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Polydopamine-modified biochar supported polylactic acid and zero-valent iron affects the functional microbial community structure for 1,1,1-trichloroethane removal in simulated groundwater 聚多巴胺改性生物炭(支持聚乳酸和零价铁)影响模拟地下水中去除 1,1,1- 三氯乙烷的功能微生物群落结构
IF 9.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-08-02 DOI: 10.1016/j.cclet.2024.110313
Haitao Yin , Liang Meng , Li Li , Jiamu Xiao , Longrui Liang , Nannan Huang , Yansong Shi , Angang Zhao , Jingwen Hou
In-situ enhanced bioreduction by functional materials is a cost-effective technology to remove chlorinated hydrocarbons in groundwater. Herein, a novel polydopamine (PDA)-modified biochar (BC)-based composite containing nanoscale zero-valent iron (nZVI) and poly-l-lactic acid (PLLA) (PB-PDA-Fe) was synthesized to enhance the removal of 1,1,1-trichloroethane (1,1,1-TCA) in simulated groundwater with actual site sediments. Its impact on functional microbial community structure in system was also investigated. The typical characterizations revealed uniform dispersion of PLA and nZVI particles on the BC surface, being smoother after PDA coating. The composite exhibited a significantly higher performance on 1,1,1-TCA removal (82.38%, initial concentration 100 mg/L) than Fe-PDA and PB-PDA treatments. The diversity and richness of the microbial community in the composite treatment consistently decreased during incubation due to a synergistic effect between PLLA-BC and nZVI. Desulfitobaterium, Pedobacter, Sphaerochaeta, Shewanella, and Clostridium were identified as enriched genera by the composite through DNA-stable isotope probing (DNA-SIP), playing a crucial role in the bioreductive dechlorination process. All the above results demonstrate that this novel composite selectively enhances the activity of microorganisms with extracellular respiration functions to efficiently dechlorinate 1,1,1-TCA. These findings could contribute to understanding the responsive microbial community by carbon-iron composites and expedite the application of in-situ enhanced bioreduction for effective remediation of chlorinated hydrocarbon-contaminated groundwater.
利用功能材料原位增强生物还原是一种去除地下水中氯化碳氢化合物的经济有效的技术。本文合成了一种新型聚多巴胺(PDA)改性生物炭(BC)复合材料,其中含有纳米级零价铁(nZVI)和聚乳酸(PLLA)(PB-PDA-Fe),用于提高实际场地沉积物模拟地下水中 1,1,1-三氯乙烷(1,1,1-TCA)的去除率。同时还研究了其对系统中功能微生物群落结构的影响。典型的表征结果表明,聚乳酸和 nZVI 颗粒在 BC 表面均匀分散,在涂覆 PDA 后更加光滑。该复合材料对 1,1,1-三氯乙酸的去除率(82.38%,初始浓度 100 mg/L)明显高于 Fe-PDA 和 PB-PDA 处理。由于 PLLA-BC 和 nZVI 的协同作用,复合处理中微生物群落的多样性和丰富度在培养过程中持续下降。通过 DNA 稳定同位素探针(DNA-SIP),确定了脱硫杆菌、Pedobacter、Sphaerochaeta、Shewanella 和 Clostridium 是复合材料中的富集菌属,它们在生物还原脱氯过程中发挥着重要作用。上述结果表明,这种新型复合材料可选择性地增强具有细胞外呼吸功能的微生物有效脱氯 1,1,1-TCA 的活性。这些发现有助于了解碳-铁复合材料对微生物群落的响应,并加快应用原位增强生物还原法有效修复受氯烃类污染的地下水。
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引用次数: 0
Advances in virus-host interaction research based on microfluidic platforms 基于微流控平台的病毒-宿主相互作用研究进展
IF 9.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-31 DOI: 10.1016/j.cclet.2024.110302
Cheng Wang , Ji Wang , Dong Liu , Zhi-Ling Zhang

Viral epidemics pose a serious threat to global public health, making it essential to explore virus-host interactions for uncovering the pathogenesis of viral diseases and developing effective antiviral strategies. Traditional in vitro cell infection models struggle to replicate physiological microenvironment, while animal infection models may encounter obstacles such as species gap, high-cost, and ethical issues. Additionally, potential heterogeneous infection outcomes are usually inaccessible by population-based experiments. Microfluidics, as an emerging interdisciplinary platform, has proven to be a powerful tool for inquiring virus-host interactions. In this review, conventional virological methods were introduced first and remarkable advantages of microfluidics in viral cell biology were highlighted. Next, the in-depth applications of microfluidics in analyzing heterogeneity of virus-host interplays, dynamic monitoring of events related to viral life cycle, and modeling of viral infectious diseases were fully elaborated from the perspective of single-cell chip, multi-cell culture chip and organ-on-a-chip (organ chip). Finally, the opportunities and challenges in developing robust microfluidic methods for virology were discussed. Overall, this review aims to provide an overview of microfluidic-based research on virus-host interaction and promote multidisciplinary collaborations for better understanding and responding to viral threats.

