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Ionic–Covalent Bond-Mediated Electron-Rich Lattice Oxygen for Solar-Driven Acetic Acid Abatement 离子共价键介导的富电子点阵氧用于太阳能驱动的醋酸减排
IF 12.2 1区 环境科学与生态学
环境科学与技术 Pub Date : 2026-10-20 Epub Date: 2026-09-07 DOI: 10.1021/acs.est.6c07573
Tongzhou Xu, Zhixin Hu, Bosheng Chen, Ang Gao, Zhenguo Wang, Biluan Zhang, Lei Miao, Jinlong Wang, Yanbing Guo
{"title":"Ionic–Covalent Bond-Mediated Electron-Rich Lattice Oxygen for Solar-Driven Acetic Acid Abatement","authors":"Tongzhou Xu,&nbsp;Zhixin Hu,&nbsp;Bosheng Chen,&nbsp;Ang Gao,&nbsp;Zhenguo Wang,&nbsp;Biluan Zhang,&nbsp;Lei Miao,&nbsp;Jinlong Wang,&nbsp;Yanbing Guo","doi":"10.1021/acs.est.6c07573","DOIUrl":"https://doi.org/10.1021/acs.est.6c07573","url":null,"abstract":"<p>Domestic waste generates volatile fatty acids (VFAs)and emitsstrong malodors that reduce environmental comfort. The generationof these odor-causing molecules usually occurs in relatively high-humidityconditions, which speed up the deterioration of adsorbents, creatingsecondary waste from frequent replacement. Herein, we report a lithium-dopedmanganese dioxide (Li–MnO<sub>2</sub>) photothermal systemthat sustainably degrades acetic acid (CH<sub>3</sub>COOH, a key VFA).Mechanistic studies reveal the ionic bond in Li–O localizeselectrons at the oxygen atom, while the covalent bond in Mn–Oestablishes an efficient electron transport channel. This electron-richoxygen can cleave the O–H bond in H<sub>2</sub>O with an ultra-lowenergy barrier of 0.01 eV, generating dihydroxy groups, which subsequentlyinitiate a nucleophilic attack on the O–H and C–H bondsin CH<sub>3</sub>COOH molecules. The introduction of light not onlyefficiently converts the material surface into thermal energy, butit also triggers electron rearrangement. The engineered Li–MnO<sub>2</sub> catalyst demonstrates complete CH<sub>3</sub>COOH degradationat 291 mW cm<sup>–2</sup>. A modular photothermal purificationdevice demonstrates above 1000 h odor removal efficiency in municipalwaste scenario. We anticipate this work will enable perpetual CH<sub>3</sub>COOH removal from domestic waste without external energy input,offering a sustainable solution for odor control in waste management.</p>","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"60 41","pages":"29640–29650"},"PeriodicalIF":12.2,"publicationDate":"2026-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149218999","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}
引用次数: 0
Three Distinct Binding Modes Govern High-Affinity Ligand Interactions with Amyloid Fibrils 三种不同的结合模式支配着高亲和力配体与淀粉样蛋白原纤维的相互作用
IF 2.7 3区 生物学
Biochemistry Biochemistry Pub Date : 2026-10-20 Epub Date: 2026-10-02 DOI: 10.1021/acs.biochem.6c00489
Timothy S. Chisholm
{"title":"Three Distinct Binding Modes Govern High-Affinity Ligand Interactions with Amyloid Fibrils","authors":"Timothy S. Chisholm","doi":"10.1021/acs.biochem.6c00489","DOIUrl":"https://doi.org/10.1021/acs.biochem.6c00489","url":null,"abstract":"<p>Fibrillar proteinaggregates are a defining feature of neurodegenerativediseases and represent attractive biomarkers and therapeutic targets.However, the rational design of small-molecule ligands and probestargeting these aggregates is limited by a poor understanding of howligands bind to amyloid fibrils. This work outlines an experimentalapproach to determine the binding mode of ligands to amyloid fibrilsusing previously overlooked information contained within standardbinding assays. Using a mathematical framework to analyze bindingbehavior, three distinct high-affinity binding modes were identified:discrete, overlapping, and interacting binding. Reanalysis of publishedbinding data indicates that these binding modes are widespread amongcommon amyloid-binding ligand scaffolds. Two ligands were designedusingprinciples informed by these binding modes, yielding improved bindingaffinities and characteristic fluorescence responses. These findingsestablish a practical framework for determining how small moleculesbind amyloid fibrils using straightforward binding assays and forguiding the design of future fibril-binding ligands and probes.</p>","PeriodicalId":28,"journal":{"name":"Biochemistry Biochemistry","volume":"65 20","pages":"3299–3309"},"PeriodicalIF":2.7,"publicationDate":"2026-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149219000","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}
