic matter content, bulk density, microbial biomass and pH, and anthropogenic activities, including application of ammonium-based fertilizers and manure, were the most important factors regulating NNM and NN. The land use change effect was the strongest in tropical and subtropical regions, where NNM was negatively affected and NN positively affected by land use change. Our findings indicate that increasing soil organic matter content and enhancing soil structural development post land use change can boost soil N supply and reduce the risk for N loss.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"24 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-08-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144851055","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":"Global Decarbonization Enabled by a Novel Strategy of Biomineralization for Concrete Corrosion Inhibition.","authors":"Xiaohao Sun,Yong Wang,Jiadong Ren,Onyx W H Wai,Xiangdong Li","doi":"10.1021/acs.est.5c00261","DOIUrl":"https://doi.org/10.1021/acs.est.5c00261","url":null,"abstract":"With rapid urban population growth, predominantly in coastal regions, decarbonizing concrete structures in coastal cities is crucial. Extending the lifespan of concrete is highly efficient in achieving net-zero greenhouse gas (GHG) emissions by 2050. Biomineralization for concrete corrosion inhibition (BCCI) was previously proposed and demonstrated to effectively protect marine concrete in laboratory experiments, showing promise for decarbonization due to potentially increased lifespans. The potential of BCCI for decarbonization and sustainability warrants further investigation. Therefore, this study evaluated its impact on GHG emissions for insights into global decarbonization. Field corrosion experiments were conducted to ascertain its effectiveness as a valuable GHG calculation input, including biofilm community analysis and microstructure and macroscopic measurements of concrete. Results show that BCCI decreased the total/relative abundances of corrosive bacteria, inhibited sulfate and chloride diffusion, and enhanced carbon functions, irrespective of concrete type. Moreover, BCCI significantly reduced GHG emissions, particularly in 20 MPa concrete. BCCI demonstrated substantial GHG mitigation potential in China, Indonesia, and the USA, which enabled a competitive 37-65% reduction in global GHG from producing underwater concrete. In the long term, this strategy would yield more sustainable development benefits. Findings contribute to achieving global decarbonization and multiple sustainable development goals for concrete sectors and coastal infrastructures.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"79 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-08-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144851119","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":"Deciphering the Effects of Quenching on the Chemodiversity of Low- and Non-volatile Disinfection Byproducts in Drinking Source Water Using ESI(-)-FT-ICR MS.","authors":"Shixi Wu,Yiming Feng,Xinyi Chen,Qing-Long Fu,Huiyu Dong,Xin Yang,Rui Ma,Pingqing Fu,Yanxin Wang","doi":"10.1021/acs.est.5c06175","DOIUrl":"https://doi.org/10.1021/acs.est.5c06175","url":null,"abstract":"Quenching is essential for terminating chlorination and preserving halogenated disinfection byproducts (Xn-DBPs) in disinfected waters. However, the effects of quenchers on the chemodiversity and stability of low- and non-volatile Xn-DBPs are still poorly understood. Four quenchers─sodium sulfite (SS), sodium thiosulfate (STS), ascorbic acid (AA), and 1,3,5-trimethoxybenzene (TMB)─were employed to elucidate their influences on the non-targeted analysis of Xn-DBPs using Fourier transform ion cyclotron resonance mass spectrometry under negative electrospray ionization mode (ESI(-)-FT-ICR MS). Compared with the insignificant difference in decomposed Xn-DBPs, the average number of additionally formed Xn-DBPs for AA was significantly lower than that for SS (31 ± 18 versus 67 ± 35) at their optimum doses. The decomposition and additional formation caused by three reductive quenchers on the characterization of Xn-DBPs and their precursors followed the order: AA < STS < SS. Moreover, TMB was recommended to quench residual chlorine for one hour at the quencher-to-residual chlorine molar ratio of 2.00 because of its advantages in avoiding the decomposition of redox-sensitive Xn-DBPs and additional formation of Xn-DBPs by ESI(-)-FT-ICR MS, while exhibiting insignificant impacts on the overall molecular characteristics of DOM. This study provides novel insights into the effects of quenching on the non-targeted analysis of Xn-DBPs.