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Additive-free synthesis of S-substituted isothioureas via visible-light-induced four-component reaction ofα-diazoesters,aryl isothiocyanates,amines and cyclic ethers

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Chinese chemical Letters 2024年第2期35卷 415-419页

作者： Yufen Lv Hongyu Ding Jinmao You Wei Wei Dong Yi key laboratory of Catalytic Conversion and clean Energy in universities of shandong province School of Chemistry and Chemical EngineeringQufu Normal UniversityQufu 273165China College of Chemistry and chemical engineering Shaoxing UniversityShaoxing 312000China School of Pharmacy Southwest Medical UniversityLuzhou 646000China

An additive-free and environmentally friendly strategy has been realized for the construction of S-substituted isothioureas through visible-light-induced multicomponent reaction starting fromα-diazoesters,aryl isothiocyanates,amines and cyclic ethers.This methodology features simple operation,mild reaction conditions,favorable functional group tolerance,easily available starting materials and high efficiency.

关键词： Visible-light Additive-free Four-component reaction S-Substituted isothioureas

用于能源转化和环境修复的TiO_(2)基梯型异质结光催化剂

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Science China Materials 2024年第2期67卷 424-443页

作者：张宝龙孙彬刘方璇高婷婷周国伟 key laboratory of Fine chemicals in universities of shandong Jinan Engineering Laboratory for Multi-scale Functional MaterialsSchool of Chemistry and Chemical EngineeringQilu University of Technology(Shandong Academy of Sciences)Jinan 250353China

太阳能驱动的半导体光催化技术被认为是缓解能源短缺和环境污染的潜在策略.因此,探索高效的光催化剂是推动光催化技术发展和实际应用的关键.作为一种典型的半导体光催化剂,TiO_(2)因其化学稳定、环境友好、成本低廉等特性而备受关注.然... 详细信息

太阳能驱动的半导体光催化技术被认为是缓解能源短缺和环境污染的潜在策略.因此,探索高效的光催化剂是推动光催化技术发展和实际应用的关键.作为一种典型的半导体光催化剂,TiO_(2)因其化学稳定、环境友好、成本低廉等特性而备受关注.然而,TiO_(2)光生载流子的快速复合、光吸收范围窄以及还原能力不足等缺点严重阻碍了其光催化性能.通过将TiO_(2)与其他半导体复合以构建梯型异质结可以有效的解决上述问题.在此光催化体系中,梯型异质结不仅可以整合各组分的优点,实现光生载流子的有效分离和光捕获能力的增强,而且还能保留最强的氧化还原能力.基于此,本文综述了利用构建梯型异质结来提高TiO_(2)光催化性能的最新研究进展,着重介绍了TiO_(2)基梯型异质结光催化剂的分类,主要包括金属氧化物、金属硫属化物、有机半导体和其他类型半导体.在此基础上,本文还总结了TiO_(2)基梯型异质结光催化剂在析氢、CO_(2)还原、H_(2)O_(2)生成和污染物降解等领域中的应用.同时,为了更好地理解光生载流子的转移途径,本文还简要介绍了梯型异质结的一些表征方法.最后,对TiO_(2)基梯型异质结光催化剂所面临的问题和未来的发展方向进行了展望.综上,本文旨在为构建用于能源转换和环境修复的高效TiO_(2)基梯型异质结光催化剂提供参考.

关键词： TiO_(2) step-scheme heterojunction photocatalysis energy conversion environmental remediation

Fluorinated graphene quantum dots with long-term lubrication for visual drug loading and joint inflammation therapy

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摩擦:英文版 2023年第12期11卷 2204-2220页

作者： Peiwei GONG Changmin QI Dandan WANG Mianran CHAO Jianxi LIU Meirong CAI Weimin LIU key laboratory of Catalytic Conversion and clean Energy in universities of shandong province School of Chemistry and Chemical EngineeringQufu Normal UniversityJining 273165China State key laboratory of Solidification Processing Center of Advanced Lubrication and Seal MaterialsNorthwestern Polytechnical UniversityXi’an 710072China State key laboratory of Solid Lubrication Lanzhou Institute of Chemical PhysicsChinese Academy of SciencesLanzhou 730000China

