Chem最新文献_第9页

Unstructured protein mimics have enzymatic activity 非结构蛋白质模拟物具有酶活性

IF 19.6 1区化学

Chem Pub Date : 2026-03-12 Epub Date: 2026-02-26 DOI: 10.1016/j.chempr.2026.102996

Felipe Jiménez-Ángeles , Monica Olvera de la Cruz

引用次数: 0

A redesigned aldehyde dehydrogenase enables intermolecular biocatalytic amide formation from aldehydes and amines 重新设计的醛脱氢酶使分子间的生物催化酰胺形成从醛和胺

IF 19.6 1区化学

Chem Pub Date : 2026-03-12 Epub Date: 2026-02-25 DOI: 10.1016/j.chempr.2026.102994

Francesco Mascia , Magdalena Abramiuk , Aneta Swárovská , Wolfgang Kroutil

引用次数: 0

Vacancy-interface coupling in nanomaterials for photocatalytic energy and environmental applications 纳米材料在光催化能源和环境方面的应用

IF 19.6 1区化学

Chem Pub Date : 2026-03-12 Epub Date: 2026-02-19 DOI: 10.1016/j.chempr.2025.102913

Meijun Guo , Shuai Zhang , Jingrun Ran , Shi-Zhang Qiao

{"title":"Vacancy-interface coupling in nanomaterials for photocatalytic energy and environmental applications","authors":"Meijun Guo , Shuai Zhang , Jingrun Ran , Shi-Zhang Qiao","doi":"10.1016/j.chempr.2025.102913","DOIUrl":"10.1016/j.chempr.2025.102913","url":null,"abstract":"<div><div>Vacancy-interface coupling has emerged as a powerful strategy for boosting photocatalytic performance through the synergistic regulation of charge dynamics, interfacial structure, and surface pathways. Engineering vacancies at interfaces allow photogenerated carriers to be trapped, separated, and directed to reactive sites, enhancing activity and selectivity. This perspective highlights recent advances in vacancy-mediated interfacial engineering for solar-driven transformations through representative cases in plastics and biomass photoreforming, H<sub>2</sub>O<sub>2</sub> evolution, water splitting, and CO<sub>2</sub> reduction. Particular emphasis is placed on <em>in situ</em> spectroscopic evidence for the dynamic evolution of vacancies and their real-time interactions with reactive sites. By integrating experimental insights with theoretical modeling, we demonstrate how vacancy-interface coupling results in robust, tunable, and efficient photocatalysts. Finally, we outline key challenges and opportunities for developing robust and application-oriented systems that fully exploit defect-interface synergy for sustainable energy and environmental applications.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"12 3","pages":"Article 102913"},"PeriodicalIF":19.6,"publicationDate":"2026-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147428672","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

Understanding and mitigating degradation in amine-based sorbents for CO2 direct air capture 了解和减轻胺基吸附剂对二氧化碳直接空气捕获的降解

IF 19.6 1区化学

Chem Pub Date : 2026-03-12 Epub Date: 2026-02-26 DOI: 10.1016/j.chempr.2026.102958

Anthony J. Varni , Wade A. Braunecker , Marcos F. Calegari Andrade , G. Michael Carroll , Yoseph A. Guta , Elwin Hunter-Sellars , Christopher W. Jones , Noemi Leick , Sichi Li , Amitesh Maiti , Maxwell A.T. Marple , Hyun June Moon , Miles A. Sakwa-Novak , Carsten Sievers , Nicholas A. Strange , Simon H. Pang

