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Superior performance in visible-light-driven hydrogen evolution reaction of three-dimensionally ordered macroporous SrTiO_(3) decorated with Zn_(x)Cd_(1−x)S

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Frontiers of Chemical Science and Engineering 2021年第6期15卷 1561-1571页

作者： Huiying Quan Kejiang Qian Ying Xuan Lan-Lan Lou Kai Yu Shuangxi Liu moe key laboratory of Pollution Processes and environmental Criteria Tianjin Key Laboratory of Environmental Technology for Complex Transmedia PollutionCollege of Environmental Science and EngineeringNankai UniversityTianjin300350China Institute of New Catalytic Materials Science and moe key laboratory of Advanced Energy Materials chemistry School of Materials Science and EngineeringNational Institute of Advanced MaterialsNankai UniversityTianjin300350China

It is of broad interest to develop emerging photocatalysts with excellent light-harvesting capacity and high charge carrier separation efficiency for visible light photocatalytic hydrogen evolution ***,achieving satisfying hydrogen evolution efficiency under noble metal-free conditions remains *** this study,we demonstrate the fabrication of three-dimensionally ordered macroporous SrTiO_(3)decorated with Zn_(x)Cd_(1−x)S nanoparticles for hydrogen production under visible light irradiation(λ>420 nm).Synergetic enhancement of photocatalytic activity is achieved by the slow photon effect and improved separation efficiency of photogenerated charge *** obtained composites could afford very high hydrogen production efficiencies up to 19.67 mmol·g^(−1)·h^(−1),with an apparent quantum efficiency of 35.9%at 420 nm,which is 4.2 and 23.9 times higher than those of pure Zn_(0.5)Cd_(0.5)S(4.67 mmol·g^(−1)·h^(−1))and CdS(0.82 mmol·g^(−1)·h^(−1)),*** particular,under Pt-free conditions,an attractive hydrogen production rate(3.23 mmol·g^(−1)·h^(−1))was achieved,providing a low-cost and high-efficiency strategy to produce hydrogen from water ***,the composites showed excellent stability,and no obvious loss in activity was observed after five cycling tests.

关键词： three-dimensionally ordered macroporous SrTiO_(3) Zn_(x)Cd_(1−x)S visible light hydrogen production promotion mechanism

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theoretical Design of Blue-light-emitting Material Based on 1,2,3-Benzotriazole-based Derivative

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Chinese Journal of Structural chemistry 2011年第10期30卷 1447-1451页

作者：胡波姚婵黄旭日 Faculty of chemistry Jilin Normal University key laboratory of Preparation and Applications of environmental Friendly Materials Jilin Normal University State key laboratory of theoretical and Computational chemistry Jilin University

theoretically,1,2,3-benzotriazole（BT）-based derivative is designed by the struc-tural tuning in 2,1,3-benzothiadiazole（BTD）-based derivative and presents potential for applications in organic light-emitting diodes（OLEDs）.Calculations show that the emission spectrum of BT-based derivative is located at the blue scope,so it can act as a blue-light-emitting ***,the oscillator strength of emission spectrum is significantly enhanced by replacing BTD with BT,implying it possess large fluorescent ***,BT-based derivative exhibits improved hole transportation with respect to the BTD-based derivative.

关键词： OLEDs 1 2 3-benzotriazole electronic and optical properties charge transport

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Sub-micrometer-scale chemical analysis by nanosecond-laser-induced tip-enhanced ablation and ionization time-of-flight mass spectrometry

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Nano Research 2018年第11期11卷 5989-5996页

作者： Xiaoping Li Zhisen Liang Shudi Zhang Tongtong Wang Wei Hang Department of chemistry and the moe key Lab ofSpectrochemicalAnalysis & Instrumentation College of Chemistry and ChemicalEngineering Xiamen University Xiamen 361005 China State key laboratory of Marine environmental Science Xiamen University Xiamen 361005 China

