In this article the affiliation of Jin-Ke Shen,Nai-Teng Wu,Li-Yuan Wang,Gang Jiang,Jin Li,Gui-Long Liu,Xian-Ming Liu were incorrectly given as:State Key Laboratory of Chemistry and Utilization of Carbon Based Energy R...In this article the affiliation of Jin-Ke Shen,Nai-Teng Wu,Li-Yuan Wang,Gang Jiang,Jin Li,Gui-Long Liu,Xian-Ming Liu were incorrectly given as:State Key Laboratory of Chemistry and Utilization of Carbon Based Energy Resources,School of Chemical Engineering and Technology,Xinjiang University,Urumqi 830046,China.展开更多
For the efficient electrolytic extraction of Er from spent nuclear fuel,a series of electrochemical methods was used to research the electrochemical behavior of Er(Ⅲ)in the LiCl—KCl system on inert(Mo)electrode and ...For the efficient electrolytic extraction of Er from spent nuclear fuel,a series of electrochemical methods was used to research the electrochemical behavior of Er(Ⅲ)in the LiCl—KCl system on inert(Mo)electrode and on reactive(Ni)electrodes.On the inert Mo electrode,the reduction of Er(Ⅲ)to Er(0)is a onestep with three-electron and quasi-reversible reaction process.Meanwhile,the apparent generation Gibbs free energy and activity coefficients of Er(Ⅲ)on the inert electrode were determined.Thereafter,the electrochemical reduction of Er(Ⅲ)on the Ni electrode was emphatically investigated.Er(Ⅲ)is reduced at a corrected potential owing to the formation of Ni-Er alloys.In addition,thermodynamic parameters such as partial excess Gibbs free energy change of Er in Ni,activity and apparent generation Gibbs free energy of the Ni-Er alloys were determined by the electromotive force method.Finally,different Ni-Er alloys were produced using potentiostatic electrolysis on the Ni cathode by controlling different potentials,Moreover,electrolytic extraction was carried out on the Ni cathode at the potential of-2.0 V,and the separation efficiency of Er reaches 99.72%,which proves the practicability of separating Er from LiCl-KCl eutectic on the reactive Ni cathode.展开更多
All-solid-state lithium batteries(ASSLBs)are strongly considered as the next-generation energy storage devices for their high energy density and intrinsic safety.The solid-solid contact between lithium metal and solid...All-solid-state lithium batteries(ASSLBs)are strongly considered as the next-generation energy storage devices for their high energy density and intrinsic safety.The solid-solid contact between lithium metal and solid electrolyte plays a vital role in the performance of working ASSLBs,which is challenging to investigate quantitatively by experimental approach.This work proposed a quantitative model based on the finite element method for electrochemical impedance spectroscopy simulation of different solid-solid contact states in ASSLBs.With the assistance of an equivalent circuit model and distribution of relaxation times,it is discovered that as the number of voids and the sharpness of cracks increase,the contact resistance Rcgrows and ultimately dominates the battery impedance.Through accurate fitting,inverse proportional relations between contact resistance Rcand(1-porosity)as well as crack angle was disclosed.This contribution affords a fresh insight into clarifying solid-solid contact states in ASSLBs.展开更多
The growing demands for energy storage systems,electric vehicles,and portable electronics have significantly pushed forward the need for safe and reliable lithium batteries.It is essential to design functional separat...The growing demands for energy storage systems,electric vehicles,and portable electronics have significantly pushed forward the need for safe and reliable lithium batteries.It is essential to design functional separators with improved mechanical and electrochemical characteristics.This review covers the improved mechanical and electrochemical performances as well as the advancements made in the design of separators utilizing a variety of techniques.In terms of electrolyte wettability and adhesion of the coating materials,we provide an overview of the current status of research on coated separators,in situ modified separators,and grafting modified separators,and elaborate additional performance parameters of interest.The characteristics of inorganics coated separators,organic framework coated separators and inorganic-organic coated separators from different fabrication methods are compared.Future directions regarding new modified materials,manufacturing process,quantitative analysis of adhesion and so on are proposed toward next-generation advanced lithium batteries.展开更多
La-Mg-Ni-based hydrogen storage alloys with superlattice structures are the new generation anode material for nickel metal hydride(Ni-MH)batteries owing to the advantages of high capacity and exceptional activation pr...La-Mg-Ni-based hydrogen storage alloys with superlattice structures are the new generation anode material for nickel metal hydride(Ni-MH)batteries owing to the advantages of high capacity and exceptional activation properties.However,the cycling stability is not currently satisfactory enough which plagues its application.Herein,a strategy of partially substituting La with the Y element is proposed to boost the capacity durability of La-Mg-Ni-based alloys.Furthermore,phase structure regulation is implemented simultaneously to obtain the A5 B19-type alloy with good crystal stability specifically.It is found that Y promotes the phase formation of the Pr5 Co19-type phase after annealing at 985℃.The alloy containing Y contributes to the superior rate capability resulting from the promoted hydrogen diffusion rate.Notably,Y substitution enables strengthening the anti-pulverization ability of the alloy in terms of increasing the volume match between[A_(2)B_(4)]and[AB5]subunits,and effectively enhances the anti-corrosion ability of the alloy due to high electronegativity,realizing improved long-term cycling stability of the alloy from 74.2%to 78.5%after cycling 300 times.The work is expected to shed light on the composition and structure design of the La-Mg-Ni-based hydrogen storage alloy for Ni-MH batteries.展开更多
