Science China Chemistry最新文献_第5页

Facile and efficient synthesis of 1,4-dihydropyridine drug molecules via Hantzsch condensation reaction catalyzed by isostructural crystalline Cd-Pd/Pt heterometallic-organic frameworks Cd-Pd/Pt异质金属-有机框架催化Hantzsch缩合反应制备1,4-二氢吡啶类药物分子

IF 9.8 1区化学

Science China Chemistry Pub Date : 2026-07-29 DOI: 10.1007/s11426-026-3497-x

Yiduo Wang, Xiangmei Lu, Yajuan Wang, Guo-Ping Yang, Yao-Yu Wang

{"title":"Facile and efficient synthesis of 1,4-dihydropyridine drug molecules via Hantzsch condensation reaction catalyzed by isostructural crystalline Cd-Pd/Pt heterometallic-organic frameworks","authors":"Yiduo Wang, Xiangmei Lu, Yajuan Wang, Guo-Ping Yang, Yao-Yu Wang","doi":"10.1007/s11426-026-3497-x","DOIUrl":"10.1007/s11426-026-3497-x","url":null,"abstract":"<div><p>1,4-Dihydropyridine N-heterocyclic compounds are the core skeleton of essential cardiovascular drugs. The Hantzsch condensation reaction is a key synthetic approach for these compounds, yet the currently available catalytic systems suffer from harsh reaction conditions and low yields, necessitating the development of novel heterogeneous catalysts. Herein, two isostructural porous heterometallic organic frameworks (<b>Cd-Pd/Pt PDA</b>) were designed and synthesized using the bifunctional ligand 3,5-pyridinedicarboxylic acid (H<sub>2</sub>PDA). Of these, <b>Cd-Pt PDA</b> exhibits outstanding catalytic activity in the one-pot Hantzsch condensation reaction, demonstrating a broad substrate scope (22 examples) with a low catalyst loading (1.2 mol%), minimal Pt leaching (1.46 ppm), and excellent recyclability over five consecutive cycles without significant loss of activity. Notably, high-quality single crystals of nitrendipine, felodipine, and nimodipine were obtained for the first time from the MOF-catalyzed reaction, and their molecular structures were conclusively identified through single-crystal X-ray diffraction (SC-XRD) analysis. Furthermore, theoretical calculations provide strong validation for the feasibility and mechanism of the Hantzsch condensation reaction catalyzed by this material. This research not only provides an efficient platform for the green and sustainable production of important drug molecules but also establishes a rational design paradigm for the creation of multifunctional heterogeneous catalysts.</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"69 10","pages":"5673 - 5679"},"PeriodicalIF":9.8,"publicationDate":"2026-07-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149176851","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

Azaphenanthrene-based polycyclic acceptors regulated by N/halogen engineering achieving over 20% efficiency in binary organic solar cells 氮/卤素工程调控的氮杂蒽基多环受体在二元有机太阳能电池中实现了20%以上的效率

IF 9.8 1区化学

Science China Chemistry Pub Date : 2026-07-29 DOI: 10.1007/s11426-026-3507-9

Ruohan Wang, Jian Liu, Guangkun Song, Wenkai Zhao, Wendi Shi, Zhaoyang Yao, Guankui Long, Chenxi Li, Xiangjian Wan, Yongsheng Chen

{"title":"Azaphenanthrene-based polycyclic acceptors regulated by N/halogen engineering achieving over 20% efficiency in binary organic solar cells","authors":"Ruohan Wang, Jian Liu, Guangkun Song, Wenkai Zhao, Wendi Shi, Zhaoyang Yao, Guankui Long, Chenxi Li, Xiangjian Wan, Yongsheng Chen","doi":"10.1007/s11426-026-3507-9","DOIUrl":"10.1007/s11426-026-3507-9","url":null,"abstract":"<div><p>The molecular core-expansion strategy has proved effective in reducing energy loss (<i>E</i><sub>loss</sub>) and improving acceptor packing behavior, thereby achieving a better balance of open-circuit voltage (<i>V</i><sub>oc</sub>), short-circuit current density (<i>J</i><sub>sc</sub>) and fill factor (FF). However, most reported core-expansion designs still focus on quinoxaline-fused frameworks, whereas investigations into larger multi-ring systems (<i>n</i> ⩾ 5) remain scarce. The limited progress stems mainly from the fact that extensive ring fusion often disrupts molecular packing, leading to poor device performance. To address this challenge, we employed a heteroatom-guided design strategy by constructing a series of azaphenanthrene-fused acceptors and systematically incorporating halogen atoms (F, Cl, and Br) into the central core. As the halogen radius increases, both the crystallinity and packing order of the acceptors are progressively enhanced. Ultimately, the Br-substituted azaphenanthrene-fused acceptor CHNBr delivers an impressive fill factor of 78.84%, enabling the binary organic solar cells to surpass the 20% power conversion efficiency (PCE) among multi-ring-expanded acceptor systems.</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"69 10","pages":"5768 - 5776"},"PeriodicalIF":9.8,"publicationDate":"2026-07-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149176907","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