The tip-enhanced near-field technique has drawn great attention recently because it is a promising technique for nanoscale chemical analysis when combined with other spectroscopic methods. Furthermore, this integration can improve the spatial resolution of mass spectrometry. In this study, a nanosecond-laser (ns-laser)-induced tip-enhanced ablation and ionization source was coupled to an in-house-built laser ionization time-of-flight mass spectrometer. Sub-micrometer-sized craters (with diameters of 200-300 nm) were observed on titanium (Ti) film coated onto a gold (Au) substrate. The corresponding mass spectra were acquired, which verified that sub-micrometer-sized ablation (and subsequently ionization) could be achieved by the ns-laser-induced tip-enhanced electromagnetic field. In addition, formation of the crater was studied with an increased number of laser pulses. Furthermore, a mass spectrometry imaging (MSI) experiment was performed with potassium chloride (KCl) residue dropped onto nano-patterned gold pillars, achieving 80-nm lateral resolution.

关键词： tip-enhanced near-field technique time-of-flight mass spectrometer nanosecond laser sub-micrometer-scale spatial resolution

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Construction of cobalt vacancies in cobalt telluride to induce fast ionic/electronic diffusion kinetics for lithium-ion half/full batteries

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Journal of Materials Science & Technology 2022年第32期127卷 124-132页

作者： Lei Hu Lin Li Yuyang Zhang Xiaohong Tan Hao Yang Xiaoming Lin Yexiang Tong Anhui laboratory of Functional Coordinated Complexes for Materials chemistry and Application School of Chemical and Environmental EngineeringAnhui Polytechnic UniversityWuhu 241000China moe of the key laboratory of Bioinorganic and Synthetic chemistry The Key Laboratory of Low-Carbon Chemistry&Energy Conservation of Guangdong ProvinceSchool of ChemistrySun Yat-Sen UniversityGuangzhou 510275China Guangxi key laboratory of Electrochemical Energy Materials School of Chemistry&Chemical EngineeringGuangxi UniversityNanning 530004China key laboratory of theoretical chemistry of Environment Ministry of EducationSchool of ChemistrySouth China Normal UniversityGuangzhou 510006China

Designing novel electrode materials with unique structures is of great significance for improving the performance of lithium ion batteries(LIBs).Herein,copper-doped Co_(1-x)Te@nitrogen-doped carbon hollow nanoboxes(Cu-Co_(1-x)Te@NC HNBs)have been fabricated by chemical etching of Cu Co-ZIF nanoboxes,followed by a successive high-temperature tellurization *** as-synthesized Cu-Co_(1-x)Te@NC HNBs composite demonstrated faster ionic and electronic diffusion kinetics than the pristine Co Te@NC HNBs *** existence of Co-vacancy promotes the reduction of Gibbs free energy change(ΔG_(H^(*)))and effectively improves the Li~+diffusion *** and theoretical calculations show that performance improvement is ascribed to the electronic interactions between Cu-Co_(1-x)Te and nitrogen-doped carbon(NC)that trigger the shift of the p-band towards facilitation of interfacial charge transfer,which in turn helps boost up the lithium storage ***,the proposed Cu-doping-induced Co-vacancy strategy can also be extended to other conversion-type cobalt-based material(CoSe_(2))in addition to asobtained Cu-Co_(1-x)Se_(2)@NC HNBs anodes for long-life and high-capacity *** importantly,the fabricated LiCoO_(2)//Cu-Co_(1-x)Te@NC HNBs full cell exhibits a high energy density of 403 Wh kg^(-1)and a power density of 6000 W kg^(-1).We show that the energy/power density reported herein is higher than that of previously studied cobalt-based anodes,indicating the potential application of Cu-Co_(1-x)Te@NC HNBs as a superior electrode material for LIBs.