Under the condition of solvothermal synthesis,the viologen ligand 1,1′-bis(3-carboxyphenyl)-(4,4′-bipyri-dine)dichloride(H_(2)bcbpy·2Cl)and KI are coordinated with the metal cadmium ions.A case of thermochromic...Under the condition of solvothermal synthesis,the viologen ligand 1,1′-bis(3-carboxyphenyl)-(4,4′-bipyri-dine)dichloride(H_(2)bcbpy·2Cl)and KI are coordinated with the metal cadmium ions.A case of thermochromic coor-dination polymer[Cd(bcbpy)I_(2)]·2H_(2)O(1)was constructed.Complex 1 displays a 1D chain structure and exhibits thermochromic behavior.Under different temperature stimulation,the complex(ground)slowly changed from green to yellow-green,and with the increase of temperature,the color of complex 1 gradually deepened,and finally became orange-yellow.Therefore,complex 1 was prepared as a thermochromic film.In addition,we also performed electrochemical tests on complex 1,which showed that the complex is a semiconductor material.CCDC:2391802.展开更多
A cobalt-based metal-organic framework[Co_(3)(L)_(2)(1,4-bib)_(4)]·4H_(2)O(Co-MOF)was prepared using 5-[(4-carboxyphenoxy)methyl]isophthalic acid(H_(3)L)and 1,4-bis(1H-imidazol-1-yl)benzene(1,4-bib)as ligands.The...A cobalt-based metal-organic framework[Co_(3)(L)_(2)(1,4-bib)_(4)]·4H_(2)O(Co-MOF)was prepared using 5-[(4-carboxyphenoxy)methyl]isophthalic acid(H_(3)L)and 1,4-bis(1H-imidazol-1-yl)benzene(1,4-bib)as ligands.Then,an electrochemical sensor modified with Co-MOF on a glassy carbon electrode(Co-MOF@GCE)was constructed for detecting Cd^(2+)and Pb^(2+)in aqueous solutions.The sensor exhibited a linear range of 1.0-16.0µmol·L^(-1)with a detection limit(LOD)of 4.609 nmol·L^(-1)for Cd^(2+),and 0.5-10.0µmol·L^(-1)with an LOD of 1.307 nmol·L^(-1)for Pb^(2+).Simultaneous detection of both ions within 0.5-7.0µmol·L^(-1)achieved LOD values of 0.47 nmol·L^(-1)(Cd^(2+))and 0.008 nmol·L^(-1)(Pb^(2+)),respectively.Analysis of real water samples(tap water,mineral water,and river water)yielded recoveries of 95%-105%,validating practical applicability.Density functional theory(DFT)calculations reveal that synergistic interactions between cobalt centers and N/O atoms enhance adsorption and electron-transfer efficiency.CCDC:2160744.展开更多
Biomass-derived heteroatom self-doped cathode catalysts has attracted considerable interest for electrochemical advanced oxidation processes(EAOPs)due to its high performance and sustainable synthesis.Herein,we illust...Biomass-derived heteroatom self-doped cathode catalysts has attracted considerable interest for electrochemical advanced oxidation processes(EAOPs)due to its high performance and sustainable synthesis.Herein,we illustrated the morphological fates of waste leaf-derived graphitic carbon(WLGC)produced from waste ginkgo leaves via pyrolysis temperature regulation and used as bifunctional cathode catalyst for simultaneous H_(2)O_(2) electrochemical generation and organic pollutant degradation,discovering S/N-self-doping shown to facilitate a synergistic effect on reactive oxygen species(ROS)generation.Under the optimum temperature of 800℃,the WLGC exhibited a H_(2)O_(2) selectivity of 94.2%and tetracycline removal of 99.3%within 60 min.Density functional theory calculations and in-situ Fourier transformed infrared spectroscopy verified that graphitic N was the critical site for H_(2)O_(2) generation.While pyridinic N and thiophene S were the main active sites responsible for OH generation,N vacancies were the active sites to produce ^(1)O_(2) from O_(2).The performance of the novel cathode for tetracycline degradation remains well under a wide pH range(3–11),maintaining excellent stability in 10 cycles.It is also industrially applicable,achieving satisfactory performance treating in real water matrices.This system facilitates both radical and non-radical degradation,offering valuable advances in the preparation of cost-effective and sustainable electrocatalysts and hold strong potentials in metal-free EAOPs for organic pollutant degradation.展开更多
Pitch is a complex mixture of polycyclic aromatic hydrocarbons and their non-metal derivatives that has a high carbon content.Using pitch as a precursor for carbon materials in alkali metal ion(Li^(+)/Na^(+)/K^(+))bat...Pitch is a complex mixture of polycyclic aromatic hydrocarbons and their non-metal derivatives that has a high carbon content.Using pitch as a precursor for carbon materials in alkali metal ion(Li^(+)/Na^(+)/K^(+))batteries has become of great interest.However,its direct pyrolysis often leads to microstructures with a high orientation and small interlayer spacing due to uncontrolled liquid-phase carbonization,resulting in subpar electrochemical performance.It is therefore important to control the microstructures of pitch-derived carbon materials in order to improve their electrochemical properties.We evaluate the latest progress in the development of these materials using various microstructural engineering approaches,highlighting their use in metal-ion batteries and supercapacitors.The advantages and limitations of pitch molecules and their carbon derivatives are outlined,together with strategies for their modification in order to improve their properties for specific applications.Future research possibilities for structure optimization,scalable production,and waste pitch recycling are also considered.展开更多
