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Alkane recognition enhanced by solvophobic interactions enables site-selective aliphatic C–H oxidation 疏溶剂相互作用增强的烷烃识别使位置选择性脂肪族C-H氧化成为可能
IF 19.1 1区 化学
Chem Pub Date : 2025-04-10 DOI: 10.1016/j.chempr.2025.102539
Marco Galeotti , Laia Vicens , Miquel Costas
{"title":"Alkane recognition enhanced by solvophobic interactions enables site-selective aliphatic C–H oxidation","authors":"Marco Galeotti ,&nbsp;Laia Vicens ,&nbsp;Miquel Costas","doi":"10.1016/j.chempr.2025.102539","DOIUrl":"10.1016/j.chempr.2025.102539","url":null,"abstract":"<div><div>Site-selective C–H oxidation in substrates devoid of functional groups is a standing chemical problem. In the March issue of <em>Chem</em>, Tiefenbacher and co-workers combine solvophobic interactions and substrate recognition via dispersion interactions between a supramolecular catalyst and methyl groups of the substrate to implement unprecedented selectivity control in aliphatic C–H oxidation.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"11 4","pages":"Article 102539"},"PeriodicalIF":19.1,"publicationDate":"2025-04-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143703449","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
Emerging trends in CO carbonylation CO羰基化的新趋势
IF 23.5 1区 化学
Chem Pub Date : 2025-04-10 DOI: 10.1016/j.chempr.2025.102503
Chang-Sheng Kuai, Yang Yuan, Xiao-Feng Wu
{"title":"Emerging trends in CO carbonylation","authors":"Chang-Sheng Kuai, Yang Yuan, Xiao-Feng Wu","doi":"10.1016/j.chempr.2025.102503","DOIUrl":"https://doi.org/10.1016/j.chempr.2025.102503","url":null,"abstract":"Carbon monoxide (CO), a simple yet versatile C1 building block, plays a pivotal role in modern synthetic chemistry, offering unique reactivity and sustainability potential. Recent advances in carbonylation chemistry have expanded the field. Transition-metal-catalyzed carbonylation has seen progress in catalyst design, including earth-abundant metals and innovative ligands, improving selectivity, efficiency, and sustainability. Ionic carbonylation has benefited from frustrated Lewis pairs, enabling milder conditions and broader substrate scopes, while radical carbonylation, leveraging photochemical and single-electron pathways, has unlocked novel transformations. These advancements highlight CO’s potential to address key challenges in catalysis and carbon neutrality by converting industrial CO emissions into value-added products. Moving forward, opportunities include expanding substrate compatibility, replacing noble metals, and integrating emerging technologies like flow chemistry and AI-driven catalyst design. These developments underscore the transformative impact of CO chemistry on sustainable synthesis and its vital role in addressing global environmental challenges.","PeriodicalId":268,"journal":{"name":"Chem","volume":"90 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2025-04-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143814149","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
Enhancing multi-resonance thermally activated delayed fluorescence emission via through-space heavy-atom effect 通过穿透空间重原子效应增强多共振热激活延迟荧光发射
IF 19.1 1区 化学
Chem Pub Date : 2025-04-10 DOI: 10.1016/j.chempr.2024.10.020
Qi Zheng , Yang-Kun Qu , Peng Zuo , Hai-Tian Yuan , Yue-Jian Yang , Yu-Chen Qiu , Liang-Sheng Liao , Dong-Ying Zhou , Zuo-Quan Jiang
