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Cellular Consequences, Citrullination Substrates, and Antigenicity of Targeting PAD4 to Cell Surfaces 细胞后果,瓜氨酸化底物和靶向PAD4到细胞表面的抗原性
IF 11.1 1区 化学
ACS Central Science Pub Date : 2026-08-26 Epub Date: 2026-07-21 DOI: 10.1021/acscentsci.6c00032
Sophie Kong, Trenton M. Peters-Clarke, Corleone S. Delaveris, Paul Phojanakong, Veronica Steri, James A. Wells
{"title":"Cellular Consequences, Citrullination Substrates, and Antigenicity of Targeting PAD4 to Cell Surfaces","authors":"Sophie Kong,&nbsp;Trenton M. Peters-Clarke,&nbsp;Corleone S. Delaveris,&nbsp;Paul Phojanakong,&nbsp;Veronica Steri,&nbsp;James A. Wells","doi":"10.1021/acscentsci.6c00032","DOIUrl":"https://doi.org/10.1021/acscentsci.6c00032","url":null,"abstract":"<p>Protein arginine deiminase-4 (PAD4) catalyzes hydrolysisof arginineto citrulline in proteins that promote widespread cellular changesthat can induce innate immunity and promote cancer. Hyperactivityof PAD4 leads to a form of cell death called NETosis, releasing PAD4to the extracellular space to promote various autoimmune diseasesthrough the generation of anticitrulline protein antibodies (ACPAs).Little is known about the specific citrullinated substrates that leadto autoimmunity, but there is growing evidence that PAD4 is localizedto the cell surface in response to inflammation. Here, we characterizethe cellular consequences of exogenous PAD4, showing that it inducesmorphological changes that increase cell migration, a hallmark ofcancer. We then devised a robust proteomics approach to identify PAD4substrates. We identified ∼ 3000 citrullinated peptides from1300 proteins upon exogenous addition of PAD4 both inside and outsideof cells. This extracellular set can be further augmented by targetingPAD4 to cancer cells using a HER2 binding protein conjugate. Finally,we studied how citrullinated cells can induce a humoral response <em>in vivo</em> to produce ACPAs. We believe these studies furtherour understanding of cellular consequences of extracellular PAD4 andidentify new PAD4 substrates that are potential neoepitopes for ACPAgeneration.</p>","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"12 8","pages":"1207–1222"},"PeriodicalIF":11.1,"publicationDate":"2026-08-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148815794","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
His Start-up Wants to Mimic Human Breast Milk Using Plants 他的创业公司想用植物模仿人类的母乳
IF 11.1 1区 化学
ACS Central Science Pub Date : 2026-08-26 Epub Date: 2026-08-06 DOI: 10.1021/acscentsci.6c01284
Kristel Tjandra
{"title":"His Start-up Wants to Mimic Human Breast Milk Using Plants","authors":"Kristel Tjandra","doi":"10.1021/acscentsci.6c01284","DOIUrl":"https://doi.org/10.1021/acscentsci.6c01284","url":null,"abstract":"","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"12 8","pages":"1060–1061"},"PeriodicalIF":11.1,"publicationDate":"2026-08-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148815699","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Multimodal FRACTAL-MSI and Image Fusion Improves Detection and Resolution of Biomolecule Imaging 多模态分形- msi和图像融合提高了生物分子成像的检测和分辨率
IF 11.1 1区 化学
ACS Central Science Pub Date : 2026-08-26 Epub Date: 2026-07-06 DOI: 10.1021/acscentsci.6c00422
Mika T. Westerhausen, Rosemary J. Bergin, Connor R. Phillips, Jake P. Violi, Thomas E. Lockwood, Reggie Ridlen, David P. Bishop
{"title":"Multimodal FRACTAL-MSI and Image Fusion Improves Detection and Resolution of Biomolecule Imaging","authors":"Mika T. Westerhausen,&nbsp;Rosemary J. Bergin,&nbsp;Connor R. Phillips,&nbsp;Jake P. Violi,&nbsp;Thomas E. Lockwood,&nbsp;Reggie Ridlen,&nbsp;David P. Bishop","doi":"10.1021/acscentsci.6c00422","DOIUrl":"https://doi.org/10.1021/acscentsci.6c00422","url":null,"abstract":"<p>Elemental mass spectrometry imaging (MSI) of biomoleculesvia metal-conjugatedantibodies enables highly multiplexed, <em>in situ</em> quantitativeanalyses. However, the detection of low abundance analytes by elementalMSI and the spatial resolution of the images obtained are inhibitedby detector sensitivity. To overcome this constraint, we introduceFRACTAL-MSI, a