ACS Central Science最新文献_第5页

Cascade Catalysis for CO2 Upgrading to Long-Chain Products CO2升级为长链产物的级联催化

IF 11.1 1区化学

ACS Central Science Pub Date : 2026-08-26 Epub Date: 2026-07-17 DOI: 10.1021/acscentsci.5c02358

Yutong Wang, Min Kuang, Gengfeng Zheng

{"title":"Cascade Catalysis for CO2 Upgrading to Long-Chain Products","authors":"Yutong Wang, Min Kuang, Gengfeng Zheng","doi":"10.1021/acscentsci.5c02358","DOIUrl":"https://doi.org/10.1021/acscentsci.5c02358","url":null,"abstract":"Cascade catalytic conversion of CO2 has recentlyemergedas a transformative strategy for multilevel CO2 valorization.By integration of electrocatalytic CO2 reduction with thermocatalyticand/or biocatalytic processes, this approach enables stepwise constructionof complex products from simple carbon feedstocks. The electrocatalyticstage supplies key intermediates or upstream products such as CO,formate, formaldehyde, or ethanol, which can be further convertedinto value-added multicarbon products including sugars, polymers,and other fine chemicals through downstream coupling. Recent demonstrations,ranging from CO2-to-sugar and CO2-to-polyketoneconversions to artificial CO2-to-polymer biocatalytic pathways,have demonstrated the great potential of cascade strategies in bridgingelectro-, thermo-, and biochemistry. This Outlook discusses recentprogress in electrochemical cascade CO2 conversion andoutlines the key design goals for this field, including full-cascadeperformances, coupled catalyst-reaction optimizations, mechanisticunderstanding across complex interfaces, and integrated reactor architectures.","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"12 8","pages":"1089–1098"},"PeriodicalIF":11.1,"publicationDate":"2026-08-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148815797","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

Correction to “Detecting Bacteria in Their Mammalian Hosts Using Metabolism-Targeted [13C]CO2 Breath Testing” 更正“使用代谢目标[13C]CO2呼气测试检测哺乳动物宿主中的细菌”

IF 11.1 1区化学

ACS Central Science Pub Date : 2026-08-26 Epub Date: 2026-08-01 DOI: 10.1021/acscentsci.6c01043

Marina López-Álvarez, Sang Hee Lee, Anju Wadhwa, Mohammad Yaqoob Bhat, Tyler S. Simmons, Jung Min Kim, Anil Bidkar, Spenser R. Simpson, Shari Dhaene, Jeffrey D. Steinberg, Joseph Blecha, Wenxing Zou, Robert R. Flavell, Marshall D. McCue, Amanda M. Green, Renuka Sriram, Tom Desmet, Joanne Engel, Jason W. Rosch, Michael A. Ohliger, Kiel D. Neumann, David M. Wilson

引用次数: 0

In Vivo Real-Time Metabolic Isotopic Tracing via Breath Analysis upon Deuterated Water Ingestion: A Proof-of-Concept Study 通过吸入氘水的呼吸分析进行体内实时代谢同位素追踪：一项概念验证研究

IF 11.1 1区化学

ACS Central Science Pub Date : 2026-08-26 Epub Date: 2026-06-25 DOI: 10.1021/acscentsci.6c00078

Zhihong Yin, Kapil Dev Singh, Zhifeng Tang, Mélina Richard, Jiafa Zeng, Urs Frey, Pablo Sinues, Xue Li

