Pub Date : 2025-09-24DOI: 10.1016/j.cclet.2025.111892
Dengke Ma , Youai Qiu
Enantioselective enamine catalysis has enriched asymmetric synthesis by enabling precise stereochemical control. While classically thermal/photochemical strategies have expanded reaction diversity, electrochemical enantiocontrol remains underexplored despite its potential for tunable redox manipulation. This review systematically evaluates electrochemical enantioselective enamine catalysis through polar/radical mediated chemical bond formation pathways, aiming to delineate current mechanistic paradigms and highlight electrochemistry’s unique role on asymmetric enamine catalysis beyond thermodynamic and photochemical conditions. Future efforts including developing enhanced compatibility of chiral catalysts and intermediates with electrochemical systems, as well as exploiting transformative techniques for mechanistic elucidation could be promising to unlock more novel transformations and stereoselectivity models.
{"title":"Electrochemical strategies for advancing enantioselective enamine catalysis","authors":"Dengke Ma , Youai Qiu","doi":"10.1016/j.cclet.2025.111892","DOIUrl":"10.1016/j.cclet.2025.111892","url":null,"abstract":"<div><div>Enantioselective enamine catalysis has enriched asymmetric synthesis by enabling precise stereochemical control. While classically thermal/photochemical strategies have expanded reaction diversity, electrochemical enantiocontrol remains underexplored despite its potential for tunable redox manipulation. This review systematically evaluates electrochemical enantioselective enamine catalysis through polar/radical mediated chemical bond formation pathways, aiming to delineate current mechanistic paradigms and highlight electrochemistry’s unique role on asymmetric enamine catalysis beyond thermodynamic and photochemical conditions. Future efforts including developing enhanced compatibility of chiral catalysts and intermediates with electrochemical systems, as well as exploiting transformative techniques for mechanistic elucidation could be promising to unlock more novel transformations and stereoselectivity models.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"37 4","pages":"Article 111892"},"PeriodicalIF":8.9,"publicationDate":"2025-09-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145974786","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}
Pub Date : 2025-09-23DOI: 10.1016/j.cclet.2025.111875
Guochao Lv , Guangzong Tian , Guodong Chen , Shengyong Zhu , Jialong Bao , Chunjun Qin , Xiaopeng Zou , Jing Hu , Peter H. Seeberger , Jian Yin
Pseudomonas aeruginosa is an opportunistic pathogen responsible for severe nosocomial infections. This multidrug-resistant bacterium can cause pneumonia and cystic fibrosis, both of which are associated with high morbidity and mortality rates. The lipopolysaccharide of P. aeruginosa serves as an attractive target for the development of effective glycoconjugate vaccines. In this article, we report the first chemical synthesis of the highly challenging tetrasaccharide repeating unit of the P. aeruginosa serotype O3 O-antigen using a two-directional [1+(2 + 1)] glycosylation strategy. The synthesis is particularly challenging due to the poor nucleophilicity of the axial C4 hydroxyl group of l-galactose and the steric hindrance imposed by the 3S-hydroxybutyryl (Hb) chain. Furthermore, the presence of an acetyl group at the ortho position relative to the glycosylation site on l-galactose can lead to undesirable acetyl migration. Additionally, it is noteworthy that the selective removal of a 2-naphthylmethyl ether (Nap) during the late stages of synthesis, particularly in the presence of multiple benzyl groups, can be somewhat challenging to predict. Through the careful selection of synthetic strategies, building blocks, and optimized reaction conditions, we achieved the stereoselective glycosylations, selective oxidation of primary alcohols, remarkable enhancement of acceptor activity, and efficient introduction of the 3S-Hb group. The synthetic methodology presented in this work serves as a valuable reference for the preparation of structurally related oligosaccharides. By incorporating an aminopropyl linker, the target tetrasaccharide facilitates glycan microarray preparation and in vivo immunological assessments, thereby accelerating progress toward a synthetic glycoconjugate vaccine for P. aeruginosa.