病毒流行对全球公共卫生构成严重威胁,因此必须探索病毒与宿主之间的相互作用,以揭示病毒性疾病的发病机理并开发有效的抗病毒策略。传统的体外细胞感染模型难以复制生理微环境,而动物感染模型可能会遇到物种差异、高成本和伦理问题等障碍。此外,基于群体的实验通常无法获得潜在的异质性感染结果。微流控技术作为一种新兴的跨学科平台,已被证明是研究病毒与宿主相互作用的有力工具。在这篇综述中,首先介绍了传统的病毒学方法,并强调了微流控技术在病毒细胞生物学中的显著优势。接着,从单细胞芯片、多细胞培养芯片和器官芯片的角度,全面阐述了微流控技术在分析病毒-宿主相互作用的异质性、动态监测病毒生命周期相关事件和病毒传染病建模等方面的深入应用。最后,还讨论了为病毒学开发稳健的微流控方法所面临的机遇和挑战。总之,本综述旨在概述基于微流控技术的病毒-宿主相互作用研究,促进多学科合作,以更好地理解和应对病毒威胁。
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引用次数: 0
IFC - Editorial Board/ Publication info 国际金融公司 - 编辑委员会/出版信息
IF 9.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-30 DOI: 10.1016/S1001-8417(24)00674-0
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引用次数: 0
Visible light excitation on CuPd/TiN with enhanced chemisorption for catalyzing heck reaction 可见光激发 CuPd/TiN 化学吸附作用增强,可催化 heck 反应
IF 9.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-28 DOI: 10.1016/j.cclet.2024.110299
Xuhui Fan , Fan Wang , Mengjiao Li , Faiza Meharban , Yaying Li , Yuanyuan Cui , Xiaopeng Li , Jingsan Xu , Qi Xiao , Wei Luo
In this work, we developed plasmonic photocatalyst composed of CuPd alloy nanoparticles supported on TiN, the optimized Cu3Pd2/TiN catalyst shows excellent conversion (>96 %) and selectivity (>99 %) for Heck reaction at 50 °C under visible light irradiation. By in-situ spectroscopic investigations, we find that visible light excitation could achieve stable metallic Cu species on the surface of CuPd alloy nanoparticles, thereby eliminating the inevitable surface oxides of Cu based catalyst. The in-situ formed metallic Cu species under irradiation take advantage of the strong interactions of Cu with visible light, and manifest in the localized surface plasmon resonances (LSPR) photoexcitation. Visible light excitation could further promote the charge transfer between catalytic Pd component and the support TiN, resulting in electron-rich Pd sites on CuPd/TiN. Moreover, light excitation on CuPd/TiN generates strong chemisorption of iodobenzene and styrene, favoring the activation of reactants for Heck reaction. DFT calculations suggest that electron-rich CuPd sites ideally lower the activation energy barrier for the coupling reaction. This work provides valuable insights for mechanistic understanding of plasmonic photocatalysis.
