Science China Chemistry最新文献_第6页

Short-range electronic engineering by coupling Fe phthalocyanines with MOF-derived N,S-doped carbon nanorods for oxygen reduction Fe酞菁与mof衍生的N， s掺杂碳纳米棒耦合用于氧还原的短程电子工程

IF 10.4 1区化学

Science China Chemistry Pub Date : 2025-01-02 DOI: 10.1007/s11426-024-2349-x

Jie Liu, Qiu Ye, Yi Wu, Junliang Chen, Yongjie Ge, Linjie Zhang, Reza Abazari, Jinjie Qian

{"title":"Short-range electronic engineering by coupling Fe phthalocyanines with MOF-derived N,S-doped carbon nanorods for oxygen reduction","authors":"Jie Liu, Qiu Ye, Yi Wu, Junliang Chen, Yongjie Ge, Linjie Zhang, Reza Abazari, Jinjie Qian","doi":"10.1007/s11426-024-2349-x","DOIUrl":"10.1007/s11426-024-2349-x","url":null,"abstract":"<div><p>Molecular catalysts like metal phthalocyanines (MPc) hold significant promise for diverse applications in renewable energy conversion and storage. Despite their inherent catalytic activity in the oxygen reduction reaction (ORR), enhancing their practical applicability necessitates addressing challenges in electrical conductivity and catalytic stability through effective control of electron distribution within the substrate. In this work, we have successfully synthesized an electrocatalyst featuring FePc molecules anchored onto N,S co-doped carbon nanorods from a pillar-layer metal-organic framework (MOF), designated as ZTB-NSCR-FePc. This MOF-derived heteroatom-doped carbon substrate could be easily obtained by direct pyrolysis of a pre-fabricated rod-like Zn-TDC-bpy. The optimized ZTB-NSCR-FePc demonstrated exceptional electrocatalytic efficiency and stability towards ORR with a positive half-wave potential of 0.890 V. When employed in a Zn-air battery, it outperformed the benchmark Pt/C air cathode, achieving a peak power density of 198.9 mW cm<sup>−2</sup>. Finally, theoretical calculations revealed that short-range electron interactions between N/S atoms and the graphene substrate significantly enhance the anchoring effect of FePc, improve the adsorption of reaction intermediates, and thereby boost the ORR performance.</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"68 5","pages":"1859 - 1868"},"PeriodicalIF":10.4,"publicationDate":"2025-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143918976","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

Engineering N3C vacancies in hierarchical porous carbon nitride nanosheets for room temperature ultradeep photocatalytic aerobic oxidative desulfurization 在层次化多孔氮化碳纳米片上设计N3C空位用于室温超深光催化好氧氧化脱硫

IF 10.4 1区化学

Science China Chemistry Pub Date : 2025-01-02 DOI: 10.1007/s11426-024-2306-1

Yina Nie, Weijie Yang, Xin Wang, Xiang Li, Lele Wei, Xiaolin Bai, Lin Liu, Feng Fu, Jun Wan