引用次数: 0
A Bistable UV-Sensitive Opsin from a Reef Building Coral Showing a Switchable and Tunable Regulation of Gs-Signaling by Different Wavelengths of Light 一种来自礁石珊瑚的双稳态紫外线敏感视蛋白显示出不同波长光对gs信号的可切换和可调调节
IF 2.7 3区 生物学
Biochemistry Biochemistry Pub Date : 2026-10-20 Epub Date: 2026-10-07 DOI: 10.1021/acs.biochem.6c00520
Yusuke Sakai, Akinari Sakayori, Tomoki Kawaguchi, Kento Takano, Keiji Iwashita, Keita Sato, Keiichi Kojima, Hideyo Ohuchi, Hisao Tsukamoto
{"title":"A Bistable UV-Sensitive Opsin from a Reef Building Coral Showing a Switchable and Tunable Regulation of Gs-Signaling by Different Wavelengths of Light","authors":"Yusuke Sakai,&nbsp;Akinari Sakayori,&nbsp;Tomoki Kawaguchi,&nbsp;Kento Takano,&nbsp;Keiji Iwashita,&nbsp;Keita Sato,&nbsp;Keiichi Kojima,&nbsp;Hideyo Ohuchi,&nbsp;Hisao Tsukamoto","doi":"10.1021/acs.biochem.6c00520","DOIUrl":"https://doi.org/10.1021/acs.biochem.6c00520","url":null,"abstract":"<p>Cnidarians possess a large number of opsins in theirgenomes fortheir various photoreceptive functions. In particular, they uniquelypossess Gs-coupled opsins that induce intracellular cAMP accumulationin a light-dependent manner. These Gs-coupled opsins, cnidopsins,are powerful optogenetic tools that manipulate cAMP-dependent cellularresponses. In this study, we characterized a cnidopsin, named AtCnidop3a,from the coral <em>Acropora tenuis</em> as aGs-coupled and UV-sensitive bistable pigment. This cnidopsin showeda large spectral shift upon activation from absorption maxima from395 to 560 nm, and the resting and activated states are interconvertibleby illumination with UV (or violet) and orange light. The activatedstate efficiently activates Gs proteins and elevates intracellularcAMP levels in mammalian cultured cells. To engineer an opsin mutantthat can be turned on and off upon long-wavelength light illuminationby utilizing the large spectral separation, negatively charged aminoacids were introduced near the retinal Schiff base region. Among thetested opsin mutants, the Y113<sup>3.28</sup>E mutant is capable ofbeing activated by green light unlike the wild-type while retainingthe property of being inactivated by orange light like the wild-type,indicating successful conversion of the opsin to a visible-light-sensitivebistable pigment. The visible-light-induced cAMP regulation of theY113<sup>3.28</sup>E mutant was enhanced by an additional L94<sup>2.61</sup>G substitution. Our characterization and engineering ofthe cnidopsin revealed the functional diversity of cnidarian opsinsand their potential utility as optogenetic tools regulating Gs-dependentphysiological responses.</p>","PeriodicalId":28,"journal":{"name":"Biochemistry Biochemistry","volume":"65 20","pages":"3183–3195"},"PeriodicalIF":2.7,"publicationDate":"2026-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149219023","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}
引用次数: 0
Dual Oxidation in the Amino Acid-Mediated Copper-Catalyzed Fenton-like System: Effects of Ligand Structure and pH-Dependent Speciation 氨基酸介导的铜催化类芬顿体系的双重氧化:配体结构和ph依赖性物种形成的影响
IF 9.028 1区 环境科学与生态学
环境科学与技术 Pub Date : 2026-10-20 DOI: 10.1021/acs.est.6c10258
Erwin Jongwoo Park,Soosan Park,Hye Kyung Nam,Junghun Lee,Jiyoon Cho,Hyunsoo Yoon,Min Sik Kim,Changha Lee
