Science China Chemistry最新文献_第6页

Azobenzene-derived coordination polymer enables integrated dilute CO2 capture and electrolysis at industrial current densities 偶氮苯衍生的配位聚合物能够在工业电流密度下集成稀二氧化碳捕获和电解

IF 9.8 1区化学

Science China Chemistry Pub Date : 2026-07-27 DOI: 10.1007/s11426-026-3464-7

Hui-Mian Zhou, Yong-Yuan Gui, Da-Gang Yu

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Biohybrid chiral hydrogel suppresses tumor stemness via mechanotransduction 生物杂化手性水凝胶通过机械转导抑制肿瘤干性

IF 9.8 1区化学

Science China Chemistry Pub Date : 2026-07-27 DOI: 10.1007/s11426-026-3457-8

Jia-Xuan Yi, Lingshan Gong, Yingxiang Ye

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Decarboxylative functionalization with redox-active esters in a single-electron transfer manner 以单电子转移方式用氧化还原活性酯进行脱羧功能化

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Science China Chemistry Pub Date : 2026-07-27 DOI: 10.1007/s11426-026-3403-4

Siyu Xia, Zhongxuan Cai, Shengyu Zhuang, Jin Xie

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Spatial modulation of photoreactivity in isoreticular metal-organic frameworks: comparative insights into single-component, multivariate, and core-shell systems 等晶格金属-有机框架中光反应性的空间调节：单组分、多元组分和核-壳体系的比较研究

IF 9.8 1区化学

Science China Chemistry Pub Date : 2026-07-27 DOI: 10.1007/s11426-026-3410-x

Ziyue Liu, Qi Liu, Jianping Lang

{"title":"Spatial modulation of photoreactivity in isoreticular metal-organic frameworks: comparative insights into single-component, multivariate, and core-shell systems","authors":"Ziyue Liu, Qi Liu, Jianping Lang","doi":"10.1007/s11426-026-3410-x","DOIUrl":"10.1007/s11426-026-3410-x","url":null,"abstract":"<div><p>Metal-organic frameworks (MOFs) incorporating multiple functional groups provide modular platforms for tailoring physical properties and photochemical reactivity. We report the synthesis and comparative photoreactivity analysis of a set of iso-reticular Zn(II)-based MOFs constructed from 1,4-bis[2-(3-pyridyl)ethenyl]benzene and benzene-1,4-dicarboxylate linkers bearing diverse substituents. These frameworks, comprising single-component, multivariate (MTV), and core-shell architectures, undergo [2+2] photocycloaddition in the solid state via a single-crystal-to-single-crystal transformation under UV irradiation. Real-time photoreaction dynamics were monitored by laser scanning confocal microscopy, revealing functional group-dependent variations in emission behavior and reaction kinetics. MTV-MOFs exhibit two distinct photoreactivity patterns: either consistent with, or markedly divergent from, the predicted linear combination of the respective single-component analogues, suggesting non-trivial linker-linker interactions. In contrast, core-shell MOFs retain the intrinsic photoreactivity and luminescence profiles of each domain, indicative of minimal interfacial coupling. These findings underscore the critical influence of linker identity, spatial arrangement, and compositional distribution on MOF photoreactivity, providing valuable insights for the rational design of photoresponsive crystalline materials.</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":"5643 - 5651"},"PeriodicalIF":9.8,"publicationDate":"2026-07-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149176536","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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Binuclear copper catalytic sites confined in a metal-organic framework for monooxygenase-mimetic C(sp3)–H oxidation 双核铜催化位限制在金属-有机框架中用于模拟单加氧酶的C(sp3) -H氧化

IF 9.8 1区化学

Science China Chemistry Pub Date : 2026-07-24 DOI: 10.1007/s11426-026-3415-4

Jun-Yu Li, Fu-Qi Mi, Jiang-Jie Zhang, Tao Huang, Zi-Yi Guo, Qiao Yao, Liang-Liang Yan, Teng Zhang

