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N-doped carbon quantum dots as fluorescent probes for highly selective and sensitive detection of Fe^3+ ions

Particuology 2018年第6期16卷 94-100页

作者： Xiangyi Deng Yali Feng Haoran Li Zhuwei Du Qing Teng Hongjun Wang School of Civil and Resource Engineering University of Science and Technology Beijing Beijing 100083China State Key Laboratory of Biochemical Engineering Institute of Process Engineering Chinese Academy of SciencesBeijing 100190China

To investigate the effect of nitrogen on the photoluminescence properties of carbon quantum dots (CO Ds), N-doped carbon quantum dots (N-CQDs)were synthesized by one-step hydrothermal treatment using biomass tar as the carbon *** an inevitable organic pollutant,the unsaturated bonds in biomass tar,such as carboxylic acids,aldehydes,and aromatics,are favorable for formation of the graphitic carbon *** obtained N-CQDs are spherical with an average particle size of 2.64nm and the crystal lattice spacing is 0.25nm,corresponding to the (100)facet of graphitic *** N-CQDs emit bright blue photoluminescence under 365nm ultraviolet light,and they have excellent water solubility and stability with a high quantum yield of 26.1%.Coordination between the functional groups on the N-CQD surface and Fe^3+ ions is promoted because of the improved electronic properties and surface chemical reactivity caused by N atoms,leading to a significant fluorescence quenching effect of the N-CQDs in the presence of Fe^3+ions with high selectivity and *** is a linear relationship between In (Fo/F)and the Fe^3+ concentration in the N-CQD concentration range 0.06-1400μmol/L with a detection limit of 60nmol/L, showing that the *** have great potential as a fluorescent probe for Fe^3+detection.

关键词： N-doped carbon quantum dots Fe^3+ion detection Fluorescence quenching Biomasstar

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Construction of Thioamide Peptides from Chiral Amino Acids

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Angewandte Chemie 2023年第26期135卷

作者： Yanyan Liao Shunmin Zhang Prof. Dr. Xuefeng Jiang Shanghai Key Laboratory of Green Chemistry and Chemical Process Institute of Eco-Chongming School of Chemistry and Molecular Engineering East China Normal University 3663 North Zhongshan Road Shanghai 200062 P. R. China State Key Laboratory of Elemento-Organic Chemistry Nankai University Tianjin 300071 P. R. China State Key Laboratory of Organometallic Chemistry Shanghai Institute of Organic Chemistry Chinese Academy of Sciences Shanghai 200032 P. R. China

Thioamide peptides were synthesized in a straightforward one-pot process via the linkage of diverse natural amino acids in the presence of thiolphosphonate and trichlorosilane, wherein carbonyl groups were replaced with thiono compounds with minimal racemization. Experimental and computational mechanistic studies demonstrated that the trichlorosilane enables the activation of carboxylic acids via intense interactions with the Si−O bond, followed by coupling of the carboxylic acids with thiolphosphonate to obtain the key intermediate S -acyl dithiophosphate. Silyl-activated quadrangular metathesis transition states afforded the thioamide peptides. The potential applications of these thioamide peptides were further highlighted via late-stage linkages of diverse natural products and pharmaceutical drugs and the thioamide moiety.

关键词： Peptides Racemization Reaction Mechanisms Thioamides

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Dual Stimuli-Responsive Rotaxanes with Tunable Vibration-Induced Emission and Switchable Circularly Polarized Luminescence

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Angewandte Chemie 2024年第12期136卷

作者： Wei-Tao Xu Xue Li Peicong Wu Dr. Wei-Jian Li Dr. Yu Wang Xiao-Qin Xu Dr. Xu-Qing Wang Prof. Dr. Jinquan Chen Prof. Dr. Hai-Bo Yang Prof. Dr. Wei Wang Shanghai Key Laboratory of Green Chemistry and Chemical Processes School of Chemistry and Molecular Engineering East China Normal University 3663 N. Zhongshan Road Shanghai 200062 China State Key Laboratory of Precision Spectroscopy School of Physics and Electronic Science East China Normal University Dongchuan Road 500 Shanghai 200241 China State Key Laboratory of Petroleum Molecular and Process Engineering (SKLPMPE) Sinopec Research Institute of Petroleum Processing Co. LTD. Beijing 100083 China East China Normal University Shanghai 200062 China Shanghai Center of Brain-inspired Intelligent Materials and Devices East China Normal University Shanghai 200241 China

