Cheng Chen, Yiyang Zhang, Guoyu Yin, Dongyao Sun, Ye Li, Lijun Hou, Min Liu
Global warming and microplastics (MPs) pollution are emerging stressors that threaten coastal ecosystems, yet their combined impacts on biogeochemical cycles remain poorly resolved. Here, we integrated a factorial microcosm experiment with stable isotope tracing and molecular techniques to disentangle how warming and MPs jointly regulate nitrogen (N) cycling in coastal sediments. We demonstrate that warming and MPs interacted nonadditively to reshape nitrification, denitrification, and associated nitrous oxide (N2O) production dynamics. Warming reversed the stimulatory effect of polyethylene (PE) on nitrification, turning it inhibitory, and amplified the suppressive impact of poly(butylene adipate-co-terephthalate) (PBAT), primarily through synergistic intensification of anoxic stress. In contrast, warming strengthened PE-driven stimulation of denitrification and mitigated PBAT-induced inhibition, likely due to the selective enrichment of nirS- and nosZ-harboring denitrifiers. Moreover, warming overturned the stimulatory effects of both PE and PBAT on N2O production, shifting toward inhibition through nitrifier denitrification, as substantiated by dual-isotope (15N–18O) tracing and genomic evidence. Collectively, these findings provide novel mechanistic insights into how warming interacts with MPs to reconfigure sedimentary N cycling, with broad implications for predicting the responses and evolution of coastal ecosystems under accelerating global change.
{"title":"Warming Modulates Microplastic Impacts on Coastal Nitrogen Cycling by Synergistically Amplifying Sediment Hypoxia and Restructuring the Denitrifying Microbiome","authors":"Cheng Chen, Yiyang Zhang, Guoyu Yin, Dongyao Sun, Ye Li, Lijun Hou, Min Liu","doi":"10.1021/acs.est.5c08930","DOIUrl":"https://doi.org/10.1021/acs.est.5c08930","url":null,"abstract":"Global warming and microplastics (MPs) pollution are emerging stressors that threaten coastal ecosystems, yet their combined impacts on biogeochemical cycles remain poorly resolved. Here, we integrated a factorial microcosm experiment with stable isotope tracing and molecular techniques to disentangle how warming and MPs jointly regulate nitrogen (N) cycling in coastal sediments. We demonstrate that warming and MPs interacted nonadditively to reshape nitrification, denitrification, and associated nitrous oxide (N<sub>2</sub>O) production dynamics. Warming reversed the stimulatory effect of polyethylene (PE) on nitrification, turning it inhibitory, and amplified the suppressive impact of poly(butylene adipate-<i>co</i>-terephthalate) (PBAT), primarily through synergistic intensification of anoxic stress. In contrast, warming strengthened PE-driven stimulation of denitrification and mitigated PBAT-induced inhibition, likely due to the selective enrichment of <i>nirS</i>- and <i>nosZ</i>-harboring denitrifiers. Moreover, warming overturned the stimulatory effects of both PE and PBAT on N<sub>2</sub>O production, shifting toward inhibition through nitrifier denitrification, as substantiated by dual-isotope (<sup>15</sup>N–<sup>18</sup>O) tracing and genomic evidence. Collectively, these findings provide novel mechanistic insights into how warming interacts with MPs to reconfigure sedimentary N cycling, with broad implications for predicting the responses and evolution of coastal ecosystems under accelerating global change.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"46 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2026-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146146398","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}
Adrià Sunyer-Caldú, Hongyu Xie, Bénilde Bonnefille, Foteini Raptopoulou, Edouard Pesquet, May Britt Rian, Daniel Schlesinger, Michael Norman, Young June Jeon, Boram Kim, Seung-Bok Lee, Ji Eun Lee, Jean Froment, Stefano Papazian, Jonathan W. Martin
Polluted air is a major global health risk factor, yet the chemical composition and toxicity of airborne gases and particles remain underexplored due to their complexity and difficulties in sampling. We recently introduced how polydimethylsiloxane (PDMS) foam─or silicone foam─can be synthesized for passive air sampling, enabling simple and cost-effective nontarget chemical profiling of indoor air. Here, we demonstrate expanded applications, indoors and outdoors, with commercial PDMS-foam, including for: (i) wide-scope target analysis of >220 priority substances by quantitative liquid- and gas chromatography-high-resolution mass spectrometry, (ii) microscopic characterization and nontarget profiling of accumulated fine particles, and (iii) effect-guided discovery of harmful substances, combining toxicological data with nontarget analysis in silico. Median method quantification limits were 0.12 ng/mL, 90% of target analytes had absolute recoveries between 70 and 130%, and hazardous substances were discovered, including ethylene glycols, insecticides, and UV filters. Microscopy revealed the accumulation of abundant fine particles, and the automated characterization of the fluorescent fraction revealed that most were <4 μm. Extracts from outdoor samples reduced human lung cell viability, and multivariate modeling flagged families of potentially toxic substances in a virtual effect-directed analysis. PDMS-foam disks require field calibration to determine their linear sampling rate(s), but current results and applications establish PDMS-foam as a multimodal passive sampler, enabling integrated chemical quantitation, toxicological analysis, and molecular discovery in air.
