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Model reduction of fractional impedance spectra for time–frequency analysis of batteries, fuel cells, and supercapacitors

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Carbon energy 2024年第1期6卷 108-141页

作者： Weiheng Li Qiu-An Huang Yuxuan Bai Jia Wang Linlin Wang Yuyu Liu Yufeng Zhao xifei Li Jiujun Zhang Institute for Sustainable energy/College of Sciences Shanghai UniversityShanghaiChina Shanxi key laboratory of Nanomaterials and Nanotechnology School of Mechanical and Electrical EngineeringXi'an University of Architecture and TechnologyXi'anShaanxiChina xi'an key laboratory of new energy materials and devices School of Materials Science and EngineeringInstitute of Advanced Electrochemical EnergyXi'an University of TechnologyXi'anShaanxiChina

Joint time–frequency analysis is an emerging method for interpreting the underlying physics in fuel cells,batteries,and supercapacitors.To increase the reliability of time–frequency analysis,a theoretical correlation between frequency-domain stationary analysis and time-domain transient analysis is urgently required.The present work formularizes a thorough model reduction of fractional impedance spectra for electrochemical energy devices involving not only the model reduction from fractional-order models to integer-order models and from high-to low-order RC circuits but also insight into the evolution of the characteristic time constants during the whole reduction process.The following work has been carried out:(i)the model-reduction theory is addressed for typical Warburg elements and RC circuits based on the continued fraction expansion theory and the response error minimization technique,respectively;(ii)the order effect on the model reduction of typical Warburg elements is quantitatively evaluated by time–frequency analysis;(iii)the results of time–frequency analysis are confirmed to be useful to determine the reduction order in terms of the kinetic information needed to be captured;and(iv)the results of time–frequency analysis are validated for the model reduction of fractional impedance spectra for lithium-ion batteries,supercapacitors,and solid oxide fuel cells.In turn,the numerical validation has demonstrated the powerful function of the joint time–frequency analysis.The thorough model reduction of fractional impedance spectra addressed in the present work not only clarifies the relationship between time-domain transient analysis and frequency-domain stationary analysis but also enhances the reliability of the joint time–frequency analysis for electrochemical energy devices.

关键词： battery,fuel cell,supercapacitor fractional impedance spectroscopy model reduction time-frequency analysis

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Photoredox catalytic alkylarylation of alkynes with arylsulfonylacetate as bifunctional reagent

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Science China Chemistry 2024年第6期67卷 2022-2028页

作者： Chonglong He Min Wang Yulong Wang Lirong Zhao Youkang Zhou keyuan Zhang Shenyu Shen Yaqiong Su xin-Hua Duan Le Liu School of Chemistry Engineering Research Center of Energy Storage Materials and DevicesMinistry of EducationXi’an Key Laboratory of Sustainable Energy Material ChemistryXi’an Jiaotong UniversityXi’an710049China

Difunctionalization of alkynes represents a powerful and straightforward approach to the synthesis of complex molecules.However,the radical difunctionalization of alkynes mediated by bifunctional reagents remains challenging and underexplored,despite significant progress having been made in alkene difunctionalization.Here,we report a novel arylsulfonylacetate skeleton in which aryl rings are attached to acetates through SO_(2),serving as a powerful bifunctional reagent for the alkylarylation of alkynes via vinyl-radical intermediate under photoredox conditions.This modular bifunctional reagent enables the simultaneous incorporation of a wide range of functional groups,including(hetero)aryl ring and alkyl carboxylate into alkynes,resulting in synthetically valuable all-carbon tetrasubstituted alkene derivatives.This transformation is distinguished by its redox-neutral nature,readily accessible starting materials,compatibility with diverse functional groups and its capacity to facilitate convergent synthesis.The utility of this approach was further demonstrated by the late-stage functionalization of complex molecules and the preparation of fluorescent molecules and anti-cancer drugs.

关键词： bifunctional reagent photoredox catalysis Smiles rearrangement alkylarylation tetrasubstituted acyclic all-carbon olefins

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S-scheme regulated Ni_(2)P-NiS/twinned Mn_(0.5)Cd_(0.5)S hetero-homojunctions for efficient photocatalytic H_(2)evolution

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Journal of materials Science & Technology 2024年第2期169卷 148-157页

作者： Qiqi Zhang Zhen Wang Yuhang Song Jun Fan Tao Sun Enzhou Liu School of Chemical Engineering/xi’an key laboratory of Special energy materials Northwest UniversityXi’an 710069China