Aiming at the construction of novel stimuli-responsive fluorescent system with precisely tunable emissions, the typical 9,14-diphenyl-9,14-dihydrodibenzo[a, c]phenazine (DPAC) luminogen with attractive vibration-induced emission (VIE) behavior has been introduced into [2]rotaxane as a stopper. Taking advantage of their unique dual stimuli-responsiveness towards solvent and anion, the resultant [2]rotaxanes reveal both tunable VIE and switchable circularly polarized luminescence (CPL). Attributed to the formation of mechanical bonds, DPAC-functionalized [2]rotaxanes display interesting VIE behaviors including white-light emission upon the addition of viscous solvent, as evaluated in detail by femtosecond transient absorption (TA) spectra. In addition, ascribed to the regulation of chirality information transmission through anion-induced motions of chiral wheel, the resolved chiral [2]rotaxanes reveal unique switchable CPL upon the addition of anion, leading to significant increase in the dissymmetry factors ( g lum ) values with excellent reversibility. Interestingly, upon doping the chiral [2]rotaxanes in stretchable polymer, the blend films reveal remarkable emission change from white light to light blue with significant 6.5-fold increase in g lum values up to −0.035 under external tensile stresses. This work provides not only a new design strategy for developing molecular systems with fluorescent tunability but also a novel platform for the construction of smart chiral luminescent materials for practical use.

关键词： mechanically interlocked molecules chiral rotaxanes vibration-induced emission circularly polarized luminescence pillar[5]arene

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12-Tungstophosphoric acid niched in Zr-based metal-organic framework:a stable and efficient catalyst for Friedel-Crafts acylation

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Science China Chemistry 2018年第4期61卷 402-411页

作者： Latif Ullah Guoying Zhao Zichen Xu Hongyan He Muhammad Usman Suojiang Zhang Beijing Key Laboratory of Ionic Liquids Clean Process Key Laboratory of Green Process EngineeringState Key Laboratory of Multiphase Complex SystemsInstitute of Process EngineeringChinese Academy of SciencesBeijing 100190China University of Chinese Academy of Sciences Beijing 100049China Center of Excellence in Nanotechnology King Fahd University of Petroleum and MineralsDhahran 3126Saudi Arabia

Heteropoly acids(HPA) are well known for their versatile solid acid catalysis in diverse chemical reactions, however they suffer from low surface area(<10 m^2/g) and leaching into the reactions media, which reduce their prospects as industrial ***, a novel hybrid material HPW@Zr-BTC,composed of 12-tungstophoric acid(HPW) and Zr^(Ⅳ)-benzene tri-carboxylate(Zr-BTC) metal-organic framework(MOF), was prepared via one-pot solvothermal method. Excellent HPW loading up to 32.3 wt% was achieved, and HPW@Zr-BTC composite proved to be highly stable, besides the crystalline morphology of Zr-BTC was intact. The catalytic activity of the hybrid composite was explored via Friedel-Crafts acylation of anisole with benzoyl *** 28.2 wt% HPW@Zr-BTC showed excellent catalytic performance, with 99.4% anisole conversion and 97.6% yield(pmethoxybenzophenone) under solvent free conditions. Excellent retention of catalytic activity was achieved after at least five consecutive runs due to non-observable HPW leaching. The promising activity and stability of the catalyst forecasted its potential industrial applications.

关键词： dodeca-tungstophosphoric acid Zr-BTC metal-organic frameworks one-pot solvothermal synthesis heterogeneouscatalysis anisole acylation high temperature XRD

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Coupling Electrochemical Sulfion Oxidation with CO2Reduction over Highly Dispersed p-Bi Nanosheets and CO2-Assisted Sulfur Extraction

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Angewandte Chemie 2023年第7期136卷

作者： Xue Teng Kai Shi Prof. Lisong Chen Prof. Jianlin Shi Shanghai Key Laboratory of Green Chemistry and Chemical Processes School of Chemistry and Molecular Engineering East China Normal University 200062 Shanghai China State Key Laboratory of Petroleum Molecular and Process engineering SKLPMPE East China Normal University 200062 Shanghai China Institute of Eco-Chongming 202162 Shanghai China Shanghai Institute of Ceramics Chinese Academy of Sciences 200050 Shanghai P. R. China