{"title":"In Vivo Real-Time Metabolic Isotopic Tracing via Breath Analysis upon Deuterated Water Ingestion: A Proof-of-Concept Study","authors":"Zhihong Yin, Kapil Dev Singh, Zhifeng Tang, Mélina Richard, Jiafa Zeng, Urs Frey, Pablo Sinues, Xue Li","doi":"10.1021/acscentsci.6c00078","DOIUrl":"https://doi.org/10.1021/acscentsci.6c00078","url":null,"abstract":"Stable isotope tracingwith deuterium oxide (D2O) offersa powerful approach for probing metabolic dynamics, yet noninvasiveand real-time tools for monitoring in vivo deuterium(D) incorporation remain scarce. This study introduces secondary electrosprayionization–high-resolution mass spectrometry (SESI-HRMS) asa noninvasive, real-time approach for tracking D incorporation inhuman exhaled breath metabolites. A total of 11 healthy volunteerswere enrolled across two independent study centers. Each participantprovided up to 20 breath samples across fasting, post-D2O intake, and postprandial phases, yielding 213 samples in total.SESI-HRMS enabled the detection of 2,691 deuterium/hydrogen (D/H)pairs and revealed distinct metabolic trajectories associated withD labeling. Short-chain fatty acids (SCFAs) exhibited biphasic kineticsconsistent with rapid orogastric exchange followed by microbial fermentation.Transient increases in pyruvaldehyde were associated with glycemicfluctuations, while dynamic alterations in medium-chain acylcarnitinessuggested shifts in mitochondrial energy metabolism. Notably, SESI-HRMSunambiguously resolved D-labeled peaks from natural 13Cisotopologues, demonstrating high analytical specificity for stableisotope tracing. Collectively, these findings demonstrate the feasibilityof SESI-HRMS real-time breath analysis for noninvasive investigationof D-labeled metabolic dynamics in humans.","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"12 8","pages":"1110–1118"},"PeriodicalIF":11.1,"publicationDate":"2026-08-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148815805","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

Advances in Porous Materials and Their Applications 多孔材料及其应用研究进展

IF 11.1 1区化学

ACS Central Science Pub Date : 2026-08-26 DOI: 10.1021/acscentsci.6c01286

Seth M. Cohen

引用次数: 0

Location, Location, Location: Main Chain Poly(cobaltocenium)s Outperform Side Chain Analogues 位置，位置，位置：主链聚钴氰胺优于侧链类似物

IF 11.1 1区化学

ACS Central Science Pub Date : 2026-08-26 Epub Date: 2026-07-21 DOI: 10.1021/acscentsci.6c01185

Edmund F. Palermo

引用次数: 0

Simple Organic Nitrogen Ligand Unlocks Perchlorate Reduction at Neutral pH 简单有机氮配体在中性pH下解锁高氯酸盐还原

IF 11.1 1区化学

ACS Central Science Pub Date : 2026-08-26 Epub Date: 2026-07-30 DOI: 10.1021/acscentsci.6c01255

Jaehyeong Park, Jong Kwon Choe

引用次数: 0

Programmed S → N Remote Cyano Migration: A Thiocyanate-Based Entry to Cyanamides and Selective Ferroptosis Inducers 程化S→N远端氰基迁移：以硫氰酸盐为基础进入氰酰胺和选择性铁下沉诱导剂

IF 11.1 1区化学

ACS Central Science Pub Date : 2026-08-26 Epub Date: 2026-08-06 DOI: 10.1021/acscentsci.6c00645

Xiyan Duan, Wanjing Feng, Fengjiao Du, Can Liu, Ning Liu, Yihao Zhao, Kun Liu, Pu Liu, Yixuan Zhang, Jingze Li, Yahui Ding, Quan Zhang