{"title":"Dual Oxidation in the Amino Acid-Mediated Copper-Catalyzed Fenton-like System: Effects of Ligand Structure and pH-Dependent Speciation","authors":"Erwin Jongwoo Park,Soosan Park,Hye Kyung Nam,Junghun Lee,Jiyoon Cho,Hyunsoo Yoon,Min Sik Kim,Changha Lee","doi":"10.1021/acs.est.6c10258","DOIUrl":"https://doi.org/10.1021/acs.est.6c10258","url":null,"abstract":"The Cu(II)/H2O2 system has attracted increasing interest as a Cu-catalyzed advanced oxidation process and serves as a useful biomimetic model for investigating Cu-mediated biomolecule redox interactions. In this system, reactive oxidants can operate in a dual-oxidation mode, where the oxidant flux partitions between coordinated ligands and coexisting bulk-phase substrates. In this study, we systematically investigated this behavior over a wide pH range (3–12), using 17 structurally diverse amino acids (AAs) as model ligands and benzoic acid (BA), which exhibits negligible Cu(II) complexation, as a model bulk-phase substrate. Speciation-based kinetic analysis identified the bis-chelated complex, [Cu(AA)2], as a key catalytic species associated with effective dual oxidation, namely, balanced oxidant allocation between ligand-centered AA oxidation and bulk-phase BA oxidation, at pH 7–10. Using quantitative structure–activity/efficiency relationships, we demonstrate that the partitioning of oxidant flux is governed by two ligand-associated properties: (i) Cu(II)-binding strength, which promotes ligand-centered oxidation, and (ii) oxidative stability (proxied by the highest occupied molecular orbital (HOMO)–lowest unoccupied molecular orbital (LUMO) gap), which favors the oxidant flux to the bulk phase. At higher pH, the possible formation of mixed hydroxo species, [Cu(AA)2(OH)]−, was associated with a shift toward ligand-centered oxidation and attenuated bulk-phase BA oxidation. Integrated machine-learning models combining ligand descriptors with pH-dependent speciation indicators further supported these trends and predicted AA and BA oxidation kinetics across pH 7–11. These results provide a predictive framework for understanding how ligand structure and pH-dependent speciation jointly control oxidant allocation in the Cu(II)/H2O2 system.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"108 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2026-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149221684","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}
引用次数: 0
Effects of an Electric Field on Hydroxide Diffusion in Aqueous Anion Exchange Membranes 电场对氢氧化物在阴离子交换膜中扩散的影响
IF 4.126 3区 化学
The Journal of Physical Chemistry C Pub Date : 2026-10-20 DOI: 10.1021/acs.jpcc.6c01812
Wenli Bao,Weiwei Zhang,Gui-Rong Zhang,Junfeng Rong,Qiugen Zhang,Donghai Mei
{"title":"Effects of an Electric Field on Hydroxide Diffusion in Aqueous Anion Exchange Membranes","authors":"Wenli Bao,Weiwei Zhang,Gui-Rong Zhang,Junfeng Rong,Qiugen Zhang,Donghai Mei","doi":"10.1021/acs.jpcc.6c01812","DOIUrl":"https://doi.org/10.1021/acs.jpcc.6c01812","url":null,"abstract":"Anion exchange membrane (AEM)-based water electrolysis represents a promising pathway for sustainable hydrogen production, leveraging nonprecious metal catalysts. A comprehensive understanding of hydroxide ion (OH–) transport mechanisms within AEMs is crucial to achieving high-performance electrolysis. However, the influence of an electric field on OH– diffusion in aqueous AEMs remains inadequately explored. This study employs reactive force field (ReaxFF) molecular dynamics (MD) simulations to investigate OH– diffusion through four distinct mechanisms: Free-Vehicular, Free-Grotthuss, Associate-Vehicular, and Associate-Grotthuss. Three poly(biphenyl alkylene) (PBPA) AEMs with varying hydration levels and hydrophilicity were analyzed under conditions with and without an applied electric field. Results indicate that the Associate-Grotthuss mechanism predominantly governs OH– diffusion across all three AEMs. Higher hydration levels enhance OH– diffusion rates, while the application of an electric field significantly increases the total diffusion coefficient of OH–. Microstructural analysis further reveals that AEMs with higher hydration levels and greater hydrophilicity promote OH– diffusion by preserving water channel continuity and pore width. Additionally, the electric field improves the orientation order of water molecules, further facilitating OH– transport. These findings provide valuable insights into the enhancement of hydroxide ion diffusion via applied electric fields and offer theoretical guidance for designing high-conductivity AEMs to advance water electrolysis technology.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"33 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2026-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149221726","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}
