Science China Chemistry最新文献

Size-selective hybridization chain reaction for accurate signal amplification in living cancer cells

IF 10.4 1区化学

Science China Chemistry Pub Date : 2024-11-12 DOI: 10.1007/s11426-024-2294-x

Ting Chen, Xiaojiao Wang, Rongrong Gao, Meihe Yuan, Mei Chen, Xiao-Bing Zhang, Guoliang Ke

{"title":"Size-selective hybridization chain reaction for accurate signal amplification in living cancer cells","authors":"Ting Chen, Xiaojiao Wang, Rongrong Gao, Meihe Yuan, Mei Chen, Xiao-Bing Zhang, Guoliang Ke","doi":"10.1007/s11426-024-2294-x","DOIUrl":"10.1007/s11426-024-2294-x","url":null,"abstract":"<div><p>Accurate signal amplification in living cells is highly important in biomedical research and medical diagnostics. Benefiting from its enzyme-free, efficient isothermal signal amplification ability, hybridization chain reaction (HCR) plays an important role in intracellular signal amplification; however, HCR fails the accurate signal amplification in the situation when the properties of some biological targets and analogues are too similar. Particularly, their signal amplification accuracy for mature miRNAs is unsatisfactory due to the signal interference of precursor microRNAs (abbreviated as pre-miRNAs), which also contain the sequence of mature miRNAs. Herein, we develop the first example of size-selective hybridization chain reaction probe for accurate signal amplification, which achieved accurate and sensitive biosensing of mature miRNAs in living cancer cells. Our probe, termed as qTcage, consists of a DNA nanocage for size-selective responsive to mature miRNAs, as well as a quadrivalent tetrahedral DNA structure for HCR signal amplification. Benefiting from the size-selectivity of DNA nanocage, shorter mature miRNAs (19–23 nt) rather than longer pre-miRNAs (60–70 nt) could enter the cavity to release triggers strand, which activates HCR reaction for fluorescence signal recovery. The probe efficiently reduces signal interference of pre-miRNAs and improves the imaging sensitivity for intracellular mature miRNAs, which was successfully applied for mature miRNAs imaging during drug treatment. Overall, this strategy provides the hybridization chain reaction with the feature of size-selective ability, which holds promise for further accurate signal amplification in biological processes study and clinical diagnostics.</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"67 12","pages":"4259 - 4266"},"PeriodicalIF":10.4,"publicationDate":"2024-11-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142758036","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

Fostering a growing chemistry community: the 2024 emerging investigator issue of Science China Chemistry

IF 10.4 1区化学

Science China Chemistry Pub Date : 2024-11-12 DOI: 10.1007/s11426-024-2414-x

Li-Jun Wan

引用次数: 0

Mechanochemistry of cyclobutanes

IF 10.4 1区化学

Science China Chemistry Pub Date : 2024-11-11 DOI: 10.1007/s11426-024-2344-0

Roberto Obregon, Junpeng Wang

引用次数: 0

Donor-acceptor modulation of coordination polymers for effective photothermal conversion

IF 10.4 1区化学

Science China Chemistry Pub Date : 2024-10-25 DOI: 10.1007/s11426-024-2253-y

Bo Zhang, Xing-Wang Li, Han Fang, Chang-Tai Li, Si-Jia Yu, Mei-Hui Yu, Ze Chang, Xian-He Bu

{"title":"Donor-acceptor modulation of coordination polymers for effective photothermal conversion","authors":"Bo Zhang, Xing-Wang Li, Han Fang, Chang-Tai Li, Si-Jia Yu, Mei-Hui Yu, Ze Chang, Xian-He Bu","doi":"10.1007/s11426-024-2253-y","DOIUrl":"10.1007/s11426-024-2253-y","url":null,"abstract":"<div><p>The targeted construction of donor-acceptor (D-A) materials featuring efficient photothermal (PT) conversion properties has been an attractive but challenging goal. Herein, a new series of coordination polymers (CPs) featuring different PT performances were constructed with flexible linker 1,1′-Ferrocenedicarboxylic acid (FCA) and 2,4,6-tri(pyridin-4-yl)-1,3,5-triazine (TPT) as acceptor and donor molecules including coronene and tetrathiafulvalene (TTF). Based on the flexible configurations of FCA ligand and the directing of donor dependent D-A interactions, the structures of <b>TF-1</b> to <b>TF-3</b> featuring distinctive dimension were obtained based on Cd(II) ions for investigating the PT property in configurational perspectives. A systematic investigation of the PT properties of the CPs was performed. Notably, <b>TF-3</b> exhibits the finest PT conversion effect under the irradiation of 560 nm laser, while <b>TF-2</b> shows optimal PT conversion under 808 nm laser irradiation required for biological PT therapy, illustrating the correlation between the structural and component features of the CPs and their PT performances. Furthermore, Zn(II) as bio-friendly ion was utilized to construct hypotoxic <b>TF-4</b> that reveals similar structure to that of <b>TF-2</b> for potential application. Polydimethylsiloxane (PDMS) patches doped with <b>TF-4</b> exhibits considerable NIR PT conversion effect under 808 nm, represented by the nearly 80 °C temperature increased in 120 s for <b>TF-4</b>@PDMS patch (1.2 wt%) under 0.9 W cm<sup>−2</sup> irradiation, the results of which herein indicate the potential of D-A CPs as versatile platform for the modulation of PT materials.</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"67 12","pages":"4175 - 4183"},"PeriodicalIF":10.4,"publicationDate":"2024-10-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142757993","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