Morphological and electronic modulation of Gd-doped HKUST metal-organic frameworks enhancing efficient CO2 electroreduction to ethanol gd掺杂的HKUST金属有机框架的形态和电子调制提高CO2电还原为乙醇的效率

IF 9.8 1区化学

Science China Chemistry Pub Date : 2026-07-29 DOI: 10.1007/s11426-026-3392-5

Yutong Chen, Honglin Cheng, Shenghua Zhou, Lifeng Deng, Jiajing Pei, Yan Guo, Xiangyu Liu, Xi Liu

{"title":"Morphological and electronic modulation of Gd-doped HKUST metal-organic frameworks enhancing efficient CO2 electroreduction to ethanol","authors":"Yutong Chen, Honglin Cheng, Shenghua Zhou, Lifeng Deng, Jiajing Pei, Yan Guo, Xiangyu Liu, Xi Liu","doi":"10.1007/s11426-026-3392-5","DOIUrl":"10.1007/s11426-026-3392-5","url":null,"abstract":"<div><p>Cu-based catalysts are promising candidates for the electrocatalytic reduction of CO<sub>2</sub> (CO<sub>2</sub>RR) toward multicarbon products. However, designing suitable active sites in Cu metal-organic frameworks (MOFs) remains a critical challenge, owing to their inherent structural instability during CO<sub>2</sub>RR and the difficulty in simultaneously optimizing morphology and electronic structure. In this work, we report a facile one-pot synthesis of gadolinium-doped HKUST (Gd<sub><i>x</i></sub>/HKUST), integrating morphological and electronic modulation to selectively electroreduce CO<sub>2</sub> to ethanol. The optimized Gd<sub>0.25</sub>/HKUST catalyst exhibits a unique wheat-ear-like morphology (thus conducive to CO<sub>2</sub> adsorption and accessibility) and a Gd-induced valence state transition from Cu<sup>+</sup> to Cu<sup>0</sup>, as corroborated by a suite of physicochemical characterizations. Electrochemical evaluation at −1.0 V presents a high Faradaic efficiency of 54.5% for ethanol, surpassing pristine HKUST, along with stability exceeding 60 h. <i>In situ</i> spectroscopic analyses indicates the rapid consumption of *CO species, followed by the subsequent hydrogenation of *CO to form *CHO and the further generation of *OC<sub>2</sub>H<sub>5</sub> on the Gd<sub>0.25</sub>/HKUST catalyst. Theoretical studies reveal that Cu-Gd bimetallic synergy lowers the energy barrier for *CHO hydrogenation, thereby facilitating C-C coupling. This work highlights a dual-strategy approach integrating morphological and electronic modifications in MOF-based catalysts, thus advancing the rational design of efficient CO<sub>2</sub>-to-C<sub>2+</sub> conversion systems.</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"69 9","pages":"5103 - 5111"},"PeriodicalIF":9.8,"publicationDate":"2026-07-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148986848","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

Tailoring 2D Zr-MOF stacking via V-shaped modulators for high-efficiency gas chromatographic separations 剪裁2D Zr-MOF堆叠通过v形调制器高效气相色谱分离