{"title":"Engineering N3C vacancies in hierarchical porous carbon nitride nanosheets for room temperature ultradeep photocatalytic aerobic oxidative desulfurization","authors":"Yina Nie, Weijie Yang, Xin Wang, Xiang Li, Lele Wei, Xiaolin Bai, Lin Liu, Feng Fu, Jun Wan","doi":"10.1007/s11426-024-2306-1","DOIUrl":"10.1007/s11426-024-2306-1","url":null,"abstract":"<div><p>The production of ultra-low sulfur clean fuels holds global significance for improving energy efficiency and reducing environmental pollution. Photocatalytic aerobic oxidative desulfurization (PODS) offers an attractive approach to efficiently remove refractory heterocyclic aromatic sulfur compounds under mild conditions. However, the sluggish charge dynamics, insufficient molecule activation, and slow mass transfer within photocatalysts restrict the overall desulfurization efficiency, hindering the widespread application of this technology. Herein, we developed a defective g-C<sub>3</sub>N<sub>4</sub> (M<sub>1</sub>U<sub>3</sub>CN) photocatalyst with bridged N<sub>3C</sub> vacancies and hierarchical porous structures to address these limitations. This catalyst not only demonstrates outstanding dibenzothiophene (DBT) removal efficiency of 99.6% for model oil with high conversion and selectivity but also achieves complete sulfur removal from gasoline as well as 96.7% sulfur removal for distilled diesel at room temperature, successfully achieving ultradeep aerobic oxidative desulfurization. The introduction of rich N<sub>3C</sub> vacancies and abundant micro-meso-macroporous distribution in M<sub>1</sub>U<sub>3</sub>CN enhances kinetic efficiencies by promoting charge carrier separation, mass transfer, and molecular activation simultaneously; resulting in exceptional PODS performance. This work provides a collaborative strategy to overcome kinetic challenges in aerobic oxidative desulfurization <i>via</i> defect and structural engineering of the catalyst.</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"68 4","pages":"1608 - 1619"},"PeriodicalIF":10.4,"publicationDate":"2025-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143716685","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

Efficient large-area flexible organic photovoltaic modules on transparent thin silver electrodes 透明薄银电极上的高效大面积柔性有机光伏组件

IF 10.4 1区化学

Science China Chemistry Pub Date : 2025-01-02 DOI: 10.1007/s11426-024-2299-7

Cong Xie, Zedong Xiong, Xinlu Liu, Wen Wang, Yang Liu, Xueshi Jiang, Xin Lu, Lulu Sun, Yinhua Zhou

{"title":"Efficient large-area flexible organic photovoltaic modules on transparent thin silver electrodes","authors":"Cong Xie, Zedong Xiong, Xinlu Liu, Wen Wang, Yang Liu, Xueshi Jiang, Xin Lu, Lulu Sun, Yinhua Zhou","doi":"10.1007/s11426-024-2299-7","DOIUrl":"10.1007/s11426-024-2299-7","url":null,"abstract":"<div><p>Large-area flexible organic photovoltaic (OPV) modules are challenging to achieve high power conversion efficiency (PCE). Electrical shunts or shortages generally occur in large-area OPV modules due to the ultrathin (100–200 nm) and soft active layers. Improving the surface smoothness of bottom transparent electrode will be able to suppress the shunts and shortages. In this work, we report a method to fabricate smooth and flexible transparent electrodes based on thin silver film, and further to fabricate efficient large-area flexible OPV modules. The fabricated thin silver transparent electrodes simultaneously have high conductivity, high optical transmittance, good mechanical flexibility and low surface roughness. Humidity exposure (h.e.) treatment on MoO<sub>3</sub> effectively facilitates the continuous growth of the thin transparent silver electrode. 6 nm silver film on MoO<sub>3</sub> (h.e.) on plastic substrate shows a transmittance up to 89%, a sheet resistance of 15 Ω/sq, and a low surface roughness with a root-mean-square value of 0.276 nm. Furthermore, 52-cm<sup>2</sup> flexible organic solar modules (15 subcells) showed a certified PCE of 12.66%. Furthermore, a 1350 cm<sup>2</sup> flexible component assembled by 25 pieces of 52–55 cm<sup>2</sup> modules showed certified PCE of 12.10% with an open-circuit voltage of 62.85 V.</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"68 3","pages":"1199 - 1206"},"PeriodicalIF":10.4,"publicationDate":"2025-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143475103","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

Stable copper boron-imidazolate cage as Cu-riched enzyme for highly efficient electrocatalytic CO2 reduction to ethylene 稳定的咪唑铜硼笼型富铜酶用于高效电催化CO2还原成乙烯

IF 10.4 1区化学

Science China Chemistry Pub Date : 2025-01-02 DOI: 10.1007/s11426-024-2290-5

Jun-Qiang Chen, Qiao-Hong Li, Qin-Long Hong, Ping Shao, Hai-Xia Zhang, Jian Zhang