{"title":"Understanding and mitigating degradation in amine-based sorbents for CO2 direct air capture","authors":"Anthony J. Varni , Wade A. Braunecker , Marcos F. Calegari Andrade , G. Michael Carroll , Yoseph A. Guta , Elwin Hunter-Sellars , Christopher W. Jones , Noemi Leick , Sichi Li , Amitesh Maiti , Maxwell A.T. Marple , Hyun June Moon , Miles A. Sakwa-Novak , Carsten Sievers , Nicholas A. Strange , Simon H. Pang","doi":"10.1016/j.chempr.2026.102958","DOIUrl":"10.1016/j.chempr.2026.102958","url":null,"abstract":"<div><div>The success of direct air capture (DAC) of CO<sub>2</sub> depends on sorbents that combine high capacity, low energy requirements, and long-term durability. Amine-based sorbents—including solid-supported aminopolymers, grafted amines, and amine-functionalized resins—remain the leading candidates, but their limited lifetimes drive up costs and constrain deployment. In this review, we outline the current understanding of amine-based sorbent degradation with an emphasis on clearly identifying what is known about structure-property-performance relationships, as well as important knowledge gaps. More specifically, we discuss how polymer chemistry, sorbent design variables, and environmental and process conditions contribute to performance loss. In parallel, we outline how advances in spectroscopy, modeling, and accelerated testing are beginning to illuminate chemical and physical degradation mechanisms. Looking forward, we identify future research directions that will be critical for gaining a deeper understanding of degradation, as well as opportunities for developing innovative mitigation strategies for improving the lifetime of amine-based sorbents.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"12 3","pages":"Article 102958"},"PeriodicalIF":19.6,"publicationDate":"2026-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147428673","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

Time-resolved exciton delocalization from transient absorption spectroscopy 瞬态吸收光谱的时间分辨激子离域

IF 19.6 1区化学

Chem Pub Date : 2026-03-12 Epub Date: 2025-10-24 DOI: 10.1016/j.chempr.2025.102790

Yuanheng Wang , Catrina P. Oberg , Yue Hu , Raina M. Morley , Emely Freytag , Christoph Lambert , Gregory D. Scholes

{"title":"Time-resolved exciton delocalization from transient absorption spectroscopy","authors":"Yuanheng Wang , Catrina P. Oberg , Yue Hu , Raina M. Morley , Emely Freytag , Christoph Lambert , Gregory D. Scholes","doi":"10.1016/j.chempr.2025.102790","DOIUrl":"10.1016/j.chempr.2025.102790","url":null,"abstract":"<div><div>The temporal evolution of exciton delocalization in aggregates determines the excitons’ dynamics. Although the equilibrium exciton delocalization length can be measured through several well-established methods, capturing its temporal dynamics remains challenging. Here, we present an experimental approach to quantifying the time-dependent evolution of exciton delocalization in aggregates through transient absorption spectroscopy. Our method employs excited-state absorption and stimulated emission to probe the exciton delocalization while utilizing ground-state absorption to track and filter out the evolution of exciton concentration through a ratio-based analysis. Through experimental validations and theoretical simulations, we demonstrate that this approach quantitatively captures the temporal evolution of exciton delocalization while remaining insensitive to concurrent competing dynamics, such as exciton-exciton annihilation. Furthermore, this methodology could be extended to measure the time-resolved quantum Fisher information in molecular aggregate systems.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"12 3","pages":"Article 102790"},"PeriodicalIF":19.6,"publicationDate":"2026-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147428978","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

Achieving well-ordered microstructure and enhanced conductivities in n-doped conjugated polymers via dual-affinity dopant 通过双亲和掺杂剂实现n掺杂共轭聚合物的有序微观结构和增强电导率

IF 19.6 1区化学

Chem Pub Date : 2026-03-12 Epub Date: 2025-09-23 DOI: 10.1016/j.chempr.2025.102755

Chen-Kai Pan , Yi-Fan Huang , Zi-Di Yu , Ze-Fan Yao , Chi-Yuan Yang , Jie-Yu Wang , Jian Pei