With the acceleration of advanced industrialization and urbanization,the environment is deteriorating rapidly,and non-renewable energy resources are depleted.The gradual advent of potential clean energy storage techno...With the acceleration of advanced industrialization and urbanization,the environment is deteriorating rapidly,and non-renewable energy resources are depleted.The gradual advent of potential clean energy storage technologies is particularly urgent.Electrochemical energy storage technologies have been widely used in multiple fields,especially supercapacitors and rechargeable batteries,as vital elements of storing renewable energy.In recent years,two-dimensional material MXene has shown great potential in energy and multiple application fields thanks to its excellent electrical properties,large specific surface area,and tunability.Based on the layered materials of MXene,researchers have successfully achieved the dual functions of energy storage and conversion by adjusting the surface terminals at the Fermi level.It is worth noting that compared with other two-dimensional materials,MXene has more active sites on the basal plane,showing excellent catalytic performance.In contrast,other two-dimensional materials have catalytic activity only at the edge sites.This article comprehensively overviews the synthesis process,structural characteristics,modification methods for MXene-based polymer materials,and their applications in electrochemical energy storage.It also briefly discusses the potential of MXene-polymer materials in electromagnetic shielding technology and sensors and looks forward to future research directions.展开更多
In response to the increasing demand of ethylene,electrochemical ethane nonoxidative dehydrogenation(EENDH)to ethylene by protonic ceramic electrolysis cells(PCECs)is developed.However,existing anode materials exhibit...In response to the increasing demand of ethylene,electrochemical ethane nonoxidative dehydrogenation(EENDH)to ethylene by protonic ceramic electrolysis cells(PCECs)is developed.However,existing anode materials exhibit poor proton conductivity and limited catalytic activity.Herein,a novel Sr_(1.95)Fe_(1.4)Co_(0.1)Mo_(0.4)Zr_(0.1)O_(6-δ)(SFCMZ)anode is prepared as PCECs anode for EENDH.Zr doping increases the oxygen vacancies and enhances the proton conductivity of SFCMZ.Moreover,an alloy-oxide heterostructure(Co Fe@SFCMZ)is formed through in-situ exsolution of Co Fe alloy nanoparticles under reduction conditions,generating abundant oxygen vacancies and improving its catalytic activity.Co Fe@SFCMZ cell achieves an electrolysis current density of 0.87 A/cm^(2) at 700℃ under 1.6 V,with an ethane conversion rate of 34.22%and corresponding ethylene selectivity of 93.4%.These results demonstrate that Co Fe@SFCMZ anode exhibits excellent electrocatalytic activity,suggesting promising applications for EENDH.展开更多
In the context of modern holistic education,integrating“ideological and political education”into specialized courses is a new requirement for professional teaching.In order to seamlessly integrate ideological educat...In the context of modern holistic education,integrating“ideological and political education”into specialized courses is a new requirement for professional teaching.In order to seamlessly integrate ideological education into academic disciplines through subtle influence,it is essential to identify and design suitable ideological elements.Based on the interdisciplinary nature of chemical engineering curricula,this paper focuses on core socialist values,patriotic sentiment,professional ethics,and the spirit of scientific innovation.It identifies key ideological elements such as“a strong chemical industry makes a strong nation”and“patriotism and maritime power,”analyzes their manifestations of value,and explores their relevance and significance in ideological education across different chemical engineering courses.展开更多
Integrating the CO_(2)capture process with the CO_(2)electrochemical reduction process into a single system can eliminate the need for storage and transportation following CO_(2)capture.This integrated process offers ...Integrating the CO_(2)capture process with the CO_(2)electrochemical reduction process into a single system can eliminate the need for storage and transportation following CO_(2)capture.This integrated process offers several advantages over multi-step cascade processes,including reduced costs and enhanced CO_(2)utilization.However,the integrated CO_(2)capture and electrochemical reduction(CCER)process encounters several challenges,including the low CO_(2)adsorption performance of the gas diffusion electrode(GDE)and catalyst,as well as the poor activity and selectivity of the catalyst for the electrochemical reduction of CO_(2).This review aims to systematically summarize the fundamentals of the CCER process.Based on an in-depth understanding of the CO_(2)mass transfer,adsorption,and electrochemical reduction processes,GDE design strategies based on the modulation of wettability and structure are discussed to enhance the CO_(2)capture capability at the GDE level.At the catalyst level,catalyst design strategies based on the introduction of CO_(2)capture sites and the construction of CO_(2)mass transfer channels were analyzed,and catalyst design strategies for enhanced CO_(2)capture were proposed.This review summarizes the most common catalysts for CO_(2)electrochemical reduction,such as Ni-based,Bi-based,and Cubased catalysts,and analyzes their design strategies based on reaction pathways for generating specific products.Finally,the problems and challenges of the CCER process are summarized and proposed,which provide ideas for the further application of this technology in the future.展开更多