Osteoarthritis(OA)treatment mainly relies on developing new drugs or nanocarriers,while little attention is paid to building novel remedial mode and improving drug loading efficiency.This work reports an integrated nanosystem that not only realizes visual drug loading and release,but also achieves enhanced lubrication and effective joint inflammation therapy based on fluorinated graphene quantum dots(FGQDs).Oxygen introduction promotes FGQDs outstanding water-stability for months,and layered nano-sized structure further guarantees excellent lubricating properties in biomimetic synovial fluid.The special design of chemistry and structure endows FGQDs robust fluorescence in a wide range of pH conditions.Also,the excitation spectrum of FGQDs well overlaps the absorption spectrum of drugs,which further constructs a new concept of internal filtering system to visually monitor drug loading by naked eyes.More importantly,extraordinary long-term lubrication performance is reported,which is the first experimental demonstration of concentration-dependent mutations of coefficient of friction(COF).Cell incubation experiments indicate that drug-loaded FGQDs have good biocompatibility,tracking property of cellular uptake and drug release,which show efficient anti-inflammation potential for H2O2-induced chondrocyte degradation by up-regulated cartilage anabolic genes.This study establishes a promising OA treatment strategy that enables to monitor drug loading and release,to enhance long-time lubricating property,and to show effective anti-inflammatory potential for cartilage protection.

关键词： fluorinated graphene(FG) structure design lubrication fluorescence drug delivery

Visualization of the process:selenocysteine activates GPX4 in ferroptosis based on a nano-fluorescent probe

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Science China Chemistry 2022年第7期65卷 1286-1290页

作者： Dongrui Luan Wenfei Guo Xiaonan Gao Kehua Xu Bo Tang College of Chemistry Chemical Engineering and Materials ScienceCollaborative Innovation Center of Functionalized Probes for Chemical Imaging in Universities of ShandongKey Laboratory of Molecular and Nano ProbesMinistry of EducationShandong Provincial Key Laboratory of Clean Production of Fine ChemicalsShandong Normal UniversityJinan 250014China Department of Clinical laboratory The Second HospitalCheeloo College of MedicineShandong UniversityJinan 250033China

Developing accurate methods for visualizing the expressions of proteins during the life process is a hotspot in the biochemical research field.Glutathione peroxidase 4(GPX4),one type of selenoproteins,was previously identified as a significant ferroptosis-regulated protein.Therefore,a novel approach was established to visualize the activation process of selenocysteine(Sec)toward GPX4 via an Au–Se bonded fluorescent nanoprobe and assisted by western blot analysis.The Au–Se nanoprobe was constructed by selenol-modified peptides for monitoring the concentration changes of Sec.The fluorescence intensity of Sec in confocal fluorescence imaging positively correlates with GPX4's activation level,proved by western blot analysis in living cells.This study provides an intuitional and visual strategy for predicting the functional expression of GPX4 during the ferroptosis process and offers new directions for the future investigation of proteins'functional expressions.

关键词： ferroptosis nano-fluorescent probe selenocysteine activates GPX4 visualization

In-situ assembly of 2D/3D porous nickel cobalt sulfide solid solution as superior pre-catalysts to boost multi-functional electrocatalytic oxidation

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Chinese chemical Letters 2023年第5期34卷 365-368页

作者： Pin Hao Xu Dong Houguang Wen Ruirui Xu Junfeng Xie Qian Wang Guanwei Cui Jian Tian Bo Tang College of Chemistry Chemical Engineering and Materials ScienceCollaborative Innovation Center of Functionalized Probes for Chemical Imaging in Universities of ShandongKey Laboratory of Molecular and Nano ProbesMinistry of EducationShandong Provincial Key Laboratory of Clean Production of Fine ChemicalsShandong Normal UniversityJi'nan 250014China School of Materials Science and engineering Shandong University of Science and TechnologyQingdao 266590China