关键词： MOF-derived material Cobalt telluride Cobalt vacancy Diffusion kinetics Lithium storage

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Ultrasmall high-entropy alloy nanoparticles on hierarchical N-doped carbon nanocages for tremendous electrocatalytic hydrogen evolution

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Nano Research 2024年第11期17卷 9518-9524页

作者： Manman Jia Jietao Jiang Jingyi Tian Xizhang Wang Lijun Yang Qiang Wu Zheng Hu key laboratory of Mesoscopic chemistry of moe and Jiangsu Provincial laboratory for Nanotechnology School of Chemistry and Chemical Engineering Nanjing University Nanjing 210023 China

High-entropy alloys (HEAs) are promising candidates for the electrocatalyst of hydrogen evolution reaction (HER) due to their unique properties such as cocktail electronic effect and lattice distortion effect. Herein, the ultrasmall (sub-2 nm) nanoparticles of PtRuCoNiCu HEA with uniform element distribution are highly dispersed on hierarchical N-doped carbon nanocages (hNCNC) via low-temperature thermal reduction, denoted as us-HEA/hNCNC. The optimal us-HEA/hNCNC exhibits excellent HER performance in 0.5 M H_(2)SO4 solution, achieving an ultralow overpotential of 19 mV at 10 mA·cm^(−2) (without iR-compensation), high mass activity of 13.1 A·mgnoble metals ^(−1) at −0.10 V and superb stability with a slight overpotential increase of 3 mV after 20,000 cycles of cyclic voltammetry scans, much superior to the commercial Pt/C (20 wt.%). The combined experimental and theoretical studies reveal that the Pt&Ru serve as the main active sites for HER and the CoNiCu species modify the electron density of active sites to facilitate the H* adsorption and achieve an optimum M-H binding energy. The hierarchical pore structure and N-doping of hNCNC support also play a crucial role in the enhancement of HER activity and stability. This study demonstrates an effective strategy to greatly improve the HER performance of noble metals by developing the HEAs on the unique hNCNC support.

关键词： high-entropy alloys acidic hydrogen evolution ultrasmall nanoparticles hierarchical carbon nanocages high activity

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Impact of Pd single-site coordination structure on catalytic performance for semihydrogenation of acetylene

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Nano Research 2024年第9期17卷 8243-8249页

作者： Yu Zeng Minqi Xia Fujie Gao Changkai Zhou Xueyi Cheng Liwei Liu Liu Jiao Qiang Wu Xizhang Wang Lijun Yang Yining Fan Zheng Hu key laboratory of Mesoscopic chemistry of moe and Jiangsu Provincial laboratory for Nanotechnology School of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China

Semihydrogenation of trace acetylene in an ethylene gas stream is a vital step for the industrial production of polyethylene,in which Pd single-site catalysts(SSCs)have great ***,two Pd SSCs with different coordination structures are prepared on hierarchical nitrogen-doped carbon nanocages(hNCNC)by regulating the nitrogen species with or without using *** using dicyandiamide,the obtained Pd1-Ndicy/hNCNC SSC features the coordinated Pd by two pyridinic N and two pyrrolic N(PdN^(py)_(2)N^(pr)_(2)).Without using dicyandiamide,the obtained Pd1/hNCNC SSC features the coordinated Pd by pyridinic N and C(PdN^(py_(x)C_(4-x)),x=1-4).The former exhibits an 18-fold increase in catalytic activity compared to the *** results reveal the abundant unoccupied orbital states above the Fermi level of moiety,which can facilitate the activation of substrate molecules and dynamics of acetylene hydrogenation as supported by the combined theoretical and experimental *** addition,PdN^(py)_(2)N^(pr)_(2)the moiety presents a favorable desorption of ***,the Pd1-Ndicy/hNCNC SSC exhibits high C2H2 conversion(99%)and C2H4 selectivity(87%)at 160℃.This study demonstrates the impact of Pd single-site coordination structure on catalytic performance,which is significant for the rational design of advanced Pd SSCs on carbon-based supports.

