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Work-function effect of Ti_(3)C_(2)/Fe-N-C inducing solid electrolyte interphase evolution for ultra-stable sodium storage

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Nano Research 2024年第8期17卷 7163-7173页

作者： Huicong Xia Lingxing Zan Hongliang Dong Yifan Wei Yue Yu Jinfu Shu Jia-Nan Zhang Chong-Xin Shan key laboratory of Advanced Energy Catalytic and Functional material Preparation of Zhengzhou College of Materials Science and EngineeringZhengzhou UniversityZhengzhou 450001China key laboratory of materials Physics of ministry of education School of Physics and MicroelectronicsZhengzhou UniversityZhengzhou 450001China key laboratory of Chemical Reaction Engineering of Shaanxi Province College of Chemistry and Chemical EngineeringYan’an UniversityYan’an 716000China Center for High Pressure Science and technology Advanced Research PudongShanghai 201203China key laboratory of Advanced Energy materials Chemistry(ministry of education) Nankai UniversityTianjin 300071China

In the quest to enhance the efficiency of sodium-ion batteries,the dynamics of solid electrolyte interphase(SEI)formation are of paramount *** SEI layer’s integrity is integral to the charge–discharge efficiency and the overall longevity of the ***,a novel two-dimensional Ti_(3)C_(2) fragments enmeshed on iron-nitrogen-carbon(Fe-N-C)nanosheets(Ti_(3)C_(2)/Fe-NC)has been *** electrode features a matrix which has been shown to expedite SEI layer formation through the facilitation of selective anion adsorption,thus augmenting battery *** functional theory calculation reveals that the SEI evolution energy of NaPF6 at the Ti_(3)C_(2)/Fe-N-C interface is 0.81 eV,significantly lower than the Ti_(3)C_(2)(1.23 eV).This process is driven by the electron transportation from Ti_(3)C_(2) to Fe-N-C substrate,facilitated by their work-function difference,leading to the formation of ferromagnetic Fe species,which possesses Fe 3d d_(xz)d_(z)2 orbitals and undergoes hybridization with theπandσorbitals of NaF,creating a key intermediate during *** process diminishes the antibonding energy and attenuates the orbital interaction with NaF,thus reducing the activation energy and improving the SEI formation reaction ***,it leads to the creation of multi-interface SEI characterized by high-throughput ion transport and an efficient reaction network.

关键词： Ti_(3)C_(2)/Fe-N-C heterostructure work-function electron interaction solid electrolyte interphase sodium storage

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Peracetic acid catalytic activation using Co3O4 nanocluster decorated graphitic carbon nitride for cefapirin degradation in water

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Science China Technological Sciences 2024年第10期67卷 3103-3115页

作者： YIN ShiMei GAO YiXuan CHEN Long LI Fan LIU XiaoNa QI Fei LIU Wen Beijing key Lab for Source Control technology of Water Pollution College of Environmental Science and EngineeringBeijing Forestry University key laboratory of Water and Sediment Sciences (ministry of education) College of Environmental Sciences and EngineeringPeking University School of Environmental Science and Engineering Taiyuan University of Technology State Environmental Protection key laboratory of All material Fluxes in River Ecosystems Peking University Beijing National laboratory for Molecular Sciences Peking University