在这项工作中,我们开发了由 CuPd 合金纳米粒子支撑在 TiN 上组成的等离子体光催化剂,优化后的 Cu3Pd2/TiN 催化剂在可见光照射下于 50 °C,对 Heck 反应具有优异的转化率(96%)和选择性(99%)。通过原位光谱研究,我们发现可见光激发可以在 CuPd 合金纳米颗粒表面形成稳定的金属 Cu 物种,从而消除了 Cu 基催化剂不可避免的表面氧化物。辐照下原位形成的金属铜物种利用了铜与可见光的强相互作用,表现为局部表面等离子体共振(LSPR)光激发。可见光激发可进一步促进催化钯成分与支持物 TiN 之间的电荷转移,从而在 CuPd/TiN 上形成富电子钯位。此外,CuPd/TiN 上的光激发会产生强烈的碘苯和苯乙烯化学吸附,有利于活化 Heck 反应的反应物。DFT 计算表明,富电子 CuPd 位点能理想地降低偶联反应的活化能垒。这项工作为从机理上理解等离子体光催化提供了宝贵的见解。
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引用次数: 0
The controlled oxidation states of the H4PMo11VO40 catalyst induced by plasma for the selective oxidation of methacrolein 等离子体诱导 H4PMo11VO40 催化剂的可控氧化态,用于选择性氧化甲基丙烯醛
IF 9.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-28 DOI: 10.1016/j.cclet.2024.110298
Gang Hu , Chun Wang , Qinqin Wang , Mingyuan Zhu , Lihua Kang
In this paper, low-temperature dielectric-blocked discharge plasma (DBD) was employed for the first time to treat silica-doped H4PMo11VO40 (HPAV) catalysts (DBD(Ar/x)-MF-Catal) and apply them in the catalytic methacrolein (MAL) selective oxidation to produce methacrylic acid (MAA). This work investigates in detail the controllable regulation of the concentration of oxidation states on silica-doped HPAV catalysts by adjusting the DBD discharge with controlled changes in voltage, current, treatment time, and treatment medium. It reports the intrinsic correlation between oxidation states and MAL oxidation performance. The research results indicated that the catalytic performance was related to the presence of oxygen vacancies and oxygen species (VO2+), and are the main reason for the selective oxidation of MAL to MAA. Besides, the generation of oxygen vacancies and VO2+ altered localized electrons, which resulted in the easier activation of O2. Theoretical calculations of DFT also proved the formation mechanism of oxygen vacancies and VO2+ and electron properties on high-performance polymers, which elucidated the intrinsic influence of catalyst components. The DBD(Ar/10)-MF-Catal catalysts with suitable VO2+ and oxygen vacancy concentrations exhibited the highest catalytic performance with 90 % MAL conversion and 70 % MAA selectivity and showed good stability (500 h).
本文首次采用低温介质阻挡放电等离子体(DBD)处理二氧化硅掺杂的 H4PMo11VO40(HPAV)催化剂(DBD(Ar/x)-MF-Catal),并将其应用于催化甲基丙烯醛(MAL)选择性氧化生成甲基丙烯酸(MAA)。这项工作详细研究了通过控制电压、电流、处理时间和处理介质的变化来调节 DBD 放电,从而可控地调节二氧化硅掺杂 HPAV 催化剂上氧化态的浓度。报告了氧化态与 MAL 氧化性能之间的内在联系。研究结果表明,催化性能与氧空位和氧物种(VO2+)的存在有关,是将 MAL 选择性氧化为 MAA 的主要原因。此外,氧空位和 VO2+ 的产生改变了局部电子,使 O2 更容易活化。DFT 理论计算也证明了氧空位和 VO2+ 的形成机理以及电子在高性能聚合物上的特性,阐明了催化剂组分的内在影响。具有合适 VO2+ 和氧空位浓度的 DBD(Ar/10)-MF-Catal 催化剂具有最高的催化性能,MAL 转化率为 90%,MAA 选择性为 70%,并表现出良好的稳定性(500 h)。
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引用次数: 0
Direct identification of energy transfer mechanism in CeIII-MnII system by constructing molecular heteronuclear complexes 通过构建分子异核配合物直接确定 CeIII-MnII 系统的能量传递机制
IF 9.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-26 DOI: 10.1016/j.cclet.2024.110296
Huanyu Liu , Gang Yu , Ruoyao Guo, Hao Qi, Jiayin Zheng, Tong Jin, Zifeng Zhao, Zuqiang Bian, Zhiwei Liu
Sensitization of metal-centered forbidden transitions is of great significance. Solid MnII-based phosphors with d-d forbidden transition sensitized by CeIII with d-f allowed transition are promising light conversion materials, but the energy transfer mechanism in CeIII-MnII is still in dispute for the uncertainty of distances between metal centers. Herein, for the first time, we explored the energy transfer mechanism in two well-designed luminescent heteronuclear complexes with clear crystal structures, i.e. Ce-N8-Mn and Ce-N2O6-Mn (N8 = 1,4,7,10,13,16,21,24-octaazabicyclo[8.8.8]hexacosane; N2O6 = 4,7,13,16,21,24-hexaoxa-1,10-diazabicyclo[8.8.8]hexacosane). Short distances between metal centers facilitate efficient energy transfer from CeIII to MnII in both complexes, resulting in high photoluminescence quantum yield up to unity. After systematic study of the two heteronuclear complexes as well as two reference complexes Ce(N8)Br3 and Ce(N2O6)Br3, we concluded that dipole-quadrupole interaction is the dominant energy transfer mechanism in the heteronuclear complexes.