Engineering of sulfur vacancies on the basal plane of molybdenum disulfide(MoS_(2))may provide effective way to promote the catalytic activity.Although the sulfur vacancy density has previously been correlated with ca...Engineering of sulfur vacancies on the basal plane of molybdenum disulfide(MoS_(2))may provide effective way to promote the catalytic activity.Although the sulfur vacancy density has previously been correlated with catalytic activity,direct evidence that vacancies create surfaces with enhanced electrocatalytic activity is still lacking.Here,we used a combination of scanning electrochemical cell microscopy(SECCM)with submicrometer resolution and photoluminescence imaging to show that sulfur vacancies in monolayer MoS_(2)microflakes lead to significant spatial heterogeneity in the electrochemical hydrogen evolution reaction(HER)activity.Specifically,colocated multi-microscopy unveils that regions with superior HER activity are associated with sulfur vacancy defects.As the vacancy density increases,the triangular flakes display significantly enhanced and spatially uniformly distributed electrocatalytic activity.Our multi-microscopic imaging approach using SECCM convincingly highlights the spatial heterogeneity of electrocatalytic activity across monolayer MoS_(2)by sulfur vacancy engineering.展开更多
Single-atom Fe catalysts show significant promise in the electrocatalytic reduction of CO_(2)(CO_(2)RR),while their performance remains inferior to that of precious metal catalysts due to the overly strong binding of^...Single-atom Fe catalysts show significant promise in the electrocatalytic reduction of CO_(2)(CO_(2)RR),while their performance remains inferior to that of precious metal catalysts due to the overly strong binding of^(*)CO intermediates.Although the introduction of heteroatoms or transition metal sites can modulate the binding strength of^(*)CO on Fe sites,these regulators often induce competitive hydrogen evolution reaction(HER)with reduced Faraday efficiency(FE).In this work,we employ HER-inert Sn as a regulator to tune the electronic structure of Fe,weakening^(*)CO adsorption and enhancing CO_(2)RR performance.Diatomic Fe-Sn pairs supported on N-doped carbon(Fe-Sn/NC)were synthesized,achieving FE for CO exceeding 90%over a broad potential range from−0.4 to−0.9 V versus the reversible hydrogen electrode.Fe-Sn/NC shows a high turnover frequency of 1.5×10^(4)h^(-1),much higher than that of Fe/NC.Characterization results and theoretical calculations demonstrate that bonding Sn site to Fe generates electron-rich Fe centers,effectively reducing the adsorption strength of^(*)CO without triggering HER.Additionally,Fe-Sn/NC exhibits exceptional activity in hydrazine oxidation performance(HzOR).The HzOR-assisted CO_(2)RR system using Fe-Sn/NC as electrodes reduces energy consumption by 38%compared with the conventional CO_(2)RR coupled oxygen evolution reaction system.展开更多
This study innovatively proposes a“chemical prelithiation/alloying-induced interfacial reconstruction”synergistic strategy that fundamentally improves the performance of Si-based anodes.Through a precisely controlle...This study innovatively proposes a“chemical prelithiation/alloying-induced interfacial reconstruction”synergistic strategy that fundamentally improves the performance of Si-based anodes.Through a precisely controlled process leveraging orbital energetics and Lewis acid catalysis,we successfully engineer a Li-Al-F phase on the interface of SiO(denoted as Pre-SiO-Al)anodes via sequential chemical prelithiation and AlF_(3)-driven interfacial alloying reactions.This novel approach breaks through the ion transport limitations of traditional LiF-dominated solid electrolyte interphase(SEI)layers,while concurrently addressing the critical challenges of low initial Coulombic efficiency(ICE)and severe volume expansion.Mechanism studies reveal that the Li-Al-F offers an ultralow Li^(+)diffusion barrier(0.1 eV),significantly enhancing interfacial ion transport kinetics.Meanwhile,the high mechanical strength and dynamic stress dissipation capability of LiAl-F effectively suppress SEI fracture caused by volume expansion,enabling coordinated deformation compatibility between the electrode and the interfacial layer.The Pre-SiO-Al anode maintains a high capacity of 682.6 m A h g^(-1)after 2000 cycles at 1.0 A g^(-1)with near 100% capacity retention.When paired with LiFePO_(4)cathode,the Pre-SiO-Al||LFP full cell achieves impressive rate capability and cycling stability(93.8% capacity retention after 150 cycles at 0.5 C),demonstrating strong commercialization potential.展开更多
