化学•材料最新文献

{"title":"The Active Component of Dehydrophos Covalently Binds to Acetohydroxyacid Synthase and Inhibits the Growth of Uropathogenic Escherichia coli","authors":"Xin Lin,&nbsp;Sharon Chow,&nbsp;Paul Malek Mirzayans,&nbsp;Jiahui Tng,&nbsp;Gerhard Schenk,&nbsp;Craig M. Williams,&nbsp;Luke W. Guddat","doi":"10.1021/acs.biochem.6c00555","DOIUrl":"https://doi.org/10.1021/acs.biochem.6c00555","url":null,"abstract":"<p>Acetohydroxyacid synthase (AHAS) is the first enzymein the branched-chainamino acid biosynthesis pathway and is the target for more than 50commercially deployed herbicides. This enzyme has also been suggestedas a target for the discovery of novel antimicrobial and antifungaltherapeutics. Dehydrophos, a natural product antibiotic, is a potentialnew lead inhibitor of AHASs for drug development, whereby the biologicallyactive component is proposed to be methyl acetylphosphonate (MAP).MAP has been suggested as a pyruvate analog that inhibits ThDP-dependentenzymes, including AHAS. Here, the crystal structure of <em>Saccharomyces cerevisiae</em> AHAS in complex with MAPhas been determined to 2.22 Å resolution, showing that it bindscovalently with ThDP. We have also shown that MAP alone is effectivein inhibiting the growth of uropathogenic <em>Escherichia coli</em> (UPEC) in cell susceptibility assays and thatthis activity is lost when exogenous branched-chain amino acids (BCAAs)are added. This suggests that AHAS is a target for the antibioticactivity of MAP and dehydrophos. Our crystal structure provides astarting point for the rational design of ThDP covalently bound AHASinhibitors that are also structurally different from those that havebeen developed previously as commercial herbicides that inhibit AHAS.</p>","PeriodicalId":28,"journal":{"name":"Biochemistry Biochemistry","volume":"65 20","pages":"3286–3298"},"PeriodicalIF":2.7,"publicationDate":"2026-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149218985","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":"60 Years of Biogeochemistry and Remediation Science","authors":"Paul G. Tratnyek,&nbsp;Heileen Hsu-Kim,&nbsp;Sukhwan Yoon","doi":"10.1021/acs.est.6c15296","DOIUrl":"https://doi.org/10.1021/acs.est.6c15296","url":null,"abstract":"","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"60 41","pages":"29211–29212"},"PeriodicalIF":12.2,"publicationDate":"2026-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149219010","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":"Resource-Oriented Wastewater Treatment through Quorum Quenching─Integration of AnMBR and Donnan Dialysis","authors":"Hongyu Zhang,Yuxuan Wan,Liqiu Zhang,Huarong Yu,Haiyang Yang,Fangshu Qu","doi":"10.1021/acs.est.6c05848","DOIUrl":"https://doi.org/10.1021/acs.est.6c05848","url":null,"abstract":"Aligned with United Nations Sustainable Development Goal 6, water treatment is shifting from pollution removal to resource recovery and circularity. An integration of AnMBR and a Donnan dialysis (DD) (AnMBR-DD) was proposed to simultaneously recover methane and ammonium, and quorum quenching (QQ) was further incorporated to mitigate membrane fouling and enhance process efficiency. The COD removal efficiency was stably maintained above 80%, and the methane conversion efficiency reached 51.6%. The effluent NH4+-N concentration was controlled at 3–5 mg/L, with a recovery efficiency of 47.1% in the AnMBR-DD. The QQ effectively alleviated biofouling on the ultrafiltration membrane in the AnMBR and ion exchange membrane in the DD, while improving methane production and ammonia recovery by 20.6% and 6.6%, respectively. These improvements were mainly attributed to QQ-induced reductions in extracellular polymeric substances (EPS), which weakened microbial adhesion and decreased biofilm compactness. Life cycle assessment showed that coupled methane and ammonium recovery in AnMBR-DD-QQ were the decided advantages in alleviating the environmental impact. These results highlight the great potential of AnMBR-DD-QQ as a resource-oriented wastewater treatment strategy.