signal amplification method that adapts FluoRescentsignal Amplification via Cyclic staining of TArget moLecules (FRACTAL)for multimodal laser ablation-inductively coupled plasma-mass spectrometry(LA-ICP-MS) and immunofluorescence (IF) imaging by alternating fluorescent-and lanthanide-tagged secondary antibodies on the same histologicalsection. Using NeuN as a model neuronal marker, we demonstrate 23–80×amplification of IF and LA-ICP-MS signals in fresh-frozen murine brain,FFPE tissue, and SH-SY5Y cells. Two image fusion methods that didnot require machine learning were then developed that exploited trueprobe colocalization to generate quantitative elemental images atIF resolution. The enhanced sensitivity permitted super-resolutionreconstruction of LA-ICP-MS data to obtain subcellular images witha 250 nm resolution, or greater than that of the 40× IF obtainedvia image fusion. We also demonstrated selective target amplificationwithin a 4-plex elemental panel. Together, FRACTAL-MSI provides apractical, broadly accessible strategy to improve detection, and thereforethe resolution, of low-abundance biomolecules.</p>","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"12 8","pages":"1119–1131"},"PeriodicalIF":11.1,"publicationDate":"2026-08-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148815818","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Spectroscopic Evidence in Optical Absorption for the Formation and Transformation of Prenucleation Clusters of CdS Quantum Dots CdS量子点预成核团簇形成和转变的光吸收光谱证据。
IF 11.1 1区 化学
ACS Central Science Pub Date : 2026-07-22 Epub Date: 2026-06-29 DOI: 10.1021/acscentsci.6c00394
Yang Li, Kui Yu*, Yusha Yang, Andrei Sapelkin, Sanwei Guo, Xiaobo Zhu, Sijie Zhang and Xiaoqin Chen*, 
{"title":"Spectroscopic Evidence in Optical Absorption for the Formation and Transformation of Prenucleation Clusters of CdS Quantum Dots","authors":"Yang Li,&nbsp;Kui Yu*,&nbsp;Yusha Yang,&nbsp;Andrei Sapelkin,&nbsp;Sanwei Guo,&nbsp;Xiaobo Zhu,&nbsp;Sijie Zhang and Xiaoqin Chen*,&nbsp;","doi":"10.1021/acscentsci.6c00394","DOIUrl":"10.1021/acscentsci.6c00394","url":null,"abstract":"<p>Prenucleation clusters (PNCs) that occupy a local minimumin theenergy landscape have been suggested to form via chemical self-assemblyprior to the nucleation and growth of colloidal semiconductor quantumdots (QDs) in reactions of individual cation and anion containingmolecules. However, firm spectroscopic evidence for the PNC has previouslyproven elusive. Using two model reactions of cadmium oleate + 1-dodecanethioland cadmium oleate + sulfur, we show the first signature signal ofoptical absorption between 260 and 290 nm for CdS PNCs. Controllingthe PNC transformation into magic-size clusters (MSCs) in dispersion,we demonstrate a clear reciprocal relationship of the absorption strengthbetween the PNC and the MSC. Our findings build a solid foundationfor PNC formation in QD reactions and bring a deeper insight intothe molecule–PNC–QD/MSC transition sequence, the knowledgeof which enables the transformation of nanochemistry from an empiricalart to a science.</p>","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"12 7","pages":"996–1007"},"PeriodicalIF":11.1,"publicationDate":"2026-07-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148583051","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Catalytic Reduction of Aqueous Perchlorate at Neutral pH 中性pH下高氯酸盐水溶液的催化还原。
IF 11.1 1区 化学
ACS Central Science Pub Date : 2026-07-22 Epub Date: 2026-07-08 DOI: 10.1021/acscentsci.6c00532
Jinyu Gao*, Shaohua Xie, Jianjun Chen, Qingsong Luo, Juchen Guo, Yadong Yin, Fudong Liu and Jinyong Liu*, 