The synthesis ofα-amino acid from imines with different carbonyl sources is attractive for both synthetic organic and medicinal chemistry communities.Imines,which were easily available from the corresponding ketones ...The synthesis ofα-amino acid from imines with different carbonyl sources is attractive for both synthetic organic and medicinal chemistry communities.Imines,which were easily available from the corresponding ketones and amines,were employed as one of the most ideal precursors.Traditionally,cyanation and subsequent hydrolysis were required to install the carboxyl group^([1]).In these cases,the toxicity of the cyanation reagents limited its further synthetic applications in organic chemsitry.Besides,metal activation of imine substrates to make the organometallic intermediate and trap CO_(2) to give the desiredα-amino acid were also developed by many groups(Scheme 1A).The utilization of stoiochiometric amounts of metal reagents was required to realize the transformation.Recently,Yu reported a novel photocatalytic reductive carboxylation protocol for synthesis ofα-amino acid from imines with CO_(2)as the carbonyl source^([2]).展开更多
Electrochemical synthesis of value-added chemicals represents a promising approach to address multidisciplinary demands.This technology establishes direct pathways for electricity-to-chemical conversion while signific...Electrochemical synthesis of value-added chemicals represents a promising approach to address multidisciplinary demands.This technology establishes direct pathways for electricity-to-chemical conversion while significantly reducing the carbon footprint of chemical manufacturing.It simultaneously optimizes chemical energy storage and grid management,offering sustainable solutions for renewable energy utilization and overcoming geographical constraints in energy distribution.As a critical nexus between renewable energy and green chemistry,electrochemical synthesis serves dual roles in energy transformation and chemical production,emerging as a vital component in developing carbon-neutral circular economies.Focusing on key small molecules(H_(2)O,CO_(2),N_(2),O_(2)),this comment examines fundamental scientific challenges and practical barriers in electrocatalytic conversion processes,bridging laboratory innovations with industrial-scale implementation.展开更多
Currently,chemical furnaces play an important role in the chemical industry.It is necessary to ensure their quality and operation performance,so as to guarantee the efficiency of chemical production.Compared with othe...Currently,chemical furnaces play an important role in the chemical industry.It is necessary to ensure their quality and operation performance,so as to guarantee the efficiency of chemical production.Compared with other furnaces,chemical furnaces have strong particularity,which puts forward higher requirements for the thermal shock resistance of the refractories of furnace linings.This paper studied the thermal shock resistance of the refractories for chemical furnace linings,and proposed measures for improvement,providing experience and technical support for the safe production of chemical enterprises.展开更多
To enhance the electrochemical performance of the reversible solid oxide cell(RSOC),a facile way through adopting A-site deficient Pr_(0.94)PrBaCo_(1.5)Fe_(0.5)O_(5+δ)(PBCF94)as an air electrode for RSOC is reported....To enhance the electrochemical performance of the reversible solid oxide cell(RSOC),a facile way through adopting A-site deficient Pr_(0.94)PrBaCo_(1.5)Fe_(0.5)O_(5+δ)(PBCF94)as an air electrode for RSOC is reported.The designed A-site Pr-deficient air electrode is expected to provide abundant oxygen vacancies,macroscopic nanoparticle generation,excellent redox properties and oxygen mobility,which ultimately contribute to the enhanced electrocatalytic activity.The results confirm that the RSOC with an A-site deficient air electrode exhibits considerable peak power density up to 1.53 W·cm^(-2),and the desirable electrolysis current density reaches 2.29 A·cm^(-2)at 1.5 V and 800℃.Correspondingly,the RSOC exhibits remarkable long-term reversible stability of 200 h.Thus,the A-site deficient Pr_(0.94)PrBaCo_(1.5)Fe_(0.5)O_(5+δ)air electrode could be the potential one for RSOC application.展开更多
文摘In this article the affiliation of Jin-Ke Shen,Nai-Teng Wu,Li-Yuan Wang,Gang Jiang,Jin Li,Gui-Long Liu,Xian-Ming Liu were incorrectly given as:State Key Laboratory of Chemistry and Utilization of Carbon Based Energy Resources,School of Chemical Engineering and Technology,Xinjiang University,Urumqi 830046,China.
基金Project supported by Ph.D.Student Research and Innovation Fund of the Fundamental Research Funds for the Central Universities(3072023GIP1005)。
文摘For the efficient electrolytic extraction of Er from spent nuclear fuel,a series of electrochemical methods was used to research the electrochemical behavior of Er(Ⅲ)in the LiCl—KCl system on inert(Mo)electrode and on reactive(Ni)electrodes.On the inert Mo electrode,the reduction of Er(Ⅲ)to Er(0)is a onestep with three-electron and quasi-reversible reaction process.Meanwhile,the apparent generation Gibbs free energy and activity coefficients of Er(Ⅲ)on the inert electrode were determined.Thereafter,the electrochemical reduction of Er(Ⅲ)on the Ni electrode was emphatically investigated.Er(Ⅲ)is reduced at a corrected potential owing to the formation of Ni-Er alloys.In addition,thermodynamic parameters such as partial excess Gibbs free energy change of Er in Ni,activity and apparent generation Gibbs free energy of the Ni-Er alloys were determined by the electromotive force method.Finally,different Ni-Er alloys were produced using potentiostatic electrolysis on the Ni cathode by controlling different potentials,Moreover,electrolytic extraction was carried out on the Ni cathode at the potential of-2.0 V,and the separation efficiency of Er reaches 99.72%,which proves the practicability of separating Er from LiCl-KCl eutectic on the reactive Ni cathode.