{"title":"Silicone-Foam Passive Air Samplers for Combined Target and Nontarget Chemical Profiling and Toxicity Assessment of Airborne Exposomes","authors":"Adrià Sunyer-Caldú, Hongyu Xie, Bénilde Bonnefille, Foteini Raptopoulou, Edouard Pesquet, May Britt Rian, Daniel Schlesinger, Michael Norman, Young June Jeon, Boram Kim, Seung-Bok Lee, Ji Eun Lee, Jean Froment, Stefano Papazian, Jonathan W. Martin","doi":"10.1021/acs.est.5c16613","DOIUrl":"https://doi.org/10.1021/acs.est.5c16613","url":null,"abstract":"Polluted air is a major global health risk factor, yet the chemical composition and toxicity of airborne gases and particles remain underexplored due to their complexity and difficulties in sampling. We recently introduced how polydimethylsiloxane (PDMS) foam─or silicone foam─can be synthesized for passive air sampling, enabling simple and cost-effective nontarget chemical profiling of indoor air. Here, we demonstrate expanded applications, indoors and outdoors, with commercial PDMS-foam, including for: (i) wide-scope target analysis of >220 priority substances by quantitative liquid- and gas chromatography-high-resolution mass spectrometry, (ii) microscopic characterization and nontarget profiling of accumulated fine particles, and (iii) effect-guided discovery of harmful substances, combining toxicological data with nontarget analysis in silico. Median method quantification limits were 0.12 ng/mL, 90% of target analytes had absolute recoveries between 70 and 130%, and hazardous substances were discovered, including ethylene glycols, insecticides, and UV filters. Microscopy revealed the accumulation of abundant fine particles, and the automated characterization of the fluorescent fraction revealed that most were <4 μm. Extracts from outdoor samples reduced human lung cell viability, and multivariate modeling flagged families of potentially toxic substances in a virtual effect-directed analysis. PDMS-foam disks require field calibration to determine their linear sampling rate(s), but current results and applications establish PDMS-foam as a multimodal passive sampler, enabling integrated chemical quantitation, toxicological analysis, and molecular discovery in air.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"247 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2026-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146146395","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}
Max I. Kessler, Richard Randall, Gang Wan, Kun Xu, Yirui Zhang, Jennifer A. Dionne, Robert B. Jackson, Arun Majumdar
To mitigate the climate impacts of methane, there has been substantial interest in the complete oxidation of methane to carbon dioxide by using photocatalysis at ambient temperatures. However, previous studies have primarily examined methane concentrations well above those found at most emission sources and have overlooked the role of realistic humidity. This work reports methane oxidation rates at 25 °C for oxide-based photocatalysts for methane concentrations ranging from 2 to 5000 ppm. Even under dry conditions with less than 2% relative humidity, residual water attracted to the hydrophilic surfaces of these photocatalysts severely inhibits methane oxidation. Thinning this water layer boosts methane oxidation rates by up to 1 order of magnitude. Furthermore, surface modification of titanium dioxide with a hydrophobic fluorosilane coating (1H,1H,2H,2H-perfluorooctyltriethoxysilane) enables room temperature photocatalytic removal of dilute methane even under conditions with up to 80% relative humidity. These findings and engineering solutions offer guidance for the development of light-driven approaches for scalable methane removal.
