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Electrolyte and interphase engineering through solvation structure regulation for stable lithium metal batteries

Chinese Chemical Letters 2023年第12期34卷 401-408页

作者： Hai Su Haikuo Zhang Zifeng Chen Mengjie Li Jiwei Zhao Haiyan Xun Jie Sun Yunhua Xu School of Materials Science and Engineering Key Laboratory of Advanced Ceramics and Machining Technology(Ministry of Education)and Tianjin Key Laboratory of Composite and Functional MaterialsTianjin UniversityTianjin 300072China State Key Laboratory of Silicon Materials School of Materials Science and EngineeringZhejiang UniversityHangzhou 310027China Key Laboratory for Green Chemical Technology of Ministry of Education School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China

Lithium metal batteries(LMBs)are considered to be one of the most promising high-energy-density battery ***,their practical application in carbonate electrolytes is hampered by lithium dendrite growth,resulting in short cycle ***,an electrolyte regulation strategy is developed to improve the cyclability of LMBs in carbonate electrolytes by introducing LiNO3 using trimethyl phosphate with a slightly higher donor number compared to NO_(3)^(-)as a *** not only allows the formaion of Li^(+)-coordinated NO3 but also achieves the regulation of electrolyte solvation structures,leading to the formation of robust and ion-conductive solid-electrolyte interphase films with inorganic-rich inner and organic-rich outer layers on the Li metal *** a result,high Coulombic efficiency of 99.1%and stable plating/stripping cycling of Li metal anode in LilCu cells were ***,excellent performance was also demonstrated in Li||LiNi_(0.83)Co_(0.11)Mn_(0.06)O_(2)(NCM83)full cells and Cul/NCM83 anodefree cells using high mass-loading *** work provides a simple interphase engineering strategy through regulating the electrolyte solvation structures for high-energy-density LMBs.

关键词： Lithium metal batteries Lithium nitrate Trimethyl phosphate Solvation structures Solid-electrolyte interphases

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Ensemble of single-atom catalysis and defect engineering in Cu_(1)/CeO_(2) nanozymes for tumor therapy

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science China Chemistry 2023年第9期66卷 2590-2599页

作者： Hao-Xin Liu Zhiliang Gao Han Yan Shan-Qing Li Wei-Wei Wang Xuetao Qin Hongning Sun Jiwei Cui Chun-Jiang Jia Key Laboratory of Colloid and Interface Chemistry Key Laboratory of Special Aggregated Materials of the Ministry of EducationSchool of Chemistry and Chemical EngineeringShandong UniversityJinan 250100China School of Materials and Environmental Engineering Chizhou UniversityChizhou 247000China

As a class of nanomaterials with natural enzyme-like characteristics, nanozymes have shown their great potential in various applications. Reducible metal oxides featured with defect structures, and single-atom catalysts with isolated metal sites are regarded as two of the most promising nanozymes. However, the strategies to construct highly performed nanozymes by combining these advantages are rarely reported. Herein, we report the coordination-unsaturated single-atomic Cu species supported on sintered CeO_(2), which combines the advantages of defect engineering and single-atom catalysis, exhibiting a largely enhanced peroxidase(POD)-like activity. The high-temperature calcination induces the transformation of inert Cu_(1)O_(4) species into coordination-unsaturated Cu_(1)O_(3) sites. This novel Cu_(1)O_(3) active sites with an unsaturated coordination work as a new type of defect sites to greatly activate the isolated Cu atoms and accelerate the dissociation of H_(2)O_(2) to form hydroxyl radicals(·OH). The obtained nanozyme with a high POD-like activity possesses low cytotoxicity, showing potential applications for the tumor inhibition in vitro and in vivo.

关键词： single-atom catalysis oxygen defect Cu/CeO_(2) peroxidase-like activity tumor inhibition

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Hierarchical Zn_(3)V_(2)O_(8)microspheres interconnected via conductive carbon nanotubes as promising anode materials for lithium-ion battery applications

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Rare Metals 2023年第8期42卷 2601-2611页

作者： Ming-Ming Liu Hai-Tao Yu Lang Yuan Ting-Feng Yi Fei He Ying Xie Key Laboratory of Functional Inorganic Material Chemistry Ministry of EducationSchool of Chemistry and Materials ScienceHeilongjiang UniversityHarbin 150080China School of Materials Science and Engineering Northeastern UniversityShenyang 110819China Key Laboratory of Superlight Materials and Surface Technology Ministry of EducationCollege of Materials Science and Chemical EngineeringHarbin Engineering UniversityHarbin 150001China