{"title":"Catalytic Reduction of Aqueous Perchlorate at Neutral pH","authors":"Jinyu Gao*,&nbsp;Shaohua Xie,&nbsp;Jianjun Chen,&nbsp;Qingsong Luo,&nbsp;Juchen Guo,&nbsp;Yadong Yin,&nbsp;Fudong Liu and Jinyong Liu*,&nbsp;","doi":"10.1021/acscentsci.6c00532","DOIUrl":"10.1021/acscentsci.6c00532","url":null,"abstract":"<p>Perchlorate (ClO<sub>4</sub><sup>–</sup>) is a pervasiveand inert pollutant threatening human health. Catalytic reductionof ClO<sub>4</sub><sup>–</sup> is imperative for water environmentremediation and promising for space exploration. Previous catalystsusing oxo Mo<sup>IV</sup> and Re<sup>V</sup> species required acidicpH to reduce aqueous ClO<sub>4</sub><sup>–</sup>. Herein, wedeveloped a ligand-enhanced Ru<sup>0</sup> nanoparticle catalyst forrapid ClO<sub>4</sub><sup>–</sup> reduction by 1 atm H<sub>2</sub> at pH 7 and 20 °C. Molecular organic nitrogen ligands,particularly <em>cis</em>-1,2-diaminocyclohexane (<em>cis</em>-DACH), accelerated Ru<sup>0</sup>-catalyzed ClO<sub>4</sub><sup>–</sup> reduction by up to 80-fold. Nitrogen-functionalizedcarbon (NC) support also provided up to 5-fold acceleration. The final[<em>cis</em>-DACH]Ru/NC catalyst demonstrated unprecedentedactivity and robustness for ClO<sub>4</sub><sup>–</sup> reductionat neutral pH. Kinetic analyses and instrumental characterizationsfound that the nitrogen ligands not only boosted the reactivity ofexposed Ru<sup>0</sup> sites by 63-fold (31-fold by <em>cis</em>-DACH and 2-fold by the NC support) but also enhanced ClO<sub>4</sub><sup>–</sup> adsorption by 180%. This novel paradigm of tuningnanostructured catalysts by organic ligands will benefit environmentaland energy applications for the degradation and utilization of ClO<sub>4</sub><sup>–</sup>.</p>","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"12 7","pages":"1038–1047"},"PeriodicalIF":11.1,"publicationDate":"2026-07-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148583131","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Making Prodrugs Stick Around: Engineering Protease-Activated Tumor Retention 使前药停留:工程蛋白酶激活的肿瘤保留
IF 11.1 1区 化学
ACS Central Science Pub Date : 2026-07-22 Epub Date: 2026-07-09 DOI: 10.1021/acscentsci.6c01098
Robin Kryštůfek,  and , Jan Konvalinka​, 
{"title":"Making Prodrugs Stick Around: Engineering Protease-Activated Tumor Retention","authors":"Robin Kryštůfek,&nbsp; and ,&nbsp;Jan Konvalinka​,&nbsp;","doi":"10.1021/acscentsci.6c01098","DOIUrl":"https://doi.org/10.1021/acscentsci.6c01098","url":null,"abstract":"","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"12 7","pages":"888–890"},"PeriodicalIF":11.1,"publicationDate":"2026-07-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148596536","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
MOF-Based Lithium Oxygen Batteries: Status and Prospects from Material Design to System Integration 基于mof的锂氧电池:从材料设计到系统集成的现状与展望
IF 11.1 1区 化学
ACS Central Science Pub Date : 2026-07-22 Epub Date: 2026-06-11 DOI: 10.1021/acscentsci.6c00644
Shuaiyu Gao, Yuqing Dong, Malin Li, Yuelin Zhao, Genban Sun* and Jihong Yu*, 
{"title":"MOF-Based Lithium Oxygen Batteries: Status and Prospects from Material Design to System Integration","authors":"Shuaiyu Gao,&nbsp;Yuqing Dong,&nbsp;Malin Li,&nbsp;Yuelin Zhao,&nbsp;Genban Sun* and Jihong Yu*,&nbsp;","doi":"10.1021/acscentsci.6c00644","DOIUrl":"https://doi.org/10.1021/acscentsci.6c00644","url":null,"abstract":"<p>Lithium oxygen batteries (LOBs) offer exceptional theoreticalenergydensity but face formidable challenges due to the sluggish kineticsof the oxygen reduction and evolution reactions (ORR/OER). This reviewdelineates the pivotal role of metal–organic frameworks (MOFs)in overcoming these hurdles. We systematically dissect how the uniquestructural programmability, ultrahigh surface area, and atomicallydispersed active sites of MOFs and their derivatives are ingeniouslyexploited to engineer high-performance cathodes, functional separators,and solid-state electrolytes. The discussion is extended to pristineMOFs, MOF-derived carbons, and heteroatom-doped composites, highlightingtheir efficacy in regulating Li<sub>2</sub>O<sub>2</sub> growth andreducing overpotentials. Furthermore, strategic hybridization withconductive matrices such as carbon nanotubes and MXenes to enhanceelectron transfer is elaborated. Finally, we provide critical perspectiveson future research directions, encompassing stability enhancement,artificial intelligence-guided discovery, and advanced interfacialengineering, charting a course for MOF-based materials to propel thedevelopment of next-generation LOBs.</p>","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"12 7","pages":"895–940"},"PeriodicalIF":11.1,"publicationDate":"2026-07-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148596550","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Expanding the Trifluoroborate Toolbox: Pyridinium Scaffolds for PET Tracer Development 扩展三氟硼酸盐工具箱:PET示踪剂开发的吡啶支架
