Chem最新文献_第3页

Isotope interface design for high-energy aqueous proton batteries 高能水质子电池的同位素界面设计

IF 19.6 1区化学

Chem Pub Date : 2025-09-11 DOI: 10.1016/j.chempr.2025.102551

Hongwei Cai , Kai Fu , Ruixi Chen , Wenyuan Bao , Deyang Guan , Xiangchen Zhang , Zhaohui Deng , Xinfei Wu , Xingbao Chen , Jean-Jacques Gaumet , Wen Luo , Liqiang Mai

{"title":"Isotope interface design for high-energy aqueous proton batteries","authors":"Hongwei Cai , Kai Fu , Ruixi Chen , Wenyuan Bao , Deyang Guan , Xiangchen Zhang , Zhaohui Deng , Xinfei Wu , Xingbao Chen , Jean-Jacques Gaumet , Wen Luo , Liqiang Mai","doi":"10.1016/j.chempr.2025.102551","DOIUrl":"10.1016/j.chempr.2025.102551","url":null,"abstract":"<div><div><span><span><span>The stability of the electrode-electrolyte interface is crucial for the long-term operation of battery </span>chemistries, particularly under harsh conditions with corrosive acidic/alkaline </span>aqueous electrolytes. Here, we report the design of a H</span><sub>2</sub><sup>18</sup>O-H<sub>2</sub><sup>16</sup>O isotope interface to promote the formation of a protective electrode-electrolyte interphase, as demonstrated by a model investigation based on an aqueous proton battery (APB) utilizing strongly acidic aqueous electrolytes. This design enables the manganese-iron Prussian blue analog (MnFe-PBA), typically considered acid intolerant, to cycle stably over 10,000 cycles in corrosive H<sub>3</sub>PO<sub>4</sub> electrolytes. This acid resistance is attributed to the isotope interface-governed <em>in situ</em><span> formation of interphases comprising hydrogen-bonded frameworks. With the high-energy MnFe-PBA cathode, the full battery attains a high voltage plateau (⁓1.2 V) and energy density (77.6 Wh kg</span><sup>−1</sup><span>), both surpassing all previously reported APBs. Our findings provide a novel approach for enhancing the performance of aqueous batteries subject to extremely corrosive conditions and encourage the integration of isotopic science with battery technology.</span></div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"11 9","pages":"Article 102551"},"PeriodicalIF":19.6,"publicationDate":"2025-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143893371","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

Ligand-enabled override of the memory effect in Rh-catalyzed asymmetric Suzuki reactions 铑催化的不对称铃木反应中配体激活的记忆效应

IF 19.6 1区化学

Chem Pub Date : 2025-09-11 DOI: 10.1016/j.chempr.2025.102550

Ke Liu , David Egea-Arrebola , Ruchuta Ardkhean , Laura Cunningham , Kirsten E. Christensen , Robert S. Paton , Stephen P. Fletcher

{"title":"Ligand-enabled override of the memory effect in Rh-catalyzed asymmetric Suzuki reactions","authors":"Ke Liu , David Egea-Arrebola , Ruchuta Ardkhean , Laura Cunningham , Kirsten E. Christensen , Robert S. Paton , Stephen P. Fletcher","doi":"10.1016/j.chempr.2025.102550","DOIUrl":"10.1016/j.chempr.2025.102550","url":null,"abstract":"<div><div>Chiral non-racemic allylic species are key building blocks for many carbon-containing molecules, including pharmaceuticals and polymers. Metal-catalyzed asymmetric additions of nucleophiles to allylic species undergo different pathways depending on the metal and nucleophile combination, hindering the development of useful addition reactions with aromatic nucleophiles. We report an asymmetric cross-coupling method between aryl boronic acids and linear allylic phosphates to give branched allylic products. This Suzuki-type reaction overcomes the “memory effect” in Rh catalysis, enabling an overall SN2′ transformation by rate-determining reductive elimination and forming a new stereogenic center adjacent to a terminal vinyl moiety. The method tolerates preexisting stereogenic centers, allowing for synthetic strategies where drugs and natural products are elaborated via diastereoselective allylic arylations. The method is used, as the catalyst-controlled stereochemistry-setting step, in an iterative strategy to give arrays of aryl-substituted contiguous stereogenic centers. This approach will complement existing catalyst-controlled stereoselective methods for forming C–C bonds.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"11 9","pages":"Article 102550"},"PeriodicalIF":19.6,"publicationDate":"2025-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143853600","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

Functional liquid layer enables superior performance of air purification filter 功能液层使空气净化过滤器性能优越

IF 19.6 1区化学

Chem Pub Date : 2025-09-11 DOI: 10.1016/j.chempr.2025.102526

Qifei Wang , Yuheng Sheng , Xiaowei Song , Yuchen Qiu , Xiao Li , Chao Shang , Yang Wang , Jihong Yu