引用次数: 0
Ligand Binding Remodels the Oligomeric State and Active Site of Klebsiella pneumoniae Azoreductase 配体结合重塑肺炎克雷伯菌偶氮还原酶的低聚态和活性位点
IF 2.7 3区 生物学
Biochemistry Biochemistry Pub Date : 2026-10-20 Epub Date: 2026-10-07 DOI: 10.1021/acs.biochem.6c00568
Reese Hitchings, Agnidipta Ghosh, Arthur J. Arcinas, Steven C. Almo, Libusha Kelly, Ali Ryan
{"title":"Ligand Binding Remodels the Oligomeric State and Active Site of Klebsiella pneumoniae Azoreductase","authors":"Reese Hitchings,&nbsp;Agnidipta Ghosh,&nbsp;Arthur J. Arcinas,&nbsp;Steven C. Almo,&nbsp;Libusha Kelly,&nbsp;Ali Ryan","doi":"10.1021/acs.biochem.6c00568","DOIUrl":"https://doi.org/10.1021/acs.biochem.6c00568","url":null,"abstract":"<p>Azo dyes are widespread in the environment, and humansingest arange of these dyes present in food and drugs. The human gut microbiomesignificantly impacts the fate of ingested azo dyes primarily throughthe reduction of the azo bond (R–N = N–R′). Flavin-dependentazoreductases have been considered the key enzymatic drivers of thisprocess. To challenge this paradigm, we constructed a sequence similaritynetwork of known azoreductases and focused on AzoA of <em>Klebsiella pneumoniae</em>, a central representative withinthe gut microbiome cluster. Unexpectedly, <em>K. pneumoniae</em> AzoA displayed relatively low <em>in vitro</em> activityagainst a range of azo compounds. While the physiological implicationsremain unclear, these findings are consistent with the possibilitythat nonenzymatic mechanisms contribute substantially to azo compoundreduction in the gut. Furthermore, structural characterization ofAzoA, as a holoenzyme and in its ligand-bound state, revealed a previouslyunrecognized ligand-coupled mechanism involving remodeling of theactive site and oligomeric state.</p>","PeriodicalId":28,"journal":{"name":"Biochemistry Biochemistry","volume":"65 20","pages":"3236–3246"},"PeriodicalIF":2.7,"publicationDate":"2026-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149218975","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}
引用次数: 0
Discovery and Modulation of an Unusual Terminal Mismatch Bypass Activity Involving 3′-Phosphorothioated Primers and Commercial Strand Displacement DNA Polymerases 涉及3 ' -磷酸化引物和商业链置换DNA聚合酶的不寻常末端错配旁路活性的发现和调节
IF 2.7 3区 生物学
Biochemistry Biochemistry Pub Date : 2026-10-20 Epub Date: 2026-10-08 DOI: 10.1021/acs.biochem.6c00108
Shrawan Kumar, Hira Singh Gariya, Chandrika Sharma, Saba Parveen, Vandana K Nair, Mrittika Sengupta, Chitra Gurnani, Souradyuti Ghosh
{"title":"Discovery and Modulation of an Unusual Terminal Mismatch Bypass Activity Involving 3′-Phosphorothioated Primers and Commercial Strand Displacement DNA Polymerases","authors":"Shrawan Kumar,&nbsp;Hira Singh Gariya,&nbsp;Chandrika Sharma,&nbsp;Saba Parveen,&nbsp;Vandana K Nair,&nbsp;Mrittika Sengupta,&nbsp;Chitra Gurnani,&nbsp;Souradyuti Ghosh","doi":"10.1021/acs.biochem.6c00108","DOIUrl":"https://doi.org/10.1021/acs.biochem.6c00108","url":null,"abstract":"<p>Phosphorothioated (PST) oligonucleotides are extensivelyused inRNA therapeutics and biosensing applications. PST-modified linkagesremain part of 13 approved oligonucleotide drug backbones (out of23 total approved drugs). Despite the widespread utilization of PSTlinkages in oligonucleotide therapeutics, the full spectrum of theirinteractions with nontarget nucleic acids and DNA polymerases remainsinadequately characterized. In this study, we report a novel discoveryand the modalities (sequence dependence and length) of an unusual3′-mismatch bypass activity involving 3′-PST primers,circular DNA (CD) template, and