{"title":"Stable copper boron-imidazolate cage as Cu-riched enzyme for highly efficient electrocatalytic CO2 reduction to ethylene","authors":"Jun-Qiang Chen, Qiao-Hong Li, Qin-Long Hong, Ping Shao, Hai-Xia Zhang, Jian Zhang","doi":"10.1007/s11426-024-2290-5","DOIUrl":"10.1007/s11426-024-2290-5","url":null,"abstract":"<div><p>Single-atom catalyst has garnered widespread attention to mimic mature enzymes due to its well-defined atomic structure and coordination environments. However, since the carbon-carbon (C–C) coupling reactions require synergistic catalysis of multiple sites, single-atom catalysts suffer from insufficient active sites and unclear reaction mechanisms. Controlling the reaction intermediates in a precisely targeted pocket through careful metal-organic cage design is therefore crucial. Here, we prepare a tetrahedral [Cu<sub>6</sub>L<sub>4</sub>]-type boron–imidazolate cage integrating highly active Cu sites and optimized cavity, which exhibits enzyme like specific catalytic performance in electrochemical CO<sub>2</sub> reduction reaction (CO<sub>2</sub>RR) to enhance the selectivity of C<sub>2</sub>H<sub>4</sub>. Electrochemical analyses and computational calculations suggest that the single Cu site together with neighboring boron-imidazolate ligands provides suitably synergistic effects that enable the energetically favorable formation of an *COCHO intermediate, a key step determining selectivity. As a result, the [Cu<sub>6</sub>L<sub>4</sub>]-type cage of BIC-145 achieves a Faradaic efficiency of 28% for C<sub>2</sub>H<sub>4</sub> maintaining an average current density of −3.54 mA cm<sup>−2</sup> over a 5-hour electrolysis period. This work represents the first example for studying single-metal site catalysts with ultra-low coordination numbers through the rational design of metal-organic cages.</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"68 3","pages":"943 - 950"},"PeriodicalIF":10.4,"publicationDate":"2025-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143475122","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

Impregnating photo-stable gold precursor onto uncalcined TS-1 to boost catalytic hydro-oxidation of propane 在未煅烧的TS-1上浸渍光稳定金前驱体以促进丙烷的催化加氢氧化

IF 10.4 1区化学

Science China Chemistry Pub Date : 2025-01-02 DOI: 10.1007/s11426-024-2403-7

Zhihua Zhang, Erchuan Yang, Fan Liu, Kesheng Xu, Yuxia Zhong, Jinwei Sun, Shudong Shi, Xuezhi Duan, Xinggui Zhou

{"title":"Impregnating photo-stable gold precursor onto uncalcined TS-1 to boost catalytic hydro-oxidation of propane","authors":"Zhihua Zhang, Erchuan Yang, Fan Liu, Kesheng Xu, Yuxia Zhong, Jinwei Sun, Shudong Shi, Xuezhi Duan, Xinggui Zhou","doi":"10.1007/s11426-024-2403-7","DOIUrl":"10.1007/s11426-024-2403-7","url":null,"abstract":"<div><p>Immobilizing highly dispersed Au nanoparticles onto titanium silicalite-1 (TS-1) by a simple impregnation method under light is still a challenging task. In this work, a high photostable Au precursor protected by thiol ligands was firstly synthesized, and the as-prepared Au precursor displayed excellent stability under light for over 30 days, while the Au precursor without thiol ligands formed precipitates after just 2 h under light. Subsequently, the Au precursor protected by thiol ligands was immobilized on the external surface of uncalcined TS-1 (i.e., TS-1-B) by the incipient wetness impregnation method (IWI method) to prepare Au/TS-1-B catalyst. The activity of as-prepared Au/TS-1-B catalyst in the hydro-oxidation of propane to acetone was 1.4 times higher than that of the catalyst prepared by the deposition-precipitation urea method (DPU method). The structures of the Au/TS-1-B catalysts prepared by different methods were analyzed by multiple characterizations. Compared to the Au/TS-1-B catalyst prepared by the DPU method, the Au/TS-1-B catalyst synthesized by the IWI method exhibited a narrower size distribution of Au nanoparticles and had more small Au particles (<2 nm), which is the main reason for its superior activity. Additionally, the effects of gold loadings, reaction temperature and Si/Ti molar ratio on the catalytic performance of the Au/TS-1-B catalyst prepared by the IWI method were also investigated. In addition, the Au/TS-1-B catalyst prepared by the IWI method also exhibited excellent stability for over 140 h.</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"68 4","pages":"1585 - 1596"},"PeriodicalIF":10.4,"publicationDate":"2025-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143716684","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

