Science China Chemistry最新文献_第6页

Palladium-catalyzed asymmetric [4+3] cycloaddition of cycloamidines with trimethylenemethanes to access chiral bridged [3.2.2] bicycles 钯催化环脒与三甲基乙烷的不对称[4+3]环加成制备手性桥接[3.2.2]自行车

IF 9.8 1区化学

Science China Chemistry Pub Date : 2026-04-23 DOI: 10.1007/s11426-025-3300-y

Jiaxing Guo, Qianyu Chen, Chunyu Han, Xinze Wang, Wenda Xu, Wenli Yan, Huijing Xiang, Xiang Ma, Genping Huang, Xingguang Li

{"title":"Palladium-catalyzed asymmetric [4+3] cycloaddition of cycloamidines with trimethylenemethanes to access chiral bridged [3.2.2] bicycles","authors":"Jiaxing Guo, Qianyu Chen, Chunyu Han, Xinze Wang, Wenda Xu, Wenli Yan, Huijing Xiang, Xiang Ma, Genping Huang, Xingguang Li","doi":"10.1007/s11426-025-3300-y","DOIUrl":"10.1007/s11426-025-3300-y","url":null,"abstract":"<div><p>The asymmetric cycloaddition of palladium-trimethylenemethane (Pd-TMM) serves as a powerful method for constructing enantioenriched ring systems. Yet its application to cycloaddends for chiral bridged polycycles remains largely unexplored and challenging, owing to high energy barriers and difficulties in selectivity control. Herein, we report the first asymmetric [4+3] TMM cycloaddition with 4<i>π</i>-cycloaddends—cycloamidines, enabling efficient access to diverse chiral bridged azabicyclo[3.2.2]nonanones with multiple stereocenters in excellent enantio- and diastereoselectivity. This transformation is driven by the “push-pull” effect of the amidino moiety and aromatization-assisted C–C bond formation. Computational studies reveal that the initial nucleophilic addition governs both the reaction rate and stereoselectivity. Moreover, evaluations in cellular and <i>in vivo</i> models confirm the high biosafety and promising antitumor efficacy of these chiral azabicyclic compounds.</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"69 8","pages":"4477 - 4487"},"PeriodicalIF":9.8,"publicationDate":"2026-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148695540","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

Recent advances in electrocatalysts toward industrialized alkaline electrolysis 工业化碱性电解电催化剂的最新进展

IF 9.7 1区化学

Science China Chemistry Pub Date : 2026-04-16 DOI: 10.1007/s11426-025-3288-y

Ling Zhang, Wangyang Wu, Li Li, Zidong Wei

引用次数: 0

Harnessing energy-transfer catalysis for modular δ-aminoboronate synthesis via radical 1,2-boryl migration 利用能量转移催化通过自由基1,2-硼基迁移合成模δ-氨基硼酸盐

IF 9.8 1区化学

Science China Chemistry Pub Date : 2026-04-16 DOI: 10.1007/s11426-025-3285-0

Shan-Shan Li, Yu-Shi Jiang, Dan-Na Chen, Fu-Qin Zhang, Yan Lei, Hai-Tao Tang, Peng-Ju Xia

{"title":"Harnessing energy-transfer catalysis for modular δ-aminoboronate synthesis via radical 1,2-boryl migration","authors":"Shan-Shan Li, Yu-Shi Jiang, Dan-Na Chen, Fu-Qin Zhang, Yan Lei, Hai-Tao Tang, Peng-Ju Xia","doi":"10.1007/s11426-025-3285-0","DOIUrl":"10.1007/s11426-025-3285-0","url":null,"abstract":"<div><p>Aminoboron compounds are privileged scaffolds in pharmaceutical chemistry, yet general and efficient access to <i>δ</i>-aminoborates remains underdeveloped. Herein, we report a photocatalytic energy transfer (EnT)-enabled radical 1,2-boron migration strategy for the modular assembly of <i>δ</i>-aminoboronate frameworks. Under mild conditions, photoexcitation of readily designed <i>β</i>-boryl oxime esters triggers decarboxylative radical generation and subsequent intramolecular 1,2-boron shift, delivering distal carbon-centered radicals. This platform enables chemo- and regioselective 1,4-difunctionalization of a wide range of unsaturated systems, including alkenes, C=N, and N=N bonds. Remarkably, the strategy is further extended to alkyne–alkene relay systems, enabling direct 1,6-aminoborylation for efficient construction of distal aminoboronic esters. This EnT-based approach overcomes limitations in atom economy and regioselectivity inherent in conventional single-electron-transfer (SET) manifolds. The reaction exhibits broad substrate scope (>70 examples), excellent functional group tolerance, and scalability. Synthetic utility is demonstrated through downstream transformations to access valuable <i>δ</i>-amino alcohols and related pharmacophores, establishing a versatile route to distal aminoboronates with potential applications in synthetic and medicinal chemistry.</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"69 8","pages":"4457 - 4463"},"PeriodicalIF":9.8,"publicationDate":"2026-04-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148695140","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