金属中心禁止跃迁的敏化具有重要意义。具有 d-f 允许跃迁的 CeIII 对具有 d-d 禁止跃迁的 MnII 固体荧光粉的敏化是一种很有前景的光转换材料,但由于金属中心间距离的不确定性,CeIII-MnII 的能量传递机制仍存在争议。在此,我们首次探索了两种具有清晰晶体结构的设计良好的发光异核配合物(即 Ce-N8-MnII 和 CeIII-MnII)的能量传递机制。即 Ce-N8-Mn 和 Ce-N2O6-Mn (N8 = 1,4,7,10,13,16,21,24-octaazabicyclo[8.8.8]hexacosane; N2O6 = 4,7,13,16,21,24-hexaoxa-1,10-diazabicyclo[8.8.8]hexacosane )。金属中心之间的短距离促进了这两种配合物中 CeIII 向 MnII 的有效能量转移,从而使光致发光量子产率高达一倍。经过对这两种异核配合物以及两种参考配合物 Ce(N8)Br3 和 Ce(N2O6)Br3 的系统研究,我们得出结论:偶极子-四极相互作用是异核配合物中最主要的能量转移机制。
{"title":"Direct identification of energy transfer mechanism in CeIII-MnII system by constructing molecular heteronuclear complexes","authors":"Huanyu Liu ,&nbsp;Gang Yu ,&nbsp;Ruoyao Guo,&nbsp;Hao Qi,&nbsp;Jiayin Zheng,&nbsp;Tong Jin,&nbsp;Zifeng Zhao,&nbsp;Zuqiang Bian,&nbsp;Zhiwei Liu","doi":"10.1016/j.cclet.2024.110296","DOIUrl":"10.1016/j.cclet.2024.110296","url":null,"abstract":"<div><div>Sensitization of metal-centered forbidden transitions is of great significance. Solid Mn<sup>II</sup>-based phosphors with d-d forbidden transition sensitized by Ce<sup>III</sup> with d-f allowed transition are promising light conversion materials, but the energy transfer mechanism in Ce<sup>III</sup>-Mn<sup>II</sup> is still in dispute for the uncertainty of distances between metal centers. Herein, for the first time, we explored the energy transfer mechanism in two well-designed luminescent heteronuclear complexes with clear crystal structures, <em>i.e.</em> Ce-N8-Mn and Ce-N2O6-Mn (N8 = 1,4,7,10,13,16,21,24-octaazabicyclo[8.8.8]hexacosane; N2O6 = 4,7,13,16,21,24-hexaoxa-1,10-diazabicyclo[8.8.8]hexacosane). Short distances between metal centers facilitate efficient energy transfer from Ce<sup>III</sup> to Mn<sup>II</sup> in both complexes, resulting in high photoluminescence quantum yield up to unity. After systematic study of the two heteronuclear complexes as well as two reference complexes Ce(N8)Br<sub>3</sub> and Ce(N2O6)Br<sub>3</sub>, we concluded that dipole-quadrupole interaction is the dominant energy transfer mechanism in the heteronuclear complexes.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 2","pages":"Article 110296"},"PeriodicalIF":9.4,"publicationDate":"2024-07-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141841515","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
Rationally constructing metallic Sn-ZnO heterostructure via in-situ Mn doping for high-rate Na-ion batteries 通过原位掺杂锰合理构建用于高倍率钠离子电池的金属锡锌氧化物异质结构
IF 9.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-25 DOI: 10.1016/j.cclet.2024.110273
Bin Feng , Tao Long , Ruotong Li , Yuan-Li Ding
Developing a heterostructure for alloying-based anode for sodium-ion batteries (SIBs) is an efficient solution to accommodate volume change upon sodiation/desodiation and boost sodium storage since it combines the merits of each component. Herein, we report a metallic and microphone-like Sn-Zn0.9Mn0.1O heterostructure via an in-situ Mn doping strategy. Based on theoretical calculations and experimental results, the introduction of Mn into ZnO (a small amount of Mn also diffuses into the Sn lattice) can not only enhance intrinsic electronic conductivity but also reduce the Na+ diffusion barrier inside the Sn phase. When evaluated as anode for SIBs, the obtained heterostructures show a high reversible capacity of 395.1 mAh/g at 0.1 A/g, rate capability of 332 mAh/g at 5 A/g, and capacity retention of almost 100 % after 850 cycles at 5 A/g, indicating its great potential for high-power application of SIBs.
