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Systematic study of the structure-property relationship of a series of near-infrared absorbing push-pull heptamethine chromophores for electro-optics

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science China chemistry 2021年第2期64卷 263-273页

作者： Di Zhang Jie Zou Wen Wang Qian Yu Guowei Deng Jieyun Wu Zhong-An Li Jingdong Luo Shenzhen Research institute City University of Hong KongShenzhen518057China Department of chemistry City University of Hong KongKowloonHong Kong SARChina College of chemistry and Life science Sichuan Provincial Key Laboratory for Structural Optimization and Application of Functional MoleculesChengdu Normal UniversityChengdu611130China School of Optoelectronic science and Engineering University of Electronic Science and Technology of ChinaChengdu611731China key laboratory for Material chemistry of Energy Conversion and Storage Ministry of EducationSchool of Chemistry and Chemical EngineeringHuazhong University of Science and TechnologyWuhan430074China

This study reports the facile synthesis,characterization and quantitative structure-property relationship analysis of molecular and material properties of tricyanofuran-based(TCF)dipolar heptamethines with different electron donors of indoline(F1),benzo[e]-indoline(F2),benz[cd]indoline(F3),and Michler’s base derivatives(Ml and M2).The linear and nonlinear optical(NLO)properties of these chromophores have been thoroughly investigated,and the relationship between molecular and bulk response has been analyzed and compared with dipolar tetraene AJLZ53 as one of the best chromophores for electro-optic(EO)*** particular,we provide responsible data collection and analysis of optical and EO properties for poled thin films using a widelyrecognized and accredited methodology of prism coupling system with the help of rigid oriented gas *** found that these push-pull heptamethines with synthetic efficacy exhibit high near-infrared absorption,excellent chemical stability and large hyperpolarizabilities(β)varied from 1,023×10^-30 esu for F1,3,047×10^-30 esu for M1,and 3,547×10^-30 esu for F3 at 1,304 nm in poled films,***βvalues of these molecules are among the highest ones for TCF-based dipolar chromophores,and also agree well with reported analytical results in the *** poled polymers with a modest chromophoric loading density of1.3×10^20 cm^-3,Ml and M2 give a high poled-induced noncentrosymmetric order and relatively large r33 values around40 pm V^-1 at 1,304 nm,indicative of largeμβvalues and suitable structural modification for high poling ***,a binary EO polymer based on the co-loading of Ml and AJLZ53 achieve a large r33 value of 143.3 pm V^-1 at 1,304 *** studies suggest that concise synthesis and molecular design of push-pull polymethines can be well guided by the tabulation of their linear and NLO properties in bulk materials,and streamline future development of high performance organic EO materials for photonic ap

关键词： electro-optics Pockels coefficient hyperpolarizability dipolar chromophores organic nonlinear optics

Recent advances in carbon-based electrocatalysts for oxygen reduction reaction

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Chinese Chemical Letters 2020年第3期31卷 626-634页

作者： Lulu Chen Xiaolong Xu Wenxiu Yang Jianbo Jia State key laboratory of electroanalytical chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China University of science and Technology of China Hefei 230026China Department of Materials science&Engineering&Department of Energy and Resources Engineering College of EngineeringPeking UniversityBeijing 100871China School of Chemical and Environmental Engineering Wuyi UniversityJiangmen 529020China

Fuel cells are one of the most promising clean energy devices to substitute for fossil fuel in the future to alleviate energy crisis and environmental *** the key reaction on the cathode in the fuel cells,oxygen reduction reaction(ORR)still requires efficient noble metal catalysts such as the comme rcial Pt/C to boost the reaction for its sluggish ***,it is critical to design earth-abundant carbonbased catalysts with high efficiency and long-term stability to replace the noble metal-based *** review focuses on the recent progress about carbon-based ORR catalysts including non-metal doped carbon materials,transition metal-nitrogen-carbon species,transition metal carbides/carbon,single atom catalysts,and other carbon *** we further infer that the excellent ORR performances can be achieved by the balance of geometric and electronic structures of catalysts such as conductivity,surface area,hierarchical porous structure,defect and doping ***,the perspective development trend is also proposed to guide the rational designation of carbon-based catalysts for ORR and even extend to other energy storage and conversion fields in the future.