This study innovated cobalt-based catalytic nanocomposites（CCNs） for the heterogeneous activation of peracetic acid（PAA）,a green and efficient advanced oxidation process for removing antibiotics from *** Co3O4catalysts exhibit limited activity due to stable electronic *** overcome this,CCNs were synthesized using a one-step condensation method,incorporating a size control strategy that anchors Co3O4nanoclusters within 4-5 nm onto six-fold cavity of g-C3N4,simultaneously modifying the coordination environment of *** alteration significantly enhances the adsorption energy of PAA and catalytic activity compared to commercial *** improved performance of CCN2,in particular,is attributed to a shift in the cobalt d band center towards the Fermi level,facilitating electron delocalization and transfer,enhancing Co-O bonding,and accelerating PAA ***2's superior activity,with a cefapirin（CFP） degradation kinetic rate constant(k1=0.760 min-1)～11 times that of PAA direct oxidation(k1=0.070 min-1) and～5 times that of commercial Co3O4/PAA system(k1=0.164 min-1),is due to its ability to generate dominant reactive species for antibiotic degradation,including alkoxy radicals(CH3C（=O）OO·),high valence metal(CoⅣ（=O）2+),and singlet oxygen（1O2）,with the latter two being crucial for the degradation *** degradation of CFP involved three mechanisms,including direct oxidation by PAA,decarboxylation,and open-ring reactions at nitrogen *** research provides insights into developing high-activity catalysts for efficient PAA activation and antibiotic removal,leveraging the strategy of shifting the transition metal d band center.

关键词： peracetic acid Co3O4 nanocluster high valence metal singlet oxygen cefapirin

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Solvothermal synthesis and adsorption performance of layered boehmite using aluminum chloride and high-alumina fly ash

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Chinese Journal of Chemical Engineering 2024年第6期70卷 280-290页

作者： Jing Wen Ruirui Yuan Tao Jiang Tangxia Yu Yufan Zhang School of Metallurgy Northeastern UniversityShenyang 110819China key laboratory for Ecological Metallurgy of Multimetallic Mineral(ministry of education) Northeastern UniversityShenyang 110819China Liaoning key laboratory for Metallurgical Sensor and technology Shenyang 110819China

High alumina fly ash(FAHAl)is a kind of bulk solid waste unique to China,whose availability of high-value aluminum and the threat to the environment makes its high-value utilization *** this work,the alumina containing leaching solution obtained from Na_(2)CO_(3) roasting and HCl leaching of FAHAl was used as the mother liquor to prepare layered boehmite in *** preparation process with AlCl_(3) as the raw material was also *** formation process and mechanism of boehmite,the choice of solvent,along with the adsorption capability of Congo red were analyzed by X-ray diffraction,scanning electron microscopy,Fourier transform infrared spectroscopy,Brunauer-Emmett-Teller method and adsorption *** showed that during the preparation of layered boehmite,the precursor Al(OH)_(3) from the reaction of Al^(3+) and OH-is transformed into boehmiteγ-*** existence of ethanol is beneficial to regulate and promote the growth of boehmite crystal *** water and ethanol are mixed with a volume ratio of 2:1 and used as the solvent,the maximum specific surface area of the boehmite is obtained at 135.7 m^(2)·g^(-1),and 99.16%of Congo red can be absorbed after 10 min when AlCl3 is used as a raw *** purified leaching solution is used as the mother liquid,the crystallinity of boehmite decreases slightly when the pH value decreases from 12.5 to *** pH is 11,the removal efficiency of Congo red reaches a maximum of 72.25%.This process not only achieves the extraction of aluminum and high-value utilization of FAHAl but also provides a thought to prepare layered boehmite with adsorption properties.

关键词： High-alumina fly ash Layered boehmite In-situ preparation Solvothermal synthesis Adsorption High-value utilization

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Enhanced thermoelectric performance enabled by compositing ZrO_(2)in n-type SiGe alloy with low thermal conductivity

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Rare Metals 2024年第3期43卷 1167-1176页

作者： Meng-Fei Wang Hua-Jun Lai Ji-Sheng Liang Jun-Liang Chen Wang-Yang Ding Qi Zhou Ying Peng Cheng-Yan Liu Lei Miao Guangxi key laboratory for Relativity Astrophysics State Key Laboratory of Featured Metal Materials and Life-Cycle Safety for Composite StructuresSchool of Physical Science and TechnologyGuangxi UniversityNanning530004China Guangxi Academy of Sciences Nanning530007China key laboratory of Information material Engineering Research Center of Electronic Information Materials and DevicesGuilin University of Electronic TechnologyMinistry of EducationGuilin541004China Guangxi key laboratory of Precision Navigation technology and Application School of Information and CommunicationGuilin University of Electronic TechnologyGuilin541004China