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"45 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-08-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144851230","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":"Regioselectivity Switching in the Tandem Reaction of Skipped Diynones with Allylic Alcohols: Stereoselective Synthesis of 4-Allyl-2-Methylene-3(2H)-Furanones.","authors":"Sofia O Karnakova,Marina Yu Dvorko,Anton V Kuzmin,Igor' A Ushakov,Dmitrii A Shabalin","doi":"10.1021/acs.joc.5c01422","DOIUrl":"https://doi.org/10.1021/acs.joc.5c01422","url":null,"abstract":"A novel base-catalyzed synthesis of hitherto unknown 4-allyl-2-methylene-3(2H)-furanones from skipped diynones and allylic alcohols via nucleophilic addition/Claisen rearrangement/cyclization reaction is described. An important role of the employed catalytic system for the regioselective switching in the cyclization step from 3-allyl-4-pyrones to isomeric 4-allyl-3(2H)-furanones is discussed. The isolation of main intermediates of the tandem reaction and study of their reactivity allowed us to develop a convenient two-stage protocol for stereoselective 4-allyl-2-methylene-3(2H)-furanone formation featuring a good substrate tolerance and good yields of target products.","PeriodicalId":57,"journal":{"name":"Journal of Organic Chemistry","volume":"37 1","pages":""},"PeriodicalIF":4.354,"publicationDate":"2025-08-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144851296","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 Cross-Linkable Silane Additive Enables High-Performance Air-Processed Inverted CsPbI3 Perovskite Solar Cells.","authors":"Jiaying Liu,Xiaohui Liu,Jianwei Wang,Zhongyu Liu,Chenyu Zhou,Hubin Zeng,Heng Qiao,Jing Zhang,Like Huang,Ning Chen,Yuejin Zhu","doi":"10.1021/acs.jpclett.5c02129","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c02129","url":null,"abstract":"The extreme sensitivity of inorganic CsPbI3 perovskites to moisture imposes stringent humidity requirements during fabrication, severely limiting their practical applications. Herein, 3-iodopropyltrimethoxysilane (IPTMS) is introduced as a multifunctional additive into the perovskite precursor to address these limitations. During thermal annealing, IPTMS molecules undergo an in situ hydrolysis-driven cross-linking reaction, consuming residual water while constructing a hydrophobic polysiloxane network at grain boundaries, thus effectively shielding films against moisture infiltration. Concurrently, IPTMS can modulate crystallization kinetics via slowing down crystal growth to generate high-quality films. Furthermore, the iodine groups in IPTMS can favorably interact with the electron-rich sites in the CsPbI3 film, resulting in a notable reduction of trap states and enhanced stability of the perovskite octahedral framework. Consequently, the optimized inverted devices deliver a champion efficiency of 20.36% with much improved long-term device stability. Besides, the incorporation of IPTMS endows the fabrication of efficient devices even in a high humid atmosphere, yielding an impressive efficiency of 19.50%.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"749 1","pages":"8632-8641"},"PeriodicalIF":6.475,"publicationDate":"2025-08-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144851031","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":"Invariance of Energy Exchange Rates for Light-Dressed Systems.","authors":"Yujie Jiao,Bing Gu,Siying Peng","doi":"10.1021/acs.jpclett.5c01663","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c01663","url":null,"abstract":"Light-driven matter can exhibit electronic and optical properties qualitatively distinct from those observed at equilibrium. We demonstrate that while strong driving can tune the absorption properties, the energy exchange rate of any light-dressed system remains invariant compared to its bare counterpart. This invariance is evidenced experimentally by the vanishing integrated area of the transient absorption spectrum. We present a general theory alongside experimental results obtained from halide perovskite nanocrystals under strong off-resonance driving. This unexpected result provides useful insights into the optical properties of matter that is driven far from equilibrium.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"14 1","pages":"8627-8631"},"PeriodicalIF":6.475,"publicationDate":"2025-08-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144851032","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":"Flexible heat pipes in thermal management applications – A comprehensive review","authors":"Nidhin A R ,&nbsp;A.R. Anand ,&nbsp;Akhil Jaiswal ,&nbsp;Madhu Ganesh ,&nbsp;Brusly Solomon","doi":"10.1016/j.rser.2025.116167","DOIUrl":"10.1016/j.rser.2025.116167","url":null,"abstract":"<div><div>Flexible heat pipes represent an innovative heat transfer technology that offers significant advantages over conventional heat pipes for thermal management. Their ability to easily adapt to complex shapes and geometries enhances their potential in renewable energy applications. This review begins with the fundamental principles and explores the diverse applications of flexible heat pipes, highlighting their unique benefits in each field. Key design considerations, such as container material, wicking structure, and working fluid are discussed in detail to provide a comprehensive understanding of their fabrication methods. Additionally, the review offers insights into experimental studies related to flexible heat pipes, recent advancements, parameters for enhancing thermal performance, and optimization methods. Addressing current challenges requires the use of advanced materials, cutting-edge manufacturing techniques, and custom-designed heat pipes for specific applications. This paper aims to develop a thorough understanding of flexible heat pipes, thereby paving the way for their implementation as a sustainable thermal management solution.