关键词： Oxygen reduction reaction Carbon materials Transition metal catalysts Single atom catalysts Fuel cells

Facile synthesis of gold nanoflowers as SERS substrates and their morphological transformation induced by iodide ions

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science China chemistry 2016年第8期59卷 1045-1050页

作者： Shujun Zhen Tong Wu Xin Huang Yuanfang Li Chengzhi Huang key laboratory of Luminescent and Real-Time analytical chemistry (Southwest University) Ministry of Education College of Chemistry and Chemical Engineering Southwest University 400715 Chongqing China Department of chemistry and Chemical Engineeringl Yibin University Yibin 644000 China College of Pharmaceutical science Southwest University Chongqing 400715 China

We report a new strategy to prepare gold nanoflowers （AuNFs） using a two-step seed-mediated method. The as-prepared AuNFs were employed as surface-enhance Raman scattering （SERS） substrates, showing strong signal enhancement. We further found that iodide ions （I^-） could selectively induce the morphological transformation of AuNFs to spheres, resulting in a blue-shift of the localized surface plasmon resonance （LSPR） bands, a color change of the AuNFs solution from blue to red, and decreased SERS activity. This behavior allows the AuNFs to be used in the determination of I^-.

关键词： gold nanoflowers SERS iodide ions

Interplay of Crosslinking Structures and Segmental Dynamics in Solid-Liquid Elastomers

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Chinese Journal of Polymer science 2022年第10期40卷 1297-1306,I0012页

作者： Hao Wang Wan-Su Peng Qi Wu Yan Zhao Shi-Tai Wang Yi Yang Jin-Rong Wu Xiao-Liang Wang Rong-Chun Zhang South China Advanced institute for Soft Matter science and Technology(AISMST) School of Emergent Soft MatterSouth China University of TechnologyGuangzhou 510640China key laboratory of High-Performance Polymer Materials and Technology of Ministry of Education Department of Polymer Science and EngineeringSchool of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210093China State key laboratory of Polymer Materials Engineering College of Polymer Science and EngineeringSichuan UniversityChengdu 610065China Suzhou Niumag analytical Instrument Corporation Chengdu 610065China Guangdong provincial key laboratory of Functional and Intelligent Hybrid Materials and Devices South China University of TechnologyGuangzhou 510640China

There have been significant interests in recent years for incorporating dynamic bonds into polymer materials for achieving multiple functionalities,such as self-healing,recycling,stimuli-responsiveness,and so ***,the impact of dynamic bonds on the polymer dynamics is actually less *** this study,we investigate a self-healing solid-liquid elastomer(SLE),which is a dual-crosslinked network made by coupling a permanently crosslinked polydimethylsiloxane(PDMS)network with polyborosiloxane(PBS)via abundant dynamic boron/oxygen dative *** double-quantum(DQ)NMR reveals that the crosslinking degree is reduced while the structural heterogeneity of network is enhanced with increasing PBS content,i.e.,increasing the content of dynamic boron/oxygen dative *** experiments clearly reveal two chain relaxation modes in the SLE samples with a characteristic relaxation time of around 2.1 s and 11.8 s,corresponding to the relaxation of coupled PBS and PDMS chains,*** master curves obtained from variable-temperature frequency-dependent rheological experiments also reveal enhanced heterogeneity of chain relaxation with increasing PBS ***,the impact of boron/oxygen dative bonds on the Rouse dynamics is further revealed by fast-field-cycling(FFC)NMR experiments,where the spinlattice relaxation rate(R_(1))of all SLE samples follows the same power law of R_(1)(ω)∝ω^(-0.33).Nevertheless,the incorporation of PBS did slightly increase the energy barrier of Rouse *** study well demonstrates a combined use of rheology and solid-state NMR spectroscopy can provide piercing insights into the interplay of crosslinking structures and dynamics of polymer materials.

关键词： Fast-field-cycling NMR Multiple-quantum NMR Rheology Dynamics Dynamic bonds

A novel heterogeneous Co(Ⅱ)-Fenton-like catalyst for efficient photodegradation by visible light over extended pH

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science China chemistry 2020年第12期63卷 1825-1836页

作者： Wu-Hua Chen Jin-Hua Xiong Xue Teng Jin-Xiao Mi Zhi-Biao Hu Haifeng Wang Zuofeng Chen Fujian provincial Colleges and University Engineering Research Center of Solid Waste Resource Utilization(Longyan University) College of Chemistry and Material ScienceLongyan UniversityLongyan 364012China Shanghai key laboratory of Chemical Assessment and Sustainability School of Chemical Science and EngineeringTongji UniversityShanghai 200092China key laboratory for Advanced Materials Centre for Computational Chemistry and Research Institute of Industrial CatalysisEast China University of Science and TechnologyShanghai 200237China Department of Materials science and Engineering College of MaterialsXiamen UniversityXiamen 361005China