{"title":"Achieving well-ordered microstructure and enhanced conductivities in n-doped conjugated polymers via dual-affinity dopant","authors":"Chen-Kai Pan , Yi-Fan Huang , Zi-Di Yu , Ze-Fan Yao , Chi-Yuan Yang , Jie-Yu Wang , Jian Pei","doi":"10.1016/j.chempr.2025.102755","DOIUrl":"10.1016/j.chempr.2025.102755","url":null,"abstract":"<div><div>Doping is a key approach to adjusting the electrical conductivities of polymer devices. However, the disruption to the microstructure of conjugated polymers from counterions of the dopant is the crucial factor limiting performance improvement. Herein, we propose a dual-affinity strategy for dopant design and present a novel n-type dopant, pTAM, with a 2-aminobenzimidazole triaminomethane structure. This pTAM dopant can significantly improve the electrical conductivity of several classic conjugated polymers with a 40%–240% increase in electrical conductivities compared with polymers doped by the widely used dopant 1,3-dimethyl-2-phenylbenzimidazoline (N-DMBI), reaching 83.3 ± 5.1 S cm<sup>−1</sup>. The enhanced performance is attributed to the matched interaction between pTAM cation and doped conjugated polymer, maintaining a well-ordered microstructure. Our work emphasizes the importance of the dopant-polymer microstructure relationship to the electrical performance, providing a corresponding effective strategy of dopant design for organic electronics and modern semiconductors.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"12 3","pages":"Article 102755"},"PeriodicalIF":19.6,"publicationDate":"2026-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145116788","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

Robust B–H perdeuteration of polyhedral boron clusters with D2O by Pd(II)-catalytic electrophilic H/D exchange and intermolecular Pd migration 通过Pd（II）催化亲电H/D交换和分子间Pd迁移，D2O对多面体硼团簇进行稳健的B-H过氘

IF 19.6 1区化学

Chem Pub Date : 2026-03-12 Epub Date: 2025-10-15 DOI: 10.1016/j.chempr.2025.102788

Yu-He Liang , Jia-Xin Kang , Yan Wang , Yi-Ge Li , Hou-Ji Cao , Qianyi Zhao , Xuenian Chen , Yan-Na Ma

{"title":"Robust B–H perdeuteration of polyhedral boron clusters with D2O by Pd(II)-catalytic electrophilic H/D exchange and intermolecular Pd migration","authors":"Yu-He Liang , Jia-Xin Kang , Yan Wang , Yi-Ge Li , Hou-Ji Cao , Qianyi Zhao , Xuenian Chen , Yan-Na Ma","doi":"10.1016/j.chempr.2025.102788","DOIUrl":"10.1016/j.chempr.2025.102788","url":null,"abstract":"<div><div>The selective B–H functionalization of carboranes has received considerable attention because of their wide applications in functional materials, catalysis, and pharmaceuticals. Deuterium-labeling experiments and kinetic-isotope-effect experiments are two important tools for mechanistic studies on the selective B–H activation of carboranes. Thus, developing an effective method for the synthesis of perdeuterated carboranes is highly desirable. Herein, we present a practical method for synthesizing perdeuterated carboranes via Pd(II)-catalyzed B–H activation by using D<sub>2</sub>O as a deuterium source. This protocol features extraordinary functional-group tolerance, high levels of deuterium incorporation, and ease of scaling. Mechanistic studies illustrate that the deuteration reaction proceeds via Pd(II)-catalytic electrophilic H/D exchange and subsequent intermolecular Pd migration. The same degree of deuterium incorporation across all boron vertices indicates that the Pd-migration step is faster than the electrophilic palladation step. Additionally, the versatility of this method is reflected in the deuteration of other boron clusters.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"12 3","pages":"Article 102788"},"PeriodicalIF":19.6,"publicationDate":"2026-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145289331","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

Primitive genotype-phenotype coupling in fuel-dependent synthetic cells with an autocatalyst 燃料依赖合成细胞的原始基因型-表型偶联

IF 19.6 1区化学

Chem Pub Date : 2026-03-12 Epub Date: 2025-11-05 DOI: 10.1016/j.chempr.2025.102816