Effective bulk phase and surface charge separation is critical for charge utilization during the photo-catalytic energy conversion process.In this work,the ternary Ni_(2)P-NiS/twinned Mn_(0.5)Cd_(0.5)S(T-MCS)nanohybrids were successfully constructed via combining Ni_(2)P-NiS with T-MCS solid solution for visible light photocatalytic H_(2)evolution.T-MCS is composed of zinc blende Mn_(0.5)Cd_(0.5)S(ZB-MCS)and wurtzite Mn_(0.5)Cd_(0.5)S(WZ-MCS)and those two alternatively arranged crystal phases endow T-MCS with excellent bulk phase charge separation performance for the slight energy level difference between ZB-MCS and WZ-MCS.S-scheme carriers transfer route between NiS and T-MCS can accelerate the interfacial charge separation and retain the active electrons and holes,meanwhile,co-catalyst Ni_(2)P as electron receiver and proton reduction center can further optimize the H_(2)evolution reaction kinetics based on the surface Schottky barrier effect.The above-formed homo-heterojunctions can establish multiple charge transfer channels in the bulk phase of T-MCS and interface of T-MCS and Ni_(2)P-NiS.Under the synergistic effect of twinned homojunction,S-scheme heterojunction,and Schottky barrier,the ternary Ni_(2)P-NiS/T-MCS com-posite manifested an H_(2)production rate of 122.5 mmol h^(-1)g^(-1),which was 1.33,1.24,and 2.58 times higher than those of the NiS/T-MCS(92.4 mmol h^(-1)g^(-1)),Ni_(2)P/T-MCS(98.4 mmol h^(-1)g^(-1)),and T-MCS(47.5 mmol h^(-1)g^(-1)),respectively.This work demonstrates a promising strategy to develop efficient sul-fides photocatalyst toward targeted solar-driven H_(2)evolution through homo-heterojunction engineering.

关键词： Photocatalytic H_(2)evolution Twinned Mn_(0.5)Cd_(0.5)S Homojunction S-scheme heterojunction Schottky barrier

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Metal–organic framework wafer enabled fast response radiation detection with ultra-low dark current

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Nano Research 2024年第4期17卷 2988-2993页

作者： Meng Xu Jianxi Liu Wei Wu Yang Chen Donghao Ma Sixin Chen Wanqi Jie Menghua Zhu Yadong Xu State key laboratory of Solidification Processing MIIT Key Laboratory of Radiation Detection Materials and Devices&School of Materials Science and EngineeringNorthwestern Polytechnical UniversityXi’an 710072China

Semiconductive metal–organic frameworks(MOFs)have attracted great interest for the electronic applications.However,dark currents of present hybrid organic–inorganic materials are 1000–10,000 times higher than those of commercial inorganic detectors,leading to poor charge transportation.Here,we demonstrate a ZIF-8(Zn(mim)_(2),mim=2-methylimidazolate)wafer with ultra-low dark current of 1.27 pA·mm^(-2) under high electric fields of 322 V·mm^(-1).The isostatic pressing preparation process provides ZIF-8 wafers with good transmittance.Besides,the presence of redox-active metals and small spatial separation between components promotes the charge hopping.The ZIF-8-based semiconductor detector shows promising X-ray detection sensitivity of 70.82μC·Gy^(-1)·cm^(-2) with low doses exposures,contributing to superior X-ray imaging capability with a relatively high spatial resolution of 1.2 lp·mm^(-1).Simultaneously,good peak discrimination with the energy resolution of~43.78%is disclosed when the detector is illuminated by uncollimated 241Am@5.48 MeVα-particles.These results provide a broad prospect of MOFs for future radiation detection applications.

关键词： MOFs lead-free α-particles X-ray detection and imaging dark current fast response

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Nickel-catalyzed carbonylative four-component 1,4-dicarbofunctionalization of 1,3-enynes

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Science China Chemistry 2024年第6期67卷 2029-2038页

作者： Yan Zhao Qi-Chao Shan Hong xin Pin Gao Xu Yang xin-Hua Duan Li-Na Guo Department of Chemistry School of ChemistryXi’an Key Laboratory of Sustainable Energy Material Chemistry and Engineering Research Center of Energy StorageMaterials and DevicesMinistry of EducationXi’an Jiaotong UniversityXi’an710049China School of Electrical Engineering Xi’an Jiaotong UniversityXi’an710049China

An efficient Ni-catalyzed four-component 1,4-carbocarbonylation of 1,3-enynes with activated alkyl halides and arylboronic acids under atmospheric pressure of CO is presented.By tuning the electronic and steric effects of alkyl radicals,both electronrich and electron-deficient 1,3-enynes were compatible with this cascade.This protocol features mild conditions,broad substrate scope,excellent functional group compatibility and facile gram-scale synthesis,providing a practical approach to the quaternary carbon center-containing allenyl ketones.Mechanistic study revealed that the acyl-NiIIspecies plays an important role in both the coupling and the alkyl radical generation processes.