基金supported by the Beijing Natural Science Foundation(Z200011,L233004)the National Key Research and Development Program(2021YFB2500300)+3 种基金the National Natural Science Foundation of China(52394170,52394171,22109011,22393900,and 22108151)the Tsinghua-Jiangyin Innovation Special Fund(TJISF)(2022JYTH0101)the S&T Program of Hebei(22344402D)the Tsinghua University Initiative Scientific Research Program.
文摘All-solid-state lithium batteries(ASSLBs)are strongly considered as the next-generation energy storage devices for their high energy density and intrinsic safety.The solid-solid contact between lithium metal and solid electrolyte plays a vital role in the performance of working ASSLBs,which is challenging to investigate quantitatively by experimental approach.This work proposed a quantitative model based on the finite element method for electrochemical impedance spectroscopy simulation of different solid-solid contact states in ASSLBs.With the assistance of an equivalent circuit model and distribution of relaxation times,it is discovered that as the number of voids and the sharpness of cracks increase,the contact resistance Rcgrows and ultimately dominates the battery impedance.Through accurate fitting,inverse proportional relations between contact resistance Rcand(1-porosity)as well as crack angle was disclosed.This contribution affords a fresh insight into clarifying solid-solid contact states in ASSLBs.
基金the Center of Lithium Battery Membrane Materials jointly established by School of Chemistry and Chemical Engineering of Huazhong University of Science and Technology and Shenzhen Senior Technology Material Co.Ltd.,the National Natural Science Foundation of China(52020105012,52303084)the Young Scientists Fund of Natural Science Foundation of Hubei Province(2023AFB220)for the support of this work.
文摘The growing demands for energy storage systems,electric vehicles,and portable electronics have significantly pushed forward the need for safe and reliable lithium batteries.It is essential to design functional separators with improved mechanical and electrochemical characteristics.This review covers the improved mechanical and electrochemical performances as well as the advancements made in the design of separators utilizing a variety of techniques.In terms of electrolyte wettability and adhesion of the coating materials,we provide an overview of the current status of research on coated separators,in situ modified separators,and grafting modified separators,and elaborate additional performance parameters of interest.The characteristics of inorganics coated separators,organic framework coated separators and inorganic-organic coated separators from different fabrication methods are compared.Future directions regarding new modified materials,manufacturing process,quantitative analysis of adhesion and so on are proposed toward next-generation advanced lithium batteries.
基金the financial support by the National Nat-ural Science Foundation of China(Nos.52201282,52071281,52371239)the China Postdoctoral Science Foundation(No.2023M742945)+4 种基金Hebei Provincial Postdoctoral Science Foundation(No.B2023003023)the Science Research Project of Hebei Education Department(No.BJK2022033)the Natural Science Foundation of Hebei Province(No.C2022203003)the Inner Mongolia Science and Technology Major Project(No.2020ZD0012)the Baotou Science and Technology Planning Project(No.XM2022BT09).
文摘La-Mg-Ni-based hydrogen storage alloys with superlattice structures are the new generation anode material for nickel metal hydride(Ni-MH)batteries owing to the advantages of high capacity and exceptional activation properties.However,the cycling stability is not currently satisfactory enough which plagues its application.Herein,a strategy of partially substituting La with the Y element is proposed to boost the capacity durability of La-Mg-Ni-based alloys.Furthermore,phase structure regulation is implemented simultaneously to obtain the A5 B19-type alloy with good crystal stability specifically.It is found that Y promotes the phase formation of the Pr5 Co19-type phase after annealing at 985℃.The alloy containing Y contributes to the superior rate capability resulting from the promoted hydrogen diffusion rate.Notably,Y substitution enables strengthening the anti-pulverization ability of the alloy in terms of increasing the volume match between[A_(2)B_(4)]and[AB5]subunits,and effectively enhances the anti-corrosion ability of the alloy due to high electronegativity,realizing improved long-term cycling stability of the alloy from 74.2%to 78.5%after cycling 300 times.The work is expected to shed light on the composition and structure design of the La-Mg-Ni-based hydrogen storage alloy for Ni-MH batteries.
文摘Under the condition of solvothermal synthesis,the viologen ligand 1,1′-bis(3-carboxyphenyl)-(4,4′-bipyri-dine)dichloride(H_(2)bcbpy·2Cl)and KI are coordinated with the metal cadmium ions.A case of thermochromic coor-dination polymer[Cd(bcbpy)I_(2)]·2H_(2)O(1)was constructed.Complex 1 displays a 1D chain structure and exhibits thermochromic behavior.Under different temperature stimulation,the complex(ground)slowly changed from green to yellow-green,and with the increase of temperature,the color of complex 1 gradually deepened,and finally became orange-yellow.Therefore,complex 1 was prepared as a thermochromic film.In addition,we also performed electrochemical tests on complex 1,which showed that the complex is a semiconductor material.CCDC:2391802.
