{"title":"Sequence-activated chemiluminescence probes: programmable illumination for high-contrast in vivo sensing and imaging","authors":"Yutao Zhang, Juan Li, Wei-Hong Zhu, Zhiqian Guo","doi":"10.1007/s11426-024-2143-0","DOIUrl":"10.1007/s11426-024-2143-0","url":null,"abstract":"<div><p>Sequence-activated chemiluminescence (CL) technique offers a unique approach to detecting specific biomolecules or cellular events with high sensitivity and spatial resolution. The fundamental principle behind sequence-activated CL probes involves tailoring highly-controllable CL signals in response to specific sequences or events of interest, thus enabling high-contrast signals under complex physiological conditions. This sequential activation could be triggered by enzymes, reactive oxygen species (ROS), biothiols or changes in the microenvironment. These unique sequence-activated CL probes bestow several advantages, including minimal background, deep-tissue penetration, and the ability of non-invasive or minimally invasive detection. The sequence-activated CL techniques represent a significant advancement in molecular imaging and diagnostics. In this mini-review, we focus on the latest developments in sequential CL probes, addressing the technical challenges and discussing the future trajectory by harnessing CL signaling and molecular recognition.\u0000</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"68 1","pages":"26 - 34"},"PeriodicalIF":10.4,"publicationDate":"2024-09-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142197172","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}
{"title":"Supramolecular metallopolymer for hypoxia-activated ruthenium complexes delivery and smart chemo-photodynamic therapy","authors":"Maomao He, Zhiyuan Ma, Zongwei Zhang, Linhao Zhang, Shengqi Zhang, Ran Wang, Xuefei Leng, Yang Li, Jiangli Fan, Wen Sun, Xiaojun Peng","doi":"10.1007/s11426-024-2065-2","DOIUrl":"10.1007/s11426-024-2065-2","url":null,"abstract":"<div><p>The Ru complexes have garnered a great deal of attention for antitumor phototherapy; however, achieving efficient cellular uptake and tumor-specific activation represents a major challenge. Herein, we synthesize a hypoxia-activated Ru complex (RuANM) and construct it into supramolecular polymers (PolyRuANM) through high binding affinity interaction. The amphiphilic supramolecular polymers possess self-assembly, resulting in the formation of diverse nanostructures exhibiting a range of morphologies by simply adjusting the host-guest ratio. As the polymer nanostructure size and morphology have been optimized, PolyRuANM prevents premature drug leakage and accumulates rapidly in the tumor cells. In the tumor hypoxia microenvironment, the polymer undergoes selective activation and disintegration, leading to the unlock of Ru complexes. Notably, the subsequent application of red light irradiation exacerbates the hypoxia and potentiates the liberation of the Ru complexes. This polymer design concept provides some novel insights into on-demand drug delivery and smart chemophotodynamic therapy.\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":"3875 - 3885"},"PeriodicalIF":10.4,"publicationDate":"2024-09-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://link.springer.com/content/pdf/10.1007/s11426-024-2065-2.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142197171","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}
{"title":"Cyano migration-mediated radical-polar crossover cyclopropanation","authors":"Ziqiang Wang, Yasu Chen, Jie Li, Chen Zhu","doi":"10.1007/s11426-024-2172-1","DOIUrl":"10.1007/s11426-024-2172-1","url":null,"abstract":"<div><p>We report a novel cyano migration-mediated radical-polar crossover process, whereby both the sulfonylcyanation of aliphatic alkenes and the formation of cyclopropanes are concurrently achieved. This transformation yields a diverse array of multi-substituted cyclopropanes under mild photocatalytic conditions. Mechanistic studies elucidate that the reaction proceeds via intramolecular nucleophilic substitution, leading to the formation of the cyclopropane derivatives.\u0000</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"68 1","pages":"241 - 248"},"PeriodicalIF":10.4,"publicationDate":"2024-09-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142225143","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}