关键词： Ni catalysis four-component 1 4-carbocarbonylation 1 3-enynes

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Recent progress in CdS-based S-scheme photocatalysts

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Journal of materials Science & Technology 2024年第4期171卷 162-184页

作者： Yajing Ren Yunfeng Li Guixu Pan Ning Wang Yan xing Zhenyi Zhang College of Environmental and Chemical Engineering Xi’an Polytechnic UniversityXi’an 710048China Jilin Provincial key laboratory of Advanced energy materials Department of ChemistryNortheast Normal UniversityChangchun 130024China key laboratory of new energy and Rare Earth Resource Utilization of State Ethnic Affairs Commission Key Laboratory of Photosensitive Materials and Devices of Liaoning ProvinceSchool of Physics and Materials EngineeringDalian Minzu UniversityDalian 116600China

Photocatalytic technology with sunlight as driving force can convert solar energy into other energy sources for storage and further use.Cadmium sulfide(CdS),as a typical reducing semiconductor of metal sulfides,represents an interesting research hotspot in photocatalysis due to its suitable bandgap(2.4 eV)for utilizing visible light and strong reducing ability for inducing surface catalytic reactions.Unfortunately,the photocatalytic performance of CdS is still limited by its fast carrier recombination and serious pho-tocorrosion.So far,CdS semiconductor has been widely developed as a typical reducing photocatalyst in constructing novel S-scheme heterojunction to overcome the above drawbacks.In this review,the de-sign concepts,basic principles,and charge transfer characteristics of CdS-based S-scheme heterojunction photocatalysts have been comprehensively introduced.Several advanced and effective characterization methods for studying the mechanism of CdS-based S-scheme heterojunction are analyzed in detail.Fur-thermore,we also summarize the typical applications of CdS-based S-scheme heterojunctions for water splitting,CO_(2) reduction,pollutant degradation,etc.Eventually,according to the current investigation sta-tus,some drawbacks in the current synthetic strategy,mechanism exploration,and application prospect of CdS-based S-scheme heterojunction are proposed,which need to be addressed by further expansion and innovative research.

关键词： Photocatalysis CdS semiconductor Heterojunction S-scheme Metal sulfide

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An effective catalyst carrier SiO_(2):Enhancing catalytic and combustion properties of CuFe_(2)O_(4)on energetic components

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Defence Technology（防务技术） 2024年第2期32卷 383-392页

作者： Li Ding Chong Wan Suhang Chen Zhao Qin Kangzhen Xu School of Chemical Engineering/xi'an key laboratory of Special energy materials Northwest UniversityXi'an710069China xi’an Modern Chemistry Research Institute Xi'an710065China

To enhance the catalytic activity of copper ferrite(CuFe_(2)O_(4))nanoparticle and promote its application as combustion catalyst,a low-cost silicon dioxide(SiO_(2))carrier was employed to construct a novel CuFe_(2)O_(4)/SiO_(2)binary composites via solvothermal method.The phase structure,morphology and catalytic activity of CuFe_(2)O_(4)/SiO_(2)composites were studied firstly,and thermal decomposition,combustion and safety performance of ammonium perchlorate(AP)and 1,3,5-trinitroperhydro-1,3,5-triazine(RDX)with it affecting were then systematically analyzed.The results show that CuFe_(2)O_(4)/SiO_(2)composite can remarkably either advance the decomposition peak temperature of AP and RDX,or reduce the apparent activation energy at their main decomposition zone.Moreover,the flame propagation rate of RDX was promoted by about 2.73 times with SiO_(2)content of 3 wt%,and safety property of energetic component was also improved greatly,in which depressing the electrostatic discharge sensitivity of pure RDX by about 1.89 times.In addition,the effective range of SiO_(2)carrier content in the binary catalyst is found to be 3 to 5 wt%.Therefore,SiO_(2)opens a new insight on the design of combustion catalyst carrier and will promote the application of CuFe_(2)O_(4)catalyst in solid propellant.