IF 9.8 1区化学

Science China Chemistry Pub Date : 2026-07-29 DOI: 10.1007/s11426-026-3479-4

Ye-Qin Zhou, Wen-Qi Tang, Jian-Ping Zhu, Xing-Feng Hu, Ming Xu, Zhi-Yuan Gu

{"title":"Tailoring 2D Zr-MOF stacking via V-shaped modulators for high-efficiency gas chromatographic separations","authors":"Ye-Qin Zhou, Wen-Qi Tang, Jian-Ping Zhu, Xing-Feng Hu, Ming Xu, Zhi-Yuan Gu","doi":"10.1007/s11426-026-3479-4","DOIUrl":"10.1007/s11426-026-3479-4","url":null,"abstract":"<div><p>Controlling the interlayer stacking of two-dimensional metal-organic frameworks (2D MOFs) is crucial and challenging for optimising their mass transfer and separation performance. Herein, we proposed a V-shaped modulator strategy to control the stacking modes of 2D Zr-BTB by employing three metatopic dicarboxylic acid (CPA = 3,5-di(4-carboxylphenyl)aniline, CPB = 1,3-di(4-carboxylphenyl)benzene, and CPP = 2,6-di(4-carboxylphenyl)-4-(phenyl)pyridine) modulators with distinct terminal functional groups. Quantitative high-angle annular dark-field images analysis revealed that the amino-functionalized modulator (CPA) induced a high proportion of untwisted stacking (≈ 64.6%), whereas the phenyl-terminated modulators (CPB and CPP) predominantly resulted in twisted stacking, with untwisted fractions of only 32.0% and 20.6%, respectively. Density functional theory calculations and independent gradient model analysis indicated that strongly polar–NH<sub>2</sub> interactions of CPA effectively anchored adjacent layers, suppressed interlayer rotational freedom, and promoted untwisted stacking. Furthermore, the untwisted Zr-BTB-CPA as a stationary phase exhibited efficient separation performance for all C<sub>7</sub> to C<sub>10</sub> alkane isomers and benzene derivative isomers with complete separation (<i>R</i> values > 1.5). In contrast, twisted stacking of Zr-BTB-CPB and Zr-BTB-CPP showed poor separation performance because of their restricted diffusion. Thermodynamic and kinetic analyses further indicated that the ordered channels in Zr-BTB-CPA enable both effective thermodynamic discrimination and rapid mass transfer. This work introduced a strategy for regulating 2D MOF stacking through rational modulator functionalization, achieving efficient gas chromatographic separation.</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"69 10","pages":"5689 - 5697"},"PeriodicalIF":9.8,"publicationDate":"2026-07-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149176850","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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Efficient uranium recovery from wastewater via flexocatalysis 柔性催化从废水中高效回收铀

IF 9.8 1区化学

Science China Chemistry Pub Date : 2026-07-29 DOI: 10.1007/s11426-026-3723-9

Yinghui Xie, Xishi Tai, Suhua Wang

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Simultaneous ultrafast permeance and high selectivity in ultrathin conjugated polymer framework membranes 超薄共轭聚合物框架膜同时具有超快渗透和高选择性

IF 9.8 1区化学

Science China Chemistry Pub Date : 2026-07-29 DOI: 10.1007/s11426-026-3526-7

Jingjing Zhao, Jingyu Chen, Jiong Zhou

引用次数: 0

Melamine-induced defect-rich carbon supporting Fe-Mo heteronuclear dual-atom catalyst for high-efficiency Zn-air batteries 高效锌空气电池用三聚氰胺诱导富碳负载Fe-Mo杂核双原子催化剂

IF 9.8 1区化学

Science China Chemistry Pub Date : 2026-07-28 DOI: 10.1007/s11426-026-3451-3

Hao Wang, Yongjuan Yuan, Jingkun Yu, Tingting Zhai, Ran Zhang, Dan Pan, Yaojia Cheng, Siyu Lu