{"title":"A Humidity-Tolerant Photocatalyst for Methane Removal","authors":"Max I. Kessler, Richard Randall, Gang Wan, Kun Xu, Yirui Zhang, Jennifer A. Dionne, Robert B. Jackson, Arun Majumdar","doi":"10.1021/acs.est.5c16764","DOIUrl":"https://doi.org/10.1021/acs.est.5c16764","url":null,"abstract":"To mitigate the climate impacts of methane, there has been substantial interest in the complete oxidation of methane to carbon dioxide by using photocatalysis at ambient temperatures. However, previous studies have primarily examined methane concentrations well above those found at most emission sources and have overlooked the role of realistic humidity. This work reports methane oxidation rates at 25 °C for oxide-based photocatalysts for methane concentrations ranging from 2 to 5000 ppm. Even under dry conditions with less than 2% relative humidity, residual water attracted to the hydrophilic surfaces of these photocatalysts severely inhibits methane oxidation. Thinning this water layer boosts methane oxidation rates by up to 1 order of magnitude. Furthermore, surface modification of titanium dioxide with a hydrophobic fluorosilane coating (1<i>H</i>,1<i>H</i>,2<i>H</i>,2<i>H</i>-perfluorooctyltriethoxysilane) enables room temperature photocatalytic removal of dilute methane even under conditions with up to 80% relative humidity. These findings and engineering solutions offer guidance for the development of light-driven approaches for scalable methane removal.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"5 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2026-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146146396","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}
The enantioselective synthesis of chiral diaryl alcohols, crucial pharmaceutical intermediates, remains challenging due to the poor stereochemical differentiation between similar aryl groups. We address this by reporting a highly enantioselective Rh-catalyzed transfer hydrogenation of cubane-aryl ketones. Leveraging the three-dimensional cubane as a sterically distinct surrogate for a flat aryl group, this method provides chiral cubane-aryl alcohol bioisosteres in excellent yield (up to 99%) and enantioselectivity (up to >99% ee). DFT studies implicate key noncovalent C–H···π interactions in the stereocontrol. Gram-scale synthesis and a TON of 5000 establish the method’s practical utility for accessing valuable, stereodefined scaffolds in drug discovery.
{"title":"Rh-Catalyzed Asymmetric Transfer Hydrogenation of Cubane-Containing Ketones to Access Bioisomers of Diaryl Alcohols","authors":"Mingyang Liu, Zichun Zhang, Congcong Yin, Zhuang Zhong, Sensheng Liu, Haifeng Zhou","doi":"10.1021/acs.joc.5c02940","DOIUrl":"https://doi.org/10.1021/acs.joc.5c02940","url":null,"abstract":"The enantioselective synthesis of chiral diaryl alcohols, crucial pharmaceutical intermediates, remains challenging due to the poor stereochemical differentiation between similar aryl groups. We address this by reporting a highly enantioselective Rh-catalyzed transfer hydrogenation of cubane-aryl ketones. Leveraging the three-dimensional cubane as a sterically distinct surrogate for a flat aryl group, this method provides chiral cubane-aryl alcohol bioisosteres in excellent yield (up to 99%) and enantioselectivity (up to >99% ee). DFT studies implicate key noncovalent C–H···π interactions in the stereocontrol. Gram-scale synthesis and a TON of 5000 establish the method’s practical utility for accessing valuable, stereodefined scaffolds in drug discovery.","PeriodicalId":57,"journal":{"name":"Journal of Organic Chemistry","volume":"133 1","pages":""},"PeriodicalIF":4.354,"publicationDate":"2026-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146146335","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}
Pub Date : 2026-02-10DOI: 10.1021/acs.jpcc.6c00389
Frederik L. Durhuus, Marco Beleggia, Cathrine Frandsen
Superparamagnetic nanoparticles (SMNPs) are essential components in a number of medical diagnostic- and drug transport techniques, and cancer therapies. It is often claimed that the rapid thermal reversals of SMNP magnetic moments negates their dipolar attraction, hence facilitating colloidal stability. We find that this is a misconception. Using Langevin dynamics, we simulate SMNP pairs and the dimer clusters they form. To quantify the tendency to aggregate, we introduce the dimer debonding time and calculate the average magnetic force of attraction which results from correlations in the fluctuating moments─a magnetic analogue of the van der Waals interaction. We find that the magnetocrystalline anisotropy, which determines the rate of superparamagnetic reversals, has no influence on debonding time, and comparing with computed Néel relaxation times this holds for both blocked and superparamagnetic particles. Hence superparamagnetism does not affect aggregation, which explains the success of previous simplified models in describing the equilibrium structure of SMNP systems. Because the key dimensionless parameter for the Néel relaxation of a lone SMNP and the one for magnetic attraction have the same size and temperature scaling, there is a strong correlation with colloidal stability, as observed experimentally, but no causal relation.