{"title":"Binuclear copper catalytic sites confined in a metal-organic framework for monooxygenase-mimetic C(sp3)–H oxidation","authors":"Jun-Yu Li, Fu-Qi Mi, Jiang-Jie Zhang, Tao Huang, Zi-Yi Guo, Qiao Yao, Liang-Liang Yan, Teng Zhang","doi":"10.1007/s11426-026-3415-4","DOIUrl":"10.1007/s11426-026-3415-4","url":null,"abstract":"<div><p>The ultimate catalytic activity of metalloenzymes relies on both primary and secondary coordination spheres of the active site, which is hard to mimic in synthetic catalytic systems. Introduction of flexible tetramethylethylenediamine (TMEDA) side chains to a UiO-67 metal-organic framework (MOF) enables the installation of non-covalently interacted, self-adaptive binuclear copper sites that synergistically activate O<sub>2</sub>, and the confined MOF pore space rich in aromatic functionalities engages organic substrates through multiple non-covalent interactions. Taking advantage of both structural features, the resulting UiO-67-TMEDA-Cu catalyst replicates the catalytic pocket of methane monooxygenase and drives aerobic C(sp<sup>3</sup>)–H oxidation under mild, additive-free conditions, exhibiting activity significantly surpassing that of its mononuclear analog and a homogeneous binuclear control catalyst lacking spatial confinement. Kinetic studies and theoretical calculations revealed that the binuclear copper pair catalyst exhibited higher activity than its mononuclear counterpart by lowering the energy demands of O–O bond cleavage and hydrogen atom abstraction, while the MOF cavity further reduces the binding energy between organic substrates and Cu<sub>2</sub> sites. This work thus demonstrates the great potential of engineering non-covalently interacted, synergistic metal pairs within MOFs to achieve enzyme-like selectivity and activity for advanced catalytic transformations.</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":"5095 - 5102"},"PeriodicalIF":9.8,"publicationDate":"2026-07-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148987113","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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Benzothiadiazole-containing heptapyrrin: modulation of diradical character and photothermal conversion via metal coordination 含苯并噻二唑七吡啶：通过金属配位调制双自由基性质和光热转化

IF 9.8 1区化学

Science China Chemistry Pub Date : 2026-07-24 DOI: 10.1007/s11426-026-3456-6

Zhen Yang, Xiandong He, Glib Baryshnikov, Bin Zhu, Chengjie Li, Shijun Li, Hans Ågren, Qizhao Li, Yongshu Xie, Yuguang Ma

{"title":"Benzothiadiazole-containing heptapyrrin: modulation of diradical character and photothermal conversion via metal coordination","authors":"Zhen Yang, Xiandong He, Glib Baryshnikov, Bin Zhu, Chengjie Li, Shijun Li, Hans Ågren, Qizhao Li, Yongshu Xie, Yuguang Ma","doi":"10.1007/s11426-026-3456-6","DOIUrl":"10.1007/s11426-026-3456-6","url":null,"abstract":"<div><p>Conjugated polypyrroles have attracted intensive attention due to their unique properties, and they have emerged as potential platforms for stabilizing radicals. With the purpose to construct stable polypyrrole radicals, a benzothiadiazole unit has been incorporated into a heptapyrrin framework to afford <b>1</b>. Thus, <b>1</b> exists as a singlet ground state diradical with a narrow singlet-triplet energy gap (Δ<i>E</i><sub>S-T</sub>) of −3.17 kcal mol<sup>−1</sup>. On this basis, <b>1</b> has been coordinated with Pd(II) and Ni(II) salts to afford binuclear complexes <b>1-Pd</b> and <b>1-Ni</b>. Notably, <b>1-Ni</b> retains the diradical character with a narrowed Δ<i>E</i><sub>S-T</sub> of −0.65 kcal mol<sup>−1</sup>, whereas <b>1-Pd</b> is a closed-shell species. As a result, <b>1, 1-Pd</b>, and <b>1-Ni</b> exhibit intense near-infrared-II (NIR-II) absorption bands at 1076, 1283, and 1309 nm, respectively, enabling them to function as NIR-II photothermal conversion materials. Thus, <b>1</b> and diradical species <b>1-Ni</b> show relatively high photothermal conversion efficiencies (<i>η</i>) of 37.6% and 38.6%, respectively. Whereas, closed-shell derivatives of <b>1</b> such as the oxidized (<b>1-ox</b>), reduced (<b>1-re</b>) and coordination (<b>1-Pd</b>) species exhibit lowered efficiencies of 24.8%, 26.5%, and 30.9%, respectively. These results provide insight into developing stable open-shell oligopyrroles as efficient photothermal materials, with the efficiencies further enhanced by coordination with transition metal ions while retaining the open-shell character.</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":"5762 - 5767"},"PeriodicalIF":9.8,"publicationDate":"2026-07-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149176799","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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High-loading asymmetric transition metal single-atom catalysts for electrocatalytic ammonia synthesis 电催化合成氨用高负荷非对称过渡金属单原子催化剂