Zn_(3)V_(2)O_(8) was considered as a promising anode material for lithium-ion battery(LIB),because of its high theoretical specific capacity,environmental friendliness,and ease of ***,the large volume change and low electronic conductivity of Zn_(3)V_(2)O_(8)in repeated charge/discharge cycles have severely limited its *** solve the above issues,hierarchical Zn_(3)V_(2)O_(8) microspheres assembled by two-dimensional(2D)nanosheets were successfully synthesized,and carbon nanotubes(CNTs)were further introduced to cross-link the Zn_(3)V_(2)O_(8) *** interconnected nature of the three-dimensional(3D)conducting network and the special hierarchical morphology were beneficial for improving the stability and conductivity of the composite,leading to the reduction of the impedance and a significant improvement of the electrochemical *** reversible capacity of the as-prepared composite can achieve 1049.5mAh·g^(-1)at a current density of 0.2 A·g^(-1)with a capacity retention of~81%after 100 *** is suggested that morphology modulation coupled with interconnecting CNT network is an effective method to boost the electrochemical performance of the anode materials for lithium-ion batteries.

关键词： Anode material Zn_(3)V_(2)O_(8) Carbon nanotube(CNT) Electrochemical performance Lithium-ion battery(LIB)

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High-selectivity electroreduction of low-concentration CO_(2)with large concentration fluctuation

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science China Chemistry 2025年第4期68卷 1620-1626页

作者： Mengyu Qi Yanbin Ma Chao Zhang Bingwei Li Xueqing Yang Zhaolin Shi Simeng Liu Changhua An Jiqing Jiao Tongbu Lu MOE International Joint Laboratory of Materials Microstructure Analysis and Testing CenterInstitute for New Energy Materials and Low Carbon TechnologiesSchool of Materials Science and EngineeringSchool of Chemistry and Chemical EngineeringTianjin University of TechnologyTianjin 300384China Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education) NankaiUniversityTianjin 300071China

Electrochemical CO_(2)reduction reaction(CO_(2)RR)has been regarded as one of the most promising solutions to achieving“zero carbon emission”.In most of the CO_(2)RR-related studies;high-purity CO_(2)has been employed as the feed gas;however;in practice;CO_(2)is generally emitted in low concentrations;so it is of great significance to realize high-selectivity electroreduction of low-concentration CO_(2)with large concentration *** this work;we constructed a dual-active-site catalyst and successfully achieved CO_(2)local enrichment and conversion for low-concentration CO_(2).Operando experiments reveal that the catalyst has one type of site for activating CO_(2)and one type of site for binding the reaction *** dual-active-site catalyst displays a selectivity for formic acid consistently above 97%over a broad potential window(from-0.9 to-1.6 V ***).Even when fed with a low-concentration CO_(2)stream(volume ratio from 50%down to 10%);the dual-active-site catalyst could display high activity and selectivity(>91%).In particular;the selectivity is still above 85%when the CO_(2)volume ratio is as low as 5%.This work offers a feasible route for converting low-concentration CO_(2)via a synergistic effect for dual-active-site catalysts.

关键词： electrochemical CO_(2)reduction low-concentration CO_(2) high-selectivity dual-active-site catalyst operando infrared spectroscopy

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Polymer: Non-fullerene acceptor heterojunction-based phototransistor for short-wave infrared photodetection

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Nano Research 2024年第4期17卷 3087-3095页

作者： Jing Li Weigang Zhu Yang Han Yanhou Geng Wenping Hu Key Laboratory of Organic Integrated Circuits of Ministry of Education&Key Laboratory of Molecular Optoelectronic Sciences School of Science&Collaborative Innovation Center of Chemical Science and Engineering(Tianjin)Tianjin UniversityTianjin 300072China Key Laboratory of Organic Integrated Circuits of Ministry of Education&Key Laboratory of Molecular Optoelectronic Sciences School of Materials Science and EngineeringTianjin UniversityTianjin 300072China

It remains full of challenge for extending short-wave infrared(SWIR)spectral response and weak-light detection in the context of broad spectral responses for *** this work,a novel poly(2,5-bis(4-hexyldodecyl)-2,5-dihydro-3,6-di-2-thienyl-pyrrolo[3,4-c]pyrrole-1,4-dione-alt-thiophene)(PDPPT3-HDO):COTIC-4F organic bulk-heterojunction is prepared as active layer for bulk heterojunction ***3-HDO serves as a hole transport material,while COTIC-4F enhances the absorption of SWIR light to 1020 *** a result,smooth and connected PDPPT3-HDO film is fabricated by blade coating method and exhibits high hole mobility up to 2.34 cm^(2)·V^(-1)·s^(-1) with a current on/off ratio of 4.72×10^(5) in organic thin film ***3-HDO:COTIC-4F heterojunction phototransistors exhibit high responsivity of 2680 A·W^(-1) to 900 nm and 815 A·W^(-1) to 1020 nm,with fast response time(rise time~20 ms and fall time~100 ms).The photosensitivity of the heterojunction phototransistor improves as the mass ratio of non-fullerene acceptors increases,resulting in an approximately two orders of magnitude enhancement compared to the bare polymer ***,the phototransistor exhibits decent responsivity even under ultra-weak light power of 43μW·cm^(-2) to 1020 *** work represents a highly effective and general strategy for fabricating efficient and sensitive SWIR light photodetectors.