{"title":"Melamine-induced defect-rich carbon supporting Fe-Mo heteronuclear dual-atom catalyst for high-efficiency Zn-air batteries","authors":"Hao Wang, Yongjuan Yuan, Jingkun Yu, Tingting Zhai, Ran Zhang, Dan Pan, Yaojia Cheng, Siyu Lu","doi":"10.1007/s11426-026-3451-3","DOIUrl":"10.1007/s11426-026-3451-3","url":null,"abstract":"<div><p>The symmetric FeN<sub>4</sub> configuration in conventional single-atom catalysts strongly binds oxygenated intermediates, creating a high energy barrier for the rate-determining *OH desorption step and limiting ORR kinetics. Herein, we construct an asymmetric Mo–Fe dual-atom catalyst on a defect-rich N-doped carbon matrix (Mo–Fe–NC (MA)) to overcome this limitation. The FeN<sub>3</sub>–MoN<sub>3</sub> coordination enables electron donation from Mo to Fe, weakening Fe–OH bonds and facilitating the rate-determining *OH desorption. The catalyst demonstrates outstanding oxygen reduction activity in 0.1 M KOH, with a half-wave potential of 0.918 V <i>vs.</i> RHE, surpassing Pt/C and single-atom references. In zinc-air batteries, it delivers a peak power density of 147.7 mW cm<sup>−2</sup> and operates stably for over 725 h. Flexible solid-state devices also show robust performance under bending, highlighting their promise for wearable energy applications.</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"69 9","pages":"5065 - 5073"},"PeriodicalIF":9.8,"publicationDate":"2026-07-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148986994","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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Nickel/photoredox-catalyzed boryl radical relay dual arylation/acylation of alkenes 镍/光氧化还原催化硼基自由基接力双芳基化/酰化烯烃

IF 9.8 1区化学

Science China Chemistry Pub Date : 2026-07-27 DOI: 10.1007/s11426-026-3432-8

Jun Dong, Haowen Zhan, Jiahao Li, Jiansheng Chen, Xinjun Tang

{"title":"Nickel/photoredox-catalyzed boryl radical relay dual arylation/acylation of alkenes","authors":"Jun Dong, Haowen Zhan, Jiahao Li, Jiansheng Chen, Xinjun Tang","doi":"10.1007/s11426-026-3432-8","DOIUrl":"10.1007/s11426-026-3432-8","url":null,"abstract":"<div><p>Herein, we report a novel dual nickel/photoredox catalytic system for alkene diarylation and diacylation, centered around a unique boron-mediated radical relay mechanism. The key steps of this process involve the efficient cleavage of B–H bonds and the selective activation of inert C(sp<sup>2</sup>)–X bonds. Specifically, photocatalytically generated bromine radicals first undergo hydrogen atom transfer (HAT) with amine-boranes, cleaving the B–H bond. The resulting boryl radicals then serve as potent activators to engage inert aryl bromides or acyl chlorides via halogen atom transfer (XAT), effectively breaking the C(sp<sup>2</sup>)–X bonds and releasing key aryl and acyl radicals. These carbon-centered radicals subsequently add to alkenes, and the resulting adducts are efficiently captured by nickel species and funneled into a downstream nickel catalytic cycle to accomplish alkene difunctionalization. This strategy is distinguished by its broad substrate compatibility, excellent chemo-selectivity, capability for late-stage functionalization of drug molecules, and the use of commercially available and stable reagents. It thus provides an efficient and reliable route to synthetically valuable 1,2-diaryl- and 1,2-diacyl-substituted 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 9","pages":"5188 - 5196"},"PeriodicalIF":9.8,"publicationDate":"2026-07-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://link.springer.com/content/pdf/10.1007/s11426-026-3432-8.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148986830","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}

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Interfacial dual-electric-field dynamic regulation enables dendrite-free lithium metal batteries 界面双电场动态调节可实现无枝晶锂金属电池

IF 9.8 1区化学

Science China Chemistry Pub Date : 2026-07-27 DOI: 10.1007/s11426-026-3425-0

Cai-Yun Zhang, Rui Huang, Hui-Ling Deng, Xiang-Zu Meng, Ya-Wen Tian, Chen-Yang Wang, Min Yan, Jianhong Gao, Pu Hu, Yu Li, Henghui Xu, Zhitian Liu

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Sodium polyacrylate modulates interfacial cations for efficient ethylene electrosynthesis from water-fed CO reduction in a solid-state electrolyzer 聚丙烯酸钠调节界面阳离子的有效乙烯电合成从水馈CO还原在固态电解槽

IF 9.8 1区化学

Science China Chemistry Pub Date : 2026-07-27 DOI: 10.1007/s11426-026-3453-0

Yun Song, Weihua Guo, Ruquan Ye

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