{"title":"Palladium-catalyzed vinylation of indoles with vinyl ethers via deoxygenative coupling","authors":"Bowen Wang, Jianxiao Li, Wanqing Wu, Liangbin Huang, Huanfeng Jiang","doi":"10.1007/s11426-024-2184-x","DOIUrl":"10.1007/s11426-024-2184-x","url":null,"abstract":"<div><p>Indole is a promising heteroarene in many natural products and pharmaceuticals; therefore, various synthetic methods for indole functionalizations have arisen in recent years. Herein, we report a Pd-catalyzed deoxygenative coupling for the <i>N</i>-vinylation of indoles by employing vinyl ethers. The vinylated indoles could be readily prepared in good to excellent yields with N1-regioselectivity regardless of the electronic characteristics and substitution patterns of indole substrates. Some indole-based pharmaceutical molecules, such as gramine, evodiamine, rutaecarpine, and melatonine, are also successfully vinylated. Moreover, carbazoles and indazoles are shown to participate. Additionally, vinylated indole can readily transform into structurally interesting indole derivatives.\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":"3785 - 3790"},"PeriodicalIF":10.4,"publicationDate":"2024-09-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142197174","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}
{"title":"The secret of the magic gourd(I): biomass from various organizations of ourds as a sustainable source for high-performance supercapacitors","authors":"Shaoqing Zhang, Xuchun Wang, Tianming Lv, Baixue Dong, Jiqi Zheng, Yang Mu, Miao Cui, Ting Zhang, Changgong Meng","doi":"10.1007/s11426-024-2233-7","DOIUrl":"https://doi.org/10.1007/s11426-024-2233-7","url":null,"abstract":"<p>The classic cartoon “Calabash Brothers” describes a story of seven brothers born from a magic gourd uniting to defeat powerful enemies. In order to explore the secret of the magic gourd, several transition metals were used to synthesize metal silicates (C-MSi) by planted gourd leaves (GLs) and then the C-MSi materials were used to fabricate supercapacitor electrodes and devices with superior electrochemical performance. By integrating theoretical calculations and experimental results, the supercapacitor electrodes and devices obtained from the combination of transition metals with amorphous carbon exhibit superior electrochemical performance. In detail, in the three-electrode system, the NaOH etched materials (C-MSi) exhibited better electrochemical performance (for instance, as for C-CdSi, 607 F g<sup>−1</sup> at 0.5 A g<sup>−1</sup> and the capacitance retention of 98.2% after 10,000 cycles) than the unetched ones (i-C-MSi). Hybrid supercapacitor (HSC) devices also achieve very excellent electrochemical properties. Take C-CdSi//AC as an example, the areal specific capacitance with 691 mF cm<sup>−2</sup> at 2 mA cm<sup>−2</sup>, the energy density with 5.04 Wh m<sup>−2</sup> at the power density of 22.2 W m<sup>−2</sup> and the cycle stability with 87.3% after 6,000 cycles. This approach is very versatile and was also applied to produce many hierarchically structured metal-silicate materials of other biomass precursors, including roots, vines, flowers, fruits and seeds of the planted gourds. Thus, it is a potential way to prepare transition metal silicates using biomaterials for the enhancement of electrochemical performance and improvement of energy storage and conversion. Also, this paper preliminarily reveals the secret of the magic gourd.</p>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"5 1","pages":""},"PeriodicalIF":9.445,"publicationDate":"2024-09-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142197173","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}