{"title":"Programmed S → N Remote Cyano Migration: A Thiocyanate-Based Entry to Cyanamides and Selective Ferroptosis Inducers","authors":"Xiyan Duan, Wanjing Feng, Fengjiao Du, Can Liu, Ning Liu, Yihao Zhao, Kun Liu, Pu Liu, Yixuan Zhang, Jingze Li, Yahui Ding, Quan Zhang","doi":"10.1021/acscentsci.6c00645","DOIUrl":"https://doi.org/10.1021/acscentsci.6c00645","url":null,"abstract":"Ferroptosis representsa promising strategy to overcome apoptosis-associateddrug resistance, yet access to diverse and drug-like ferroptosis-inducingchemical space remains limited. Among potential scaffolds for populatingthis high-value space, cyanamide-bearing molecules are attractivebut synthetically challenging due to the long-standing difficultyof constructing the N–CN bond. Here we disclose a thiocyanate-enabledcascade cyclization that leverages inexpensive, low-toxicity inorganicthiocyanate as an unconventional electrophilic CN surrogate. Thistransformation proceeds through a cascade sequence involving SCN installation,remote S → N cyano migration, and subsequent intramolecularthiazine annulation under mild, metal-free conditions. The resultingcyanamide 3,4-dihydro-2H-1,4-thiazines exhibited nanomolar ferroptosis-inducingpotency; lead compounds 3b and 3c achievedIC50 values of 6.8 nM and 14 nM, respectively; and significantlysuppressed tumor growth in a lung cancer PDX model.","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"12 8","pages":"1237–1245"},"PeriodicalIF":11.1,"publicationDate":"2026-08-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148815702","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

Domino Strategies in Heterocycle Synthesis: Advancing from Organocatalysis to Photo-/Organo-Autocatalysis 杂环合成中的多米诺骨牌策略：从有机催化到光/有机自催化

IF 11.1 1区化学

ACS Central Science Pub Date : 2026-08-26 Epub Date: 2026-07-13 DOI: 10.1021/acscentsci.6c00561

Abdulaziz A. Al-Romema, Felix Heckmann, Svetlana B. Tsogoeva

{"title":"Domino Strategies in Heterocycle Synthesis: Advancing from Organocatalysis to Photo-/Organo-Autocatalysis","authors":"Abdulaziz A. Al-Romema, Felix Heckmann, Svetlana B. Tsogoeva","doi":"10.1021/acscentsci.6c00561","DOIUrl":"https://doi.org/10.1021/acscentsci.6c00561","url":null,"abstract":"The increasing structuralcomplexity of heterocycles in pharmaceuticals,agrochemicals, and functional materials continues to challenge syntheticdesign, particularly when step economy, scalability, and sustainabilityare considered simultaneously. Domino reactions, in which multiplebond-forming events proceed sequentially in a single operation, offeran inherently concise strategy to transform simple building blocksinto densely functionalized architectures while minimizing purificationsteps and waste. In this Outlook, we examine theevolution of domino heterocycle synthesis from classical organocatalysisto photo- and organo-autocatalytic systems, highlighting how metal-freeactivation, visible-light processes, and in situ-generatedcatalytic species expand reactivity while improving catalyst, energy,and atom economy. We discuss key advances in domino reactions towardchiral heterocycles, heteroaromatic construction, total synthesis,and self-catalyzed photochemical processes, emphasizing challengessuch as catalyst loading, robustness, photon efficiency, and reactionscalability. The future development of domino synthesis will relyon combining new mechanistic ideas with sustainability and rationalreaction design. By focusing on the deliberate development of efficient,low-input organo- and photo/organo-autocatalyzeddomino reactions, we aim to spur progress toward streamlined and industriallypractical methods for heterocycle synthesis.","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"12 8","pages":"1068–1088"},"PeriodicalIF":11.1,"publicationDate":"2026-08-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148815762","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

Isomer-Resolved Mass Spectrometry Imaging Reveals Regional and Age-Dependent Glycolipid Metabolism in Rat Brain 同分异构体分辨质谱成像揭示大鼠脑中区域和年龄依赖性糖脂代谢

IF 11.1 1区化学

ACS Central Science Pub Date : 2026-08-26 Epub Date: 2026-07-10 DOI: 10.1021/acscentsci.6c00340

Hsi-Chun Chao, Marisa Asadian, Stanislav S. Rubakhin, Fan Lam, Jonathan V. Sweedler