We report herein an electrocatalytic CO 2 reduction-coupled sulfion oxidation system for the co-productions of valuable formate and sulfur at much enhanced atom utilization. Specifically, an organic ligand-assisted two-step reconstruction approach has been developed to fabricate the highly dispersed p-Bi nanosheets (p-Bi NSs) for cathodic CO 2 reduction reaction (CO 2 RR), and meanwhile porous Co−S nanosheets (Co−S NSs) was applied for anodic sulfion oxidation reaction (SOR). Significantly high Faradaic Efficiencies of about 90 % for formate production by CO 2 RR in a wide potential range from −0.6 V to −1.1 V, and excellent SOR performances including an ultra-low onset potential of about 0.2 V and recycle capacity of S 2− in the 0.1 M and 0.5 M S 2− solutions, have been simultaneously achieved. In the meantime, both the structure transformation of the catalysts and the reaction pathways are explored and discussed in detail. A two-electrode CO 2 RR||SOR electrolyzer equipped with above electrocatalysts has been established, which features as low as about 1.5 V to run the electrolyzer at 100 mA cm −2 , manifesting extremely lowered electricity consumption in comparison to conventional CO 2 RR system. Moreover, a sulfur separation approach has been proposed by using CO 2 , which is efficient, environmentally friendly and cost effective with value-added NaHCO 3 be obtained as the byproduct.

关键词： CO2 Assisted Sulfur Extraction Electrocatalytic CO2RR Sulfion Oxidation Reaction p-Bi Nanosheets

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The application of sulfur-containing peptides in drug discovery

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Chinese Chemical Letters 2018年第7期29卷 1079-1087页

作者： Jiaoyan Zhao Xuefeng Jiang Shanghai Key Laboratory of Green Chemistry and Chemical Process School of Chemistry and Molecular EngineeringEast China Normal University State Key Laboratory of Elemento-organic Chemistry Nankai University

In recent decades, peptides as potential drugs were more and more explored with the development of non-oral medicine. There into, sulfur-containing peptide is one of the most popular aspects in peptide drugs due to the introduction of sulfur atoms leading unique *** purpose of the present review is to focus on the discovery of various sulfur-containing peptides with particular emphasis on their pharmacological mechanisms. This review is organized according to the structures of the sulfurcontaining peptides.

关键词： Peptides Disulfide Thioether Thiazole Drug discovery

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Corrigendum to "Novel Platinum(IV) complexes intervene oxaliplatin resistance in colon cancer via inducing ferroptosis and apoptosis" [Eur. J. Med. Chem. 263 (2024) 115968]

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European journal of medicinal chemistry 2024年 280卷 116976页

作者： Zhikun Liu Jinyuan Cai Guiyang Jiang Meng Wang Chuang Wu Kangning Su Weiwei Hu Yaxian Huang Chunhao Yu Xiaochao Huang Guoxiu Cao Hengshan Wang Green Chemistry and Process Enhancement Technology National & Local Joint Engineering Research Center for Mineral Salt Deep Utilization Huaiyin Institute of Technology Huai'an 223003 China. Green Chemistry and Process Enhancement Technology National & Local Joint Engineering Research Center for Mineral Salt Deep Utilization Huaiyin Institute of Technology Huai'an 223003 China State Key Laboratory for the Chemistry and Molecular Engineering of Medicinal Resources Collaborative Innovation Center for Guangxi Ethnic Medicine School of Chemistry and Pharmaceutical Sciences of Guangxi Normal University Guilin 541004 China. State Key Laboratory for the Chemistry and Molecular Engineering of Medicinal Resources Collaborative Innovation Center for Guangxi Ethnic Medicine School of Chemistry and Pharmaceutical Sciences of Guangxi Normal University Guilin 541004 China. Electronic address: viphuangxc@***. Green Chemistry and Process Enhancement Technology National & Local Joint Engineering Research Center for Mineral Salt Deep Utilization Huaiyin Institute of Technology Huai'an 223003 China. Electronic address: CaoGuoxiu@***. State Key Laboratory for the Chemistry and Molecular Engineering of Medicinal Resources Collaborative Innovation Center for Guangxi Ethnic Medicine School of Chemistry and Pharmaceutical Sciences of Guangxi Normal University Guilin 541004 China. Electronic address: whengshan@***.