Research progress in metal-organic frameworks and their derivatives in electrochemistry 电化学中金属有机骨架及其衍生物的研究进展

IF 10.4 1区化学

Science China Chemistry Pub Date : 2025-01-02 DOI: 10.1007/s11426-024-2277-2

Lingling Chen, Yuxin Liu, Yichun Su, Wenchen Zhu, Guangyu Du, Huan Pang

{"title":"Research progress in metal-organic frameworks and their derivatives in electrochemistry","authors":"Lingling Chen, Yuxin Liu, Yichun Su, Wenchen Zhu, Guangyu Du, Huan Pang","doi":"10.1007/s11426-024-2277-2","DOIUrl":"10.1007/s11426-024-2277-2","url":null,"abstract":"<div><p>Metal-organic frameworks (MOFs) are distinguished by their unique porosity and meticulously ordered framework structures, setting them apart from conventional complexes. These materials are defined by their highly organized crystalline and pore structures, extensive surface areas, robust porosity, and superior adsorption capabilities. Owing to their exceptional structural and functional attributes, MOFs and their derivatives are leveraged across a broad spectrum of applications, demonstrating significant potential across diverse sectors. In recent times, the scientific community has increasingly focused on MOFs, underscoring their growing importance in research. Despite the promising array of applications for MOFs and their derivatives, challenges persist in practical deployments, and the pathway to research advancement remains daunting. This document delves into the synthesis and various applications of MOFs and their derivatives, particularly in the domains of energy storage, catalysis, sensing, and water treatment. It also highlights the ongoing research progress in the field of electrochemistry, including developments in lithium ion batteries (LIBs), lithium-sulfur batteries (LSBs), zinc-ion batteries (ZIBs), aqueous nickel-zinc batteries (NZBs), and supercapacitors. Finally, it provides an outlook on the future prospects and potential hurdles facing the development of MOF materials.</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"68 4","pages":"1287 - 1316"},"PeriodicalIF":10.4,"publicationDate":"2025-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143716766","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

Physarum polycephalum-inspired adaptive optimization design of artificial microtubular networks 基于多头绒泡菌的人工微管网络自适应优化设计

IF 10.4 1区化学

Science China Chemistry Pub Date : 2025-01-02 DOI: 10.1007/s11426-024-2305-8

Si-Min Zeng, Di-Wei Zheng, Ting Pan, Xing-Lan Ding, Yun Zhang, Chi-Hui Yang, Si-Xue Cheng, Xian-Zheng Zhang