SiGe-based thermoelectric(TE)materials have gained increasing interests due to their low maintenance costs,environmental friendliness and long ***,the intrinsically high thermal conductivity of Si-based materials also results in poor TE *** this investigation,a zirconia(ZrO_(2))composite strategy was applied to an n-type SiGe alloy,tremendously elevating its TE *** mechanical alloying and spark plasma sintering(SPS)processes,the ZrO_(2)induced the formation of nanopores in the SiGe matrix via phosphorus ***,such increase in porosity enhanced the phonon scattering and dramatically suppressed lattice thermal conductivity,from 2.83 to 1.59 W·m^(-1)·K^(-1)at 873 ***,reduced phosphorus doping led to an increase in Seebeck coefficients and a relatively minor decrease in electrical conductivity,The power factor didn't deteriorate significantly,either,as its maximum of~3.43 mW·m^(-1-)K^(-2)was achieved at 873 K with(Si_(0.8)Ge_(0.2))_(0.097)P_(0.03)(ZrO_(2))_(0.003).In short,a peak figure of merit(ZT)of~1.27 at 873 K and an average ZT~0.7 from 323 to 873 K were *** study demonstrates that the electrical and thermal transportation of SiGe material can be synergistically tuned by compositing ZrO_(2),illustrating a novel strategy to optimize the TE properties of bulk materials.

关键词： Thermoelectric SiGe alloy ZrO2 composting P element adsorption nanopores

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Inhibiting shuttle effect of lithium polysulfides by double metal selenides for high-performance lithium-sulfur batteries

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Rare Metals 2024年第6期43卷 2546-2559页

作者： Lei Li Xue-Jing Yang Yi-Yang Li Bo Jin Hui Liu Meng-Yang Cui Dong-Bo Guan Xing-You Lang Qing Jiang key laboratory of Automobile materials Ministry of Educationand College of Materials Science and EngineeringJilin UniversityChangchun 130022China

Lithium-sulfur batteries(LSBs)have attracted the attention of more and more researchers due to the advantages of high energy density,environmental friendliness,and low production ***,the low electronic conductivity of active material and shuttling effect of lithium polysulfides(LiPSs)limit the commercial development of *** solve these problems,we design a core-shell composite with nitrogen-doped carbon(NC)and two types of selenides(FeSe_(2)-NC@ZnSe-NC).The FeSe_(2)-NC@ZnSe-NC has a strong adsorption capacity,and can effectively adsorb *** the same time,it also effectively alleviates the shuttling effect of LiPSs,and improves the utilization of the active substance during the charge/discharge reaction *** mechanism involved in FeSe_(2)-NC@ZnSe-NC is demonstrated by both experiments and density-functional theory(DFT)*** electrochemical test results indicate that LSB with S/FeSe_(2)-NC@ZnSe-NC delivers an initial discharge capacity of 1260 mAh·g^(-1)at *** after 500 cycles at 1C,the capacity decay rate per cycle is 0.031%,and the capacity retention rate is 85%.The FeSe_(2)-NC@ZnSe-NC core-shell structure verifies a rational strategy to construct an electrode material for high-performance LSBs.

关键词： Lithium-sulfur batteries Shuttling effect Metal selenide Nitrogen-doped carbon Lithium polysulfides

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Electrosynthesis of H_(2)O_(2)via two-electron oxygen reduction over carbon-based catalysts:From microenvironment control to electrode/reactor design

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Energy Reviews 2024年第2期3卷 117-135页

作者： Jingjing Jia Zhenxin Li Yunrui Tian Xia Li Rui Chen Jiachen Liu Ji Liang key laboratory of Advanced Ceramics and Machining technology Ministry of EducationSchool of Materials Science and EngineeringTianjin UniversityTianjinChina