Héctor Soria-Carrera , Leonie Kauling , Job Boekhoven

引用次数: 0

Ion-exchange-mediated pre-association gates interfacial PCET 离子交换介导的预缔合门界面

IF 19.6 1区化学

Chem Pub Date : 2026-03-12 Epub Date: 2025-11-21 DOI: 10.1016/j.chempr.2025.102813

Noah B. Lewis , Joseph Kelly , Joel G. Gardner , Neil K. Razdan , Shane Ardo , Thomas E. Markland , Yogesh Surendranath

{"title":"Ion-exchange-mediated pre-association gates interfacial PCET","authors":"Noah B. Lewis , Joseph Kelly , Joel G. Gardner , Neil K. Razdan , Shane Ardo , Thomas E. Markland , Yogesh Surendranath","doi":"10.1016/j.chempr.2025.102813","DOIUrl":"10.1016/j.chempr.2025.102813","url":null,"abstract":"<div><div>Interfacial proton-coupled electron transfer (I-PCET) is typically viewed as a single elementary reaction despite general recognition that analogous solution-phase reactivity requires proton donor-acceptor pre-association. Herein, we examine the role of pre-association in I-PCET to a graphite-conjugated carboxylic acid (GC-COOH) surface by quantifying electrolyte pH and I-PCET kinetics as a function of NaClO<sub>4</sub> concentrations up to 17 mol kg<sup>−1</sup>. In acidic and acetate-buffered media, we observed attenuations in the I-PCET rate relative to those expected given the solution pH. To account for the influence of electrolyte concentration on I-PCET rate, we propose a multiple-step model wherein the exchange of interfacial Na<sup>+</sup> for H<sub>3</sub>O<sup>+</sup> to form a hydrogen-bonded pre-association complex precedes rate-limiting concerted proton-electron transfer. In this model, the increased electrolyte concentration inhibits H<sub>3</sub>O<sup>+</sup> pre-association, a phenomenon that is recovered in molecular dynamics simulations. These studies demonstrate the non-innocence of supporting electrolyte and expose the key role that pre-association equilibria play in I-PCET mechanisms.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"12 3","pages":"Article 102813"},"PeriodicalIF":19.6,"publicationDate":"2026-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145560485","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

Second near-infrared fluorophores: Rational design, optical enhancement strategies, and recent advances in imaging-guided biomedical applications 第二近红外荧光团：合理设计，光学增强策略，以及成像引导生物医学应用的最新进展

IF 19.6 1区化学

Chem Pub Date : 2026-03-12 Epub Date: 2026-02-02 DOI: 10.1016/j.chempr.2025.102867

Honglei Yu , Lin Ai , Siyu Lu

{"title":"Second near-infrared fluorophores: Rational design, optical enhancement strategies, and recent advances in imaging-guided biomedical applications","authors":"Honglei Yu , Lin Ai , Siyu Lu","doi":"10.1016/j.chempr.2025.102867","DOIUrl":"10.1016/j.chempr.2025.102867","url":null,"abstract":"<div><div>Fluorescence imaging in the second near-infrared window (NIR-II, 1,000–3,000 nm), where biological tissues exhibit optical transparency, has garnered significant attention. Owing to the minimal tissue absorption, scattering, and autofluorescence in this spectral region, NIR-II fluorescence imaging enables non-invasive <em>in vivo</em> imaging at millimeter-scale depths. Over the past decade, studies have focused on the development of NIR-II fluorophores with minimal background interference from tissues. This review focuses on strategies to optimize fluorophore performance, aiming to enhance the tissue penetration depth and imaging contrast. First, we discuss recent strategies for wavelength tuning and brightness enhancement of functional NIR-II fluorophores, categorized by their composition into organic and inorganic fluorophores. Subsequently, we summarize the latest biomedical applications and discuss the opportunities and challenges of their clinical translation, aiming to advance the clinical application of the NIR-II imaging technology. Overall, this review provides a forward-looking perspective to guide the future development of NIR-II fluorophores.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"12 3","pages":"Article 102867"},"PeriodicalIF":19.6,"publicationDate":"2026-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146101831","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