关键词： Copper ferrite Silicon dioxide Combustion catalyst Thermal decomposition Laser ignition

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Organic interfacial engineering of gold nanowires for selective glycerol electrooxidation

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Chinese Chemical Letters 2024年第3期35卷 502-507页

作者： Zhe Wang Qingling Hong Boqiang Miao Tianjiao Wang Yu Ding Pujun Jin Pei Chen Yu Chen key laboratory of Macromolecular Science of Shaanxi Province Key Laboratory of Applied Surface and Colloid Chemistry(Ministry of Education)Shaanxi Key Laboratory for Advanced Energy DevicesSchool of Materials Science and EngineeringShaanxi Normal UniversityXi'an 710062China

The selective electrochemical conversion of glycerol into value-added products is a green and sustainable strategy for the biomass utilization.In this work,Au nanowires(Au-NW)modified with polyethyleneimine(PEI)molecule(Au-NW@PEI)is obtained by an up-bottom post-modification approach.Physical characterization,molecular dynamics simulation and density functional theory demonstrate that the loose-packed PEI monolayer firmly and uniformly distribute on the Au-NW surface due to the strong Au-N interaction.Electrochemical experiments and product analysis display that PEI modification significantly enhance the electro-activity of Au-NW for the glycerol electro-oxidation reaction(GEOR)due to the electronic effect.Meanwhile,the steric hindrance and electrostatic effect of PEI layer make the optimizing adsorption of intermediates possible.Therefore,the selectivity of C3 product glyceric acid over Au-NW@PEI is increased by nearly 20%.The work thus indicates that the rational design of metal-organic interface can effectively elevate the electro-activity and selectivity of Au nanostructures,which may have wide application in biomass development.

关键词： Glycerol electrooxidation reaction Organic interface engineering Gold-based nanomaterials Electrocatalysis Selectivity

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Miura origami based reconfigurable polarization converter for multifunctional control of electromagnetic waves

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Photonics Research 2024年第3期12卷 581-586页

作者： ZHIBIAO ZHU YONGFENG LI ZHE QIN LIxiN JIANG WENJIE WANG HONGYA CHEN JIAFU WANG YONGQIANG PANG SHAOBO QU Shaanxi key laboratory of Artificially-Structured Functional materials and devices Air Force Engineering UniversityXi’an 710051China School of Electronic Science and Engineering Xi’an Jiaotong UniversityXi’an 710049China

Polarization is one of the basic characteristics of electromagnetic(EM)waves,and its flexible control is very important in many practical applications.At present,most of the multifunction polarization metasurfaces are electrically tunable based on PIN and varactor diodes,which are easy to operate and have strong real-time performance.However,there are still some problems in them,such as few degrees of freedom of planar structure control,complex circuit,bulky sample,and high cost.In view of these shortcomings,this paper proposes a Miura origami based reconfigurable polarization conversion metasurface for multifunctional control of EM waves.The interaction between the electric dipoles is changed by adjusting the folding angleθ,thereby tuning the operating frequency of the polarization conversion and the polarization state of the reflected wave.This mechanical control method brings more degrees of freedom to manipulate EM waves.And the processed sample is with lightweight and low cost.To verify the performance of the proposed origami polarization converter,a Miura origami structure loaded with metal split rings is designed and fabricated.The operating frequency of the structure can be tuned in different folding states.In addition,by controlling the folding angleθ,linear-to-linear and linear-to-circular polarization converters can be realized at different folding states.The proposed Miura origami polarization conversion metasurface provides a new idea for reconfigurable linear polarization conversion and multifunctional devices.

关键词： polarization reconfigurable tuning

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Photoinduced copper-catalyzed alkoxyl radical-triggered ring-expansion/aminocarbonylation cascade

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Chinese Chemical Letters 2024年第6期35卷 331-336页

作者： Jing-Qi Tao Shuai Liu Tian-Yu Zhang Hong xin Xu Yang xin-Hua Duan Li-Na Guo Department of Chemistry School of ChemistryXi’an Key Laboratory of Sustainable Energy Material Chemistry and Engineering Research Center of Energy Storage Materials and DevicesMinistry of EducationXi’an Jiaotong UniversityXi’an 710049China School of Electrical Engineering Xi’an Jiaotong UniversityXi’an 710049China State key laboratory of Applied Organic Chemistry Lanzhou UniversityLanzhou 730000China

A photoinduced copper-catalyzed alkoxyl triggered C-C bond cleavage/aminocarbonylation cascade is presented.Through adjusting the structure of alkoxyl radical precursors,functionalized lactones and ketoamides were synthesized with good yields and excellent functional group tolerance under redox-neutral conditions.Notably,this protocol enables the integration of lactone fragments with many amine drugs and drug fragments.

关键词： Copper catalysis Ring-expansion Aminocarbonylatioin Macrolactones Keto-amides

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