Chem最新文献_第3页

Precise synthesis of non-equilibrium rotaxanes via pumping in water 泵入水中精确合成非平衡轮烷

IF 19.6 1区化学

Chem Pub Date : 2026-04-09 Epub Date: 2026-02-04 DOI: 10.1016/j.chempr.2025.102878

Guangcheng Wu , Jihye Park , Wei-Guang Liu , Yang Jiao , Long Zhang , Han Han , Chun Tang , Taehwan Jang , Minho M. Kim , Bo Song , Xuesong Li , Ruihua Zhang , Enxu Liu , Huang Wu , Yong Wu , Xingang Zhao , Yuanning Feng , Qing Li , Hyungjun Kim , R. Dean Astumian , J. Fraser Stoddart

{"title":"Precise synthesis of non-equilibrium rotaxanes via pumping in water","authors":"Guangcheng Wu , Jihye Park , Wei-Guang Liu , Yang Jiao , Long Zhang , Han Han , Chun Tang , Taehwan Jang , Minho M. Kim , Bo Song , Xuesong Li , Ruihua Zhang , Enxu Liu , Huang Wu , Yong Wu , Xingang Zhao , Yuanning Feng , Qing Li , Hyungjun Kim , R. Dean Astumian , J. Fraser Stoddart","doi":"10.1016/j.chempr.2025.102878","DOIUrl":"10.1016/j.chempr.2025.102878","url":null,"abstract":"<div><div>Water is the matrix of life in which biomolecular machines carry out vital functions through ordered mechanical movements. The controlled active transport in artificial systems within aqueous environments, however, remains challenging at the molecular level, resulting from the inherent difficulties in manipulating molecular motions accurately in water. Herein, we present artificial molecular pumps (AMPs) capable of forming and maintaining non-equilibrium concentration differences of cucurbit[7]uril rings (up to 350 times) in aqueous media. Acid-base neutralization energy is exploited to add efficiently and precisely one ring per cycle to the dumbbells of both a solo and a duet pump by a rationally optimized pumping cassette. Operation is achieved under ambient conditions through simple pH modulation (2–7). A combination of kinetic investigations, computational modeling, and theoretical analysis provides a mechanistic understanding of how the aqueous AMPs harness chemical energy to produce and sustain high-energy oligorotaxanes in a non-equilibrium steady state.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"12 4","pages":"Article 102878"},"PeriodicalIF":19.6,"publicationDate":"2026-04-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147636778","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

Chirality’s journey: Pasteur, Kelvin, the origins of life, chiral nanotechnologies, and insights from AI 手性之旅：巴斯德，开尔文，生命的起源，手性纳米技术，以及人工智能的见解

IF 19.6 1区化学

Chem Pub Date : 2026-04-09 DOI: 10.1016/j.chempr.2026.102991

Alexander Govorov , Denis A. Govorov , Sofia Hoffman

引用次数: 0

Write and erase: Macrocyclic effectors regulate imine expression in water 写和擦除：大环效应物调节亚胺在水中的表达

IF 19.6 1区化学

Chem Pub Date : 2026-04-09 Epub Date: 2026-01-23 DOI: 10.1016/j.chempr.2025.102834

Ferran Esteve , Martina Mazzaferro , Jean-Marie Lehn

{"title":"Write and erase: Macrocyclic effectors regulate imine expression in water","authors":"Ferran Esteve , Martina Mazzaferro , Jean-Marie Lehn","doi":"10.1016/j.chempr.2025.102834","DOIUrl":"10.1016/j.chempr.2025.102834","url":null,"abstract":"<div><div>Enzymatic molecular recognition and post-modification of specific amino acids on proteins allows for writing, reading, and erasing processes that regulate a wide range of biological processes. Herein, we investigate reversible-imine-formation-based model dynamic chemical systems that adapt their expression in response to macrocyclic effectors. The writing action relies on the formation of the host-guest supramolecular adduct between the macrocycles and the components and constituents. The dynamic condensation reaction changes imine expression accordingly, giving a specific constitutional pattern. The strength of the upregulating or downregulating effect can be tuned according to the supramolecular match between the guests and the microenvironments provided by the different macrocycles. The addition of an external scavenger that is a better fit for the host erases the action and reestablishes the initial equilibrium state, regulating the whole process. Control over dynamic covalent libraries triggers the emergence of complex behaviors, such as constituent selection, (non-)selective amplification and inhibition, and sorting-to-scrambling transitions.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"12 4","pages":"Article 102834"},"PeriodicalIF":19.6,"publicationDate":"2026-04-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146033871","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

Oxygen reduction active-site regulation enables reverse photocurrent in photoelectrochemical sensing 氧还原活性位点调节实现了光电化学传感中的反向光电流

IF 19.6 1区化学

Chem Pub Date : 2026-04-09 Epub Date: 2025-11-20 DOI: 10.1016/j.chempr.2025.102821