为钠离子电池(SIB)的合金基阳极开发一种异质结构是适应钠化/解钠时的体积变化并提高钠存储量的有效解决方案,因为它结合了每种成分的优点。在此,我们通过原位掺杂锰的策略,报告了一种金属和麦克风状的 Sn-Zn0.9Mn0.1O 异质结构。根据理论计算和实验结果,在 ZnO 中引入 Mn(少量 Mn 也扩散到锡晶格中)不仅能提高本征电子电导率,还能降低锡相内部的 Na+ 扩散阻抗。在作为 SIB 的阳极进行评估时,所获得的异质结构在 0.1 A/g 条件下显示出 395.1 mAh/g 的高可逆容量,在 5 A/g 条件下显示出 332 mAh/g 的速率能力,在 5 A/g 条件下循环 850 次后容量保持率几乎达到 100%,这表明它在 SIB 的大功率应用方面具有巨大潜力。
{"title":"Rationally constructing metallic Sn-ZnO heterostructure via in-situ Mn doping for high-rate Na-ion batteries","authors":"Bin Feng ,&nbsp;Tao Long ,&nbsp;Ruotong Li ,&nbsp;Yuan-Li Ding","doi":"10.1016/j.cclet.2024.110273","DOIUrl":"10.1016/j.cclet.2024.110273","url":null,"abstract":"<div><div>Developing a heterostructure for alloying-based anode for sodium-ion batteries (SIBs) is an efficient solution to accommodate volume change upon sodiation/desodiation and boost sodium storage since it combines the merits of each component. Herein, we report a metallic and microphone-like Sn-Zn<sub>0.9</sub>Mn<sub>0.1</sub>O heterostructure <em>via</em> an <em>in-situ</em> Mn doping strategy. Based on theoretical calculations and experimental results, the introduction of Mn into ZnO (a small amount of Mn also diffuses into the Sn lattice) can not only enhance intrinsic electronic conductivity but also reduce the Na<sup>+</sup> diffusion barrier inside the Sn phase. When evaluated as anode for SIBs, the obtained heterostructures show a high reversible capacity of 395.1 mAh/g at 0.1 A/g, rate capability of 332 mAh/g at 5 A/g, and capacity retention of almost 100 % after 850 cycles at 5 A/g, indicating its great potential for high-power application of SIBs.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 2","pages":"Article 110273"},"PeriodicalIF":9.4,"publicationDate":"2024-07-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141838859","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
Robust free-base and metalated corrole radicals with reduction-induced emission 具有还原诱导发射功能的强效游离基和金属化珊瑚自由基
IF 9.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-23 DOI: 10.1016/j.cclet.2024.110292
Pengfei Li , Chulin Qu , Fan Wu , Hu Gao , Chengyan Zhao , Yue Zhao , Zhen Shen
Preparing free-base porphyrinoid radicals that can function as coordination ligands is a challenging task. Here we report the synthesis of a stable, free-base benzocorrole (BC) radical containing only two inner NH protons via a retro-Diels-Alder conversion. The radical character of BC was fully supported by crystallographic analysis, spectroscopic evidence, and theoretical calculations. This neutral radical ligand allowed easy insertion of Zn(II), Ga(III), and Pd(II) ions to produce radical complexes. All these radicals exhibited luminescence-on responses under weak reducing atmosphere, corresponding to the conversion to their aromatic anions. The red fluorescence was observed for BC and its Zn(II) and Ga(III) complexes, and the near-infrared phosphorescence (>900 nm) was detected for Pd(II) complex at room temperature. Furthermore, Ga(III) corrole exhibited a variation in fluorescence in response to axial coordination. Our findings provide a promising radical platform for coordination and developing novel functional materials with switchable spin and emission.