{"title":"Functional liquid layer enables superior performance of air purification filter","authors":"Qifei Wang , Yuheng Sheng , Xiaowei Song , Yuchen Qiu , Xiao Li , Chao Shang , Yang Wang , Jihong Yu","doi":"10.1016/j.chempr.2025.102526","DOIUrl":"10.1016/j.chempr.2025.102526","url":null,"abstract":"<div><div><span>Particulate air contaminations adversely impact the public and have thereby prompted the development of air purification<span> systems. Herein, we show a novel liquid-mediated purification system (LMS) based on a core-shell liquid-mediated membrane filter<span><span> for high-efficient capture of almost all hazardous airborne particles. This system overcomes the unavoidable instability and fouling/clogging problems of conventional filtering systems, driven by unstable surface attractive sites (e.g., electrostatic charges). The optimized liquid layer in LMS (e.g., glycerol) affords strong </span>surface tension effect<span> and high particle detachment energy to enable an integrated three-step particle-capturing process (particle attraction, adhesion, and retention), achieving an overall outperforming filtration efficiency over 99% without resistance increase within 3 months usage. Such a liquid-interface-guided purification strategy performs judicious combinability and </span></span></span></span>adjustability with the liquid layer acting as the primary filtering layer, promoting the development of universal, highly effective, environmentally friendly, and cost-effective air purification.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"11 9","pages":"Article 102526"},"PeriodicalIF":19.6,"publicationDate":"2025-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143776227","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

Reductive coupling of acrylamides and carbonyls via solvated electrons from excited-state acridyl radicals 丙烯酰胺和羰基通过激发态吖啶基自由基溶剂化电子的还原偶联

IF 19.6 1区化学

Chem Pub Date : 2025-09-11 DOI: 10.1016/j.chempr.2025.102647

Roukaya K. El Mokadem , Tanya M. Lazarus , David A. Nicewicz

引用次数: 0

An M60L60 metal-peptide capsid with a 60-crossing woven network M60L60金属肽衣壳具有60交叉编织网络

IF 19.6 1区化学

Chem Pub Date : 2025-09-11 DOI: 10.1016/j.chempr.2025.102555

Yuuki Inomata , Sota Oguma , Nao Sagara , Ami Nishijima , Yuta Saburomaru , Satoshi Yoshida , Takashi Kajitani , Koya Shimokawa , Sota Sato , Michito Yoshizawa , Makoto Fujita , Tomohisa Sawada

{"title":"An M60L60 metal-peptide capsid with a 60-crossing woven network","authors":"Yuuki Inomata , Sota Oguma , Nao Sagara , Ami Nishijima , Yuta Saburomaru , Satoshi Yoshida , Takashi Kajitani , Koya Shimokawa , Sota Sato , Michito Yoshizawa , Makoto Fujita , Tomohisa Sawada","doi":"10.1016/j.chempr.2025.102555","DOIUrl":"10.1016/j.chempr.2025.102555","url":null,"abstract":"<div><div>Controlling topologies of highly entangled molecular strands from scratch has long been challenging. For its realization, repeated cycles of prediction, considering the geometrical constraints behind molecular self-assembly, and synthetic trial-and-error are crucial. Here, we report the chemical construction of an unexplored topological molecule—a dodecahedral link with 60 crossings. This structure, predicted through theoretical considerations, represents an advancement from previous tetrahedral and cubic links. The resulting capsid-like structure, measuring 6.3 nm in size, has an M<sub>60</sub>L<sub>60</sub> composition (M, metal; L, ligand), formed through the folding and assembly of 60 trivalent Cu<sup>+</sup> ions and 60 tritopic pentapeptide ligands. This entangled topological framework formed a 4.0 nm-sized inner cavity (∼34,000 Å<sup>3</sup>). The 60-crossing dodecahedral link topology was, in another way using both knot and graph theories, also characterized as a Goldberg <em>T</em> = 3 polyhedron (<em>T</em>, triangulation number) consisting of trefoil knot panels, providing a new roadmap to further giant capsid structures.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"11 9","pages":"Article 102555"},"PeriodicalIF":19.6,"publicationDate":"2025-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143893323","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

Designing generative dissipative networks for programming complex temporal dynamics and functions 设计生成耗散网络规划复杂的时间动态和函数

IF 19.6 1区化学

Chem Pub Date : 2025-09-11 DOI: 10.1016/j.chempr.2025.102593

Xiarui Wang , Shan Wang , Liang Yue , Weihong Tan

{"title":"Designing generative dissipative networks for programming complex temporal dynamics and functions","authors":"Xiarui Wang , Shan Wang , Liang Yue , Weihong Tan","doi":"10.1016/j.chempr.2025.102593","DOIUrl":"10.1016/j.chempr.2025.102593","url":null,"abstract":"<div><div><span><span>Complex temporal dynamics orchestrated by natural networks are essential for cellular functions. Replicating these dynamics in simplified synthetic networks could elucidate underlying mechanisms, facilitating the creation of life-like systems. Herein, we introduce a versatile, modular, and programmable framework for constructing hierarchical and multifunctional generative dissipative networks (GDNs) capable of producing complex temporal dynamics. This framework involves two types of modules. Generative modules produce fuels, and dissipative modules consume these fuels to activate transient signals. By integrating multiple modules, hierarchical GDNs with diverse compositions, sizes, connections, and topologies were constructed to produce controllable complex temporal dynamics, like precise pulse-multiphase control, pulse-repetition </span>frequency modulation, and programmed timing of multiple pulses. These dynamics stem from coordination among heterogeneous modules and competition among homogeneous modules, as corroborated by kinetic modeling. Furthermore, GDNs offer a robust platform for programming autonomous temporal functions, exemplified by GDN-mediated temporal programming of </span>RNA<span> transcription and DNA condensate dynamics.</span></div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"11 9","pages":"Article 102593"},"PeriodicalIF":19.6,"publicationDate":"2025-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144145616","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

