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Ultralong nitrogen/sulfur Co-doped carbon nano-hollowsphere chains with encapsulated cobalt nanoparticles for highly efficient oxygen electrocatalysis

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Carbon Energy 2023年第8期5卷 15-30页

作者： Wei Zhang Xingmei Guo Cong Li Jiang-Yan Xue Wan-Ying Xu Zheng Niu Hongwei Gu carl redshaw Jian-Ping Lang College of Chemistry Chemical Engineering and Materials ScienceSoochow UniversitySuzhouChina State Key Laboratory of Organometallic Chemistry Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghaiChina College of Environmental and Chemical Engineering Jiangsu University of Science and TechnologyZhenjiangChina Department of Chemistry University of HullHullUK

The development of simple and effective strategies to prepare electrocatalysts,which possess unique and stable structures comprised of metal/nonmetallic atoms for oxygen reduction reaction(ORR)and oxygen evolution reaction(OER),is currently an urgent ***,an efficient bifunctional electrocatalyst featured by ultralong N,S-doped carbon nano-hollow-sphere chains about 1300 nm with encapsulated Co nanoparticles(Co-CNHSCs)is *** multifunctional catalytic properties of Co together with the heteroatom-induced charge redistribution(i.e.,modulating the electronic structure of the active site)result in superior catalytic activities toward OER and ORR in alkaline *** optimized catalyst Co-CNHSC-3 displays an outstanding electrocatalytic ability for ORR and OER,a high specific capacity of 1023.6 mAh gZn^(-1),and excellent reversibility after 80 h at 10mA cm^(-2)in a Zn-air battery *** work presents a new strategy for the design and synthesis of efficient multifunctional carbon-based catalysts for energy storage and conversion devices.

关键词： Co nanoparticles N S co-doping oxygen electrocatalysts rechargeable Zn-air batteries ultralong carbon nano-hollow-sphere chains

Supramolecular assemblies of cucurbit[n]urils and 4-aminopyridine controlled by cucurbit[n]uril size(n=5,6,7 and 8)

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Chinese Chemical Letters 2023年第7期34卷 131-136页

作者： Yun Lu Zhichao Yu Xinan Yang Jingjing Dai Peihui Shan Xianhao Feng Zhu Tao carl redshaw Xin Xiao Key Laboratory of Macrocyclic and Supramolecular Chemistry of Guizhou Province Guizhou UniversityGuiyang 550025China Department of Chemistry University of HullHull HU67RxUnited Kingdom

The binding interactions between 4-aminopyridine(4-AP) and a series of cucurbit[n]urils(Q[5], Q[6],TMe Q[6], Q[7], Q[8]) have been studied using1H NMR spectroscopy, UV–vis absorption spectroscopy,isothermal titration calorimetry(ITC) and X-ray crystallography. The data indicates that the Q[5]@4-AP complex exhibits exo binding, which is not observed in the other four host-guest complexes. Furthermore,X-ray crystallography clearly reveals how the Q[n]s bind with 4-AP to form complexes, for example Q[5]forms an outer-surface complex, whilst Q[6], TMe Q[6] and Q[7] formed 1:1 host and guest type complexes, and Q[8] formed a stable 1:2 ternary complex due to its large cavity, which can accommodate two 4-AP molecules.

关键词： Cucurbit[n]urils 4-Aminopyridine Host-guest chemistry Supramolecular assembly Exo binding

A novel pillar[5]arene-cucurbit[10]uril based host-guest complex: Synthesis, characterization and detection of paraquat

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Chinese Chemical Letters 2023年第3期34卷 134-137页

作者： Yang Luo Wei Zhang Jie Zhao Mao-Xia Yang Qian Ren carl redshaw Zhu Tao Xin Xiao Key Laboratory of Macrocyclic and Supramolecular Chemistry of Guizhou Province Institute of Applied ChemistryGuizhou UniversityGuiyang 550025China Department of Chemistry University of HullHull HU67RXUnited Kingdom