关键词： photodetection phototransistor organic semiconductor heterojunction non-fullerene acceptor

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Boosting High-Voltage Dynamics Towards High-Energy-Density Lithium-Ion Capacitors

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Energy & Environmental materials 2023年第4期6卷 211-217页

作者： Junfeng Huang Xin Lu Teng Sun Daiyao Yu Zhong Xu Yanting Xie Xinglin Jiang Yongbin Wang Shenglong Wang Xiong Zhang Weiqing Yang Haitao Zhang Key Laboratory of Advanced Technologies of Materials Ministry of EducationSchool of Materials Science and EngineeringSouthwest Jiaotong UniversityChengdu 610031China Institute of Electrical Engineering Chinese Academy of SciencesBeijing 100190China

Lithium-ion capacitors(LICs)are becoming important electrochemical energy storage systems due to their great potential to bridge the gap between supercapacitors and lithium-ion ***,capacity lopsidedness and low output voltage greatly hinder the realization of high-energy-density ***,a strategy of balancing capacity towards fastest dynamics is proposed to enable high-voltage *** electrochemical prelithiation of Nb_(2)C to be 1.1 V with 165 mAh g^(-1),Nb_(2)C//LiFePO_(4) LICs show a broadened potential window from 3.0 to 4.2 V and an according high energy density of 420 Wh kg^(-1).Moreover,the underlying mechanism between prelithiation and high voltage is disclosed by electrochemical dynamic *** declines the Nb_(2)C anode potential that facilitates electron transmission in the interlayer of two-dimensional Nb_(2)C *** effect induces small drive force for Li^(+)ions deposition and hence weakens the repulsive force from adsorbed ions on the electrode *** from even more Li^(+)ions deposition,a higher voltage is eventually *** addition,prelithiation significantly increases Coulomb efficiency of the 1st cycle from 74%to 90%,which is crucial to commercial application of LICs.

关键词： electrochemical dynamics high voltage lithium-ion capacitors Nb2C MXene prelithiation

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Analytic continuation in the coupling constant for resonances in_(∧)^(9)Be

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Chinese Physics C 2025年第1期49卷 269-280页

作者： Hantao Zhang Dong Bai Zhongzhou Ren School of Physics Science and Engineering Tongji UniversityShanghai 200092China College of Mechanics and Engineering Science Hohai UniversityNanjing 211100China Key Laboratory of Advanced Micro-Structure Materials Ministry of EducationShanghai 200092China

The application scope of the analytic continuation in the coupling constant(ACCC)can be extended to the exchange parameters of the effective nucleon-nucleon interaction in the microscopic cluster *** on such an exchange parameter dependent ACCC(abbreviated as EPD-ACCC),we examine the_(∧)^(9)Be system in the framework of theα+Q+∧microscopic cluster *** particle emission from excited states ofα+α+∧are investigated,and the corresponding resonant energies are obtained via ***,the complex scaling method(CSM)is applied for comparison.A good agreement between these two theoretical approaches is *** study demonstrates EPD-ACCC to be a reliable method for estimating multi-cluster resonances in light hypernuclei.

关键词： hypernuclear microscopic cluster model resonance

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Grain growth behavior and properties of high-entropy pseudobrookite(Mg,Co,Ni,Zn)Ti_(2)O_(5) ceramics

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Journal of advanced Ceramics 2024年第6期13卷 757-768页

作者： Xiaohui Ma Jinyu Wu Lingyi Meng Jinfeng Zhang Heng Chen Liwen Yan Anran Guo Jiachen Liu Key Laboratory of Advanced Ceramics and Machining Technology of Ministry of Education School of Materials Science and EngineeringTianjin UniversityTianjin 300072China Xiamen Key Laboratory of Rare Earth Photoelectric Functional Materials Xiamen Institute of Rare Earth MaterialsHaixi InstitutesChinese Academy of SciencesXiamen 361021China