IF 9.8 1区化学

Science China Chemistry Pub Date : 2026-07-23 DOI: 10.1007/s11426-026-3722-x

Jiahe Peng, Dingsheng Wang, Jizhou Jiang

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Bio-inspired bifunctional Im-Ln@MOFs nanocomposites enabling instant visual tracking and ambient catalytic detoxification of nerve agent simulants 仿生双功能Im-Ln@MOFs纳米复合材料使即时视觉跟踪和环境催化解毒神经毒剂模拟

IF 9.8 1区化学

Science China Chemistry Pub Date : 2026-07-23 DOI: 10.1007/s11426-026-3393-2

Jin-Yu Guo, Man Cao, Gai-Gai Wu, Yu-Jin Zhong, Xiao-Meng Hu, Shi-Bo Lu, Jie Wu, Xuan Guo, Shuang-Quan Zang

{"title":"Bio-inspired bifunctional Im-Ln@MOFs nanocomposites enabling instant visual tracking and ambient catalytic detoxification of nerve agent simulants","authors":"Jin-Yu Guo, Man Cao, Gai-Gai Wu, Yu-Jin Zhong, Xiao-Meng Hu, Shi-Bo Lu, Jie Wu, Xuan Guo, Shuang-Quan Zang","doi":"10.1007/s11426-026-3393-2","DOIUrl":"10.1007/s11426-026-3393-2","url":null,"abstract":"<div><p>High-efficiency degradation and immediate detection of organophosphorus (OPs) nerve agents under realistic, dry conditions are of paramount significance in emerging applications. While the synthetic integration of these two distinct functions within a single material platform remains a big challenge, it is highly desirable. Herein, by mimicking phosphotriesterase’s active site and applying the lanthanides (Ln<sup>3+</sup>) luminescence mechanism, bifunctional materials <b>Im-Ln@MOF-808</b> (Ln = Eu/Tb) are designed that enable visual recognition and detoxification of a nerve agent simulant, dimethyl 4-nitrophenyl phosphate (DMNP), under ambient, unbuffered, and solvent-free conditions. The metallization of the Zr<sub>6</sub>-oxo clusters of MOF-808 with Ln<sup>3+</sup> allows for exhibiting intense fluorescence in the solid state. Notably, the ingeniously introduced Im not only provides OH<sup>−</sup> for nucleophilic attack and regenerates catalytically active Zr<sub>6</sub> sites during the hydrolysis but also dramatically enhances the 4f-5d transition probabilities and the radiative transition rate of Ln<sup>3+</sup>. After contact with OPs, obvious fluorescence quenching happens by the dissociation of Ln–Im bonds, with a sensitive fluorescence quenching response with detection limits as low as 0.328 and 0.168 µM, respectively. This work illustrates, for the first time, the feasibility of simultaneous fluorescence detection and solid-phase decontamination of nerve agents using a single material, providing new insights for developing practical protective countermeasures.</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":"5121 - 5129"},"PeriodicalIF":9.8,"publicationDate":"2026-07-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148986658","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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Single-molecule force spectroscopy unveils arsenic coordination stapling and stabilization of an oncogenic p53 mutant 单分子力谱揭示了砷配位钉接和致癌p53突变体的稳定

IF 9.8 1区化学

Science China Chemistry Pub Date : 2026-07-22 DOI: 10.1007/s11426-026-3493-9

Yuanhao Liu, Yuhan Ma, Mengdie Wang, Hongjia Liu, Tianfu Feng, Hantian Zhang, Peng Zheng

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Fluorochromic metal-organic frameworks enable self-indicating thorium remediation 荧光金属有机框架使自指示钍修复

IF 9.8 1区化学

Science China Chemistry Pub Date : 2026-07-22 DOI: 10.1007/s11426-026-3533-x

Baowei Hu, Xishi Tai, Xiangke Wang

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