The macrocyclic family comprising pillar[n]arenes and cucurbit[n]urils have received much attention recently. However, studies on the construction of supramolecular complexes formed directly with derivatized pillar[n]arenes and cucurbit[n]urils are scant. Given the interest in such systems, herein we have synthesized a new type of naphthalene-derivatized pillar[n]arene NTP5 and selected Q[10] as the host molecule. The 4-[2-(1-naphthalenyl)ethenyl]pyridine of NTP5 is encapsulated by Q[10] and formed a hostguest complex in water-acetic acid(1:1) solution accompanied by enhanced fluorescence, which changed the morphology of NTP5 from a sphere to a porous form. In addition, the fluorescence of Q[10]-NTP5 can be quenched by the addition of the highly toxic pesticide paraquat(PQ), and the mechanism was shown to be the formation of a new charge transfer ternary system of Q[10]-NTP5-PQ. This work provides new ideas for the contribution of supramolecular assemblies based on derivatized pillar[n]arenes and their combination with cucurbit[n]urils and reveals their potential applications.

关键词： Pillar[n]arene Cucurbit[n]uril Paraquat Supramolecular assembly Detection

Supramolecular Self-assembly Formed from Cucurbit[8]uril and p-Hydroxybenzoic Acid

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Chemical Research in Chinese Universities 2023年第6期39卷 1058-1063页

作者： WANG Chenghui YU Zhichao BAI Qinghong PAN Dingwu PRIOR Timothy J TAO Zhu redshaw carl XIAO Xin Key Laboratory of Macrocyclic and Supramolecular Chemistry of Guizhou Province Guizhou UniversityGuiyang 550025P.R.China Chemistry School of Natural SciencesUniversity of HullHull HU67RXUK

The binding behavior of cucurbit[8]uril(Q[8])and p-hydroxybenzoic acid(p-HBA)has been investigated using ^(1)H NMR titration experiments,UV-Vis absorption,isothermal titration calorimetry(ITC),and X-ray *** revealed that the Q[8]can accommodate two p-HBA molecules to form a 1:2 host-guest inclusion complex in solution,namely(p-HBA)2@Q[8].From a poorly scattering crystal,we were able to identify two symmetry unique Q[8]rings,but with different p-HBA *** structure can be represented as Q[8]+1.5 p-HBA,which gives Q[8]@(p-HBA)2∙Q[8]@p-HBA as the structural *** supramolecular structure was screened for its ability to capture *** experimental results showed that the adsorption efficiency of the supramolecular organic framework material for iodine capture was 43.8%,with an equilibrium adsorption capacity of 223.3 mg/g.

关键词： Supramolecular self-assembly Cucurbituril p-Hydroxybenzoic acid

一种同时分辨识别Zn^(2+)和F^-离子的双功能探针（英文）

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无机化学学报 2017年第5期33卷 769-778页

作者：曾莉赵江林牟兰曾晞卫钢 redshaw carl 金宗文贵州大学贵州省大环与超分子化学重点实验室贵阳550025 中国科学院深圳先进技术研究院生物医学与健康工程研究所微纳系统与仿生医学研究中心深圳518055 澳大利亚联邦科学与工业研究组织英国赫尔大学化学系

由8-甲酰基-7-羟基香豆素与碳酰肼经一步缩合反应可制得探针1。研究发现,探针1对Zn^(2+)和F-离子均呈现荧光增强和比率比色的高灵敏和高选择性响应,检出限低至10-8 mol·L^(-1)。通过光谱、ITC、1H NMR滴定及质谱分析,详细地研究了探针... 详细信息

由8-甲酰基-7-羟基香豆素与碳酰肼经一步缩合反应可制得探针1。研究发现,探针1对Zn^(2+)和F-离子均呈现荧光增强和比率比色的高灵敏和高选择性响应,检出限低至10-8 mol·L^(-1)。通过光谱、ITC、1H NMR滴定及质谱分析,详细地研究了探针与离子形成的配合物性质。在不同的介质中,探针不仅同时表现出对金属阳离子Zn^(2+)和对阴离子F-的识别,而且吸收和发射波长均有显著的差异:1-Zn^(2+)配合物的最大吸收波长为360 nm,而1-F-配合物为400 nm;1-Zn^(2+)配合物的荧光激发和发射波长分别为360和454 nm,而1-F-配合物分别为400和475 nm。此外,探针1还能应用于活体PC3细胞中Zn^(2+)的荧光成像。