{"title":"Chemical synthesis of the highly functionalized O-antigen repeating unit from Pseudomonas aeruginosa serotype O3 for glycoconjugate vaccine development","authors":"Guochao Lv , Guangzong Tian , Guodong Chen , Shengyong Zhu , Jialong Bao , Chunjun Qin , Xiaopeng Zou , Jing Hu , Peter H. Seeberger , Jian Yin","doi":"10.1016/j.cclet.2025.111875","DOIUrl":"10.1016/j.cclet.2025.111875","url":null,"abstract":"<div><div><em>Pseudomonas aeruginosa</em> is an opportunistic pathogen responsible for severe nosocomial infections. This multidrug-resistant bacterium can cause pneumonia and cystic fibrosis, both of which are associated with high morbidity and mortality rates. The lipopolysaccharide of <em>P. aeruginosa</em> serves as an attractive target for the development of effective glycoconjugate vaccines. In this article, we report the first chemical synthesis of the highly challenging tetrasaccharide repeating unit of the <em>P. aeruginosa</em> serotype O3 O-antigen using a two-directional [1+(2 + 1)] glycosylation strategy. The synthesis is particularly challenging due to the poor nucleophilicity of the axial C4 hydroxyl group of <span>l</span>-galactose and the steric hindrance imposed by the 3<em>S</em>-hydroxybutyryl (Hb) chain. Furthermore, the presence of an acetyl group at the ortho position relative to the glycosylation site on <span>l</span>-galactose can lead to undesirable acetyl migration. Additionally, it is noteworthy that the selective removal of a 2-naphthylmethyl ether (Nap) during the late stages of synthesis, particularly in the presence of multiple benzyl groups, can be somewhat challenging to predict. Through the careful selection of synthetic strategies, building blocks, and optimized reaction conditions, we achieved the stereoselective glycosylations, selective oxidation of primary alcohols, remarkable enhancement of acceptor activity, and efficient introduction of the 3<em>S</em>-Hb group. The synthetic methodology presented in this work serves as a valuable reference for the preparation of structurally related oligosaccharides. By incorporating an aminopropyl linker, the target tetrasaccharide facilitates glycan microarray preparation and <em>in vivo</em> immunological assessments, thereby accelerating progress toward a synthetic glycoconjugate vaccine for <em>P. aeruginosa</em>.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"37 2","pages":"Article 111875"},"PeriodicalIF":8.9,"publicationDate":"2025-09-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145578509","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}
Pub Date : 2025-09-18DOI: 10.1016/j.cclet.2025.111859
Jingying Wang , Jianhui Zhao , Shaopo Wang , Jingjie Yu , Ning Li
Catalytic CO2-to-methanol conversion presents a synergistic approach for concurrent greenhouse gas abatement and sustainable energy carrier synthesis. Single-atom catalysts (SACs) with maximized atomic utilization, tailored electronic configurations and unique metal-support interactions, exhibit superior performance in CO2 activation and methanol synthesis. This review systematically compares reaction mechanisms and pathways across thermal, photocatalytic and electrocatalytic systems, emphasizing structure-activity relationships governed by active sites, coordination microenvironments and support functionalities. Through case studies of representative SACs, we elucidate how metal-support synergies dictate intermediate binding energetics and methanol selectivity. A critical analysis of reaction parameters (e.g., temperature, pressure) reveals condition-dependent catalytic behaviors in thermal system, with fewer studies in photo/electrocatalytic systems identified as key knowledge gaps. While thermal catalysis achieves industrially viable methanol yields, the scalability is constrained by energy-intensive operation and catalyst sintering. Conversely, photo/electrocatalytic routes offer renewable energy integration but suffer from inefficient charge dynamics and mass transport limitations. To address the challenges, we propose strategic research priorities on precise design of active sites, synergy of multiple technological pathways, development of intelligent catalytic systems and diverse CO2 feedstock compatibility. These insights establish a framework for developing next-generation SACs, offering both theoretical foundations and technological blueprints for developing carbon-negative catalytic technologies.