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"2 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2026-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149221689","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":"Molecular Evolution of Dissolved Organic Nitrogen from Photoaged Nitrogen-Containing Microplastics Reveals Amine Structures as Key Nitrosamine Precursors","authors":"Run Zhou,Jiayi Shi,Yuanren Jiang,Zhuo Gao,Fei Yang,Kecheng Zhu,Hanzhong Jia","doi":"10.1021/acs.est.6c12418","DOIUrl":"https://doi.org/10.1021/acs.est.6c12418","url":null,"abstract":"Although dissolved organic nitrogen (DON) is continuously released and transformed as nitrogen-containing microplastics (N-MPs) age, the evolution of this replenished pool and its reactivity during downstream chloramination remains unresolved. Here, we tracked the compositional evolution of DON molecules in polyamide (PA) and polyacrylonitrile (PAN) suspensions under UV irradiation using a nitrogen atom-based molecular classification strategy (N1–N5). After 7 d of irradiation-induced molecular reorganization, N1–N5 molecules accounted for 87% and 79% of the molecular signal intensity in PA-DOM and PAN-DOM, respectively. Eight annotated compounds followed increasing, decreasing, or transient accumulation trajectories, revealing simultaneous molecular accumulation and depletion. Reaction-network analysis further showed that N1–N5 molecules progressively became the dominant reactants, and these trajectories were dominated by oxidation and accompanied by increasingly frequent amine-related transformation links. Structural analysis revealed amide-rich N1–N2 and N-heterocycle-rich N3–N5 molecules, while secondary and tertiary amines occurred across all N1–N5 classes. As this molecular reorganization progressed, N-MP-DON level dropped, but substantially enhanced N-nitrosodimethylamine and N-nitrosodiethylamine formation, and potential precursor identification was strongly associated with amine structures, rather than nitrogen atom number. Overall, our study highlights N-MP-DON as a potential source of nitrosamine precursors, and the need to carefully consider amine-containing additives use in plastic manufacturing.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"16 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2026-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149221691","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":"Ebullition-Enhanced Release of Microplastics from Aquatic Sediment to Overlying Water: An Overlooked Transport Pathway","authors":"Shengdong Liu,&nbsp;Zhuoqing Zhou,&nbsp;Yang Li,&nbsp;Xinghui Xia,&nbsp;Xinjie Wang,&nbsp;Jiahe Zhang,&nbsp;Baoshan Xing,&nbsp;Shoichiro Hamamoto,&nbsp;Peng Zhang,&nbsp;Wen Zhang","doi":"10.1021/acs.est.6c06432","DOIUrl":"10.1021/acs.est.6c06432","url":null,"abstract":"<p>Microplastics(MPs) in aquatic systems are typicallyattributedto wastewater, runoff and atmospheric inputs, whereas the remobilizationof sediment-associated MPs by benthic gas ebullition remains poorlyunderstood. Here, we show that air-purged ebullition mobilized fourcommon MPs, polyethylene (PE), polyethylene terephthalate (PET), polyvinylchloride (PVC), and polylactic acid (PLA), from sediments into theoverlying water, with release ratios of 8.9%–12.1% over 9 d.Suspended MP concentrations in the overlying water increased rapidlyduring the first 48 h, followed by slower release and eventual plateauing,with the decelerating release behavior empirically described by apower-law model. Theoretical calculations suggest that aggregationwith suspended sediment can reduce the flotation velocities of MPsfrom 9.38–9.99 cm·s^–1 to 8.64–9.95cm·s^–1. Combined experimental observationsand theoretical analyses support a coupled flotation mechanism involvingMPs attachment to rising bubbles, bubble-driven flow that counteractsgravitational settling, and transient pressure gradients. These processescould convert sediments from a long-term sink into a secondary sourceof MPs during ebullition. Overall, this study identifies benthic gasebullition as an underappreciated pathway for MP remobilization andprovides a mechanistic framework for understanding the fate and transportof sediment-associated MPs in aquatic environments.</p>","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"60 41","pages":"29583–29595"},"PeriodicalIF":12.2,"publicationDate":"2026-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149091518","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":"Niche Divergence-Based Identification of Microbial Indicators Tracking Cyanobacterial Bloom Succession: A Metagenomic and Machine Learning Framework","authors":"Kaiwen Yang,&nbsp;Zhen Xie,&nbsp;Wei Li,&nbsp;Yi Ren,&nbsp;Xiao Yi Chen,&nbsp;Xinze Wang,&nbsp;Hongyan Ren,&nbsp;Shunzi Xiong,&nbsp;Xiaojun Zhang","doi":"10.1021/acs.est.6c04563","DOIUrl":"10.1021/acs.est.6c04563","url":null,"abstract":"<p>Cyanobacterial harmful algal blooms (CyanoHABs) posesignificantenvironmental and public health risks through toxin production, antibioticresistance gene dissemination, and the disruption of biogeochemicalcycles. Although extensive metagenomic investigations have exploredmicrobial interactions between <em>Cyanobacteria</em> andcoexisting