制备可用作配位体的自由基卟啉基是一项具有挑战性的任务。在此,我们报告了通过逆-Diels-Alder 转化法合成稳定的、仅含两个内部 NH 质子的自由基苯并吡咯(BC)自由基的情况。晶体学分析、光谱证据和理论计算充分证明了 BC 的自由基性质。这种中性自由基配体很容易插入 Zn(II)、Ga(III) 和 Pd(II) 离子,生成自由基配合物。在弱还原气氛下,所有这些自由基都表现出发光反应,相当于转化为它们的芳香阴离子。在室温下,BC 及其 Zn(II) 和 Ga(III) 复合物可发出红色荧光,Pd(II) 复合物可发出近红外磷光(900 nm)。此外,Ga(III)络合物的荧光随轴向配位的变化而变化。我们的研究结果为配位和开发具有可切换自旋和发射的新型功能材料提供了一个前景广阔的自由基平台。
{"title":"Robust free-base and metalated corrole radicals with reduction-induced emission","authors":"Pengfei Li ,&nbsp;Chulin Qu ,&nbsp;Fan Wu ,&nbsp;Hu Gao ,&nbsp;Chengyan Zhao ,&nbsp;Yue Zhao ,&nbsp;Zhen Shen","doi":"10.1016/j.cclet.2024.110292","DOIUrl":"10.1016/j.cclet.2024.110292","url":null,"abstract":"<div><div>Preparing free-base porphyrinoid radicals that can function as coordination ligands is a challenging task. Here we report the synthesis of a stable, free-base benzocorrole (<strong>BC</strong>) radical containing only two inner NH protons <em>via</em> a <em>retro</em>-Diels-Alder conversion. The radical character of <strong>BC</strong> was fully supported by crystallographic analysis, spectroscopic evidence, and theoretical calculations. This neutral radical ligand allowed easy insertion of Zn(II), Ga(III), and Pd(II) ions to produce radical complexes. All these radicals exhibited luminescence-on responses under weak reducing atmosphere, corresponding to the conversion to their aromatic anions. The red fluorescence was observed for <strong>BC</strong> and its Zn(II) and Ga(III) complexes, and the near-infrared phosphorescence (&gt;900 nm) was detected for Pd(II) complex at room temperature. Furthermore, Ga(III) corrole exhibited a variation in fluorescence in response to axial coordination. Our findings provide a promising radical platform for coordination and developing novel functional materials with switchable spin and emission.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 2","pages":"Article 110292"},"PeriodicalIF":9.4,"publicationDate":"2024-07-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141842672","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
Tumor acidic microenvironment activatable DNA nanostructure for precise cancer cell targeting and inhibition 可激活肿瘤酸性微环境的 DNA 纳米结构,用于精确靶向和抑制癌细胞
IF 9.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-23 DOI: 10.1016/j.cclet.2024.110289
Yanfei Liu , Yaqin Hu , Yifu Tan , Qiwen Chen , Zhenbao Liu
Precise tumor targeting and therapy is a major trend in cancer treatment. Herein, we designed a tumor acidic microenvironment activatable drug loaded DNA nanostructure, in which, we made a clever use of the sequences of AS1411 and i-motif, which can partially hybridize, and designed a simple while robust DNA d-strand nanostructure, in which, i-motif sequence was designed to regulate the binding ability of the AS1411 aptamer to target tumor. In the normal physiological environment, i-motif inhibits the targeting ability of AS1411. In the acidic tumor microenvironment, i-motif forms a quadruplex conformation and dissociates from AS1411, restoring the targeting ability of AS1411. Only when acidic condition and tumor cell receptor are present, this nanostructure can be internalized by the tumor cells. Moreover, the structure change of this nanostructure can realize the release of loaded drug. This drug loaded A-I-Duplex DNA structure showed cancer cell and spheroid targeting and inhibition ability, which is promising in the clinical cancer therapy.