{"title":"Physarum polycephalum-inspired adaptive optimization design of artificial microtubular networks","authors":"Si-Min Zeng, Di-Wei Zheng, Ting Pan, Xing-Lan Ding, Yun Zhang, Chi-Hui Yang, Si-Xue Cheng, Xian-Zheng Zhang","doi":"10.1007/s11426-024-2305-8","DOIUrl":"10.1007/s11426-024-2305-8","url":null,"abstract":"<div><p>Natural biological microtubular networks have undergone adaptive evolutionary selection and may offer viable solutions to design challenges in artificial microtubular networks. The plasmodium of the slime mold <i>Physarum polycephalum</i> (<i>P. polycephalum</i>) extends continuously to form a protoplasmic microtubular network structure, directly connecting food sources. Computational simulations revealed that the formation of this adaptive <i>P. polycephalum</i> microtubular network could be captured by a mathematical algorithm. Inspired by the <i>P. polycephalum</i> microtubular networks, we propose an adaptive optimization design method for artificial microtubular networks. Specifically, we utilized hydrogels with biodegradable and tissue-adhesive properties to replicate the <i>P. polycephalum</i> microtubular networks <i>via</i> photomask. In Rhodamine B diffusion and glucose-catalyzed reaction experiments, we found that the <i>P. polycephalum</i> microtubular networks exhibited significantly enhanced efficiency compared to vascular and artificial networks. Furthermore, we demonstrated the potential for uric acid (UA) degradation of the hydrogels with a real <i>P. polycephalum</i> microtubular network loaded with urate oxidase (UOx) in a rodent model of hyperuricemia. And this network achieved more than double the effect of the artificial network. This underscores the potential of natural microtubular networks to replace artificial microtubular networks.</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"68 4","pages":"1497 - 1510"},"PeriodicalIF":10.4,"publicationDate":"2025-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143716763","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

Multivariate synergy for heightening ionic HOF robustness and proton conductivity 提高离子HOF稳健性和质子电导率的多元协同作用

IF 10.4 1区化学

Science China Chemistry Pub Date : 2025-01-02 DOI: 10.1007/s11426-024-2352-9

Xiang-Tian Bai, Li-Hui Cao, Xu-Yong Chen, Jia-Yu Wang, Zi-Ye Zhou

{"title":"Multivariate synergy for heightening ionic HOF robustness and proton conductivity","authors":"Xiang-Tian Bai, Li-Hui Cao, Xu-Yong Chen, Jia-Yu Wang, Zi-Ye Zhou","doi":"10.1007/s11426-024-2352-9","DOIUrl":"10.1007/s11426-024-2352-9","url":null,"abstract":"<div><p>Multicomponent crystalline materials construct more complex and diversified structures with different combinations and modes, which expands the material structure space and application fields. In this work, we have successfully synthesized two two-component ionic hydrogen-bonded organic frameworks (<b>iHOF-32</b> and <b>iHOF-33</b>) and a three-component iHOF (<b>iHOF-34</b>). Guanidine hydrochloride which is rich in N and H and has a short chain length strengthens the hydrogen bonding network of iHOF, thereby aiding in the efficient migration of protons. The rigid architecture of 1,1′-diamino-4,4′-bipyridine diiodide furnishes additional scaffolding for the iHOFs and enhances its robustness under harsh conditions. <b>iHOF-34</b> accomplishes the combination of the ultra-high proton conductivity of <b>iHOF-32</b> and the robustness of <b>iHOF-33</b> by the synergistic interaction among the three components of ligands. In addition, <b>iHOF-34</b> was fabricated as a composite membrane with a peak proton conductivity of 1.55 × 10<sup>−1</sup> S cm<sup>−1</sup>, which is 3.8 times higher than that of recast Nafion, and has extensive potential in fuel cells. The self-assembly strategy of multicomponent HOFs opens up new avenues for constructing diverse structures while promising new opportunities for applications in the fields of proton conduction and energy storage.</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"68 5","pages":"1879 - 1887"},"PeriodicalIF":10.4,"publicationDate":"2025-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143918975","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

Self-reporting hypoxia-responsive supramolecular phototheranostic nanomaterials based on AIEgen and azocalixarene 基于aigen和偶氮杯芳烃的自报告低氧反应超分子光疗纳米材料

IF 10.4 1区化学

Science China Chemistry Pub Date : 2025-01-02 DOI: 10.1007/s11426-024-2301-3

Xiao-Wen Han, Guo-Ling Zhang, Pu Chen, Jing Zhang, Guogang Shan, Chunxuan Qi, Ben Zhong Tang, Hai-Tao Feng