</div></div>","PeriodicalId":418,"journal":{"name":"Renewable and Sustainable Energy Reviews","volume":"225 ","pages":"Article 116167"},"PeriodicalIF":16.3,"publicationDate":"2025-08-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144842672","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":"Single-Molecule Vibrational Thermometry.","authors":"Philip A Kocheril, Dongkwan Lee, Noor Naji, Rahuljeet S Chadha, Ryan E Leighton, Haomin Wang, Lu Wei","doi":"10.1021/acs.jpcb.5c04024","DOIUrl":"https://doi.org/10.1021/acs.jpcb.5c04024","url":null,"abstract":"<p><p>Molecular probes of temperature (termed \"molecular thermometers\") have become broadly used for <i>in situ</i> temperature measurements. Here, we describe Boltzmann-edge vibrational thermometry (BET) detected by anti-Stokes fluorescence, where the relative population of vibrationally excited molecules acts as a calibration-free reporter of local temperature based on the Boltzmann distribution. We demonstrate that BET microscopy is readily compatible with biological samples and achieves single-molecule sensitivity. We then show that local environments can be characterized through the modulation of vibrational temperature by mid-infrared absorption, allowing for BET fingerprinting. This work provides a foundation for sensitive vibrational thermometry in biological imaging.</p>","PeriodicalId":60,"journal":{"name":"The Journal of Physical Chemistry B","volume":" ","pages":""},"PeriodicalIF":2.9,"publicationDate":"2025-08-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144853954","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":"Machine Learning on the Impacts of Mutations in the SARS-CoV-2 Spike RBD on Binding Affinity to Human ACE2 Based on Deep Mutational Scanning Data.","authors":"Hui Xia, Dacong Wei, Zhihong Guo, Lung Wa Chung","doi":"10.1021/acs.biochem.4c00587","DOIUrl":"https://doi.org/10.1021/acs.biochem.4c00587","url":null,"abstract":"<p><p>Severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) continues to accumulate mutations in the spike receptor-binding domain (RBD) region, leading to the emergence of new variants that potentially change the binding affinity for the human angiotensin converting enzyme 2 (hACE2) receptor. Deep mutational scanning (DMS) is a powerful biochemical experimental technique that can characterize the impact of mutations on protein sequence-function relationships, allowing for rapid assessment of new mutations. Herein, machine learning (ML) models were built using the SARS-CoV-2 DMS data set, with the input features derived from the Rosetta-computed decomposition energy terms. To improve the performance of this physics-based model, we further incorporated local environment information (the number of residue pair-specific contacts within shells at different distances) as the input features. Alternatively, a convolutional neural network (CNN) model based on amino-acid sequence information as well as their physicochemical and biochemical properties was also employed, yielding predictions that achieved good agreement with the experimental data. In addition, compared to three popular protein language models, the dual-encoding CNN model demonstrated consistently superior performance on the SARS-CoV-2 DMS data set and seven additional DMS data sets for different biological properties. Furthermore, a transfer-learning strategy was applied to fine-tune the CNN model using recently reported DMS data sets for the Alpha, Delta, and Omicron BA.1, BA.2, and XBB.1.5 variants, enabling the development of variant-specific prediction models. These ML models trained on DMS data sets can not only identify the effects of single-point mutations in mutagenesis data sets but also be useful in predicting the effects of multiple-point mutations and providing valuable information for ongoing viral surveillance efforts. Moreover, this dual-encoding CNN model, without including 3D geometric information, has the potential to be a robust and alternative ML model for other DMS studies.</p>","PeriodicalId":28,"journal":{"name":"Biochemistry Biochemistry","volume":" ","pages":""},"PeriodicalIF":3.0,"publicationDate":"2025-08-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144853973","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":"Potential-of-Mean-Force vs Free-Energy Surfaces for pH-Dependent Mechanisms: The Case of Peptide Bond Formation in Ester Aminolysis","authors":"Allan L. L. East*,&nbsp;","doi":"10.1021/acs.jpclett.5c01649","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c01649","url":null,"abstract":"<p >Potential-of-mean-force (PMF) computations, for free-energy surfaces (FES) of reactions from molecular dynamics simulations, omit a concentration-dependent entropy term, which can cause difficulties in interpretation of concentration-dependent kinetics. Here the case of aminolysis of esters (amine + ester → amide + alcohol), which has known pH-dependent kinetics, is re-examined.</p>","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 32","pages":"8298–8302"},"PeriodicalIF":4.6,"publicationDate":"2025-08-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144826272","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}