Artificial intelligence-facilitated multiscale theoretical modelling to advance battery science 人工智能促进的多尺度理论建模推进电池科学

IF 9.7 1区化学

Science China Chemistry Pub Date : 2026-04-16 DOI: 10.1007/s11426-025-3306-8

Jiawei Shi, Yun Tian, Mengwei Sun, Xu Zhang, Zhen Zhou

{"title":"Artificial intelligence-facilitated multiscale theoretical modelling to advance battery science","authors":"Jiawei Shi, Yun Tian, Mengwei Sun, Xu Zhang, Zhen Zhou","doi":"10.1007/s11426-025-3306-8","DOIUrl":"10.1007/s11426-025-3306-8","url":null,"abstract":"<div><p>The multiscale nature of battery materials and their accompanying electrochemical processes poses a fundamental challenge in theoretical modeling. Conventional methods often involve a trade-off between accuracy and computational efficiency, which constrains simulations across electronic, atomistic, and primitive particle-based resolutions and consequently limits the predictive capability of multiscale modeling. The integration of artificial intelligence (AI) is transforming theoretical modeling for battery performance prediction. Beyond offering incremental improvements, AI enables quantum-mechanical accuracy at the computational cost of classical force fields, infers cross-scale physical laws from atomistic simulations, and constructs scalable bridges across traditionally segregated modeling domains. By holistically managing the workflow from machine learning assisted material design to automated synthesis and systematic optimization, AI effectively addresses cross-scale modeling challenges. In this review, we outline simulation methodologies at diverse resolutions, chosen as paradigmatic representations of multiscale modeling, and explore the transformative role of AI in advancing battery research across these hierarchical scales. Building upon these methodological advances, we critically assess the application of AI-enhanced theoretical frameworks to tackle key challenges in battery science, underscoring AI’s pivotal role in connecting theoretical simulations with experimental synthesis and accelerating the rational design of next-generation battery systems. Finally, we discuss the current limitations and key challenges facing AI-facilitated multiscale modeling.</p><div><figure><div><div><picture><source><img></source></picture><span>The alternative text for this image may have been generated using AI.</span></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"69 6","pages":"2821 - 2835"},"PeriodicalIF":9.7,"publicationDate":"2026-04-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148060693","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

Halide and steric effects on Ir(III) carbene phosphors for blue organic light-emitting diodes 蓝色有机发光二极管用Ir（III）碳粉的卤化物和位阻效应

IF 9.8 1区化学

Science China Chemistry Pub Date : 2026-04-16 DOI: 10.1007/s11426-025-3249-2

Jie Yan, Manli Huang, Martin Kuhn, Muyu Zhou, Xinyu Li, Yufeng Sang, Guowei Ni, Jinsong Jiang, Kai Li, Xiuwen Zhou, Chuluo Yang, Yun Chi