{"title":"Self-reporting hypoxia-responsive supramolecular phototheranostic nanomaterials based on AIEgen and azocalixarene","authors":"Xiao-Wen Han, Guo-Ling Zhang, Pu Chen, Jing Zhang, Guogang Shan, Chunxuan Qi, Ben Zhong Tang, Hai-Tao Feng","doi":"10.1007/s11426-024-2301-3","DOIUrl":"10.1007/s11426-024-2301-3","url":null,"abstract":"<div><p>Hypoxia is a significant feature in most of solid tumors. Hence, developing hypoxia-responsive phototheranostic system is still a challenge. In this contribution, a supramolecular assembly strategy based on sulfonate-functionalized azocalix[4]arene (SAC4A) and cationic aggregation-induced emission photosensitizer (namely TPA-H) was proposed for hypoxia-responsive bioimaging and photodynamic therapy (PDT). Upon supramolecular complexation of TPA-H and SAC4A through electrostatic interaction, the fluorescence and reactive oxygen species (ROS) generation of TPA-H were largely inhibited. In hypoxic tumors, the azo group of SAC4A can be reduced to aniline derivative and release the included TPA-H to recover its pristine fluorescence and ROS. Interestingly, the free TPA-H undergoes cell membrane-to-mitochondria translocation during cell imaging, achieving a real-time self-reporting PDT system. <i>In vivo</i> tumor imaging and therapy reveal that this as-prepared supramolecular complexes have good biosafety and efficient antitumor activity under hypoxia. Such hypoxia-responsive supramolecular photosensitizer system will enrich image-guided photodynamic therapy.</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"68 4","pages":"1550 - 1562"},"PeriodicalIF":10.4,"publicationDate":"2025-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143716764","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

Facile synthesis of the dodecahydridododecaborate (B12H122−) from borane Lewis base adducts 硼烷路易斯碱加合物快速合成十二氢化十二十二硼酸酯（B12H122−）

IF 10.4 1区化学

Science China Chemistry Pub Date : 2025-01-02 DOI: 10.1007/s11426-024-2334-0

Yi Jing, Xin-Ran Liu, Xinghua Wang, Hui Han, Sha-Sha Liang, Xi-Meng Chen, Donghui Wei, Lai-Sheng Wang, Xuenian Chen

{"title":"Facile synthesis of the dodecahydridododecaborate (B12H122−) from borane Lewis base adducts","authors":"Yi Jing, Xin-Ran Liu, Xinghua Wang, Hui Han, Sha-Sha Liang, Xi-Meng Chen, Donghui Wei, Lai-Sheng Wang, Xuenian Chen","doi":"10.1007/s11426-024-2334-0","DOIUrl":"10.1007/s11426-024-2334-0","url":null,"abstract":"<div><p>Polyhedral boranes are a class of well-known boron molecular clusters widely used in energy, chemistry, medicine, and materials science because of their unique physical and chemical properties. Great efforts have been made in the past decades to find more effective synthetic methods for this important class of boron compounds. However, existing synthetic methods suffer from low efficiency and low selectivity. Herein, we report a facile one-pot synthesis of [(CH<sub>3</sub>)<sub>3</sub>S]<sub>2</sub>B<sub>12</sub>H<sub>12</sub> with moderate yields at mild conditions. The mechanisms for the multi-step chemoselective synthesis of B<sub>12</sub>H<sub>12</sub><sup>2−</sup> without other by-products are elucidated based on theoretical results and our previous work. The Lewis base used in B–H bond condensation reaction, which acts as a hydrogen or to balance the newly generated polyhedral borane charges, is proposed and studied in detail. The current study has led to a more effective and selective synthetic method for B<sub>12</sub>H<sub>12</sub><sup>2−</sup> and has also implicated the syntheses of other new polyhedral boranes.</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"68 4","pages":"1355 - 1361"},"PeriodicalIF":10.4,"publicationDate":"2025-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143716751","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