{"title":"Dipolar Attraction of Superparamagnetic Nanoparticles","authors":"Frederik L. Durhuus, Marco Beleggia, Cathrine Frandsen","doi":"10.1021/acs.jpcc.6c00389","DOIUrl":"https://doi.org/10.1021/acs.jpcc.6c00389","url":null,"abstract":"Superparamagnetic nanoparticles (SMNPs) are essential components in a number of medical diagnostic- and drug transport techniques, and cancer therapies. It is often claimed that the rapid thermal reversals of SMNP magnetic moments negates their dipolar attraction, hence facilitating colloidal stability. We find that this is a misconception. Using Langevin dynamics, we simulate SMNP pairs and the dimer clusters they form. To quantify the tendency to aggregate, we introduce the dimer debonding time and calculate the average magnetic force of attraction which results from correlations in the fluctuating moments─a magnetic analogue of the van der Waals interaction. We find that the magnetocrystalline anisotropy, which determines the rate of superparamagnetic reversals, has no influence on debonding time, and comparing with computed Néel relaxation times this holds for both blocked and superparamagnetic particles. Hence superparamagnetism does not affect aggregation, which explains the success of previous simplified models in describing the equilibrium structure of SMNP systems. Because the key dimensionless parameter for the Néel relaxation of a lone SMNP and the one for magnetic attraction have the same size and temperature scaling, there is a strong correlation with colloidal stability, as observed experimentally, but no causal relation.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"15 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2026-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146146484","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}
Pub Date : 2026-02-10DOI: 10.1021/acs.jpcc.5c08288
Xinyi Wang, Ying Li, Kailun Zhang, Lukai Wang, Lei Zhang, Jinhua Ye, Xuan Liu, Xuanping Tan, Jingfang Sun, Huaping Mao
The formation of NH4HSO4 is a key factor in sulfur-induced catalyst deactivation in NH3 selective catalytic reduction with NOx (NH3-SCR). This study investigates the effects of interactions between NH4HSO4 and CeO2 under high-temperature conditions on the catalytic performance of CeO2/SiO2 by systematically modulating the NH4HSO4 loading. Physicochemical characterization indicates that low loadings predominantly produce surface sulfate species, enabling the catalyst to sustain over 90% NOx conversion efficiency between 250 and 450 °C. In contrast, excessive NH4HSO4 loading beyond 1.0 mmol·g–1 triggers bulk sulfate formation, resulting in progressive activity decline and complete deactivation at 2.5 mmol·g–1. In situ diffuse reflectance infrared Fourier transform spectroscopy analysis demonstrates that the sulfated CeO2/SiO2 catalyst initially follows the Eley–Rideal mechanism, while excessive sulfation induces NH3 overadsorption on catalytic sites, thereby suppressing this pathway. These results elucidate high-temperature sulfur poisoning mechanisms and offer guidelines for the design of robust CeO2-based catalysts.