In this work,we fabricated an efficient pre-catalyst based on(Ni,Co)S2solid solution with hierarchical architecture and high porosity to boost urea oxidation reaction and electrocatalytic oxidation of organic small molecules.The interaction between Ni and Co can optimize the electronic structure,resulting in the improved conductivity and accelerated charge transfer rate.The 2D/3D architecture can enrich more active species and endow the mass and electron transport to facilitate the surface oxidation and the following catalytic process.Post-structure and catalytic characterizations confirm the surface oxidation of(Ni,Co)S_(2)during the stability test,and the in-situ formed Co(Ni)based(oxy)hydroxides exhibit superior catalytic activity and facilitated charge transfer ability.As a result,the optimal(Ni,Co)S_(2)solid solution pre-catalyst displays facilitated catalytic behavior and good stability for multifunctional electrocatalytic oxidation,in which a high conversion of benzyl alcohol(97.50%),a good selectivity to benzoic acid(93.78%)and a satisfied faraday efficiency(91.86%)can be achieved.

关键词： Electrocatalytic oxidation (Ni Co)S_(2)solid solution Pre-catalyst Urea oxidation reaction 2D/3D architecture

Synthesis,Crystal Structures and Intermolecular Magnetic Coupling Mechanism of the Mononuclear Radical Complex[1-N-methyl-1,10-phenanthrolium][Ni(dmit)_2]

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Chinese Journal of Structural Chemistry 2017年第11期36卷 1878-1888页

作者：郑鲁沂张程程王赤峰迟颜辉陈雪雪石敬民钤小平徐俊 College of Chemistry Chemical Engineering and Materials ScienceCollaborative Innovation Center of Functionalized Probes for Chemical Imaging in Universities of ShandongKey Laboratory of Molecular and Nano ProbesMinistry of EducationShandong Provincial Key Laboratory of Clean Production of Fine ChemicalsShandong Normal University

The mononuclear radical anionic complex [1-N-methyl-1,10-phenanthrolium][Ni（dmit）2]（dmit = 1,3-dithiole-2-thione-4,5-dithiolate） with a new countercation has been prepared and its crystal structure was determined by X-ray crystallography at 298 and 80 K. In the mononuclear radical anionic complex, the nickel ion assumes a slightly distorted square-planar geometry. There are two and three kinds of intermolecular interactions between adjacent mononuclear radical anionic complexes in the crystal at 298 and 80 K, respectively（i.e., Models A and B at 298 K; and Models C, D and E at 80 K）. The variable-temperature magnetic moments indicate a strong antiferromagnetic interaction between the adjacent mononuclear radical anionic complexes, and the theoretical calculations reveal that the stronger antiferromagnetic coupling strength at lower temperature should be contributed to the larger overlap integrals between the short contact atoms. This study is the first to reveal the mechanism of stronger magnetic coupling strength at lower temperature for a mononuclear radical anionic nickel complex with dmit as the ligand.

关键词： crystal structure, magnetism, nickel complex, radical

Boosting the photodynamic therapy efficiency with a mitochondria-targeted nanophotosensitizer

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Chinese chemical Letters 2019年第6期30卷 1293-1296页

作者： Limin Yang Peng Gao Yuanlei Huang Xiao Lu Qian Chang Wei Pan Na Li Bo Tang College of Chemistry Chemical Engineering and Materials Science Key Laboratory of Molecular and Nano Probes Ministry of Education Collaborative Innovation Center of Functionalized Probes for Chemical Imaging in Universities of Shandong Institute of Molecular and Nano Science Shandong Provincial Key Laboratory of Clean Production of Fine Chemicals Shandong Normal University