{"title":"Enhancing multi-resonance thermally activated delayed fluorescence emission via through-space heavy-atom effect","authors":"Qi Zheng ,&nbsp;Yang-Kun Qu ,&nbsp;Peng Zuo ,&nbsp;Hai-Tian Yuan ,&nbsp;Yue-Jian Yang ,&nbsp;Yu-Chen Qiu ,&nbsp;Liang-Sheng Liao ,&nbsp;Dong-Ying Zhou ,&nbsp;Zuo-Quan Jiang","doi":"10.1016/j.chempr.2024.10.020","DOIUrl":"10.1016/j.chempr.2024.10.020","url":null,"abstract":"<div><div>Recent research has focused on the heavy-atom effect in organic luminescent materials, especially in multi-resonance thermally activated delayed fluorescence (MR-TADF) emitters. Traditional strategies involve directly conjugating heavy atoms to the chromophore, which often broadens the emission spectrum. This study explores an unconventional approach using the through-space heavy-atom effect, positioning heavy-atom moieties with nonconjugated short-range interaction with the chromophore. This method successfully demonstrates the “intramolecular external heavy-atom effect” proposed in the 1970s in cutting-edge high-efficiency emissive materials. Comparative analysis of these emitters confirms the spatial heavy-atom effect, maintaining the spectroscopic properties of MR chromophore while significantly improving external quantum efficiency in organic light-emitting diodes (OLEDs). These emitters also mitigate efficiency roll-off, showcasing the potential of spatial interactions to enhance MR-TADF materials for OLED applications.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"11 4","pages":"Article 102353"},"PeriodicalIF":19.1,"publicationDate":"2025-04-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142610117","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
Antigen spatial-matching polyaptamer nanostructure to block coronavirus infection and alleviate inflammation 用于阻断冠状病毒感染和缓解炎症的抗原空间匹配聚aptamer 纳米结构
IF 19.1 1区 化学
Chem Pub Date : 2025-04-10 DOI: 10.1016/j.chempr.2024.10.021
Jingqi Chen , Yuqing Li , Xueliang Liu , Hongyi Li , Jiawei Zhu , Rui Ma , Linxin Tian , Lu Yu , Jiabei Li , Zhuang Liu , Weihong Tan , Yu Yang
{"title":"Antigen spatial-matching polyaptamer nanostructure to block coronavirus infection and alleviate inflammation","authors":"Jingqi Chen ,&nbsp;Yuqing Li ,&nbsp;Xueliang Liu ,&nbsp;Hongyi Li ,&nbsp;Jiawei Zhu ,&nbsp;Rui Ma ,&nbsp;Linxin Tian ,&nbsp;Lu Yu ,&nbsp;Jiabei Li ,&nbsp;Zhuang Liu ,&nbsp;Weihong Tan ,&nbsp;Yu Yang","doi":"10.1016/j.chempr.2024.10.021","DOIUrl":"10.1016/j.chempr.2024.10.021","url":null,"abstract":"<div><div>Preparation for the potential emergence of future human coronaviruses (HCoVs) calls for the development of versatile and effective treatment strategies. The signs and symptoms of HCoVs include an immune inflammatory response. Therefore, our study focuses on the simultaneous inhibition of HCoV infection and the alleviation of lung inflammation. Inspired by conformational epitope matching, we engineered a <em>de novo</em> antigen spatial-matching polyaptamer (ASM-pApt) nanostructure designed to align perfectly with multiple spike (S) proteins on severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) pseudovirus (PsV). Compared with monovalent aptamer, the dissociation constant (K<sub>D</sub>) of the ASM-pApt nanostructure decreased by over 1,000-fold, and its viral semi-inhibitory concentration (IC<sub>50</sub>) improved by over 100,000-fold to 89.7 fM (fmol/L), indicating the effectiveness of antigen spatial matching. By loading polyphenol as anti-inflammatory drug and chitosan (CS) as an excipient, the ASM-pApt nanostructure showed anti-inflammatory and long drug retention properties. Our design shows the promise of polyaptamer as an antiviral/anti-inflammatory candidate against emerging HCoVs in the future.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"11 4","pages":"Article 102354"},"PeriodicalIF":19.1,"publicationDate":"2025-04-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142678776","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
Switchable diversification of quaternary ammonium salts using photocatalysis 利用光催化实现季铵盐的可切换多样化
IF 19.1 1区 化学
Chem Pub Date : 2025-04-10 DOI: 10.1016/j.chempr.2024.11.004
Takumi Kinoshita , Yota Sakakibara , Tomoko Hirano , Kei Murakami