Not going back: Unidirectional movement by intramolecular one-way ratcheting of functionalized cyclodextrin 不回头：功能化环糊精分子内单向棘轮的单向运动

IF 19.6 1区化学

Chem Pub Date : 2025-09-11 DOI: 10.1016/j.chempr.2025.102623

Enxu Liu , Dania Daou , Bernold Hasenknopf , Guillaume Vives , Matthieu Sollogoub

{"title":"Not going back: Unidirectional movement by intramolecular one-way ratcheting of functionalized cyclodextrin","authors":"Enxu Liu , Dania Daou , Bernold Hasenknopf , Guillaume Vives , Matthieu Sollogoub","doi":"10.1016/j.chempr.2025.102623","DOIUrl":"10.1016/j.chempr.2025.102623","url":null,"abstract":"<div><div>The achievement of unidirectional molecular movement is a significant challenge due to competition by Brownian motion. Nature can overcome this problem by employing chemically fueled Brownian ratcheting mechanisms to power biomolecular motors, the understanding of which has, in turn, inspired chemists to design artificial molecular systems with similar functionality. Here, we demonstrate that a selectively functionalized cyclodextrin threaded onto an axle with three segments undergoes unidirectional movement. The cyclodextrin’s unique 3D structure enables both rim-selective functionalization and a regioselective deprotection reaction of temporary stoppers on the rotaxane axle. In this system, the cyclodextrin can actively open stoppering gates in one direction only. Its forward movement is further favored by a gate-closing reaction, which occurs faster when the cyclodextrin has crossed the gate, which is also caused by its cone shape. We have thus delineated a synergistic double-gated one-way ratchet thanks to the specific 3D structure of the cyclodextrin.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"11 9","pages":"Article 102623"},"PeriodicalIF":19.6,"publicationDate":"2025-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144252625","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

Construction of axially chiral heterobiaryls via Rh-catalyzed atroposelective single-carbon insertion 通过铑催化的单碳选择性插入构建轴手性杂二芳基

IF 19.6 1区化学

Chem Pub Date : 2025-09-11 DOI: 10.1016/j.chempr.2025.102710

Hong-Hao Zhang , Feng Shi

引用次数: 0

Molecule-resolvable SERSome for metabolic profiling 用于代谢谱分析的分子可分辨的SERSome

IF 19.6 1区化学

Chem Pub Date : 2025-09-11 DOI: 10.1016/j.chempr.2025.102528

Xinyuan Bi , Xiaohang Qian , Bingsen Xue , Miao Zhang , Shuyu Liu , Haoran Chen , Cheng Jin , Huidong Tang , Jian Ye

{"title":"Molecule-resolvable SERSome for metabolic profiling","authors":"Xinyuan Bi , Xiaohang Qian , Bingsen Xue , Miao Zhang , Shuyu Liu , Haoran Chen , Cheng Jin , Huidong Tang , Jian Ye","doi":"10.1016/j.chempr.2025.102528","DOIUrl":"10.1016/j.chempr.2025.102528","url":null,"abstract":"<div><div>Multiplexed detection is a challenging yet essential task in analytical chemistry, especially for complex systems. Surface-enhanced Raman spectroscopy (SERS) is a promising analytical tool due to its molecular fingerprinting capability, sensitivity, low cost, and tractability. Considering the molecular profusion and diversity, SERSome, namely, spectral set, facilitates robust detection but is still challenged by spectral overlapping-induced uncertainty of molecular assignment and multiplexed quantification. Herein, we introduce molecule-resolvable (MORE) SERSome, identifying specific analytes contributing to the complex SERS spectra, which are then used in spectral decomposition for multiplexed analysis. Taking metabolic profiling for Alzheimer’s disease as a proof of concept, ten metabolites are screened in human serum. A deep-learning model enables accurate and rapid diagnosis, achieving an area under the receiver operating characteristic curve as high as 91.5%. Comparing with conventional methods, MORE SERSome presents a methodological advancement in multiplexed detection with strong potential for general applications and fundamental research in analytical chemistry.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"11 9","pages":"Article 102528"},"PeriodicalIF":19.6,"publicationDate":"2025-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143776224","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

Depositing atom by atom: Pt–Ru–Co triple-atom catalysts 逐个原子沉积：Pt-Ru-Co三原子催化剂

IF 19.6 1区化学

Chem Pub Date : 2025-09-11 DOI: 10.1016/j.chempr.2025.102746

Hyunjoo Lee

引用次数: 0