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Connected three-dimensional polyhedral frames for programmable liquid processing

Nature Chemical Engineering

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Nature Chemical engineering 2024年 472-482页

作者： Yiyuan Zhang Liqiu Wang Zhandong Huang Kai Cui Kun Guo Jinjia Wei Feifei Qin Jan Carmeliet Hongzhou Wang Zheren Cai Yanlin Song Xiaobing Cai Junfeng Xiao Jun Yang Department of Mechanical Engineering The Hong Kong Polytechnic University Hong Kong China School of Chemical Engineering and Technology Xi’an Jiaotong University Xi’an China Institute of Extreme Mechanics Northwestern Polytechnical University Xi’an China Chair of Building Physics Department of Mechanical and Process Engineering ETH Zürich (Swiss Federal Institute of Technology in Zürich) Zurich Switzerland Jiangxi Institute of Mechanical Science Nanchang China Key Laboratory of Green Printing Institute of Chemistry Chinese Academy of Sciences (ICCAS) Beijing Engineering Research Center of Nanomaterials for Green Printing Technology Beijing National Laboratory for Molecular Sciences (BNLMS) Beijing China State Key Laboratory for Strength and Vibration of Mechanical Structures School of Aerospace Engineering Xi’an Jiaotong University Xi’an China Shenzhen Institute for Advanced Study University of Electronic Science and Technology of China Shenzhen China

Human civilization relies heavily on the ability to precisely process liquids. Switching between liquid capture and release plays a fundamental role in the handling of various liquids, with applications that demand reversible, spatially and temporally precise, volumetrically accurate and programmable control over the liquid, independent of the details of the employed solid tools and processed liquids. However, current fluidic techniques do not fully meet these requirements. Here we present connected polyhedral frames to effectively address this challenge by tailoring liquid continuity between frames to dictate the liquid capture or release of individual frames, with an overall network that is readily switchable locally, dynamically and reversibly. Each frame captures or releases liquids, independent of its base materials, structures and processed liquids. The connected polyhedral frames are a versatile tool that enables many important functions including three-dimensional (3D) programmable patterning of liquids, 3D spatiotemporal control of concentrations of multiple materials, packaging of 3D liquid arrays and large-scale manipulation of multiple liquids, thus considerably advancing many fields, including interface science and soft materials.

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CO2Induces Symmetry Breaking in Layered Dipeptide Crystals

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Angewandte Chemie 2022年第1期135卷

作者： Dr. Xianbao Li Dr. Qi Li Dr. Aoli Wu Prof. Dr. Junbai Li Beijing National Laboratory for Molecular Sciences (BNLMS) CAS Key Lab of Colloid Interface and Chemical Thermodynamics Institute of Chemistry Chinese Academy of Sciences 100190 Beijing China University of Chinese Academy of Sciences 100049 Beijing China State Key Laboratory of Biochemical Engineering Institute of Process Engineering Chinese Academy of Sciences 100190 Beijing China

Control of symmetry breaking of materials provides large opportunities to regulate their properties and functions. Herein, we report breaking the symmetry of layered dipeptide crystals by utilizing CO 2 to induce the adjacent monomolecular layers to stack from the opposite to the same direction. The role of CO 2 is to cover the interlayer interaction sites and force the dipeptides to adsorb at asymmetric positions. Further, the dipeptide crystals exhibit far superior piezoelectricity after symmetry breaking and the piezoelectric voltage generated from the dipeptide-based generators becomes more than 500 % higher than before. This work reveals a potential route to engineer structures and properties of layered materials and provides a deep insight into the control of non-covalent interactions.

关键词： Dipeptides Layer Stacking Piezoelectricity Supramolecular Assembly Symmetry Breaking

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Schiff Base Mediated Dipeptide Assembly toward Nanoarchitectonics

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Angewandte Chemie 2022年第43期134卷

作者： Dr. Yi Jia Prof. Xuehai Yan Prof. Junbai Li Beijing National Laboratory for Molecular Sciences CAS Key Lab of Colloid Interface and Chemical Thermodynamics Institute of Chemistry Chinese Academy of Sciences Beijing 100190 China State Key Laboratory of Biochemical Engineering Institute of Process Engineering Chinese Academy of Sciences Beijing 100190 China Center for Mesoscience Institute of Process Engineering Chinese Academy of Sciences Beijing 100049 China University of Chinese Academy of Sciences Beijing 100049 China

Dynamic covalent chemistry (DCC) is fascinating because of its dual nature. It perfectly combines the reversible nature of noncovalent bonds with the robustness of covalent bonds, effectively enhancing the stability of assemblies and meanwhile giving rise to unprecedented properties. Therefore, integration of DCC with supramolecular chemistry has emerged as a versatile and an extraordinarily useful approach in directing peptide assembly. This Minireview focuses on a recent strategy, which exploits dynamic Schiff base chemistry in combination with supramolecular chemistry, to mediate dipeptide assembly toward nanoarchitectonics. Diversified structures, new emergent properties, and their related applications are highlighted. Lastly, the opportunities and prospects in this exciting field are also introduced.

关键词： Anticancer Therapy Diphenylalanine Dynamic Covalent Chemistry Optical Waveguiding Schiff Bases

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