文摘A cobalt-based metal-organic framework[Co_(3)(L)_(2)(1,4-bib)_(4)]·4H_(2)O(Co-MOF)was prepared using 5-[(4-carboxyphenoxy)methyl]isophthalic acid(H_(3)L)and 1,4-bis(1H-imidazol-1-yl)benzene(1,4-bib)as ligands.Then,an electrochemical sensor modified with Co-MOF on a glassy carbon electrode(Co-MOF@GCE)was constructed for detecting Cd^(2+)and Pb^(2+)in aqueous solutions.The sensor exhibited a linear range of 1.0-16.0µmol·L^(-1)with a detection limit(LOD)of 4.609 nmol·L^(-1)for Cd^(2+),and 0.5-10.0µmol·L^(-1)with an LOD of 1.307 nmol·L^(-1)for Pb^(2+).Simultaneous detection of both ions within 0.5-7.0µmol·L^(-1)achieved LOD values of 0.47 nmol·L^(-1)(Cd^(2+))and 0.008 nmol·L^(-1)(Pb^(2+)),respectively.Analysis of real water samples(tap water,mineral water,and river water)yielded recoveries of 95%-105%,validating practical applicability.Density functional theory(DFT)calculations reveal that synergistic interactions between cobalt centers and N/O atoms enhance adsorption and electron-transfer efficiency.CCDC:2160744.
基金financially supported by National Key R&D Program International Cooperation Project(2023YFE0108100)Natural Science Foundation of China(No.52170085)+2 种基金Key Project of Natural Science Foundation of Tianjin(No.21JCZDJC00320)Tianjin Post-graduate Students Research and Innovation Project(2021YJSB013)Fundamental Research Funds for the Central Universities,Nankai University.
文摘Biomass-derived heteroatom self-doped cathode catalysts has attracted considerable interest for electrochemical advanced oxidation processes(EAOPs)due to its high performance and sustainable synthesis.Herein,we illustrated the morphological fates of waste leaf-derived graphitic carbon(WLGC)produced from waste ginkgo leaves via pyrolysis temperature regulation and used as bifunctional cathode catalyst for simultaneous H_(2)O_(2) electrochemical generation and organic pollutant degradation,discovering S/N-self-doping shown to facilitate a synergistic effect on reactive oxygen species(ROS)generation.Under the optimum temperature of 800℃,the WLGC exhibited a H_(2)O_(2) selectivity of 94.2%and tetracycline removal of 99.3%within 60 min.Density functional theory calculations and in-situ Fourier transformed infrared spectroscopy verified that graphitic N was the critical site for H_(2)O_(2) generation.While pyridinic N and thiophene S were the main active sites responsible for OH generation,N vacancies were the active sites to produce ^(1)O_(2) from O_(2).The performance of the novel cathode for tetracycline degradation remains well under a wide pH range(3–11),maintaining excellent stability in 10 cycles.It is also industrially applicable,achieving satisfactory performance treating in real water matrices.This system facilitates both radical and non-radical degradation,offering valuable advances in the preparation of cost-effective and sustainable electrocatalysts and hold strong potentials in metal-free EAOPs for organic pollutant degradation.
文摘Pitch is a complex mixture of polycyclic aromatic hydrocarbons and their non-metal derivatives that has a high carbon content.Using pitch as a precursor for carbon materials in alkali metal ion(Li^(+)/Na^(+)/K^(+))batteries has become of great interest.However,its direct pyrolysis often leads to microstructures with a high orientation and small interlayer spacing due to uncontrolled liquid-phase carbonization,resulting in subpar electrochemical performance.It is therefore important to control the microstructures of pitch-derived carbon materials in order to improve their electrochemical properties.We evaluate the latest progress in the development of these materials using various microstructural engineering approaches,highlighting their use in metal-ion batteries and supercapacitors.The advantages and limitations of pitch molecules and their carbon derivatives are outlined,together with strategies for their modification in order to improve their properties for specific applications.Future research possibilities for structure optimization,scalable production,and waste pitch recycling are also considered.
基金supported by the Natural Science Basic Research Plan in the Shaanxi Province of China(No.2023-JC-ZD-25)Shaanxi Province(Qin ChuangYuan)“Scientist+Engineer”Team Building(No.2022KXJ-040)+1 种基金Shaanxi Provincial Department of Education Key Scientific Research Project(No.22JY024)Science and Technology Guidance Project Plan of China National Textile and Apparel Council(No.2022038,2023018).