It is well known that the grain size of high-entropy ceramics is quite small owing to the sluggish diffusion effect. However, abnormal grain growth often occurs in high-entropy pseudobrookite ceramics, ultimately resulting in the formation of many abnormally grown grains with a grain size as large as 50 μm. To study this phenomenon, the grain growth behavior of high-entropy pseudobrookite ceramics was systematically investigated in this paper. The results demonstrate that the starting material powders first react with each other to form a high-entropy intermediate phase and calcined TiO_(2) powders (TiO_(2)-1100 ℃), and then as the sintering temperature increases, the formed high-entropy intermediate phase further reacts with TiO_(2)-1100 ℃ to form high-entropy pseudobrookite ceramics. Thus, in this system, in addition to the sluggish diffusion effect, the grain sizes of the high-entropy intermediate phase and TiO_(2)-1100 ℃ also affect the morphology of high-entropy pseudobrookite. Compared to nanosized TiO_(2), micron-sized TiO_(2) has a lower sintering activity. Therefore, the high-entropy intermediate phases (Mg,Co,Ni,Zn)TiO_(3) and TiO_(2)-1100 ℃ prepared with micron-sized starting materials exhibit lower grain sizes, finally resulting in the formation of high-entropy (Mg,Co,Ni,Zn)Ti_(2)O_(5) with small grain sizes. Moreover, nano-indentation and thermal conductivity tests were carried out on high-entropy (Mg,Co,Ni,Zn)Ti_(2)O_(5) with different morphologies. The results show that the hardness of high-entropy (Mg,Co,Ni,Zn)Ti_(2)O_(5) increases from 6.05 to 9.95 GPa as the grain size increases, whereas the thermal conductivity decreases from 2.091±0.006 to 1.583±0.006 W·m^(−1)·K^(−1). All these results indicate that high-entropy (Mg,Co,Ni,Zn)Ti_(2)O_(5) with a small grain size is a potential material for thermal protection.

关键词： grain size sluggish diffusion effect two-step solid phase process high-entropy intermediate phase high-entropy pseudobrookite ceramic

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Highly dispersed atomic-level Ni active sites confined in defects for efficient electrocatalytic reduction of carbon dioxide

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Journal of Energy Chemistry 2024年第12期99卷 1-10页

作者： Wenjun Zhang Chen Zhao Yang Yang Ruotong Chen Yue Wu Jiaqi Dai Yuxing Zhang Huajie Liu Mingyang Liu College of Environmental Science and Engineering State Key Laboratory of Medicinal Chemical BiologyNankai UniversityTianjin 300350China School of Chemical Science and Engineering Key Laboratory of Advanced Civil Engineering Materials of Ministry of Education and Shanghai Research Institute for Intelligent Autonomous SystemsTongji UniversityShanghai200092China

Electrocatalytic CO_(2) reduction reaction (eCO_(2)RR) presents a promising approach for harnessing renewable energy and converting greenhouse gas (CO_(2)) into high value-added CO products.N-doped single atom (SA) and atomic-level metal nanocluster (MN) tandem catalysts with rich defects for eCO_(2)RR are reported,which achieved a maximum CO Faraday efficiency (FE_(CO)) of 97.7%(-0.7 V ***) in the H-type cell and maintained over 95% FE_(CO)at potentials from -0.18 to -0.73 V *** in the flow ***,the catalyst in the flow cell demonstrated a remarkably low onset potential of-0.14 V *** and the current density was approximately three times that of the H-type ***,XPS analysis indicates that carbon substrates containing defects have more pyridine-N *** calculations and in-situ attenuated total reflection Fourier transform infrared support this finding by showing that the Ni-(N-C_(2))_(3) active sites with defect favors preferentially convert CO_(2)-to-CO.

关键词： Electrocatalytic CO_(2)RR Atomic-level nanoclusters Defects Catalytic mechanism

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A CuO/TiO_(2)Heterojunction Based CO Sensor with High Response and Selectivity

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Energy & Environmental materials 2023年第3期6卷 409-416页

作者： Wei Wei Huanhuan Zhang Tiyue Tao Xiaohong Xia Yuwen Bao Manon Lourenco Kevin Homewood Zhongbing Huang Yun Gao Ministry-of-Education Key Laboratory for the Green Preparation and Application of Functional Materials Collaborative Innovation Center for Advanced Organic Chemical Materials Co-constructed by the Province and MinistrySchool of Materials Science&EngineeringHubei UniversityWuhan 430062China

The use of heterojunctions is a promising solution to the problem of cross-sensitivity in gas *** this work,a carbon monoxide sensor based on the CuO/TiO_(2)heterojunction was designed and *** to the good adsorption properties of CuO materials to CO,and the heterojunction interface charge transfer,the CuO/TiO_(2)thin film sensor exhibits high sensitivity to CO at room *** response is as high as 10.8–200 ppm CO,about 10 times its response to H_(2).Interference from H_(2)is greatly reduced by optimizing the structure of the CuO/TiO_(2)*** reliable detection of carbon monoxide with excellent discrimination against H_(2)is of great significance for the development of CO gas sensors.

关键词： carbon monoxide cross-sensitivity gas sensor heterojunction hydrogen

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