{"title":"NH4HSO4 Loading-Dependent NH3-Selective Catalytic Reduction Performance of a CeO2/SiO2 Catalyst via High-Temperature Calcination","authors":"Xinyi Wang, Ying Li, Kailun Zhang, Lukai Wang, Lei Zhang, Jinhua Ye, Xuan Liu, Xuanping Tan, Jingfang Sun, Huaping Mao","doi":"10.1021/acs.jpcc.5c08288","DOIUrl":"https://doi.org/10.1021/acs.jpcc.5c08288","url":null,"abstract":"The formation of NH<sub>4</sub>HSO<sub>4</sub> is a key factor in sulfur-induced catalyst deactivation in NH<sub>3</sub> selective catalytic reduction with NO<sub><i>x</i></sub> (NH<sub>3</sub>-SCR). This study investigates the effects of interactions between NH<sub>4</sub>HSO<sub>4</sub> and CeO<sub>2</sub> under high-temperature conditions on the catalytic performance of CeO<sub>2</sub>/SiO<sub>2</sub> by systematically modulating the NH<sub>4</sub>HSO<sub>4</sub> loading. Physicochemical characterization indicates that low loadings predominantly produce surface sulfate species, enabling the catalyst to sustain over 90% NO<sub><i>x</i></sub> conversion efficiency between 250 and 450 °C. In contrast, excessive NH<sub>4</sub>HSO<sub>4</sub> loading beyond 1.0 mmol·g<sup>–1</sup> triggers bulk sulfate formation, resulting in progressive activity decline and complete deactivation at 2.5 mmol·g<sup>–1</sup>. In situ diffuse reflectance infrared Fourier transform spectroscopy analysis demonstrates that the sulfated CeO<sub>2</sub>/SiO<sub>2</sub> catalyst initially follows the Eley–Rideal mechanism, while excessive sulfation induces NH<sub>3</sub> overadsorption on catalytic sites, thereby suppressing this pathway. These results elucidate high-temperature sulfur poisoning mechanisms and offer guidelines for the design of robust CeO<sub>2</sub>-based catalysts.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"46 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2026-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146146483","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}
Pub Date : 2026-02-10DOI: 10.1021/acs.jpclett.5c03993
Noah Garrett, Michael Rose, David A. Mazziotti
Hybrid quantum-classical algorithms have begun to leverage quantum devices to efficiently represent many-electron wave functions, enabling early demonstrations of molecular simulations on real hardware. A key prerequisite for scalable quantum chemistry, however, is size consistency: the energy of non-interacting subsystems must scale linearly with system size. While many algorithms are theoretically size-consistent, noise on quantum devices may couple nominally independent subsystems and degrade this fundamental property. Here, we systematically evaluate size consistency on quantum hardware by simulating systems composed of increasing numbers of non-interacting H2 molecules using optimally shallow unitary circuits. We find that molecular energies remain size-consistent within chemical accuracy for an estimated 118 and 71 H2 subsystems for one- and two-qubit unitary designs, respectively, demonstrating that current quantum devices preserve size consistency over chemically relevant system sizes and supporting the feasibility of scalable, noise-resilient simulation of strongly correlated molecules and materials.
{"title":"Size-Consistent Quantum Chemistry on Quantum Computers","authors":"Noah Garrett, Michael Rose, David A. Mazziotti","doi":"10.1021/acs.jpclett.5c03993","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c03993","url":null,"abstract":"Hybrid quantum-classical algorithms have begun to leverage quantum devices to efficiently represent many-electron wave functions, enabling early demonstrations of molecular simulations on real hardware. A key prerequisite for scalable quantum chemistry, however, is size consistency: the energy of non-interacting subsystems must scale linearly with system size. While many algorithms are theoretically size-consistent, noise on quantum devices may couple nominally independent subsystems and degrade this fundamental property. Here, we systematically evaluate size consistency on quantum hardware by simulating systems composed of increasing numbers of non-interacting H<sub>2</sub> molecules using optimally shallow unitary circuits. We find that molecular energies remain size-consistent within chemical accuracy for an estimated 118 and 71 H<sub>2</sub> subsystems for one- and two-qubit unitary designs, respectively, demonstrating that current quantum devices preserve size consistency over chemically relevant system sizes and supporting the feasibility of scalable, noise-resilient simulation of strongly correlated molecules and materials.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"387 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2026-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146146447","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}
Jacky Lim, Julia B. DiSapio, Stewart K. Richardson, Amy R. Howell
A one-pot preparation of highly functionalized furans from two readily accessible starting materials, 2-methyleneoxetanes (or 2-alkylideneoxetanes) and α-diazoketones, is reported. The mild, convergent process takes advantage of transition-metal-mediated cyclopropanation/rearrangement (CP/RA), followed by elimination, to give controlled furan functionalization.