IF 11.1 1区 化学
ACS Central Science Pub Date : 2026-07-22 Epub Date: 2026-06-16 DOI: 10.1021/acscentsci.6c00966
Antonio A. W. L. Wong,  and , David M. Perrin​, 
{"title":"Expanding the Trifluoroborate Toolbox: Pyridinium Scaffolds for PET Tracer Development","authors":"Antonio A. W. L. Wong,&nbsp; and ,&nbsp;David M. Perrin​,&nbsp;","doi":"10.1021/acscentsci.6c00966","DOIUrl":"https://doi.org/10.1021/acscentsci.6c00966","url":null,"abstract":"","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"12 7","pages":"881–884"},"PeriodicalIF":11.1,"publicationDate":"2026-07-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148596553","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Ben Katz Will “Mass Spec Everything” to Figure out What Is in Our Food 本·卡茨将“质谱仪所有东西”来找出我们的食物中有什么。
IF 11.1 1区 化学
ACS Central Science Pub Date : 2026-07-22 Epub Date: 2026-06-16 DOI: 10.1021/acscentsci.6c00954
Victoria Atkinson, 
{"title":"Ben Katz Will “Mass Spec Everything” to Figure out What Is in Our Food","authors":"Victoria Atkinson,&nbsp;","doi":"10.1021/acscentsci.6c00954","DOIUrl":"10.1021/acscentsci.6c00954","url":null,"abstract":"","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"12 7","pages":"868–870"},"PeriodicalIF":11.1,"publicationDate":"2026-07-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148583050","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Hydride and Seek: Comparing Crystallographic Hydride Placement Techniques with an Open-Shell Cobalt Complex 氢化物与Seek:用开壳钴配合物比较晶体学氢化物放置技术。
IF 11.1 1区 化学
ACS Central Science Pub Date : 2026-07-22 Epub Date: 2026-06-23 DOI: 10.1021/acscentsci.6c00632
Ryan S. Donnelly, Theodore J. Gerard, Sebastian M. Krajewski, Brandon Q. Mercado, Xiaoping Wang* and Patrick L. Holland*, 
{"title":"Hydride and Seek: Comparing Crystallographic Hydride Placement Techniques with an Open-Shell Cobalt Complex","authors":"Ryan S. Donnelly,&nbsp;Theodore J. Gerard,&nbsp;Sebastian M. Krajewski,&nbsp;Brandon Q. Mercado,&nbsp;Xiaoping Wang* and Patrick L. Holland*,&nbsp;","doi":"10.1021/acscentsci.6c00632","DOIUrl":"10.1021/acscentsci.6c00632","url":null,"abstract":"<p>Locating hydridesis crucial in organometallic chemistrybut difficultto do accurately using X-ray diffraction. Electron diffraction hasbeen proposed as a way to overcome this problem but has not been systematicallycompared to neutron diffraction and to quantum crystallography (Hirshfeldatom refinement, HAR) to test this hypothesis. Here, we present acomparative analysis of methods for a terminal cobalt hydride complexby comparing a single-crystal neutron diffraction reference structureto results from single-crystal X-ray diffraction with and withoutHirshfeld atom refinement (HAR, NoSpherA2), density functional theory(DFT), and electron diffraction (3D-ED/MicroED) refined under kinematicaland dynamical formalisms. Conventional X-ray diffraction gives lowerprecision than neutron diffraction as expected. Despite expected improvements,HAR gives systematic deviation from the neutron benchmark. Interestingly,optimized DFT equilibrium geometries are closer to the neutron valuethan the value from HAR. On the other hand, electron diffraction witha high-quality data set coupled with dynamical refinement localizesthe hydride in difference maps and gives excellent agreement withthe neutron data. Dynamical refinement is crucial, as kinematicalrefinement does not allow assignment of a hydride peak. This cross-modalcomparison defines the conditions under which 3D-ED/MicroED delivershigh-precision metal–hydride distances for this open-shellcobalt hydride.</p>","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"12 7","pages":"972–980"},"PeriodicalIF":11.1,"publicationDate":"2026-07-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148583085","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
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