Ying Qin (覃滢) , Yuanxing Chen (陈渊兴) , Wenhong Yang (杨文鸿) , Rong Tan (谭蓉) , Jingyi Zhang (张靖怡) , Runshi Xiao (肖润石) , Mingwang Liu (刘名旺) , Liuyong Hu (胡六永) , Wenling Gu (顾文玲) , Chengzhou Zhu (朱成周)

{"title":"Oxygen reduction active-site regulation enables reverse photocurrent in photoelectrochemical sensing","authors":"Ying Qin (覃滢) , Yuanxing Chen (陈渊兴) , Wenhong Yang (杨文鸿) , Rong Tan (谭蓉) , Jingyi Zhang (张靖怡) , Runshi Xiao (肖润石) , Mingwang Liu (刘名旺) , Liuyong Hu (胡六永) , Wenling Gu (顾文玲) , Chengzhou Zhu (朱成周)","doi":"10.1016/j.chempr.2025.102821","DOIUrl":"10.1016/j.chempr.2025.102821","url":null,"abstract":"<div><div>The bidirectional photocurrent holds great research significance in numerous photoelectrochemical (PEC) applications, owing to its superior accuracy and multifunctionality. Herein, we introduce an innovative concept of reverse photocurrent (|I<sub>light</sub>| < |I<sub>dark</sub>|), where the photocurrent direction switches within the cathode due to differing oxygen reduction activities at dual sites. When platinum nanoparticles are incorporated with carbon nitride nanosheets, a facile conversion of the traditional photocurrent (|I<sub>light</sub>| > |I<sub>dark</sub>|) into a reverse photocurrent with an enhancement of 22 times is achieved. Compared with traditional photocurrent characteristics, this reverse photocurrent not only reveals a new mechanism for PEC light/dark reactions but also serves as a new strategy to induce the changeover of photocurrent direction. Leveraging this bidirectional-photocurrent approach, more sensitive evaluation of aptamer-target interactions and target detection has been successfully realized. This study will offer fresh insights into photoelectrode design in the PEC analysis and surface reaction monitoring.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"12 4","pages":"Article 102821"},"PeriodicalIF":19.6,"publicationDate":"2026-04-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145554870","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

Intrinsic circularly polarized luminescence with a record-high dissymmetry factor via dynamic through-space conjugation 具有创纪录的高不对称因子的本征圆偏振光通过动态通过空间共轭

IF 19.6 1区化学

Chem Pub Date : 2026-04-09 Epub Date: 2026-02-02 DOI: 10.1016/j.chempr.2025.102858

Zuping Xiong (熊祖平) , Xiong Liu (刘雄) , Ziteng Zhang (张子腾) , Shuaitong Wei (卫帅彤) , Jiyong Liu (刘继永) , Qingyang Xu (徐清洋) , Jing Zhi Sun (孙景志) , Jianyu Zhang (张鉴予) , Ben Zhong Tang (唐本忠) , Haoke Zhang (张浩可)

{"title":"Intrinsic circularly polarized luminescence with a record-high dissymmetry factor via dynamic through-space conjugation","authors":"Zuping Xiong (熊祖平) , Xiong Liu (刘雄) , Ziteng Zhang (张子腾) , Shuaitong Wei (卫帅彤) , Jiyong Liu (刘继永) , Qingyang Xu (徐清洋) , Jing Zhi Sun (孙景志) , Jianyu Zhang (张鉴予) , Ben Zhong Tang (唐本忠) , Haoke Zhang (张浩可)","doi":"10.1016/j.chempr.2025.102858","DOIUrl":"10.1016/j.chempr.2025.102858","url":null,"abstract":"<div><div>How can non-covalent interactions be harnessed in the design of multifunctional materials beyond the constraints of traditional bonding frameworks? Inspired by weak interactions in biological systems and motivated to overcome the constraints imposed by valence-shell electron-pair repulsion, we explore excited-state through-space conjugation (TSC) between adjacent nitrogen atoms as an efficient strategy for modulating material properties. Photoisomerizable molecular switches activate dynamic TSC in the excited state, markedly enhancing both optical and mechanical properties. In the crystalline phase, this dynamic TSC enables robust red circularly polarized luminescence (CPL) at 610 nm, sustained over 300 reversible cycles, with a record-high asymmetry factor (∼0.20) among non-assembled organic small molecules. Concurrently, the system exhibits reversible changes in both elasticity and hardness. These findings uncover a counterintuitive lone-pair/lone-pair conjugation mechanism, presenting a novel strategy for designing smart crystalline materials that integrate photoswitchable and photomechanical functionalities.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"12 4","pages":"Article 102858"},"PeriodicalIF":19.6,"publicationDate":"2026-04-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146101829","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