Mechanically robust and dynamic supramolecular polymer networks enabled by [an]daisy chain backbones

IF 10.4 1区化学

Science China Chemistry Pub Date : 2024-10-21 DOI: 10.1007/s11426-024-2329-7

Yongming Wang, Yi Ding, Yuhang Liu, Shaolei Qu, Wenbin Wang, Wei Yu, Zhaoming Zhang, Feng Liu, Xuzhou Yan

{"title":"Mechanically robust and dynamic supramolecular polymer networks enabled by [an]daisy chain backbones","authors":"Yongming Wang, Yi Ding, Yuhang Liu, Shaolei Qu, Wenbin Wang, Wei Yu, Zhaoming Zhang, Feng Liu, Xuzhou Yan","doi":"10.1007/s11426-024-2329-7","DOIUrl":"10.1007/s11426-024-2329-7","url":null,"abstract":"<div><p>Supramolecular polymer networks (SPNs) have garnered significant research interest due to their dynamic properties. However, while current developments primarily focus on managing supramolecular crosslinks, the role of polymer backbones—equally crucial to SPN properties—has not yet been sufficiently explored. Herein, we utilize mechanically interlocked [<i>a</i>n]daisy chain as backbone to prepare a class of SPNs, where the force-induced motion of successive mechanical bonds toughens and reinforces the networks. In specific, the [<i>a</i>n]daisy chain backbones connect with polynorbornene chains through quadruple H-bonding in the SPN networks. Compared to the control with non-slidable backbone, The representative SPN-<b>2</b> exhibits a robust feature in tensile tests with high maximum stress (14.7 vs. 7.89 MPa) and toughness (83.8 vs. 48.6 MJ/m<sup>3</sup>). Moreover, it also has superior performance in energy dissipation benefitting from the [<i>a</i>n]daisy chain backbones as well as supramolecular crosslinks. Additionally, the SPN-<b>2</b> displayed exceptional self-healing and reprocessing capabilities due to their dynamic quadrable H-bonding crosslinkers. These findings demonstrate the untapped potential of [<i>a</i>n]daisy chain as a polymer skeleton to develop SPNs and open the door to design mechanically robust supramolecular materials with diverse smart functions.</p></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"67 12","pages":"4234 - 4241"},"PeriodicalIF":10.4,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142757929","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

Molecular catalysts for electrocatalytic ammonia oxidation

IF 10.4 1区化学

Science China Chemistry Pub Date : 2024-10-14 DOI: 10.1007/s11426-024-2137-5

Jun Li, Feiyang Zhang, Huatian Xiong, Yuanyuan Cai, Biaobiao Zhang

引用次数: 0

Relay C(sp3)-H bond trifluoromethylthiolation and amidation by visible light photoredox catalysis 利用可见光光氧化催化中继 C(sp3)-H键三氟甲基硫代和酰胺化反应

IF 10.4 1区化学

Science China Chemistry Pub Date : 2024-10-12 DOI: 10.1007/s11426-024-2259-7

Junheng Liu, Suqi Yang, Shunruo Yao, Chengjian Zhu, Yong Liu, Weipeng Li, Jin Xie

引用次数: 0

Ionic solid-like conductor-assisted polymer electrolytes for solid-state lithium metal batteries