{"title":"Recent advancements and perspectives of fast-charging composite anodes for lithium-ion batteries","authors":"Qinghui Zeng, Yongteng Dong, Yuanmao Chen, Xinyang Yue, Zheng Liang","doi":"10.1007/s11426-024-2265-9","DOIUrl":"10.1007/s11426-024-2265-9","url":null,"abstract":"<div><p>The escalating demand for fast-charging lithium-ion batteries (LIBs) has mirrored the rapid proliferation and widespread adoption of electric vehicles and portable electronic devices. Nonetheless, the sluggish diffusion kinetics of lithium ions and electrode degradation in conventional graphite-based anodes pose formidable hurdles in achieving optimal fast-charging capabilities for LIBs. To overcome these challenges, the innovative concept of fast-charging composite anodes, a paradigm shift from traditional single-component designs, has emerged as a promising avenue to enhance the overall performance of LIBs under rapid charging conditions. This paper provides a comprehensive review of the recent advancements in fast-charging composite anodes for LIBs, with a pivotal emphasis on the design principles and material selection strategies employed in various composite anode formulations. Furthermore, it outlines the future prospects and research trajectories in this burgeoning field, offering insights into potential breakthroughs and directions for further exploration.</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":"3952 - 3963"},"PeriodicalIF":10.4,"publicationDate":"2024-08-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142197197","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}
Zihao Wang, Yue Liu, Wenmin Pang, Ao Chen, Min Chen
{"title":"Polyolefin vitrimers bearing acetoacetate functionality","authors":"Zihao Wang, Yue Liu, Wenmin Pang, Ao Chen, Min Chen","doi":"10.1007/s11426-024-2070-3","DOIUrl":"10.1007/s11426-024-2070-3","url":null,"abstract":"<div><p>Polyolefin vitrimers are polymer networks bearing reversible covalent crosslinking points, enabling them to be reprocessed and recycled. In this contribution, a series of polyolefin vitrimers were designed based on the acetoacetate-functionalized polyolefin copolymers, which were produced through the direct copolymerization of ethylene with polar comonomers using a phosphine-sulfonate palladium catalyst. The pendant acetoacetate group could mediate several characteristic reactions, such as the Michael addition reaction, ketone-amine condensation and metal coordination reaction. As such, structurally adjustable polyolefin vitrimers can be accessed by introducing various dynamic crosslinking bonds, including disulfide exchange, transamination of vinylogous urethane and labile metal coordination bond. The utilization of different crosslinking reactions and the mole ratio of crosslinkers significantly impact the material properties of the resultant polymers. Specifically, the generated polyolefin vitrimers demonstrated excellent reprocessability and closed-loop recycling properties. The study in this work provides an efficient strategy to access various polyolefin vitrimers.\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":"3861 - 3867"},"PeriodicalIF":10.4,"publicationDate":"2024-08-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142197194","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}
{"title":"Applications of in-situ solid-state nuclear magnetic resonance in methanol to olefins reaction","authors":"Jing Niu, Shutao Xu, Yingxu Wei, Zhongmin Liu","doi":"10.1007/s11426-024-2266-8","DOIUrl":"10.1007/s11426-024-2266-8","url":null,"abstract":"<div><p>The methanol-to-olefins (MTO) reaction offers an alternative pathway for the production of low-carbon olefins from non-oil feedstocks. Fundamental research has been impeded by a lack of comprehensive understanding of its underlying mechanism, despite the significant progress made in industry. <i>In-situ</i> solid-state nuclear magnetic resonance (ssNMR) spectroscopy has emerged as a pivotal tool, offering crucial insights into key species under real-time <i>operando</i> conditions. Furthermore, the host–guest interaction between zeolites or surface species residing on zeolites and the reactant/active intermediates is revealed by the combination of <i>in-situ</i><sup>13</sup>C MAS NMR and 2D correlation spectroscopy. Moreover, recent technological advancements in hyperpolarization (HP) methods, including HP <sup>129</sup>Xe NMR and dynamic nuclear polarization (DNP), have significantly improved the sensitivity of ssNMR, enabling detailed structural and kinetic analysis as well as the detection of trace species. In this feature article, we summarized recent advancements in (<i>in-situ</i>) ssNMR spectroscopy applied to MTO reaction processes, encompassing mechanistic investigations at various stages and the intricate host–guest interactions. These theoretical insights into the dynamic evolution of MTO reactions lay a solid foundation for the optimization of catalytic processes and the development of efficient catalysts, thereby advancing the techniques towards more sustainable and economical production route for olefins.\u0000</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"68 1","pages":"134 - 151"},"PeriodicalIF":10.4,"publicationDate":"2024-08-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142197191","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}