关键词： 8-甲酰基-7-羟基香豆素 Zn2+ F- 分辨波长细胞成像

New Quinoxaline-Based Blue Emitters: Molecular Structures, Aggregation-Induced Enhanced Emission Characteristics and OLED Application

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Chinese Journal of Chemistry 2021年第8期39卷 2154-2162页

作者： Xiaoyu Mao Fuli Xie Xiaohui Wang Qingsong Wang Zhipeng Qiu Mark R.J.Elsegood Jie Bai Xing Feng carl redshaw Yanping Huo Jian-Yong Hu Qing Chen Guangdong Provincial Key Laboratory of Functional Soft Condensed Matter School of Material and EnergyGuangdong University of TechnologyGuangzhouGuangdong 510006China Shaanxi Key Laboratory for Advanced Energy Devices School of Materials Science and EngineeringShaanxi Normal UniversityXi'anShaanxi 710119China School of Chemical Engineering and Light Industry Guangdong University of TechnologyGuangzhouGuangdong 510006China Chemistry Department Loughborough UniversityLoughboroughLE113TUUK Department of Chemistry University of HullCottingham RoadHullYorkshire HU67RXUK Chinese Research Academy of Environmental Sciences No.8DayangfangBeiyuanBeijingChina

Three new deep blue light emitters,bearing quinoxaline with different substituents(biphenyl/pyrene)at the 1-or 2-position,were synthesized by a Pd-catalysed coupling reaction in high yields,and were fully characterize... 详细信息

关键词： Quinoxaline Pyrene Aggregation-induced emission Solid-state structures Substituent effects

一种用于水中次氯酸根检测的高选择性裸眼比色探针

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光谱学与光谱分析 2022年第1期42卷 322-332页

作者：余青陈晓丽张奇龙刘华杨先炯徐红黄亚励冯星 redshaw carl 贵州医科大学公共卫生学院教育部环境污染监测与控制重点实验室贵州贵阳550004 贵州医科大学临床医学院贵州贵阳550004 贵州医科大学基础医学院贵州贵阳550004 广东工业大学材料与能源学院广东省功能性软冷凝物质重点实验室广东广州510006 Department of Chemistry&Biochemistry University of HullCottingham RoadHullYorkshire HU67RXUK

实时检测和监测水中的次氯酸根离子(ClO-)是极富挑战性的研究工作。报道了一种光学性能优异、“裸眼”可分辨的比色型探针分子(PAH)。首先利用高分辨质谱,核磁共振氢谱和核磁共振碳谱等方法对目标探针分子(PAH)的结构进行表征。随后,利... 详细信息

实时检测和监测水中的次氯酸根离子(ClO-)是极富挑战性的研究工作。报道了一种光学性能优异、“裸眼”可分辨的比色型探针分子(PAH)。首先利用高分辨质谱,核磁共振氢谱和核磁共振碳谱等方法对目标探针分子(PAH)的结构进行表征。随后,利用紫外-可见吸收光谱考察了不同pH缓冲溶液条件下探针PAH与次氯酸根离子的相互作用。结果显示,水溶性的探针分子PAH在pH值为2.0~5.0的磷酸盐缓冲液中为黄色溶液,其最大吸收峰在424 nm处;在pH值为6.0~12.0的磷酸盐缓冲液中PAH为紫色溶液,最大吸收峰在532 nm处;在不同pH缓冲液体系中分别加入次氯酸根离子,肉眼可观察PAH溶液颜色褪去,紫外-可见吸收光谱显示在424 nm处的特征吸收峰逐渐降低并在532 nm处出现新的吸收峰,溶液颜色从黄色到紫色然后到无色,特征峰明显消失。进一步优化了实验条件,发现在pH 5.0的磷酸盐缓冲液中,探针分子PAH对ClO-离子具有特定的选择性和灵敏度,并且具有较低检出限等优点;在优化的条件下,探究了常见的金属离子、阴离子等共存条件下,对探针分子PAH检测次氯酸根离子的干扰影响。实验发现,常见的金属离子(Li^(+),Co 2^(+),Cr 3^(+),K^(+),Cd 2^(+),Pb 2^(+),Ca 2^(+),Hg 2^(+),Ba 2^(+),Cu 2^(+),Mg 2^(+),Ni 2^(+),Zn^(2^(+)),Al 3^(+)和Fe 3^(+)),阴离子(NO-2,I-,AcO-,ClO-4,SO_(2)-4,CN-,Br-,CO_(2)-3和F-),活性氧(ROO·,·OH,H_(2)O_(2),·O-2,tBuOOH,tBuO·和^(1)O_(2)),和活性氮(ONOO-和NO·)等33种物质对探针分子检测ClO-离子的干扰较小。同时,探针PAH可以定量检测次氯酸根离子(y=1.58678-0.52451x,R^(2)=0.99852),检出限为5.39μmol·L^(-1)。此外,对水体系(84消毒剂和自来水)中的次氯酸根离子浓度进行分析,三次平行试验测得自来水中次氯酸根离子的平均浓度为7.96μmol·L^(-1),平均加标回收率高,表明探针PAH还可用于定量检测实际水体系中的次氯酸根离子。