IF 10.4 1区化学

Science China Chemistry Pub Date : 2024-10-12 DOI: 10.1007/s11426-024-2353-9

Shuaishuai Yan, Hao Liu, Xiaoxia Chen, Yang Lu, Qingbin Cao, Kai Liu

{"title":"Ionic solid-like conductor-assisted polymer electrolytes for solid-state lithium metal batteries","authors":"Shuaishuai Yan, Hao Liu, Xiaoxia Chen, Yang Lu, Qingbin Cao, Kai Liu","doi":"10.1007/s11426-024-2353-9","DOIUrl":"10.1007/s11426-024-2353-9","url":null,"abstract":"<div><p>Solid polymer electrolytes (SPEs) have attracted extensive attention by virtue of lightweight and flexible processability for solid-state lithium metal batteries (LMBs) with high energy density and intrinsic safety. However, the SPEs suffer from the trade-off effect between ionic conductivity and mechanical strength. Herein, we report an ionic solid-like conductor with high Li<sup>+</sup> conductivity and good thermal stability as the conductive phase of polymer electrolytes for advanced LMBs. Using poly (vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) as the polymer matrix, the ionic solid-like conductor can be regarded as a solid plasticizer due to its advantages of non-fluidity and non-leakage. It increases the amorphous region and the dissociation degree of lithium salts in SPEs, while minimizing the loss of mechanical properties. As a result, the Li<sup>+</sup> conductivity of SPEs incorporating the ionic solid-like conductor is enhanced by four orders of magnitude compared to the blank PVDF-HFP-based electrolyte. The optimized SPE membranes can be processed as thin as 50 µm with a high Young’s modulus of 16.8 MPa, therefore ensuring stable long-term cycling of solid-state LMBs. The Li/Li symmetric cells stably cycled for more than 750 h without short circuits, and the LiFePO<sub>4</sub>/Li solid-state batteries demonstrate excellent electrochemical performance over 350 cycles with a capacity retention of 82.5%. This work provides a new strategy for designing ionic solid-like conductors as solid plasticizers for high-performance polymer electrolytes.</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"67 12","pages":"4116 - 4124"},"PeriodicalIF":10.4,"publicationDate":"2024-10-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142758037","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

Progress of photocatalytic CO2 reduction toward multi-carbon products

IF 10.4 1区化学

Science China Chemistry Pub Date : 2024-10-08 DOI: 10.1007/s11426-024-2148-2

Jiaojiao Fang, Chengyang Zhu, Huiling Hu, Jiaqi Li, Licheng Li, Haiyan Zhu, Junjie Mao

{"title":"Progress of photocatalytic CO2 reduction toward multi-carbon products","authors":"Jiaojiao Fang, Chengyang Zhu, Huiling Hu, Jiaqi Li, Licheng Li, Haiyan Zhu, Junjie Mao","doi":"10.1007/s11426-024-2148-2","DOIUrl":"10.1007/s11426-024-2148-2","url":null,"abstract":"<div><p>The photocatalytic CO<sub>2</sub> reduction reaction (CO<sub>2</sub>RR) represents a promising solution to alleviate environmental and energy issues stemming from CO<sub>2</sub> emissions while simultaneously enabling the production of high-value multi-carbon fuels. However, the efficient generation of multi-carbon products remains challenging due to high kinetic barriers, sluggish C–C coupling processes, and intricate reaction pathways. This review provides a comprehensive overview of the latest advancements in synthesizing C<sub>2+</sub> products through CO<sub>2</sub> photoreduction, highlighting the crucial role of active site design and the C–C coupling mechanism. Specifically, we emphasize the correlation between the structure of active sites and the key intermediates of C–C coupling, which is fundamental for achieving deep photoconversion of CO<sub>2</sub>. Finally, we offer a glimpse into future challenges and prospects, outlining potential directions for the development of CO<sub>2</sub>-to-multicarbon photoconversion, aiming to contribute novel insights to this exciting field.</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"67 12","pages":"3994 - 4013"},"PeriodicalIF":10.4,"publicationDate":"2024-10-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142757991","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

Enantioselective iridium-catalyzed allylic substitution with a Reformatsky reagent: direct construction of β-stereogenic homoallylic esters 铱催化烯丙基取代与 Reformatsky 试剂的对映选择性：直接构建 β-立体同源烯丙基酯

IF 10.4 1区化学

Science China Chemistry Pub Date : 2024-09-30 DOI: 10.1007/s11426-024-2284-x

Debasis Pal, Kirana D. Veeranna, Yuk Fai Wong, P. Andrew Evans

{"title":"Enantioselective iridium-catalyzed allylic substitution with a Reformatsky reagent: direct construction of β-stereogenic homoallylic esters","authors":"Debasis Pal, Kirana D. Veeranna, Yuk Fai Wong, P. Andrew Evans","doi":"10.1007/s11426-024-2284-x","DOIUrl":"10.1007/s11426-024-2284-x","url":null,"abstract":"<div><p>The Reformatsky reagent derived from ethyl bromoacetate circumvents the challenge associated with the direct regio- and enantioselective iridium-catalyzed allylic alkylation with an unstabilized aliphatic ester enolate. Notably, this work represents the first example of using a Reformatsky reagent in a metal-allyl reaction, which permits the direct construction of enantioenriched β-stereogenic homoallylic esters without preactivation of the pronucleophile or post-reaction modification of the product (e.g., thermal decarboxylation of a 1,3-dicarbonyl). Moreover, the process allows the coupling of a broad range of sterically and electronically diverse electrophiles bearing aryl, heteroaryl and alkenyl derivatives, including the significantly more challenging alkyl-substituted allylic carbonates. The versatility of the ester product is exemplified by a series of functional group manipulations and the development of a concise and efficient enantioselective total synthesis of the natural product, (+)-descurainolide A. Finally, mechanistic studies indicate that the zinc enolate behaves as a soft nucleophile that undergoes outer-sphere alkylation.\u0000</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"67 11","pages":"3791 - 3797"},"PeriodicalIF":10.4,"publicationDate":"2024-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142519159","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