Yue Yu, Jianqiu Wang, Zhihao Chen, Yang Xiao, Zhen Fu, Tao Zhang, Haoyu Yuan, Xiao-Tao Hao, Long Ye, Yong Cui, Jianhui Hou
{"title":"Naphthalene diimide-based cathode interlayer material enables 20.2% efficiency in organic photovoltaic cells","authors":"Yue Yu, Jianqiu Wang, Zhihao Chen, Yang Xiao, Zhen Fu, Tao Zhang, Haoyu Yuan, Xiao-Tao Hao, Long Ye, Yong Cui, Jianhui Hou","doi":"10.1007/s11426-024-2244-8","DOIUrl":"10.1007/s11426-024-2244-8","url":null,"abstract":"<div><p>Cathode interlayer (CIL) materials play an important role in improving the power conversion efficiency (PCE) of organic photovoltaic (OPV) cells. However, the current understanding of the structure-property relationship in CIL materials is limited, and systematic studies in this regard are scarce. Here, two new CIL materials, NDI-PhC4 and NDI-PhC6 were synthesized by varying the alkylamine chain length on the NDI-Ph core. Our investigation reveals a systematic variation in the physical and chemical properties of these materials with increasing alkylamine chain length. Specifically, we observe a sequential decrease in melting point and self-doping effect, accompanied by an enhancement in crystallinity. Among these CIL materials, NDI-PhC4 has a notable balance across various performance metrics. It also exhibits excellent surface modification capabilities, leading to a low surface roughness. Consequently, OPV cells based on NDI-PhC4 achieve a PCE of 20.2%, which is one of the highest reported efficiencies for OPV cells. In addition, the appropriate melting point of NDI-PhC4 contributes to the excellent stability of OPV cells.</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":"4194 - 4201"},"PeriodicalIF":10.4,"publicationDate":"2024-08-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142197193","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}
{"title":"Color center-rich γ-Al2O3 promotes propane dehydrogenation","authors":"Yu Wang, Xiang Wang, Mengfei Qiao, Qingyuan Wu, Kunlong Liu, Xiaodong Yi, Ruixuan Qin, Gang Fu, Nanfeng Zheng","doi":"10.1007/s11426-024-2260-2","DOIUrl":"10.1007/s11426-024-2260-2","url":null,"abstract":"<div><p>The PtSn/Al<sub>2</sub>O<sub>3</sub> catalyst is commonly used in commercial propane dehydrogenation (PDH) processes, but it faces challenges in the deactivation and periodic regeneration due to metal aggregation and coke deposition at high temperatures. Although Al<sub>penta</sub><sup>3+</sup> has been proven to be beneficial for enhancing catalytic stability, bottom-up synthesis protocols usually restrict their applications. Here, a facile post-treatment approach using acetic acid was applied to create color centers (electrons trapped within oxygen vacancies) on γ-Al<sub>2</sub>O<sub>3</sub>. Notably, the content of Al<sub>penta</sub><sup>3+</sup> was enriched to 18.3%. Then, the pre-established PtSn clusters were loaded. The electrons facilitated the formation of ultrafine PtSn nanoparticles (∼2 nm), and the Al<sub>penta</sub><sup>3+</sup> sites prevented the sintering of PtSn by constructing the strong Al<sub>penta</sub><sup>3+</sup>–O–Sn bonds. Furthermore, the catalytic durability of the catalyst prepared by conventional impregnation methods was remarkably extended from 186 h for the color center-free sample to 1,000 h using the HAc–Al<sub>2</sub>O<sub>3</sub> support. This facile post-modification was further successfully extended to commercial Al<sub>2</sub>O<sub>3</sub> pellets without altering their mechanical properties, highlighting its potential in industrial applications.</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":"4134 - 4141"},"PeriodicalIF":10.4,"publicationDate":"2024-08-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142225142","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}