{"title":"Convergent Synthesis of Highly Functionalized Furans","authors":"Jacky Lim, Julia B. DiSapio, Stewart K. Richardson, Amy R. Howell","doi":"10.1021/acs.joc.5c02670","DOIUrl":"https://doi.org/10.1021/acs.joc.5c02670","url":null,"abstract":"A one-pot preparation of highly functionalized furans from two readily accessible starting materials, 2-methyleneoxetanes (or 2-alkylideneoxetanes) and α-diazoketones, is reported. The mild, convergent process takes advantage of transition-metal-mediated cyclopropanation/rearrangement (CP/RA), followed by elimination, to give controlled furan functionalization.","PeriodicalId":57,"journal":{"name":"Journal of Organic Chemistry","volume":"315 1","pages":""},"PeriodicalIF":4.354,"publicationDate":"2026-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146146332","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}
Min Lin, Zi-Xin Ye, Fei-Fei Zou, Cheng Liang, Si-Qi Xiong, Qing-Hua Li, Tang-Lin Liu
Copper powder-catalyzed α-alkynylation of secondary alcohols via an isodesmic reaction was established. The synergistic interaction between copper powder and 1,10-phenanthroline was identified as the pivotal factor in significantly boosting the activity of the reaction. This α-alkynylation of secondary alcohols provides a step-economic procedure for preparing CF3-substituted propargylic alcohols. This reaction proceeds under open-air conditions, exhibiting a broad substrate scope and excellent compatibility with the late-stage modification of bioactive molecules.
{"title":"Copper Powder-Catalyzed α-Alkynylation of Secondary Alcohols via Isodesmic Reaction","authors":"Min Lin, Zi-Xin Ye, Fei-Fei Zou, Cheng Liang, Si-Qi Xiong, Qing-Hua Li, Tang-Lin Liu","doi":"10.1021/acs.joc.5c02835","DOIUrl":"https://doi.org/10.1021/acs.joc.5c02835","url":null,"abstract":"Copper powder-catalyzed α-alkynylation of secondary alcohols via an isodesmic reaction was established. The synergistic interaction between copper powder and 1,10-phenanthroline was identified as the pivotal factor in significantly boosting the activity of the reaction. This α-alkynylation of secondary alcohols provides a step-economic procedure for preparing CF<sub>3</sub>-substituted propargylic alcohols. This reaction proceeds under open-air conditions, exhibiting a broad substrate scope and excellent compatibility with the late-stage modification of bioactive molecules.","PeriodicalId":57,"journal":{"name":"Journal of Organic Chemistry","volume":"53 1","pages":""},"PeriodicalIF":4.354,"publicationDate":"2026-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146146334","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}
Urban environments are shaped by intricate interactions among water, soil, air, and infrastructure, where traditional models often fail to capture nonlinear, non-Euclidean dynamics. Spatiotemporal graph learning (STGL) has emerged as a powerful framework to represent such complexity, enabling accurate forecasting and real-time decision support from urban districts to national and even global scales. This review provides the first comprehensive synthesis of STGL tailored to urban environments. We summarize advances in graph construction, spatial and temporal modeling, and fusion strategies, and examine applications across urban water systems, soil and agriculture, air quality, and urban risk. Landmark case studies, including Microsoft’s Aurora, NVIDIA’s Earth-2, and Google’s GraphCast/GenCast, demonstrate STGL’s potential as a foundation model for environmental intelligence. We conclude by identifying key limitations and outlining future directions, emphasizing federated learning, machine unlearning, and meta-learning to enhance next-generation STGL frameworks that ultimately support resilient and adaptive urban environments.
{"title":"Spatiotemporal Graph Learning on Urban Environments","authors":"Hewen Li, Linlin Hou, Jing Cui, Yuqi Wang, Yu Tao, Hongcheng Wang, Dragan Savic, Aijie Wang, Nanqi Ren","doi":"10.1021/acs.est.5c12640","DOIUrl":"https://doi.org/10.1021/acs.est.5c12640","url":null,"abstract":"Urban environments are shaped by intricate interactions among water, soil, air, and infrastructure, where traditional models often fail to capture nonlinear, non-Euclidean dynamics. Spatiotemporal graph learning (STGL) has emerged as a powerful framework to represent such complexity, enabling accurate forecasting and real-time decision support from urban districts to national and even global scales. This review provides the first comprehensive synthesis of STGL tailored to urban environments. We summarize advances in graph construction, spatial and temporal modeling, and fusion strategies, and examine applications across urban water systems, soil and agriculture, air quality, and urban risk. Landmark case studies, including Microsoft’s Aurora, NVIDIA’s Earth-2, and Google’s GraphCast/GenCast, demonstrate STGL’s potential as a foundation model for environmental intelligence. We conclude by identifying key limitations and outlining future directions, emphasizing federated learning, machine unlearning, and meta-learning to enhance next-generation STGL frameworks that ultimately support resilient and adaptive urban environments.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"60 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2026-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146146394","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}
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