肿瘤精准靶向治疗是癌症治疗的一大趋势。本文设计了一种可在肿瘤酸性微环境中激活药物的DNA纳米结构,其中,我们巧妙地利用了AS1411和i-motif可部分杂交的序列,设计了一种简单而稳健的DNA d-链纳米结构,其中,i-motif序列被设计用来调节AS1411 aptamer靶向肿瘤的结合能力。在正常生理环境中,i-motif 会抑制 AS1411 的靶向能力。在酸性肿瘤微环境中,i-motif 形成四重构象并与 AS1411 解离,从而恢复 AS1411 的靶向能力。只有在酸性条件和肿瘤细胞受体存在的情况下,这种纳米结构才能被肿瘤细胞内化。此外,这种纳米结构的结构变化还能实现载药释放。这种负载药物的A-I-双链DNA结构对癌细胞和球形细胞具有靶向和抑制能力,在临床癌症治疗中具有广阔的应用前景。
{"title":"Tumor acidic microenvironment activatable DNA nanostructure for precise cancer cell targeting and inhibition","authors":"Yanfei Liu ,&nbsp;Yaqin Hu ,&nbsp;Yifu Tan ,&nbsp;Qiwen Chen ,&nbsp;Zhenbao Liu","doi":"10.1016/j.cclet.2024.110289","DOIUrl":"10.1016/j.cclet.2024.110289","url":null,"abstract":"<div><div>Precise tumor targeting and therapy is a major trend in cancer treatment. Herein, we designed a tumor acidic microenvironment activatable drug loaded DNA nanostructure, in which, we made a clever use of the sequences of AS1411 and i-motif, which can partially hybridize, and designed a simple while robust DNA <span>d</span>-strand nanostructure, in which, i-motif sequence was designed to regulate the binding ability of the AS1411 aptamer to target tumor. In the normal physiological environment, i-motif inhibits the targeting ability of AS1411. In the acidic tumor microenvironment, i-motif forms a quadruplex conformation and dissociates from AS1411, restoring the targeting ability of AS1411. Only when acidic condition and tumor cell receptor are present, this nanostructure can be internalized by the tumor cells. Moreover, the structure change of this nanostructure can realize the release of loaded drug. This drug loaded A-I-Duplex DNA structure showed cancer cell and spheroid targeting and inhibition ability, which is promising in the clinical cancer therapy.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 1","pages":"Article 110289"},"PeriodicalIF":9.4,"publicationDate":"2024-07-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141844767","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
Interfacial B-O bonding modulated S-scheme B-doped N-deficient C3N4/O-doped-C3N5 for efficient photocatalytic overall water splitting 用于高效光催化整体水分离的界面 B-O 键调制 S 型 B 掺杂缺 N C3N4/O 掺杂 C3N5
IF 9.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-20 DOI: 10.1016/j.cclet.2024.110288
Entian Cui , Yulian Lu , Zhaoxia Li , Zhilei Chen , Chengyan Ge , Jizhou Jiang
Photocatalytic overall pure water splitting is a promising method for generating green hydrogen energy under mild conditions. However, this process is often hindered by sluggish electron-hole separation and transport. To address this, a step-scheme (S-scheme) B-doped N-deficient C3N4/O-doped C3N5 (BN-C3N4/O-C3N5) heterojunction with interfacial B-O bonds has been constructed. Utilizing Pt and Co(OH)2 as co-catalysts, BN-C3N4/O-C3N5 S-scheme heterojunction demonstrates significantly enhanced photocatalytic activity for overall pure water splitting under visible light, achieving H2 and O2 evolution rates of 40.12 and 19.62 µmol/h, respectively. Systematic characterizations and experiments revealed the performance-enhancing effects of the enhanced built-in electric field and the interfacial B-O bonding. Firstly, the strengthened built-in electric field provides sufficient force for rapid interfacial electron transport. Secondly, by reducing the transport energy barrier and transfer distance, the interfacial B-O bonds facilitate rapid recombination of electrons and holes with relatively low redox potential via the S-scheme charge-transfer route, leaving the high-potential electrons and holes available for H+ reduction and OH oxidation reactions. Overall, the photocatalytic efficiency of BN-C3N4/O-C3N5 S-scheme heterojunction was significantly improved, making it a promising approach for green hydrogen production through overall pure water splitting.