The electrochemical production of hydrogen peroxide(H_(2)O_(2))by the two-electron oxygen reduction(2e^(-)ORR)process has the advantages of high safety,low energy consumption,and environmental *** 2e^(-)ORR,the catalyst/electrode is the key component as it strongly affects catalytic performance and *** materials have the advantages of high electronic conductivity,good structural stability,easy control of nanostructures,and low ***,it has been regarded as a promising catalyst/electrode material for the electrosynthesis of H_(2)O_(2)via 2e^(-)*** addition,studies have also considered the optimization of the liquid/gas interface by tuning the electrode surface,electrolyte pH,and reactor configurations for further improving the activity and selectivity of *** this review,we provide an in-depth discussion of the recent research on the carbon-based electrocatalysts for 2e^(-)ORR,especially in terms of microenvironment tuning,catalyst/electrode interface engineering,and reactor design for achieving stable and efficient production of H_(2)O_(2).The challenges that we are still facing and the future development prospects will then be concluded,which we believe should help the future development in this field.

关键词： Oxygen reduction Hydrogen peroxide Carbon-based catalyst Electrode surface Reactor design

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Polyolefin vitrimers bearing acetoacetate functionality

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Science China Chemistry 2024年第11期67卷 3861-3867页

作者： Zihao Wang Yue Liu Wenmin Pang Ao Chen Min Chen Chinese Academy of Sciences (CAS) key laboratory of Soft Matter Chemistry Department of Polymer Science and Engineering University of Science and Technology of China Institutes of Physical Science and Information technology Key Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of Education Anhui University

Polyolefin vitrimers are polymer networks bearing reversible covalent crosslinking points, enabling them to be reprocessed and recycled. In this contribution, a series of polyolefin vitrimers were designed based on the acetoacetate-functionalized polyolefin copolymers, which were produced through the direct copolymerization of ethylene with polar comonomers using a phosphinesulfonate palladium catalyst. The pendant acetoacetate group could mediate several characteristic reactions, such as the Michael addition reaction, ketone-amine condensation and metal coordination reaction. As such, structurally adjustable polyolefin vitrimers can be accessed by introducing various dynamic crosslinking bonds, including disulfide exchange, transamination of vinylogous urethane and labile metal coordination bond. The utilization of different crosslinking reactions and the mole ratio of crosslinkers significantly impact the material properties of the resultant polymers. Specifically, the generated polyolefin vitrimers demonstrated excellent reprocessability and closed-loop recycling properties. The study in this work provides an efficient strategy to access various polyolefin vitrimers.

关键词： polyolefin vitrimers acetoacetate group polar monomer olefin copolymerization

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Triggering triplet excitons of carbon nanodots through nanospace domain confinement for multicolor phosphorescence in aqueous solution

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Nano Research 2024年第7期17卷 6534-6543页

作者： Ya-Chuan Liang Qing Cao Yuan Deng Yong Wang Kai-Kai Liu Chong-Xin Shan School of Electronics and Information Zhengzhou University of Light IndustryZhengzhou 450002China Henan key laboratory of Diamond Optoelectronic material and Devices Key Laboratory of Material PhysicsMinistry of EducationSchool of Physics and MicroelectronicsZhengzhou UniversityZhengzhou 450001China Academy for Quantum Science and technology Zhengzhou University of Light IndustryZhengzhou 450002China Institute of Quantum materials and Physics Henan Academy of SciencesZhengzhou 450046China

Easy non-radiative decay property of long-lived triplet excitons in aqueous solution obstructs their applications in aquatic *** reported phosphorescence phenomena in aqueous solution have excited researchers enormously but achieving full-color water-soluble phosphorescent carbon nanodots(CNDs)is still a challenging ***,full-color phosphorescence of water-soluble CNDs has been demonstrated by triggering their triplet excitons through nanospace domain confinement,and Förster energy resonance transfer is used for further tuning phosphorescence *** phosphorescence spans across most of the visible spectrum,ranging from 400 to 700 *** an aqueous solution,the CNDs exhibits blue,green,and red phosphorescence,lasting for approximately 6,10,and 7 s,***,the phosphorescence quantum yields are 11.85%,8.6%and 3.56%,making them readily discernible to the naked eyes and laying a solid foundation for practical ***,phosphorescence flexible optical display and bioimaging have been demonstrated by using the multicolor CNDs-based nanomaterials,showing distinct superiority for accuracy and complete display and imaging in complex emission background.