关键词：比色探针次氯酸根离子快速反应高选择性

Alkyl chain length-regulated in situ intelligent nano-assemblies with AIE-active photosensitizers for photodynamic cancer therapy

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Asian Journal of Pharmaceutical Sciences 2024年第6期19卷 84-100页

作者： Lingyi Shen Qilong Zhang Yongchao Yao Yali Huang Zhichang Zheng Ming Li Hong Xu Lin Tan Xukun Liao Binyi Xia Lin Li carl redshaw Yang Bai Chengli Yang Department of Pharmacy The Affiliated Hospital of Guizhou Medical UniversityGuiyang 550004China School of Basic Medicine Guizhou Medical UniversityGuiyang 550025China Chemistry School of Natural SciencesUniversity of HullYorkshire HU67RXUK Department of Biotherapy Cancer Center and State Key Laboratory of BiotherapyWest China HospitalSichuan UniversityChengdu 610041China Clinical Research Center The Affiliated Hospital of Guizhou Medical UniversityGuiyang 550004China

Photodynamic therapy(PDT)brings new hope for the treatment of breast cancer due to few side effects and highly effective cell killing;however,the low bioavailability of traditional photosensitizers(PSs)and their dependence on oxygen severely limits their ***-induced emission(AIE)PSs can dramatically facilitate the photosensitization effect,which can have positive impacts on tumor ***-date,most AIE PSs lack tumor targeting capability and possess poor cell delivery,resulting in their use in large quantities that are harmful to healthy *** this study,a series of AIE PSs based on pyridinium-substituted triphenylamine salts(TTPAs 1-6)with different alkyl chain lengths are *** reveal that TTPAs 1-6 promote the generation of type I and II ROS,including·OH and 1O_(2).In particular,the membrane permeability and targeting of TTPAs 4-6 bearing C8-C10 side-chains are higher than TTPAs 1-3 bearing shorter alkyl ***,they can assemble with albumin,thereby forming nanoparticles(TTPA 4-6 NPs)in situ in blood,which significantly facilitates mitochondrial-targeting and strong ROS generation ***,the TTPA 4-6 NPs are pH-responsive,allowing for increased accumulation or endocytosis of the tumor and enhancing the imaging or therapeutic ***,the in vivo distributions of TTPA 4-6 NPs are visually enriched in tumor sites and exhibited excellent PDT *** work demonstrates a novel strategy for AIE PDT and has the potential to play an essential role in clinical applications using nano-delivery systems.

关键词： Aggregation-induced emission Photosensitizers Photodynamic therapy ROS generation Self-assembled nanoparticles

[ZnCl4]2-Induced Coordination and Supramolecular Self-Assembly of Lanthanide Metal Ions to Cucurbit[6]uril:Potential Application in Separation of Light Lanthanides

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[ZnCl4]2-Induced Coordination and Supramolecular Self-Assemb...