{"title":"Switchable diversification of quaternary ammonium salts using photocatalysis","authors":"Takumi Kinoshita ,&nbsp;Yota Sakakibara ,&nbsp;Tomoko Hirano ,&nbsp;Kei Murakami","doi":"10.1016/j.chempr.2024.11.004","DOIUrl":"10.1016/j.chempr.2024.11.004","url":null,"abstract":"<div><div>Over the past few decades, significant advances have been made in the radical chemistry of amine molecules. However, the radical reactions of related quaternary ammonium salts remain comparatively underexplored. If radicals could be generated from ammonium salts in a controlled manner, this could lead to a method for producing distonic radical cations, offering valuable synthetic applications for quaternary ammonium salts and their tertiary amine derivatives. In this study, we developed a photoredox-catalyzed method for derivatizing quaternary ammonium salts by reacting α-haloalkylammonium salts with olefins. The key to success is the photocatalytic generation of distonic α-ammonio radicals under both oxidative and reductive quenching conditions. This chemistry enables selective and switchable alkylations and alkenylations, affording structurally new quaternary ammonium salts. The utility of this procedure is showcased in the divergent synthesis and derivatization of bioactive quaternary ammonium salts, a deuterated tertiary amine, and the identification of salinity-tolerance-conferring molecules.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"11 4","pages":"Article 102366"},"PeriodicalIF":19.1,"publicationDate":"2025-04-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142816436","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
Electrophilic selenium drives electron leakage 亲电性硒驱动电子泄漏
IF 19.1 1区 化学
Chem Pub Date : 2025-04-10 DOI: 10.1016/j.chempr.2025.102499
Ruyi Zhou , Jicheng Yu , Zhen Gu
{"title":"Electrophilic selenium drives electron leakage","authors":"Ruyi Zhou ,&nbsp;Jicheng Yu ,&nbsp;Zhen Gu","doi":"10.1016/j.chempr.2025.102499","DOIUrl":"10.1016/j.chempr.2025.102499","url":null,"abstract":"<div><div>Disrupting redox homeostasis in cancer cells represents a promising strategy for minimizing toxicity and improving chemotherapy outcomes. In <em>Cell Biomaterials</em>, Chen, Ma, and colleagues describe an approach that employs a selenium electrophilic center with rapid electron-shuttle properties to boost mitochondrial electron leakage and thus convert antioxidants into pro-oxidants for cancer therapy.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"11 4","pages":"Article 102499"},"PeriodicalIF":19.1,"publicationDate":"2025-04-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143635553","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
BINOLates as potent reducing photocatalysts for inert-bond activation and reduction of unsaturated systems 作为惰性键活化和还原不饱和体系的强效还原光催化剂的双乙醇酸盐
IF 19.1 1区 化学
Chem Pub Date : 2025-04-10 DOI: 10.1016/j.chempr.2024.10.026
Can Liu , Yan Zhang , Rui Shang
{"title":"BINOLates as potent reducing photocatalysts for inert-bond activation and reduction of unsaturated systems","authors":"Can Liu ,&nbsp;Yan Zhang ,&nbsp;Rui Shang","doi":"10.1016/j.chempr.2024.10.026","DOIUrl":"10.1016/j.chempr.2024.10.026","url":null,"abstract":"<div><div>Phenolates are increasingly studied as photocatalysts because of their abundance and easy accessibility. However, their potential as potent and broadly applicable reducing photoredox catalysts is hindered by the high electronegativity of oxygen and the reactivity of phenoxy radicals. Herein, we discovered that renowned 1,1′-Bi-2-naphtholate derivatives (BINOLates) are potent reducing photocatalysts. These catalysts are effective for the activation of inert bonds and the reduction of unsaturated bonds, including selective CF activation of activated –CF<sub>3</sub>,–CF<sub>2</sub>H, –C<sub>2</sub>F<sub>5</sub>, and aryl fluoride, activation of alkyl and aryl chlorides, detosylation, Birch reduction, and alkene reduction, demonstrating potent reducing ability and catalytic versatility. Defluoroalkylation using PhCF<sub>3</sub> as a limiting reagent, a challenging substrate for reported catalysts, proceeded smoothly. BINOLates were applicable as photoredox catalysts even under green light. This work introduces a new catalytic application for the renowned BINOLates, suggesting the potential for future expansion of their applications in the realm of photocatalysis.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"11 4","pages":"Article 102359"},"PeriodicalIF":19.1,"publicationDate":"2025-04-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142805258","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