关键词： coordination structure hierarchical nitrogen-doped carbon nanocages palladium semihydrogenation of acetylene singlesite catalysts

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Insights into Photothermally Enhanced Photocatalytic U(VI)Extraction by a Step-Scheme Heterojunction

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Research 2023年第1期2022卷 285-299页

作者： Yifeng Zhang Haorong Sun Feixue Gao Shuo Zhang Qingzhi Han Jing Li Ming Fang Yawen Cai Baowei Hu Xiaoli Tan Xiangke Wang moe key laboratory of Resources and environmental System Optimization College of Environmental Science and EngineeringNorth China Electric Power UniversityBeijing 102206China key laboratory of theoretical and Computational Photochemistry Ministry of EducationCollege of ChemistryBeijing Normal UniversityBeijing 100875China key laboratory of Photochemical Conversion and Optoelectronic Materials Technical Institute of Physics and ChemistryChinese Academy of SciencesBeijing 100190China School of Life Science Shaoxing UniversityShaoxing 312000China

In this work,a CdS/BivO4 step-scheme(S-scheme)heterojunction with self-photothermally enhanced photocatalytic effect was synthesized and applied for efficient U(VI)*** such as transient absorption spectroscopy and Tafel test together confirmed the formation of S-scheme heterojunctions,which allows CdS/BivO_(4) to avoid photocorrosion while retaining the strong reducing capacity of CdS and the oxidizing capacity of BivO_(4).Experimental results such as radical quenching experiments and electron spin resonance show that U(VI)is rapidly oxidized by photoholes/·OH to insoluble UO(OH)2 after being reduced to U(IV)by photoelectrons/·O2,which precisely avoids the depletion of electron sacrificial *** rapid recombination of electron-hole pairs triggered by the S-scheme heterojunction is found to release large amounts of heat and accelerate the *** work offers a new enhanced strategy for photocatalytic uranium extraction and presents a direction for the design and development of new photocatalysts.

关键词： scheme retaining thermally

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Current situation and forecast of environmental risks of a typical lead-zinc sulfide tailings impoundment based on its geochemical characteristics

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Journal of environmental Sciences 2020年第7期32卷 120-128页

作者： Tao Chen Zi-Ang Yan Damao Xu Minghui Wang Jian Huang Bo Yan Xianming Xiao Xunan Ning SCNU environmental Research Institute Guangdong Provincial Key Laboratory of Chemical Pollution and Environmental Safety&MOE Key Laboratory of Environmental Theoretical ChemistrySouth China Normal UniversityGuangzhou 510006China School of Chemical Engineering and Light Industry Guangdong University of TechnologyGuangzhou 510640China State key laboratory of Organic Geochemistry Guangzhou Institute of GeochemistryChinese Academy of SciencesGuangzhou 510640China China University of Geosciences Beijing 100083China

The potential environmental implications of a Pb(Lead)-Zn(Zinc)sulfide tailing impoundment were found to be dependent on its geochemical *** typical lead-zinc sulfide tailing impoundment was *** boreholes were set with the grid method and 36 tailings were sampled and *** to the results of metal content analysis,the tailing samples contained considerably high contents of heavy metals,ranging from 6.99 to 89.0 mg/kg for Cd,75.3 to 602 mg/kg for Cu,0.53%to 2.63%for Pb and 0.30%to 2.54%for *** of the heavy metals in the sample matrix showed a uniform concentration distribution,except ***,Pb,Zn,and Mn were associated with each other,and were considered to be the dominant contributors based on hierarchical cluster ***,SEM and XPS were employed for evaluation of the tailing weathering characteristics,confirming that the tailings had undergone intensive *** maximum potential acidity of the tailings reached 244 kg H2SO4/ton;furthermore,the bioavailability of heavy metals like Pb,Cd,Cr,Cu,and Zn was 37.8%,12.9%,12.2%,5.95%,and 5.46%*** metals would be potentially released into drainage by the weathering *** of a gastrointestinal model showed that Pb,Cr,Ni and Cu contained in the tailings were high-risk ***,control of the heavy metals’migration and their environmental risks should be planned from the perspective of geochemistry.