strand displacement DNA polymerases.We demonstrate that this activity persists for at least 24 nt of mismatch,is sequence-independent, and occurs when processed by three majorcommercially available strand displacement DNA polymerases commonlyused in molecular diagnostics (phi29, BST large fragment (LF), BSUlarge fragment (LF)) with operational conditions spanning a largetemperature range and buffer conditions. The 3′-terminal mismatchbypass activity of these three polymerases additionally extended totherapeutically relevant modifications such as locked nucleic acid(LNA) and 2′-<em>O</em>-methyl (2′-OMe). Wealso found that this mismatch bypass activity could be regulated byoligonucleotides complementary to the mismatch region. The significanceof this study lies not only in the discovery and analytical investigationof the novel observation but also in its ramifications for biosensingand the nonspecific interactions of PST oligonucleotides in RNA therapeutics.</p>","PeriodicalId":28,"journal":{"name":"Biochemistry Biochemistry","volume":"65 20","pages":"3151–3166"},"PeriodicalIF":2.7,"publicationDate":"2026-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149218977","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}
引用次数: 0
Acid-Mediated [3 + 3] or [3 + 2 + 1] Cyclization between Enaminones and 6-Aminouracils to Access 2-Substituted Pyridine Derivatives or 3-Acyl-Substituted Pyrido[2,3-d]pyrimidine-2,4-diones 酸介导的胺酮和6-氨基嘧啶之间的[3 + 3]或[3 + 2 + 1]环化以获得2-取代吡啶衍生物或3-酰基取代吡啶[2,3-d]嘧啶-2,4-二酮
IF 4.354 2区 化学
Journal of Organic Chemistry Pub Date : 2026-10-20 DOI: 10.1021/acs.joc.6c01981
Wenhui Xie,Hui Liang,Zhiyong Zhu,Changyuan Zhang,Leiqing Fu,Jie-Ping Wan
{"title":"Acid-Mediated [3 + 3] or [3 + 2 + 1] Cyclization between Enaminones and 6-Aminouracils to Access 2-Substituted Pyridine Derivatives or 3-Acyl-Substituted Pyrido[2,3-d]pyrimidine-2,4-diones","authors":"Wenhui Xie,Hui Liang,Zhiyong Zhu,Changyuan Zhang,Leiqing Fu,Jie-Ping Wan","doi":"10.1021/acs.joc.6c01981","DOIUrl":"https://doi.org/10.1021/acs.joc.6c01981","url":null,"abstract":"The acid-mediated cyclization reactions of enaminones with6-aminouracils are developed. At room temperature, 2-substituted pyridinederivatives are obtained in 59–75% yields via [3 + 3] cyclization mediated bythe mixed acids FeCl3 and H2C2O4 in equimolar amounts. In addition, thereaction takes place by using FeCl3 and TBHP via a [3 + 2 + 1] cyclization tosynthesize 3-acyl-substituted pyrido[2,3-d]pyrimidine-2,4-diones. Thisprotocol showcases the unique dual reactivity of enaminones, which act notonly as reaction partners but also as one-carbon (C1) building blocks via C–C bond cleavage and C═C bond cleavage. Thismethod features easily accessible starting materials, mild divergent reaction conditions, and high synthetic efficiency. Based oncontrol experiments and previous reports, we have also proposed a plausible mechanism for this reaction.","PeriodicalId":57,"journal":{"name":"Journal of Organic Chemistry","volume":"94 1","pages":""},"PeriodicalIF":4.354,"publicationDate":"2026-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149218917","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}
引用次数: 0
Behavior-Based Thresholds Support Screening-Level Prioritization of Caffeine as a Neuroactive Wastewater Micropollutant in Coastal Waters 基于行为的阈值支持咖啡因作为沿海水域神经活性废水微污染物的筛选水平优先级
IF 12.2 1区 环境科学与生态学
环境科学与技术 Pub Date : 2026-10-20 Epub Date: 2026-10-07 DOI: 10.1021/acs.est.6c10032
Zhen Lu, Zhi Yan, Bin Liu, Jiao Wang, Yaxi Li, Ke Li