A novel Co^Ⅱ-Fenton-like heterogeneous catalyst,(H3O)2[Co^Ⅱ(phen)(H2O)2]2[Mo^Ⅵ5O15(PO4)2]·4H2O (phen=1,10-phenanthroline,C12N2H8)(1),is synthesized and utilized for photocatalytic degradation of organic dyes and antibiotic in a wide range of *** experimental results show that 1 acting as the Fenton-like catalyst with H2O2 exhibits remarkable activity at pH 3–9 under vis-light irradiation and is merited with excellent recyclability and reusability.A variety of analytical methods,including in-situ electron paramagnetic resonance (EPR) spectroscopy and density functional theory (DFT) calculations,are applied to study the mechanism on generation of·OH and O2^·-radicals for photocatalytic *** suggests that,unlike the classical Fenton process involving the redox transformation of the central cations,the generation of·OH and O2^·-radicals is associated with the substitution of the coordinating water molecules at Co(Ⅱ) by H2O2 and/or OOH^-,followed by the light-driven O–O bond cleavage and *** outcomes of this study are striking which overcome the obstacles in the classical Fe^Ⅱ-Fenton process,including the slow redox transformation between Fe(Ⅱ) and Fe(Ⅲ) and the production of massive iron precipitates especially at elevated *** opens up new avenues for the development of the high-performance Fenton(-like) catalysts for photocatalytic degradation over extended pH and provides new insight into the related process.

关键词： Co^Ⅱ-Fenton-like reagent polyoxometalate photocatalytic degradation density functional theory(DFT)calculations in-situ EPR spectroscopic analysis

SERS monitoring of photoinduced-enhanced oxidative stress amplifier on Au@carbon dots for tumor catalytic therapy

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Light(science & Applications) 2022年第10期11卷 2492-2502页

作者： Linjia Li Jin Yang Jiahui Wei Chunhuan Jiang Zhuo Liu Bai Yang Bing Zhao Wei Song State key laboratory of Supramolecular Structure and Materials College of ChemistryJilin UniversityChangchun 130012China Department of Vascular Surgery of China-Japan Union Hospital Jilin UniversityChangchun 130031China College of Basic Medical sciences Jilin UniversityChangchun 130021China Department of laboratory Animals College of Animal SciencesJilin UniversityChangchun 130062China State key laboratory of electroanalytical chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China

Currently,artificial enzymes-based photodynamic therapy(PDT)is attractive due to its efficient capacity to change the immunosuppressive tumor microenvironment(TME).It is of great significance to study the therapeutic mechanism of novel artificial enzymes in TME through a monitoring strategy and improve the therapeutic *** this study,Au@carbon dots(Au@CDs)nanohybrids with a core-shell structure are synthesized,which not only exhibit tunable enzyme-mimicking activity under near-infrared(NIR)light,but also excellent surface-enhanced Raman scattering(SERS)***,Au@CDs show a good capability for monitoring NIR-photoinduced peroxidase-like catalytic processes via a SERS strategy in ***,the Au@CDs deplete glutathione with the cascade catalyzed reactions,thus elevating intratumor oxidative stress amplifying the reactive oxygen species damage based on the NIR-photoinduced enhanced peroxidase and glutathione oxidase-like activities,showing excellent and fast PDT therapeutic effect promoted by photothermal property in 3 min,finally leading to apoptosis in cancer *** SERS monitoring,it is further found that after removing the NIR light source for 33 min,the reactive oxygen species(ROS)activity of the TME is counteracted and eliminated due to the presence of *** work presents a guidance to rationally design of artificial enzyme for ROS-involved therapeutic strategies and a new spectroscopic tool to evaluate the tumor catalytic therapy.

关键词： catalytic oxidative artificial

Sea urchin‐like NiMoO_(4) nanorod arrays as highly efficient bifunctional catalysts for electrocatalytic/photovoltage‐driven urea electrolysis

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Chinese Journal of Catalysis 2022年第5期43卷 1267-1276页

作者： Chenxin Chen Suqi He Kamran Dastafkan Zehua Zou Qingxiang Wang Chuan Zhao Department of chemistry and Environment science Fujian Provincial Key Laboratory of Modern Analytical Science and Separation TechnologyMinnan Normal UniversityZhangzhou 363000FujianChina School of chemistry and Materials&Manufacturing Futures institute The University of New South WalesSydney 2052Australia

Developing multifunctional electrocatalysts with high catalytic activity,longterm stability,and low cost is essential for electrocatalytic energy ***,sea urchinlike NiMoO_(4) nanorod arrays grown on nickel foam has been developed as a bifunctional electrocatalyst for urea oxidation and hydrogen *** NiMoO_(4)‐200/NF catalyst exhibits efficient activity toward hydrogen evolution reaction with a low overpotential of only 68 mV in 1.0 mol/L KOH to gain a current density of 10 mA cm^(–2).The NiMoO_(4)‐300/NF catalyst exhibits a prominent oxygen evolution reaction(OER)catalytic activity with an overpotential of 288 mV at 50 mA cm^(–2),as well as for urea oxidation reaction with an ultralow potential of 1.36 V at 10 mA cm^(–2).The observed difference in electrocatalytic activity and selectivity,derived by temperature variation,is ascribed to different lattice oxygen *** lattice oxygen of NiMoO_(4)‐300/NF is more than that of NiMoO_(4)‐200/NF,and the lattice oxygen is conducive to the progress of OER.A urea electrolyzer was assembled with Ni‐MoO_(4)‐200/NF and NiMoO_(4)‐300/NF as cathode and anode respectively,delivering a current density of 10 mA cm^(–2)at a cell voltage of merely 1.38 *** NiMoO_(4)nanorod arrays has also been successfully applied for photovoltage‐driven urea electrolysis and hydrogen production,revealing its great potential for solar‐driven energy conversion.