{"title":"Single-atom catalysts for CO2-to-methanol conversion: A critical review","authors":"Jingying Wang , Jianhui Zhao , Shaopo Wang , Jingjie Yu , Ning Li","doi":"10.1016/j.cclet.2025.111859","DOIUrl":"10.1016/j.cclet.2025.111859","url":null,"abstract":"<div><div>Catalytic CO<sub>2</sub>-to-methanol conversion presents a synergistic approach for concurrent greenhouse gas abatement and sustainable energy carrier synthesis. Single-atom catalysts (SACs) with maximized atomic utilization, tailored electronic configurations and unique metal-support interactions, exhibit superior performance in CO<sub>2</sub> activation and methanol synthesis. This review systematically compares reaction mechanisms and pathways across thermal, photocatalytic and electrocatalytic systems, emphasizing structure-activity relationships governed by active sites, coordination microenvironments and support functionalities. Through case studies of representative SACs, we elucidate how metal-support synergies dictate intermediate binding energetics and methanol selectivity. A critical analysis of reaction parameters (<em>e.g.</em>, temperature, pressure) reveals condition-dependent catalytic behaviors in thermal system, with fewer studies in photo/electrocatalytic systems identified as key knowledge gaps. While thermal catalysis achieves industrially viable methanol yields, the scalability is constrained by energy-intensive operation and catalyst sintering. Conversely, photo/electrocatalytic routes offer renewable energy integration but suffer from inefficient charge dynamics and mass transport limitations. To address the challenges, we propose strategic research priorities on precise design of active sites, synergy of multiple technological pathways, development of intelligent catalytic systems and diverse CO<sub>2</sub> feedstock compatibility. These insights establish a framework for developing next-generation SACs, offering both theoretical foundations and technological blueprints for developing carbon-negative catalytic technologies.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"37 2","pages":"Article 111859"},"PeriodicalIF":8.9,"publicationDate":"2025-09-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145691162","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}
Based on recently reported high-performance doubly concerted companion (DCC) dye XW96 constructed by covalently linking a porphyrin dye and an organic dye with hexyl chain protected phenothiazine and fluorenyl indoline donors, respectively, we herein employ a branched 2-ethylhexyl chain to realize better anti-charge-recombination and anti-aggregation abilities, achieving improved photovoltaic behavior. Thus, based on XW96, dye XW98 has been synthesized by introducing branched chains to the donors. As a result, the bulkier donors on both sub-dye units cause spatial repulsion, resulting in more severe twisting, decreased adsorption amount and lowered efficiency, compared to XW96. To reduce the steric hindrance, the linker between the two subdye units has been extended on the basis of XW98 (seven bonds) to give XW99 (eight bonds) and XW100 (nine bonds), affording considerably improved adsorption. Notably, XW99 affords an open-circuit voltage (VOC) of 784 mV, a short-circuit current density (JSC) of 22.08 mA/cm2, and a high power conversion efficiency (PCE) of 12.54 %. Compared with XW99, dye XW100 exhibits a larger percentage of single anchoring despite its larger adsorption amount, leading to a lowered efficiency of 12.25 %. This work indicates that combination of bulky branched chains on the donors with optimized linker length is essential for developing efficient DCC sensitizers.
{"title":"Efficient dye-sensitized solar cells based on doubly concerted companion dyes with bulky branched chains on the donors and optimized linkage length","authors":"Conglin Liu, Yinglong Li, Yuquan Hu, Qizhao Li, Chengjie Li, Yongshu Xie","doi":"10.1016/j.cclet.2025.111863","DOIUrl":"10.1016/j.cclet.2025.111863","url":null,"abstract":"<div><div>Based on recently reported high-performance doubly concerted companion (DCC) dye <strong>XW96</strong> constructed by covalently linking a porphyrin dye and an organic dye with hexyl chain protected phenothiazine and fluorenyl indoline donors, respectively, we herein employ a branched 2-ethylhexyl chain to realize better anti-charge-recombination and anti-aggregation abilities, achieving improved photovoltaic behavior. Thus, based on <strong>XW96</strong>, dye <strong>XW98</strong> has been synthesized by introducing branched chains to the donors. As a result, the bulkier donors on both sub-dye units cause spatial repulsion, resulting in more severe twisting, decreased adsorption amount and lowered efficiency, compared to <strong>XW96</strong>. To reduce the steric hindrance, the linker between the two subdye units has been extended on the basis of <strong>XW98</strong> (seven bonds) to give <strong>XW99</strong> (eight bonds) and <strong>XW100</strong> (nine bonds), affording considerably improved adsorption. Notably, <strong>XW99</strong> affords an open-circuit voltage (<em>V</em><sub>OC</sub>) of 784 mV, a short-circuit current density (<em>J</em><sub>SC</sub>) of 22.08 mA/cm<sup>2</sup>, and a high power conversion efficiency (PCE) of 12.54 %. Compared with <strong>XW99</strong>, dye <strong>XW100</strong> exhibits a larger percentage of single anchoring despite its larger adsorption amount, leading to a lowered efficiency of 12.25 %. This work indicates that combination of bulky branched chains on the donors with optimized linker length is essential for developing efficient DCC sensitizers.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"37 3","pages":"Article 111863"},"PeriodicalIF":8.9,"publicationDate":"2025-09-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145735494","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}