members, the potential of incorporating functional indicatorsinto early CyanoHAB monitoring systems remains underexplored. In thisstudy, we employed metagenomic binning combined with machine learningapproaches to analyze seasonal cyanobacterial succession and coexistingmicrobial communities across 19 sites in Erhai Lake across four seasons.We documented distinct niche shifts driven by the spatiotemporal heterogeneityin seasonal cyanobacterial succession alongside the formation of uniqueniches triggered by this asynchrony. Specialized microbial members(SN-MAGs) were identified as candidate bioindicators associated withearly-stage cyanobacterial proliferation. Functional profiling showed <em>r/K</em> selection and metabolic adaptations in these SN-MAGs,including stress resistance and altered carbon metabolism, linkedto cyanobacterial dynamics. Machine learning models leveraging thesefeatures were constructed and retrospectively evaluated. Cross-lakevalidation using an independent Lake Taihu dataset confirmed associationsamong these features and microbial community shifts preceding <em>Microcystis</em> proliferation. Our findings highlight the potentialvalue of the dynamics of specific bacteria as a sensitive indicatorof cyanobacterial dynamics. Moreover, we propose that these identifiedfunctional markers could potentially be developed into targeted molecularassays (e.g., qPCR assays), offering possible utility in predicting <em>Microcystis</em> population expansion.</p>","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"60 41","pages":"29569–29582"},"PeriodicalIF":12.2,"publicationDate":"2026-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149091521","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":"Second-Generation Synthesis of the Male Contraceptive YCT-529","authors":"Naresh Gantasala,Narsihmulu Cheryala,Gunda I. Georg","doi":"10.1021/acs.joc.6c01804","DOIUrl":"https://doi.org/10.1021/acs.joc.6c01804","url":null,"abstract":"We report a practical synthesis of the nonhormonal male contraceptive YCT-529. The method features key transformations: Grignard-mediated acetylation, the α-methylenation of a methyl ketone, and pyrrole formation via the Stetter and Paal–Knorr reaction sequence. It avoids iridium and palladium catalysts, overcoming the major limitations of an earlier synthesis. The current scalable synthesis proceeds in 6 steps from bromochromene 4 in 51% overall yield and does not require chromatographic purification.","PeriodicalId":57,"journal":{"name":"Journal of Organic Chemistry","volume":"56 1","pages":""},"PeriodicalIF":4.354,"publicationDate":"2026-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149218922","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":"Phosphorylation by the PknB Serine/Threonine Kinase Stimulates Dimer Formation by WalR","authors":"Marina Suppi,&nbsp;Ian R. Monk,&nbsp;Liam K. R. Sharkey,&nbsp;Nichollas E. Scott,&nbsp;Dweipayan Goswami,&nbsp;Aakash Natarajan,&nbsp;Stephanie Tan,&nbsp;Katharine Myler,&nbsp;Sheila Marie Pimentel-Elardo,&nbsp;Timothy P. Stinear,&nbsp;Sacha J. Pidot,&nbsp;Justin R. Nodwell","doi":"10.1021/acs.biochem.6c00334","DOIUrl":"https://doi.org/10.1021/acs.biochem.6c00334","url":null,"abstract":"<p>WalKR is a two-component system that regulates cell wallhomeostasisand other processes in low-GC Gram-positive bacteria. It is essentialfor viability in <em>Staphylococcus aureus</em> and regulates genes that encode the autolysins and other criticalproteins. The sensor kinase WalK phosphorylates WalR at the asparticacid residue 53 (D53) in the receiver domain, stimulating promoterDNA binding. Unlike most response regulators, WalR is reported tohave a second kinase, the serine/threonine kinase PknB, which phosphorylatesthe receiver domain at the threonine residue 101. We previously reportedthat a <em>walR</em> mutation that changed T101 to a methionineconferred low-level resistance to vancomycin and greatly increasedsusceptibility to tunicamycin along with several other phenotypictraits. In this work, we demonstrate similarities between <em>pknB</em> null and the WalR_T101M mutants. A combinationof <em>in vitro</em> and <em>in vivo</em> data supportsthe idea that PknB interacts with WalR in living cells (consistentwith similar experiments in <em>Bacillus subtilis</em>) and that this likely involves phosphorylation of WalR at T101.Using <em>in silico</em> modeling, we identified a possibleintermolecular hydrogen bond between the T101 phosphate group andE108. This would have the effect of stabilizing the WalR dimerizationinterface. Consistent with this, we find that T101 is important forWalR dimer formation <em>in vivo</em>. The primary activationof WalR is clearly phosphorylation at D53 by WalK. However, our datasuggest that PknB serves as a second potentiating input stabilizingthe WalR dimer.