Coaxing stubborn molecules into crystals with a silver triangle 用银三角将顽固分子诱导成晶体

IF 19.6 1区化学

Chem Pub Date : 2026-04-09 Epub Date: 2026-03-26 DOI: 10.1016/j.chempr.2026.102989

Hongliang Ye , Andrew C.-H. Sue

引用次数: 0

A new class of nickel precatalysts for cross-coupling: Nickel(I) isocyanide complexes 一类新的镍预催化剂：镍(I)异氰化物配合物

IF 19.6 1区化学

Chem Pub Date : 2026-04-09 Epub Date: 2026-03-27 DOI: 10.1016/j.chempr.2026.103029

Devi Oniani , Nilay Hazari

引用次数: 0

Tunable thermal phase-change materials from common detergents 普通洗涤剂的可调热相变材料

IF 19.6 1区化学

Chem Pub Date : 2026-04-09 Epub Date: 2025-11-18 DOI: 10.1016/j.chempr.2025.102820

Daniel W. Laorenza , Vidhya M. Dev , Claire E. Casaday , Jarad A. Mason

{"title":"Tunable thermal phase-change materials from common detergents","authors":"Daniel W. Laorenza , Vidhya M. Dev , Claire E. Casaday , Jarad A. Mason","doi":"10.1016/j.chempr.2025.102820","DOIUrl":"10.1016/j.chempr.2025.102820","url":null,"abstract":"<div><div>Phase-change materials that transform between two solid phases with a large latent heat provide an emissions-free platform for passively or actively regulating temperature across diverse environments. Layered materials with confined hydrocarbon bilayers undergo reversible solid-state, “chain-melting” phase transitions, offering a modular mechanism for thermal energy storage and barocaloric cooling. Here, we report two series of chain-melting phase-change materials based on readily available alkylsulfate salts. A broad screening of material architectures containing dodecylsulfate anions reveals hydrocarbon packing motifs that exhibit well-behaved phase transitions governed by both hydrocarbon chain length and packing density. We posit that both alkyl chain confinement and inorganic-organic interfacial interactions dictate phase-change behavior, including transition entropies and reversibility. Based on these design principles, we demonstrate large barocaloric effects below 100 bar with tetra-aquo bis-decylsulfate copper(II). The insights provided by calorimetric and structural examination of these materials offer a pathway for designing and optimizing high-performance thermal phase-change materials.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"12 4","pages":"Article 102820"},"PeriodicalIF":19.6,"publicationDate":"2026-04-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145536324","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

Reduction and deuteration of N-heteroarenes using an organic photoredox catalyst 用有机光氧化还原催化剂还原和氘化n -杂芳烃

IF 19.6 1区化学

Chem Pub Date : 2026-04-09 Epub Date: 2025-11-21 DOI: 10.1016/j.chempr.2025.102822

Amreen K. Bains , Arindam Sau , Brandon S. Portela , Robert S. Paton , Garret M. Miyake , Niels H. Damrauer

{"title":"Reduction and deuteration of N-heteroarenes using an organic photoredox catalyst","authors":"Amreen K. Bains , Arindam Sau , Brandon S. Portela , Robert S. Paton , Garret M. Miyake , Niels H. Damrauer","doi":"10.1016/j.chempr.2025.102822","DOIUrl":"10.1016/j.chempr.2025.102822","url":null,"abstract":"<div><div>Selective reduction and deuteration of heteroarenes offers a direct approach to synthesizing saturated congeners, which are vital motifs in medicinal chemistry and drug discovery. Relevant traditional synthetic methods, such as catalytic hydrogenation, primarily rely on transition-metal-mediated catalysis, elevated temperatures, and pressurized H<sub>2</sub>. Therefore, complementary metal- and H<sub>2</sub>-free methodologies that operate at room temperature and convert a wide range of heteroarenes into their saturated and, when desired, deuterium-enriched congeners are valuable. To this end, we introduce core-extended coronene-tetraesters as organic photoredox catalysts for the photoinduced reduction and deuteration of a range of heteroarenes at ambient temperature using visible light from commercially available LEDs. This protocol accommodates over nine types of heteroarenes under a common reaction condition. Mechanistic studies reveal that the reactivity is enabled by photon absorption by the <em>in situ</em>-generated closed-shell 2e<sup>−</sup>/H<sup>+</sup> super-reductant.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"12 4","pages":"Article 102822"},"PeriodicalIF":19.6,"publicationDate":"2026-04-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145560487","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

Reimagining metal-organic framework discovery: Integrating experiment, computation, and artificial intelligence 重新构想金属有机框架发现：整合实验、计算和人工智能

IF 19.6 1区化学

Chem Pub Date : 2026-04-09 Epub Date: 2026-02-25 DOI: 10.1016/j.chempr.2025.102921

Madeleine A. Gaidimas , Jiaru Bai , Yeonghun Kang , Kent O. Kirlikovali , Varinia Bernales , Alán Aspuru-Guzik , Omar K. Farha

引用次数: 0