Pub Date : 2025-09-17DOI: 10.1016/j.cclet.2025.111842
Dechao Yuan , Tianying Luo , Qiao Su , Changxing Qu , Meng Pan , Jia Xu , Mingyi Zhang , Yuanchao Luo , Renjian He , Shiwei Liu , Xiang Fang , Hong Duan , Zhiyong Qian
Nanozymes are nanomaterials with enzyme-like catalytic activities that have rapidly advanced in the biomedical field in recent years due to their high stability, low cost, and catalytic versatility. As promising alternatives to natural enzymes, nanozymes have demonstrated unique advantages in infection control, cancer therapy, and tissue regeneration. This review systematically summarizes key advances in recent years in nanozyme-based catalytic therapeutics. We focus on their mechanisms and applications in combating bacterial, viral, and fungal infections via membrane lipid peroxidation, protein/genome damage, and biofilm disruption; in cancer treatment through chemodynamic therapy (CDT), tumor microenvironment modulation, and multimodal synergistic strategies; and in bone regeneration through antioxidant, anti-inflammatory, and osteoinductive functions. Moreover, we highlight the integration of nanozymes with hydrogels, scaffolds, and microrobotic systems to enhance therapeutic outcomes. Finally, current challenges such as targeting specificity, in vivo catalytic control, biosafety, and clinical translation are discussed to provide a comprehensive roadmap for future research and clinical development in catalytic nanomedicine.
{"title":"Nanozyme-based catalytic therapeutics: Applications in infectious diseases, cancer therapy, and bone regeneration","authors":"Dechao Yuan , Tianying Luo , Qiao Su , Changxing Qu , Meng Pan , Jia Xu , Mingyi Zhang , Yuanchao Luo , Renjian He , Shiwei Liu , Xiang Fang , Hong Duan , Zhiyong Qian","doi":"10.1016/j.cclet.2025.111842","DOIUrl":"10.1016/j.cclet.2025.111842","url":null,"abstract":"<div><div>Nanozymes are nanomaterials with enzyme-like catalytic activities that have rapidly advanced in the biomedical field in recent years due to their high stability, low cost, and catalytic versatility. As promising alternatives to natural enzymes, nanozymes have demonstrated unique advantages in infection control, cancer therapy, and tissue regeneration. This review systematically summarizes key advances in recent years in nanozyme-based catalytic therapeutics. We focus on their mechanisms and applications in combating bacterial, viral, and fungal infections <em>via</em> membrane lipid peroxidation, protein/genome damage, and biofilm disruption; in cancer treatment through chemodynamic therapy (CDT), tumor microenvironment modulation, and multimodal synergistic strategies; and in bone regeneration through antioxidant, anti-inflammatory, and osteoinductive functions. Moreover, we highlight the integration of nanozymes with hydrogels, scaffolds, and microrobotic systems to enhance therapeutic outcomes. Finally, current challenges such as targeting specificity, <em>in vivo</em> catalytic control, biosafety, and clinical translation are discussed to provide a comprehensive roadmap for future research and clinical development in catalytic nanomedicine.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"37 3","pages":"Article 111842"},"PeriodicalIF":8.9,"publicationDate":"2025-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145735491","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}
Zinc ion hybrid capacitors (ZIHCs) are emerging electrochemical energy storage devices with the dual characteristics of high energy density and high power density. However, the mismatch of capacity and electrode kinetics between porous carbon cathodes and zinc metal anodes limits the development of ZIHCs. Lignin has high carbon content, high aromaticity, and three-dimensional functional molecular structures, which is an ideal raw material for preparing high-performance porous carbon electrode materials with high carbon yield, conductive carbon network and enriched heteroatom dopants. Currently, the high-value utilization ratio of industrial lignin is lower than 10%. In this review, the typical preparation methodologies of lignin-derived porous carbons are summarized. The latest research advances for the lignin-derived porous carbon cathodes in ZIHCs are critically focused from the perspectives of pore regulation, surface modification, and morphology design. The core points and development directions that lignin-derived porous carbon cathodes are expected to achieve an original breakthrough in the future are proposed from three levels of techniques, mechanisms, and applications. This review fills the blank region in the applications of lignin-derived porous carbons for ZIHCs, aiming to provide valuable guidance for the high-value utilization process of lignin and the industrialization process of ZIHCs.