关键词： carbon nanodots triplet excitons multicolor aqueous solution

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Preparation of calcium carbonate with microstructure and nanostructure from carbide slag for CO_(2) sequestration by using recyclable ammonium chloride

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Particuology 2024年第7期90卷 1-9页

作者： Jin Yao Qiuju Chen Li Zeng Wenjin Ding key laboratory of ministry of education for Solid Waste Treatment and Resource Recycle Southwest University of Science and TechnologyMianyang621010China Sichuan Engineering Lab of Non-metallic Mineral Powder modification and High-value Utilization Mianyang621010China School of Architecture and Civil Engineering Chengdu UniversityChengdu610106China

Based on the composition characteristics of carbide slag and the application of polyvinyl chloride,a method of preparing calcium carbonate with microstructure and nanostructure by using carbide slag as a raw material and ammonium chloride as a leaching agent was *** factors for the preparation of calcium carbonate and the effects of different conditions on the crystal phase,grain size,and morphology of calcium carbonate were systematically *** results showed that the nanosized calcium carbonate was prepared at 60 mL/min,25°C,no additional ammonia,and 60 *** product of spherical vaterite was in accordance with the relevant standards for the industrial precipitation of calcium ***,the reuse of carbonation filtrate was *** crystal phase,grain size,and morphology of the carbonation product could be controlled by adjusting the reaction *** manuscript provided a new idea for resource utilization of carbide slag and preparing nanocalcium carbonate.

关键词： Carbide slag Ammonium chloride Cyclic utilization Micro and nano structure Product control

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Exploring the Core-shell Structure of BaTiO3-based Dielectric Ceramics Using Machine Learning Models and Interpretability Analysis

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Journal of Wuhan University of technology(materials Science) 2024年第3期39卷 561-569页

作者：孙家乐 XIONG Peifeng 郝华 LIU Hanxing State key laboratory of Advanced technology for materials Synthesis and Processing School of Material Science and EngineeringInternational School of Material Science and EngineeringWuhan University of TechnologyWuhan 430070China Sanya Science and education Innovation Park Wuhan University of TechnologySanya 572000China Foshan Xianhu laboratory of the Advanced Energy Science and technology Guangdong laboratory Xianhu Hydrogen ValleyFoshan 528200China

A machine learning(ML)-based random forest(RF)classification model algorithm was employed to investigate the main factors affecting the formation of the core-shell structure of BaTiO_(3)-based ceramics and their interpretability was analyzed by using Shapley additive explanations(SHAP).An F1-score changed from 0.8795 to 0.9310,accuracy from 0.8450 to 0.9070,precision from 0.8714 to 0.9000,recall from 0.8929 to 0.9643,and ROC/AUC value of 0.97±0.03 was achieved by the RF classification with the optimal set of features containing only 5 features,demonstrating the high accuracy of our model and its high *** the interpretability analysis of the model,it was found that the electronegativity,melting point,and sintering temperature of the dopant contribute highly to the formation of the core-shell structure,and based on these characteristics,specific ranges were delineated and twelve elements were finally obtained that met all the requirements,namely Si,Sc,Mn,Fe,Co,Ni,Pd,Er,Tm,Lu,Pa,and *** the process of exploring the structure of the core-shell,the doping elements can be effectively localized to be selected by choosing the range of features.

关键词： machine learning BaTiO_(3) core-shell structure random forest classifier

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