{"title":"Behavior-Based Thresholds Support Screening-Level Prioritization of Caffeine as a Neuroactive Wastewater Micropollutant in Coastal Waters","authors":"Zhen Lu,&nbsp;Zhi Yan,&nbsp;Bin Liu,&nbsp;Jiao Wang,&nbsp;Yaxi Li,&nbsp;Ke Li","doi":"10.1021/acs.est.6c10032","DOIUrl":"10.1021/acs.est.6c10032","url":null,"abstract":"<p>Sensitive functional end points revealearly responses to neuroactivewastewater contaminants but are rarely translated into screening thresholds.Using caffeine as a sentinel, we evaluated a behavior-based frameworkfor coastal waters. Systematic searches of Web of Science Core Collection,PubMed, and Embase through 24 August 2026 identified 66 eligible studiesand 2181 effect sizes for meta-analysis. The near-zero grand pooledsigned ln <em>RR</em> may reflect cancellation amongend points with opposing response directions. Responses varied bylife stage, exposure duration, concentration, and end point category.Standardized light–dark assays across eight aquatic speciesrevealed taxon- and context-dependent behavioral disruptions, includingresponses at low concentration and non-monotonic patterns. Speciessensitivity distributions based on behavioral benchmark concentrationsyielded a conservative hazardous concentration affecting 5% of species(HC5; 0.0585 μg L<sup>–1</sup>) and a screening-levelbehavior-based predicted no-effect concentration (PNEC; 0.0195 μgL<sup>–1</sup>). A separate systematic literature search, supplementedwith NORMAN EMPODAT records, compiled 1421 quantifiable caffeine measurementsin coastal and estuarine waters. Concentrations were right-skewed(median, 44.9 ng L<sup>–1</sup>; IQR, 14.60–190.00 ngL<sup>–1</sup>), and 69.88% of measurements fell into the high-priorityrisk quotient category (RQ ≥ 1). These findings support behavior-basedthresholds for prioritizing neuroactive wastewater pollution in coastalwaters.</p>","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"60 41","pages":"29342–29354"},"PeriodicalIF":12.2,"publicationDate":"2026-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149091567","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}
引用次数: 0
Inhalation of Environmentally Simulated PET Nanoplastics Induces Demyelinating Disorders via the CXCL12/CXCR4 Axis 环境模拟PET纳米塑料吸入通过CXCL12/CXCR4轴诱导脱髓鞘疾病
IF 12.2 1区 环境科学与生态学
环境科学与技术 Pub Date : 2026-10-20 Epub Date: 2026-10-05 DOI: 10.1021/acs.est.6c03987
Shuang Liu, Jingcun Dong, Yu Hu, Qingqing Zhu, Huiyang Fu, Jia Gao, Xueyu Weng, Ligang Hu, Chunyang Liao, Guibin Jiang
{"title":"Inhalation of Environmentally Simulated PET Nanoplastics Induces Demyelinating Disorders via the CXCL12/CXCR4 Axis","authors":"Shuang Liu,&nbsp;Jingcun Dong,&nbsp;Yu Hu,&nbsp;Qingqing Zhu,&nbsp;Huiyang Fu,&nbsp;Jia Gao,&nbsp;Xueyu Weng,&nbsp;Ligang Hu,&nbsp;Chunyang Liao,&nbsp;Guibin Jiang","doi":"10.1021/acs.est.6c03987","DOIUrl":"10.1021/acs.est.6c03987","url":null,"abstract":"<p>Thehealth threat from airborne nanoplastics (NPs) remains unclear,as despite inhalation being a more direct brain entry route thaningestion, current understanding relies on oral exposure and commercialparticle models that obscure realistic risks. Here, by integratingenvironmentally simulated polyethylene terephthalate (PET)-NPs withan aerosol inhalation model that mirrors real-world human exposure(0.1, 1, and 10 mg/m<sup>3</sup>), we demonstrate that chronic NPinhalation translocated to the brain and induced demyelination, neuroinflammation,and cognitive deficits. The most pronounced effects were observedat the highest exposure dose (10 mg/m<sup>3</sup>), which is relevantto the occupational settings. Mechanistically, NP exposure triggeredastrocytic CXCL12 release, leading to CXCR4-dependent microglial activationand cytokine network dysregulation. <em>In vitro</em>, blockadeof CXCR4 with AMD3100 attenuated NP-induced microglial migration andoligodendrocytic myelin basic protein reduction. Our study thus definitivelylinks realistic airborne NP exposure to the key neuropathologicalfeatures of demyelinating disorders and pinpoints a modifiable molecularpathway that could inform exposure-based preventive strategies. Thesefindings underscore the need for further assessment of airborne NPrisks, particularly in occupational settings.</p>","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"60 41","pages":"29285–29298"},"PeriodicalIF":12.2,"publicationDate":"2026-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149091989","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}
引用次数: 0
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