{"title":"Isomer-Resolved Mass Spectrometry Imaging Reveals Regional and Age-Dependent Glycolipid Metabolism in Rat Brain","authors":"Hsi-Chun Chao, Marisa Asadian, Stanislav S. Rubakhin, Fan Lam, Jonathan V. Sweedler","doi":"10.1021/acscentsci.6c00340","DOIUrl":"https://doi.org/10.1021/acscentsci.6c00340","url":null,"abstract":"Glycolipids are essential for myelin integrity, but theirextensiveisomeric complexity, where isomers like galactosylceramide (GalCer)and glucosylceramide (GlcCer) have unique functions, has hinderedour ability to map their metabolism in the brain. Existing mass spectrometrymethods fail to resolve this complexity. We fundamentally overcomethis barrier with a powerful new isomer-resolved mass spectrometryimaging workflow. By coupling ion mobility and mass spectrometry imagingwith targeted enzymatic pretreatment, our method provides direct visualizationof distinct de novo metabolic pathways for GalCer and GlcCer in situ.When applied to rat brains across the lifespan (2, 6, and 12 months),this technology revealed a previously unrecognized age-related declinethat selectively affected the GalCer pathway, while the isomeric GlcCerpathway remained comparatively stable. We confirmed these metabolicalterations colocalize with myelin-associated proteins specificallyin oligodendrocyte-rich regions, providing a functional link to alteredoligodendrocyte-related lipid metabolism. This integrated approachprovides a new paradigm for dissecting isomer-specific glycolipidmetabolism, offering insight into lipid alterations in brain agingand opening new avenues for biomarker discovery in neurodegeneration.","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"12 8","pages":"1146–1157"},"PeriodicalIF":11.1,"publicationDate":"2026-08-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148810336","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

Pressure-Induced Metal-like Transport and Magnetoresistance in a Au2+–Au3+ Halide Perovskite Au2+ -Au3 +卤化物钙钛矿的压力诱导类金属输运和磁电阻

IF 11.1 1区化学

ACS Central Science Pub Date : 2026-08-26 Epub Date: 2026-06-24 DOI: 10.1021/acscentsci.6c00315

Christina R. Deschene, Armin Eghdami, Yijun Yu, Alex Smith, Zhenxian Liu, Frederick P. Marlton, Wendy L. Mao, Harold Y. Hwang, Jeffrey B. Neaton, Hemamala I. Karunadasa

{"title":"Pressure-Induced Metal-like Transport and Magnetoresistance in a Au2+–Au3+ Halide Perovskite","authors":"Christina R. Deschene, Armin Eghdami, Yijun Yu, Alex Smith, Zhenxian Liu, Frederick P. Marlton, Wendy L. Mao, Harold Y. Hwang, Jeffrey B. Neaton, Hemamala I. Karunadasa","doi":"10.1021/acscentsci.6c00315","DOIUrl":"https://doi.org/10.1021/acscentsci.6c00315","url":null,"abstract":"The Cs4AuIIAuIII2Cl12 perovskite (1), featuring AuCl4 trimersseparated by vacancies, enables the first high-pressure study of Au2+/3+mixed-valence. Our computational analysis of the goldfrontier orbitals suggests that the Au2+→Au3+ intervalence charge transfer (IVCT) occurs across the vacancies.Computational structures indicate that these vacancies rapidly shrinkwith pressure and the Au2+ and Au3+ coordinationspheres become very similar at the phase transition to nearly cubicsymmetry at ca. 15 GPa─enabling facile IVCT. Although the activationenergy of conductivity of 0.73(4) meV and far-infrared absorptionindicate a small but nonzero bandgap, ambient thermal energy drivesthe IVCT, affording metallic properties: prominent infrared reflectivityand transport values of 102 S·cm–1. This prompted us to perform the first high-pressure studies ofmagnetoresistance (MR) and Hall effect in halide perovskites. At 16GPa, the MR increases by 9.3% at 2 K and 9 T; this value is maintainedup to 27 GPa, when a local distortion drives electronic localization.By globally fitting the MR and Hall resistance to a two-carrier modelwe quantify how the carrier densities and mobilities evolve with pressure.Thus, metal-like transport and MR in 1 is driven by apressure-induced transition from localized to partially delocalizedmixed-valence.","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"12 8","pages":"1132–1145"},"PeriodicalIF":11.1,"publicationDate":"2026-08-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148810344","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