{"title":"Halide and steric effects on Ir(III) carbene phosphors for blue organic light-emitting diodes","authors":"Jie Yan, Manli Huang, Martin Kuhn, Muyu Zhou, Xinyu Li, Yufeng Sang, Guowei Ni, Jinsong Jiang, Kai Li, Xiuwen Zhou, Chuluo Yang, Yun Chi","doi":"10.1007/s11426-025-3249-2","DOIUrl":"10.1007/s11426-025-3249-2","url":null,"abstract":"<div><p>We reported Ir(III) complexes featuring a dicarbene pincer chelate, a bidentate carbene cyclometalate (with either <i>N</i>-benzyl or <i>N</i>-mesityl appendage) and a halide (X<sup>−</sup> = Cl<sup>−</sup>, Br<sup>−</sup> and I<sup>−</sup>), for probing the structure-property relationship. They exhibit blue emission with the peak<sub>max</sub> spanning 465–480 nm in toluene at RT. Particularly, <b>[Ir(DP)(MC5H)Cl]</b> and <b>[Ir(DP)(MS1)Cl]</b> showed the best performance among these Ir(III) emitters due to the high MLCT and LC components and relatively diminished XLCT contribution. This is evidenced by high photoluminescent quantum yield (PLQY) of 60% and 73% and fast radiative rate constant (<i>k</i><sub>r</sub> = 6.7 × 10<sup>6</sup> and 2.0 × 10<sup>6</sup> s<sup>−1</sup>). Phosphorescent organic light-emitting diode (PhOLED) devices based on 20 wt% of <b>[Ir(DP)(MC5H)Cl]</b> and <b>[Ir(DP)(MS1)Cl]</b> exhibited the maximum external quantum efficiency (EQE<sub>max</sub>) of 26.1% and 22.0% with peak<sub>max</sub> at 506 and 468 nm, respectively. Additionally, hyper-OLED featuring sensitizer <b>[Ir(DP)(MS1)Cl]</b> and terminal emitter v-DABNA afforded narrowband blue emission with EQE<sub>max</sub> of 26.9% and the International Commission on Illumination (CIE) coordinates of (0.129, 0.157).</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"69 7","pages":"3515 - 3523"},"PeriodicalIF":9.8,"publicationDate":"2026-04-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://link.springer.com/content/pdf/10.1007/s11426-025-3249-2.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148552939","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Usability and extensibility: imperatives for next-generation LLM agents in chemistry 可用性和可扩展性：化学中下一代LLM代理的必要性

IF 9.7 1区化学

Science China Chemistry Pub Date : 2026-04-15 DOI: 10.1007/s11426-025-3262-6

Xuefeng Bai, Xin Zhang, Hao-Tian Wang, Zhiling Zheng, Jian-Rong Li

引用次数: 0

Controlled desaturative diborylation of carbonyls 羰基的可控去饱和二硼化

IF 9.8 1区化学

Science China Chemistry Pub Date : 2026-04-14 DOI: 10.1007/s11426-025-3345-5

Chaoqun Shi, Cheng Ma, Xinni An, Minghui Sun, Shasha Geng, Yun He, Yi Yang, Shaofei Ni, Zhang Feng

{"title":"Controlled desaturative diborylation of carbonyls","authors":"Chaoqun Shi, Cheng Ma, Xinni An, Minghui Sun, Shasha Geng, Yun He, Yi Yang, Shaofei Ni, Zhang Feng","doi":"10.1007/s11426-025-3345-5","DOIUrl":"10.1007/s11426-025-3345-5","url":null,"abstract":"<div><p>We report a NaHMDS-promoted strategy for the efficient and highly selective synthesis of aryl diboronates from carbonyl compounds through controlled activation of diboron reagents. This transformation proceeds under catalyst- and additive-free conditions and offers notable advantages, including environmental sustainability, avoidance of halogenated waste, and broad functional-group compatibility. The protocol enables late-stage diborylation of biologically relevant molecules and provides a versatile platform for accessing structurally diverse naphthalene derivatives directly from carbonyl precursors. Combined experimental and computational studies indicate that the reaction proceeds via sequential alkenyl C–O bond borylation, allylic C–H bond borylation, and a desaturation process. Remarkably, the diboron reagent exhibits an unprecedented oxidative role rather than its conventional reductive behavior, ing a hydride from an anionic alkenyl boronate intermediate to promote desaturation. These findings reveal a previously unrecognized reactivity mode of base/diboron reagent systems and open new avenues for reaction design based on their oxidative potential.</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"69 8","pages":"4527 - 4534"},"PeriodicalIF":9.8,"publicationDate":"2026-04-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148695502","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