Depolymerizing off-the-shelf polymethacrylates with visible light 用可见光解聚现成的聚甲基丙烯酸酯
IF 19.1 1区 化学
Chem Pub Date : 2025-04-10 DOI: 10.1016/j.chempr.2025.102540
Nicholas Ballard , Haritz Sardon
{"title":"Depolymerizing off-the-shelf polymethacrylates with visible light","authors":"Nicholas Ballard ,&nbsp;Haritz Sardon","doi":"10.1016/j.chempr.2025.102540","DOIUrl":"10.1016/j.chempr.2025.102540","url":null,"abstract":"<div><div>As the recycling of polymer materials becomes a topic of growing societal importance, there is a need to develop robust methods for dealing with plastic waste. In a recent article in <em>Science</em>, Anastasaki and co-workers report a route for the efficient chemical recycling of commercial polymethacrylates via low-temperature depolymerization using visible light.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"11 4","pages":"Article 102540"},"PeriodicalIF":19.1,"publicationDate":"2025-04-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143703516","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
Intramolecular through-space heavy-atom effect in π-stacked MR-TADF emitters π堆叠MR-TADF发射体分子内穿越空间重原子效应
IF 19.1 1区 化学
Chem Pub Date : 2025-04-10 DOI: 10.1016/j.chempr.2024.11.015
Sheng-Yi Yang , Cheng Liu , Fei Wang , Ben Zhong Tang
{"title":"Intramolecular through-space heavy-atom effect in π-stacked MR-TADF emitters","authors":"Sheng-Yi Yang ,&nbsp;Cheng Liu ,&nbsp;Fei Wang ,&nbsp;Ben Zhong Tang","doi":"10.1016/j.chempr.2024.11.015","DOIUrl":"10.1016/j.chempr.2024.11.015","url":null,"abstract":"<div><div>In this issue of <em>Chem</em>, Jiang and colleagues utilized a spiro-fluorene unit as a π-bridge to construct a series of π-stacked multi-resonance thermally activated delayed fluorescence emitters. By introducing different heavy atoms through chemical bonding, they revealed the impact of the intramolecular through-space heavy-atom effect on the optoelectronic properties of the molecules.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"11 4","pages":"Article 102377"},"PeriodicalIF":19.1,"publicationDate":"2025-04-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143608742","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
Electrolyte: The cornerstone of commercializing the electrosynthesis of H2O2 电解液：电合成H2O2商业化的基石
IF 19.1 1区 化学
Chem Pub Date : 2025-04-10 DOI: 10.1016/j.chempr.2025.102536
Chang Long (隆昶) , Zhiyong Tang (唐智勇)
{"title":"Electrolyte: The cornerstone of commercializing the electrosynthesis of H2O2","authors":"Chang Long (隆昶) ,&nbsp;Zhiyong Tang (唐智勇)","doi":"10.1016/j.chempr.2025.102536","DOIUrl":"10.1016/j.chempr.2025.102536","url":null,"abstract":"<div><div>In this issue of <em>Chem</em>, Strasser and co-workers introduce an electrolyte design that leverages the alkali-metal enhancement effect for the sustainable electrosynthesis of H<sub>2</sub>O<sub>2</sub> from oxygen. This little electrolyte alteration, combined with a cost-effective commercial carbon-based gas-diffusion electrode, represents a significant advancement toward the green production of H<sub>2</sub>O<sub>2</sub>.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"11 4","pages":"Article 102536"},"PeriodicalIF":19.1,"publicationDate":"2025-04-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143695861","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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