{"title":"Lignin valorization towards porous carbon cathodes in zinc ion hybrid capacitors","authors":"Caiwei Wang , Cheng Zeng , Changhong Wei , Guizhen Chen , Yueling Liang , Wenli Zhang","doi":"10.1016/j.cclet.2025.111850","DOIUrl":"10.1016/j.cclet.2025.111850","url":null,"abstract":"<div><div>Zinc ion hybrid capacitors (ZIHCs) are emerging electrochemical energy storage devices with the dual characteristics of high energy density and high power density. However, the mismatch of capacity and electrode kinetics between porous carbon cathodes and zinc metal anodes limits the development of ZIHCs. Lignin has high carbon content, high aromaticity, and three-dimensional functional molecular structures, which is an ideal raw material for preparing high-performance porous carbon electrode materials with high carbon yield, conductive carbon network and enriched heteroatom dopants. Currently, the high-value utilization ratio of industrial lignin is lower than 10%. In this review, the typical preparation methodologies of lignin-derived porous carbons are summarized. The latest research advances for the lignin-derived porous carbon cathodes in ZIHCs are critically focused from the perspectives of pore regulation, surface modification, and morphology design. The core points and development directions that lignin-derived porous carbon cathodes are expected to achieve an original breakthrough in the future are proposed from three levels of techniques, mechanisms, and applications. This review fills the blank region in the applications of lignin-derived porous carbons for ZIHCs, aiming to provide valuable guidance for the high-value utilization process of lignin and the industrialization process of ZIHCs.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"37 4","pages":"Article 111850"},"PeriodicalIF":8.9,"publicationDate":"2025-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146035426","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}
Pub Date : 2025-09-16DOI: 10.1016/j.cclet.2025.111845
Linan Wu, Shenghua Gao, Peng Zhan
{"title":"Breakthrough progress in the structural determination of the monkeypox virus I7L protease and the design of targeted inhibitors","authors":"Linan Wu, Shenghua Gao, Peng Zhan","doi":"10.1016/j.cclet.2025.111845","DOIUrl":"10.1016/j.cclet.2025.111845","url":null,"abstract":"","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"37 4","pages":"Article 111845"},"PeriodicalIF":8.9,"publicationDate":"2025-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145975320","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}
Pub Date : 2025-09-13DOI: 10.1016/j.cclet.2025.111834
Feng Zhao , Hongyu Ding , Ting Sun , Chao Shen , Zu-Li Wang , Wei Wei , Dong Yi
Carbenes as one of the most important class of intermediates have been widely utilized in various organic synthetic transformations. Carbene insertion-initiated ring-opening reactions of cyclic ethers offer a valuable strategy for constructing new carbon-oxygen bonds. In comparison with traditional thermal or metal-mediated carbene transfer reactions, visible-light-promoted multi-component reaction strategy provides a mild and eco-friendly approach to access densely functionalized molecules. Recently, visible-light-induced multi-component carbene transfer reactions of diazo compounds have been rapidly developed and attracted a great deal of research interest of chemists owing to their advantages of simple operation, mild condition, high atom economy and rich structural diversity. This paper summarizes the recent research progress on the visible-light-promoted multi-component carbene transfer reactions of diazo compounds via ring-opening of cyclic ethers with various nucleophiles. The reaction patterns of different nucleophiles and their corresponding mechanism are described in this review. The future research direction and challenges in this area are also discussed.