光催化整体纯水分离是一种在温和条件下产生绿色氢能的可行方法。然而,这一过程往往受到电子-空穴分离和传输迟缓的阻碍。为解决这一问题,我们构建了一种具有 B-O 键界面的阶梯式(S-scheme)B-掺杂缺 N C3N4/O 掺杂 C3N5(BN-C3N4/O-C3N5)异质结。利用铂和 Co(OH)2 作为助催化剂,BN-C3N4/O-C3N5 S 型异质结在可见光条件下的整体纯水分离光催化活性显著增强,H2 和 O2 的进化速率分别达到 40.12 和 19.62 µmol/h。系统表征和实验揭示了增强的内置电场和界面 B-O 键的性能增强效应。首先,增强的内置电场为快速的界面电子传输提供了足够的力。其次,通过降低传输能垒和传输距离,界面 B-O 键有利于氧化还原电势相对较低的电子和空穴通过 S 型电荷转移途径快速重组,从而使高电位的电子和空穴可用于 H+ 还原和 OH- 氧化反应。总体而言,BN-C3N4/O-C3N5 S-scheme异质结的光催化效率显著提高,使其成为一种通过整体纯水分离实现绿色制氢的可行方法。
{"title":"Interfacial B-O bonding modulated S-scheme B-doped N-deficient C3N4/O-doped-C3N5 for efficient photocatalytic overall water splitting","authors":"Entian Cui ,&nbsp;Yulian Lu ,&nbsp;Zhaoxia Li ,&nbsp;Zhilei Chen ,&nbsp;Chengyan Ge ,&nbsp;Jizhou Jiang","doi":"10.1016/j.cclet.2024.110288","DOIUrl":"10.1016/j.cclet.2024.110288","url":null,"abstract":"<div><div>Photocatalytic overall pure water splitting is a promising method for generating green hydrogen energy under mild conditions. However, this process is often hindered by sluggish electron-hole separation and transport. To address this, a step-scheme (S-scheme) B-doped N-deficient C<sub>3</sub>N<sub>4</sub>/O-doped C<sub>3</sub>N<sub>5</sub> (BN-C<sub>3</sub>N<sub>4</sub>/O-C<sub>3</sub>N<sub>5</sub>) heterojunction with interfacial B-O bonds has been constructed. Utilizing Pt and Co(OH)<sub>2</sub> as co-catalysts, BN-C<sub>3</sub>N<sub>4</sub>/O-C<sub>3</sub>N<sub>5</sub> S-scheme heterojunction demonstrates significantly enhanced photocatalytic activity for overall pure water splitting under visible light, achieving H<sub>2</sub> and O<sub>2</sub> evolution rates of 40.12 and 19.62 µmol/h, respectively. Systematic characterizations and experiments revealed the performance-enhancing effects of the enhanced built-in electric field and the interfacial B-O bonding. Firstly, the strengthened built-in electric field provides sufficient force for rapid interfacial electron transport. Secondly, by reducing the transport energy barrier and transfer distance, the interfacial B-O bonds facilitate rapid recombination of electrons and holes with relatively low redox potential <em>via</em> the S-scheme charge-transfer route, leaving the high-potential electrons and holes available for H<sup>+</sup> reduction and OH<sup>−</sup> oxidation reactions. Overall, the photocatalytic efficiency of BN-C<sub>3</sub>N<sub>4</sub>/O-C<sub>3</sub>N<sub>5</sub> S-scheme heterojunction was significantly improved, making it a promising approach for green hydrogen production through overall pure water splitting.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 1","pages":"Article 110288"},"PeriodicalIF":9.4,"publicationDate":"2024-07-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141850636","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
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Chinese Chemical Letters
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