关键词： Pb-Zn tailings impoundment Geochemical characteristics Distribution of the metals Weathering process environmental risk assessment

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Towards single-atom photocatalysts for future carbon-neutral application

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SmartMat 2022年第3期3卷 417-446页

作者： Dongpeng Zhang Yanxiao Li Yi Li Sihui Zhan moe key laboratory of Pollution Processes and environmental Criteria Tianjin Key Laboratory of Environmental Remediation and Pollution ControlCollege of Environmental Science and EngineeringNankai UniversityTianjinChina Department of chemistry Tianjin UniversityTianjinChina

The implementation of carbon neutrality to achieve the goal of controlling global warming in the Paris Climate Agreement is currently the most important international climate *** utilization of solar energy through photocatalysts is of great significance to the adjustment of energy ***-atom photocatalysts have excellent catalytic activity and selectivity in a variety of applications,including sustainable energy conversion,chemical synthesis,CO_(2)reduction,environmental remediation,and other areas,owing to their unique electronic structure and high atom ***,we elaborated on the content and implementation direction of the carbon neutrality policy and demonstrated the design principles of single-atom *** single-atom synthesis strategies are summarized,and representative characterization methods have been shown to further reveal the structure–performance ***,we focus on the application of single-atom photocatalysts in CO_(2)reduction,sustainable energy conversion,and environmental ***,the opportunities and challenges in the application of single-atom photocatalysts were discussed based on its current development.

关键词： carbon neutrality CO_(2)reduction hydrogen photocatalysts single-atom catalysts synthesis strategies

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Self-Powered Piezo-Supercapacitors Based on ZnO@Mo-Fe-MnO_(2)Nanoarrays

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Energy & environmental Materials 2024年第4期7卷 304-314页

作者： Luo Sun Zhiguo Ye Xinyuan Peng Shaojie Zhuang Duosheng Li Zhong Jin School of Materials Science and Engineering Nanchang Hangkong University696#FengHeNan RoadNanchang 330063China State key laboratory of Coordination chemistry MOE Key Laboratory of Mesoscopic ChemistryMOE Key Laboratory of High Performance Polymer Materials and TechnologyJiangsu Key Laboratory of Advanced Organic MaterialsSchool of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China

The development of self-charging supercapacitor power cells(SCSPCs)has profound implications for smart electronic devices used in different ***,we epitaxially electrodeposited Mo-and Fe-codoped MnO_(2)films on piezoelectric ZnO nanoarrays(NAs)grown on the flexible carbon cloth(denoted ZnO@Mo-Fe-MnO_(2)NAs).A self-charging supercapacitor power cell device was assembled with the Mo-and Fe-codoped MnO_(2)nanoarray electrode and poly(vinylidenefluoride-co-trifluoroethylene)(PVDF-Trfe)piezoelectric film doped with BaTiO_(3)(BTO)and carbon nanotubes(CNTs)(denoted PVDF-Trfe/CNTs/BTO).The self-charging supercapacitor power cell device exhibited an energy density of 30μWh cm^(-2)with a high power density of 40 mW cm^(-2)and delivered an excellent self-charging performance of 363 mV(10 N)driven by both the piezoelectric ZnO nanoarrays and the poly(vinylidenefluoride-co-trifluoroethylene)piezoelectric film doped with BaTiO_(3)and carbon *** intriguingly,the device could also be self-charged by 184 mV due to residual stress alone and showed excellent energy conversion efficiency and low self-discharge *** work illustrates for the first time the self-charging mechanism involving electrolyte ion migration driven by both electrodes and films.A comprehensive analysis strongly confirmed the important contribution of the piezoelectric ZnO nanoarrays in the self-charging process of the self-charging supercapacitor power cell *** work provides novel directions and insights for the development of selfcharging supercapacitor power cells.

关键词： MnO_(2) piezoelectric self-charging supercapacitors ZnO nanoarray

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