{"title":"Visible-light-promoted multi-component carbene transfer reactions of diazo compounds via ring-opening of cyclic ethers","authors":"Feng Zhao , Hongyu Ding , Ting Sun , Chao Shen , Zu-Li Wang , Wei Wei , Dong Yi","doi":"10.1016/j.cclet.2025.111834","DOIUrl":"10.1016/j.cclet.2025.111834","url":null,"abstract":"<div><div>Carbenes as one of the most important class of intermediates have been widely utilized in various organic synthetic transformations. Carbene insertion-initiated ring-opening reactions of cyclic ethers offer a valuable strategy for constructing new carbon-oxygen bonds. In comparison with traditional thermal or metal-mediated carbene transfer reactions, visible-light-promoted multi-component reaction strategy provides a mild and eco-friendly approach to access densely functionalized molecules. Recently, visible-light-induced multi-component carbene transfer reactions of diazo compounds have been rapidly developed and attracted a great deal of research interest of chemists owing to their advantages of simple operation, mild condition, high atom economy and rich structural diversity. This paper summarizes the recent research progress on the visible-light-promoted multi-component carbene transfer reactions of diazo compounds <em>via</em> ring-opening of cyclic ethers with various nucleophiles. The reaction patterns of different nucleophiles and their corresponding mechanism are described in this review. The future research direction and challenges in this area are also discussed.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"37 2","pages":"Article 111834"},"PeriodicalIF":8.9,"publicationDate":"2025-09-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145578408","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}
Pub Date : 2025-09-11DOI: 10.1016/j.cclet.2025.111826
Cuiping Lin , Chenchen Wang , Shaoqi Li , Qi Shen , Xiaodong Yang , Zengsheng Guo , Haiming Feng , Cuncheng Li , Yiqing Sun , Lifeng Hang
Conversion of ammonia into hydrogen, a crucial pathway for the hydrogen economy, is severely constrained by the intricacy of the required equipment and the low efficiency. Herein, Pd@PtNiCoRuIr core-shell mesoporous bifunctional electrocatalysts were fabricated via a one-step wet-chemical reduction approach. By utilizing the limiting effect of triblock copolymers, gradient distribution control of six metal elements (Pd core and Pt/Ni/Co/Ru/Ir high-entropy alloys shell) was achieved, where the high-entropy alloy shell forms high-density active sites through lattice distortion effect. With the help of lattice distortion and mesoporous-confinement-enabled interfacial coupling effects, Pd@PtNiCoRuIr catalyst exhibited exceptional bifunctional performance in alkaline media: A low hydrogen evolution reaction (HER) overpotential of 30.5 mV at 10 mA/cm2 and a high ammonia oxidation reaction (AOR) peak current density of 19.6 mA/cm2 at 0.7 V vs. RHE, representing a 3.83-fold enhancement over commercial Pt/C. Moreover, a rechargeable Zn-NH3 battery system was constructed and achieved 92.3 % Faradaic efficiency (FE) for NH3-to-H2 conversion with outstanding stability at 16 mA/cm2, thereby providing an innovative solution for efficient ammonia decomposition-based hydrogen production.
{"title":"Pd@PtNiCoRuIr core-shell high-entropy alloys mesoporous nanospheres for temporally decoupled ammonia splitting by a Zn-NH3 battery","authors":"Cuiping Lin , Chenchen Wang , Shaoqi Li , Qi Shen , Xiaodong Yang , Zengsheng Guo , Haiming Feng , Cuncheng Li , Yiqing Sun , Lifeng Hang","doi":"10.1016/j.cclet.2025.111826","DOIUrl":"10.1016/j.cclet.2025.111826","url":null,"abstract":"<div><div>Conversion of ammonia into hydrogen, a crucial pathway for the hydrogen economy, is severely constrained by the intricacy of the required equipment and the low efficiency. Herein, Pd@PtNiCoRuIr core-shell mesoporous bifunctional electrocatalysts were fabricated <em>via</em> a one-step wet-chemical reduction approach. By utilizing the limiting effect of triblock copolymers, gradient distribution control of six metal elements (Pd core and Pt/Ni/Co/Ru/Ir high-entropy alloys shell) was achieved, where the high-entropy alloy shell forms high-density active sites through lattice distortion effect. With the help of lattice distortion and mesoporous-confinement-enabled interfacial coupling effects, Pd@PtNiCoRuIr catalyst exhibited exceptional bifunctional performance in alkaline media: A low hydrogen evolution reaction (HER) overpotential of 30.5 mV at 10 mA/cm<sup>2</sup> and a high ammonia oxidation reaction (AOR) peak current density of 19.6 mA/cm<sup>2</sup> at 0.7 V <em>vs.</em> RHE, representing a 3.83-fold enhancement over commercial Pt/C. Moreover, a rechargeable Zn-NH<sub>3</sub> battery system was constructed and achieved 92.3 % Faradaic efficiency (FE) for NH<sub>3</sub>-to-H<sub>2</sub> conversion with outstanding stability at 16 mA/cm<sup>2</sup>, thereby providing an innovative solution for efficient ammonia decomposition-based hydrogen production.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"37 1","pages":"Article 111826"},"PeriodicalIF":8.9,"publicationDate":"2025-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145414756","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}
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