关键词： NiMoO4 nanorod Bifunctional electrocatalyst Urea electrolysis Photovoltage‐driven Lattice oxygen Sea urchin‐like

A universal design for triggering the precise micro-structure reconstruction through in-situ electro-regulating to boost the pseudocapacitance of MnO_(2)

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Journal of Energy chemistry 2022年第11期31卷 184-197,I0006页

作者： Lijin Yan Jiangyu Hao Baibai Liu Xuefeng Zou Qibin Wu Jin Hou Jizhou Duan Shicheng Wei Yang Zhou Bin Xiang Baorong Hou College of chemistry and Chemical Engineering Chongqing UniversityChongqing 401331China College of Optoelectronic Engineering Chongqing UniversityChongqing 400044China Guizhou provincial key laboratory of Computational Nano-Material science Guizhou Normal UniversityGuiyang 550018GuizhouChina College of chemistry and Chemical Engineering Ocean University of ChinaQingdao 266100ShandongChina key laboratory of Marine Environmental Corrosion and Bio-fouling Institute of OceanologyChinese Academy of SciencesQingdao 266071ShandongChina National key laboratory for Remanufacturing Army Academy of Armored ForcesBeijing 100072China analytical and Testing Center of Chongqing University Chongqing UniversityChongqing 401331China

Developing a precise controllable strategy for modulating the micro-morphology,atom coordination environment,and electronic structure of electrode materials is crucial for the performance in the field of energy storage,yet still a tremendous ***,a facile and universal in-situ electrochemical self-optimization design,electro-regulating,is designed to controllably produce electrode materials with abundant *** detailed characterization studies,the microstructure of MnO_(2) is reconstructed after electro-regulating,which exhibits a structure of small fragments with numerous holes due to the partial self-dissolution of acidic oxides under an alkaline operating ***,the electro-regulating strategy not only presents the formation steps of numerous holes but is also accompanies by a number of O vacancies generation process due to the activation of an external electric *** study provides a new inspiration for reasonably designing advanced functional electrode materials for various electrochemical applications and beyond.

关键词： Electro-regulating Microstructure reconstructed MnO_(2) Corrosion resistance Supercapacitors

Continuous flow removal of acid fuchsine by dielectric barrier discharge plasma water bed enhanced by activated carbon adsorption

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Frontiers of Chemical science and Engineering 2019年第2期13卷 340-349页

作者： Rusen Zhou Renwu Zhou Xianhui Zhang Kateryna Bazaka Kostya (Ken) Ostrikov School of chemistry Physics and Mechanical EngineeringQueensland University of TechnologyBrisbaneQLD 4000Australia CSIRO-QUT Joint Sustainable Processes and Devices laboratory CSIROLindfieldNSW 2070Australia Fujian provincial key laboratory of Plasma and Magnetic Resonance Institute of Electromagnetics and AcousticsDepartment of Electronic ScienceSchool of Electronic Science and EngineeringXiamen UniversityXiamen 361005China

Continuous processes which allow for large amount of wastewater to be treated to meet drainage standards while reducing treatment time and energy consumption are urgently needed. In this study, a dielectric barrier discharge plasma water bed system was designed and then coupled with granular activated carbon (GAC) adsorption to rapidly remove acid fuchsine (AF) with high efficiency. Effects of feeding gases, treatment time and initial concentration of AF on removal efficiency were investigated. Results showed that compared to the N2 and air plasmas treatments, O2 plasma processing was most effective for AF degradation due to the strong oxidation ability of generated activated species, especially the OH radicals. The addition of GAC significantly enhanced the removal efficiency of AF in aqueous solution and shorten the required time by 50%. The effect was attributed to the ability of porous carbon to trap and concentrate the dye, increasing the time dye molecules were exposed to the plasma discharge zone, and to enhance the production of OH radicals on/in GAC to boost the degradation of dyes by plasma as well as in situ regenerate the exhausted GAC. The study offers a new opportunity for continuous effective remediation of wastewater contaminated with organic dyes using plasma technologies.

关键词： continuous removal dye-containing wastewater dielectric barrier discharge plasma water bed activated carbon adsorption