</p>","PeriodicalId":28,"journal":{"name":"Biochemistry Biochemistry","volume":"65 20","pages":"3167–3182"},"PeriodicalIF":2.7,"publicationDate":"2026-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149218986","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":"Substrate Selectivity of Viperin Probed Using Anticancer-Related Pyrimidine Nucleotide Analogs","authors":"Minshik Jo,&nbsp;Victor Rivera-Santana,&nbsp;Hanyu Su,&nbsp;Dillon P. Langford,&nbsp;E. Neil G. Marsh","doi":"10.1021/acs.biochem.6c00226","DOIUrl":"https://doi.org/10.1021/acs.biochem.6c00226","url":null,"abstract":"<p>Many antiviral and anticancer drugs are based on thestructureof pyrimidine nucleosides. Once phosphorylated, they function by interferingwith either DNA or RNA replication or transcription. The antiviralenzyme, viperin, catalyzes the dehydration of CTP to produce 3′-deoxy-3′,4′-didehydroCTP(ddhCTP), which functions as a natural antiviral nucleotide. Variousdrugs mimic the structure of CTP, and furthermore, viperin is upregulatedin some cancers and autoimmune diseases. Therefore, we examined whethersuch drugs may be substrates for viperin. A panel of eight commerciallyavailable nucleosides, including several clinically used drugs, wereenzymatically converted to their triphosphate forms and investigatedas substrates for viperin. Five of the nucleotides were not substrates,indicating that viperin has generally high specificity for CTP. Twonucleotides, 3′-deoxy-3′-fluoroCTP and cytarabine triphosphateelicited reductive cleavage of SAM and were converted to their dehydratedproducts by viperin. The last compound, gemcitabine triphosphate,elicited reductive cleavage of SAM, but no dehydrated product wasobserved, implying that it activates SAM cleavage without undergoinghydrogen atom abstraction. The implications of these results are discussed.</p>","PeriodicalId":28,"journal":{"name":"Biochemistry Biochemistry","volume":"65 20","pages":"3217–3225"},"PeriodicalIF":2.7,"publicationDate":"2026-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149218995","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":"A Multidimensional Framework for Integrated Toxicity Assessment and Prioritization of Naphthenic Acids in Marine Medaka (Oryzias melastigma): Neurotoxicity and Mechanistic Insights","authors":"Jizhuang Chu,Shixuan Cui,Yumiao Zhou,Qiang Kong,Ying Wang,Yijing Xia,Huanxin Zhang","doi":"10.1021/acs.est.6c11718","DOIUrl":"https://doi.org/10.1021/acs.est.6c11718","url":null,"abstract":"Petroleum pollution poses a major challenge to global environmental health. Petroleum-derived naphthenic acids (NAs) are frequently detected in marine environments, yet their multidimensional toxicity and mechanisms remain poorly understood. Here, we developed an integrated toxicity framework combining bioassays, toxicity screening, computational simulations, transcriptomics, and bioinformatics to characterize NAs toxicity in marine medaka (Oryzias melastigma). A concentration gradient spanning environmentally detected levels to higher-effect concentrations (0.015–30 mg/L) revealed developmental defects, cardiac suppression, behavioral disruption, and metabolic dysfunction. CRITIC–AHP-based prioritization identified neurotoxicity as the predominant toxicity dimension, with cyclopentylpropionic acid (CPPA) and cyclohexylpropionic acid (CHPA) identified as major contributors. Mechanistically, these compounds were associated with distinct candidate pathways involving CXCR3-CXCL10 neuroinflammatory responses and DPP10-Kv4.2 ion homeostasis disruption. Their divergent toxicity profiles may be associated with differences in hydrophobicity and molecular flexibility. Rescue experiments supported these pathways, restoring swimming velocity by 60.32% and 62.09%, respectively. Furthermore, NAs induced neurobehavioral alterations and transcriptional signatures overlapping with Alzheimer’s disease-associated genes, with 14 and 12 candidate genes identified for CPPA and CHPA. Collectively, this study provides a cross-scale perspective linking physicochemical properties, toxicity pathways, and adverse outcomes of NAs, offering a conceptual approach for toxicity screening and mechanism elucidation of contaminants.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"11 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2026-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149221685","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}