Tuning molecular knots by introducing remote substituents 通过引入远端取代基调整分子结

IF 9.8 1区化学

Science China Chemistry Pub Date : 2026-04-14 DOI: 10.1007/s11426-026-3395-5

Siri Froiland, Meiling Wade, Yuanning Feng

引用次数: 0

Efficient manipulation of triplet excitons for long afterglow in flexible crystals 柔性晶体长余辉中三重态激子的有效操纵

IF 9.8 1区化学

Science China Chemistry Pub Date : 2026-04-13 DOI: 10.1007/s11426-025-3283-1

Zhiqin Wu, Jian Liu, Zhenyi He, Jingyu Cao, Baolei Tang, Lei Zhou, Yang Li, Hongyu Zhang, Xiang Ma

{"title":"Efficient manipulation of triplet excitons for long afterglow in flexible crystals","authors":"Zhiqin Wu, Jian Liu, Zhenyi He, Jingyu Cao, Baolei Tang, Lei Zhou, Yang Li, Hongyu Zhang, Xiang Ma","doi":"10.1007/s11426-025-3283-1","DOIUrl":"10.1007/s11426-025-3283-1","url":null,"abstract":"<div><p>Flexible optoelectronic materials are becoming an emerging research area due to their unique flexibility and processing feasibility. However, the development of flexible crystals with long afterglow remains a formidable challenge. Herein, flexible crystals with long afterglow are achieved by enriching and stabilizing triplet excitons through crystal engineering and host-guest doping. These flexible crystals exhibit multi-channel emission and a phosphorescent lifetime of 966.24 ms under ambient conditions, significantly surpassing previously reported flexible crystals with afterglow properties. Notably, high-temperature phosphorescence, which is rarely observed in crystals, can be detected in the obtained material. Single-crystal analysis and theoretical calculation reveal that weak C–H⋯π and π⋯π interactions contribute to the flexibility of the crystals. The crystals possess an elastic modulus of 0.081 GPa and an average hardness of 0.004 GPa, characteristics that are highly uncommon in the field of flexible optoelectronics. Ultimately, flexible crystals are applied in optoelectronic information transmission and encryption. This study provides a crucial reference for the advanced application of flexible crystals in optical and material sciences.</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"69 8","pages":"4433 - 4441"},"PeriodicalIF":9.8,"publicationDate":"2026-04-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148695578","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

Nanoparticle-induced local microenvironments and their roles in electrocatalysis 纳米粒子诱导的局部微环境及其在电催化中的作用

IF 9.8 1区化学

Science China Chemistry Pub Date : 2026-04-13 DOI: 10.1007/s11426-025-3335-3

Yanwei Zhu, Li Tao, Xian-Zhu Fu, Shuangyin Wang

{"title":"Nanoparticle-induced local microenvironments and their roles in electrocatalysis","authors":"Yanwei Zhu, Li Tao, Xian-Zhu Fu, Shuangyin Wang","doi":"10.1007/s11426-025-3335-3","DOIUrl":"10.1007/s11426-025-3335-3","url":null,"abstract":"<div><p>The local reaction microenvironment within the electrochemical double layer plays a decisive role in governing electrocatalytic activity and selectivity, particularly in nanoparticle-based catalytic systems. Beyond their intrinsic electronic structures, nanoparticles (NPs) can induce distinct local microenvironments by virtue of their morphology, size, spatial distribution, and surface characteristics. In this review, we summarize recent advances in understanding how these NPs structural parameters modulate local microenvironments as well as their roles in regulating reaction kinetics, selectivity, and efficiency in energy-related electrocatalytic reactions. We also systematically analyze critical microenvironment factors such as local electric field strength, ion distribution, interfacial pH, mass transport, and intermediate coverage. Simultaneously, <i>in situ</i> and <i>operando</i> characterization techniques, together with theoretical simulations, are highlighted to elucidate the formation and dynamic evolution of nanoparticle-induced microenvironments during electrocatalysis. Finally, current challenges and future perspectives are discussed, including the precise characterization of local microenvironments, the identification of key microenvironment descriptors, and machine learning-assisted prediction of interfacial catalytic activity for advanced electrocatalyst design.</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"69 8","pages":"4280 - 4291"},"PeriodicalIF":9.8,"publicationDate":"2026-04-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148695580","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