Photodynamic therapy (PDT) is an attractive clinical technique for cancer treatment. However, the poor solubility and weak cellular internalization of the molecule-photosensitizers, as well as the exceedingly short lifetime and limited diffusion distance of the generated reactive oxygen species (ROS) in cytoplasm directly restricted the therapeutic efficiency of conventional PDT. In this study, we proposed a facile strategy for improving PDT of cancer based on a mitochondria-targeted nanophotosensitizer. The molecule-photosensitizer chlorin e6 was covalently attached on the internal and external surfaces of the mesoporous silica nanoparticles. Then, the triphenylphosphonium was anchored on the nanoparticles for selectively targeting mitochondria. When irradiated with laser, the nanophotosensitizer can generate a large amount of ROS in mitochondria, thus causing the mitochondrial dysfunction and irreversible cell apoptosis. In vitro and in vivo studies demonstrated that the nanophotosensitizer could boost the treatment efficiency against cancer cells and xenograft tumor models.

关键词： Mitochondria Nanophotosensitizer Photodynamic therapy Reactive oxygen species Enhanced treatment efficiency

Reduced Thiol Compounds-Induced Biosensing,Bioimaging Analysis and Targeted Delivery

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Chinese Journal of Chemistry 2020年第12期38卷 1793-1806页

作者： Yingshu Guo Xiaofei Zheng Xiuping Cao Wenxin Li Di Wu Shusheng Zhang Collaborative Innovation Center of Tumor Marker Detection Technology Equipment and Diagnosis-Therapy Integration in Universities of ShandongShandong Province Key Laboratory of Detection Technology for Tumor MarkersSchool of Chemistry and Chemical EngineeringLinyi UniversityLinyiShandong 276005China

Reduced thiol compounds(RTCs),such as glutathione(GSH),cysteine(Cys),and homocysteine(Hcy),are important components of many amino acids andproteins.They are also basic buiding blocks that make up organisms and play an important role in physiology and pathology.Therefore,based on thefundamental characteristics of RTCs in vivo,researchers have reported their use in biosensing and imaging analysis and as carriers inlfe sciences andhealth sciences.n this review,we will itroduce the principles of RTLs and highlight their applications in biosensing and imaging analysis and as carriersreported from 2015 to 2020.

关键词： thiol principles fundamental

The regulation of coordination structure between cobalt and nitrogen on graphene for efficient bifunctional electrocatalysis in Zn-air batteries

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Journal of Energy Chemistry 2022年第5期31卷 213-221页

作者： Xinxin Shu Maomao Yang Miaomiao Liu Wei Pan Jintao Zhang key laboratory for Colloid and Interface Chemistry of State Education Ministry School of Chemistry and Chemical EngineeringShandong UniversityJinan 250100ShandongChina College of Chemistry Chemical Engineering and Materials ScienceShandong Normal UniversityJinan 250014ShandongChina State key laboratory of Crystal Materials Shandong UniversityJinan 250100ShandongChina

Electrocatalysts with atomically dispersed metal moieties are of importance in enhancing electrocatalysis for a specific reaction including oxygen reduction. However, it is still challenging to modulate the coordination structure of metal atoms with heteroatoms on carbon supports. Herein, an innovative and facile bridging strategy to regulate the coordination structure of cobalt with nitrogen atoms on reduced graphene oxide(r GO) sheets was developed by the interfacial complexation of amino-rich folic acid with cobalt ions on graphene oxide sheets and the subsequent thermal treatment. Typically, the actual coordination interaction between cobalt and nitrogen species was revealed by using X-ray absorption spectroscopy(XAS), exhibiting the Co-N_(4) coordination structure well-dispersed on reduced graphene oxide.Such unique structure enables the efficient oxygen reduction and evolution reactions via the favorable adsorption and desorption of intermediates. With the enhanced bifunctional electrocatalytic activities,the fabricated Zn-air battery exhibited the excellent performance with large power density of 319.8 mW cm^(-2) and good long-term stability(over 300 h). This work establishes the synthesis strategy for bridging metal atom with heteroatom on graphene sheets to enhance the bifunctional electrocatalysis toward Zn-air batteries.

关键词： Oxygen reduction reaction Synergistic effect Bifunctional electrocatalysis Bridging structure