文摘With the acceleration of advanced industrialization and urbanization,the environment is deteriorating rapidly,and non-renewable energy resources are depleted.The gradual advent of potential clean energy storage technologies is particularly urgent.Electrochemical energy storage technologies have been widely used in multiple fields,especially supercapacitors and rechargeable batteries,as vital elements of storing renewable energy.In recent years,two-dimensional material MXene has shown great potential in energy and multiple application fields thanks to its excellent electrical properties,large specific surface area,and tunability.Based on the layered materials of MXene,researchers have successfully achieved the dual functions of energy storage and conversion by adjusting the surface terminals at the Fermi level.It is worth noting that compared with other two-dimensional materials,MXene has more active sites on the basal plane,showing excellent catalytic performance.In contrast,other two-dimensional materials have catalytic activity only at the edge sites.This article comprehensively overviews the synthesis process,structural characteristics,modification methods for MXene-based polymer materials,and their applications in electrochemical energy storage.It also briefly discusses the potential of MXene-polymer materials in electromagnetic shielding technology and sensors and looks forward to future research directions.
基金financially supported by the National Natural Science Foundation of China(Nos.52272190 and 22178023)the National Key R&D Program of China(No.2021YFB4001401)。
文摘In response to the increasing demand of ethylene,electrochemical ethane nonoxidative dehydrogenation(EENDH)to ethylene by protonic ceramic electrolysis cells(PCECs)is developed.However,existing anode materials exhibit poor proton conductivity and limited catalytic activity.Herein,a novel Sr_(1.95)Fe_(1.4)Co_(0.1)Mo_(0.4)Zr_(0.1)O_(6-δ)(SFCMZ)anode is prepared as PCECs anode for EENDH.Zr doping increases the oxygen vacancies and enhances the proton conductivity of SFCMZ.Moreover,an alloy-oxide heterostructure(Co Fe@SFCMZ)is formed through in-situ exsolution of Co Fe alloy nanoparticles under reduction conditions,generating abundant oxygen vacancies and improving its catalytic activity.Co Fe@SFCMZ cell achieves an electrolysis current density of 0.87 A/cm^(2) at 700℃ under 1.6 V,with an ethane conversion rate of 34.22%and corresponding ethylene selectivity of 93.4%.These results demonstrate that Co Fe@SFCMZ anode exhibits excellent electrocatalytic activity,suggesting promising applications for EENDH.
基金Undergraduate Teaching Reform Research Project of Shenyang University of Technology。
文摘In the context of modern holistic education,integrating“ideological and political education”into specialized courses is a new requirement for professional teaching.In order to seamlessly integrate ideological education into academic disciplines through subtle influence,it is essential to identify and design suitable ideological elements.Based on the interdisciplinary nature of chemical engineering curricula,this paper focuses on core socialist values,patriotic sentiment,professional ethics,and the spirit of scientific innovation.It identifies key ideological elements such as“a strong chemical industry makes a strong nation”and“patriotism and maritime power,”analyzes their manifestations of value,and explores their relevance and significance in ideological education across different chemical engineering courses.
基金supported by the National Natural Science Foundation of China(U23A20573,U23A20140)the Hebei Natural Science Foundation(B202420809,B2024208088)+2 种基金S&T Program of Hebei(242Q4301Z,22373709D)Project of Basic Research at Universities in Shijiazhuang(241790977A)Huang jin tai plan project of Hebei provincial department of education(HJZD202512)。
文摘Integrating the CO_(2)capture process with the CO_(2)electrochemical reduction process into a single system can eliminate the need for storage and transportation following CO_(2)capture.This integrated process offers several advantages over multi-step cascade processes,including reduced costs and enhanced CO_(2)utilization.However,the integrated CO_(2)capture and electrochemical reduction(CCER)process encounters several challenges,including the low CO_(2)adsorption performance of the gas diffusion electrode(GDE)and catalyst,as well as the poor activity and selectivity of the catalyst for the electrochemical reduction of CO_(2).This review aims to systematically summarize the fundamentals of the CCER process.Based on an in-depth understanding of the CO_(2)mass transfer,adsorption,and electrochemical reduction processes,GDE design strategies based on the modulation of wettability and structure are discussed to enhance the CO_(2)capture capability at the GDE level.At the catalyst level,catalyst design strategies based on the introduction of CO_(2)capture sites and the construction of CO_(2)mass transfer channels were analyzed,and catalyst design strategies for enhanced CO_(2)capture were proposed.This review summarizes the most common catalysts for CO_(2)electrochemical reduction,such as Ni-based,Bi-based,and Cubased catalysts,and analyzes their design strategies based on reaction pathways for generating specific products.Finally,the problems and challenges of the CCER process are summarized and proposed,which provide ideas for the further application of this technology in the future.
基金the Fundamental Research Funds for the Central Universities(Nos.2232023G-04 and 20720210009)National Natural Science Foundation of China(Nos.NSFC-22274019 and 92163103)National Key R&D Program of China(No.2022YFA1505200)for financial support.Q.Chen is sponsored by National Ten Thousand Talent Program for young top-notch talent。
文摘Engineering of sulfur vacancies on the basal plane of molybdenum disulfide(MoS_(2))may provide effective way to promote the catalytic activity.Although the sulfur vacancy density has previously been correlated with catalytic activity,direct evidence that vacancies create surfaces with enhanced electrocatalytic activity is still lacking.Here,we used a combination of scanning electrochemical cell microscopy(SECCM)with submicrometer resolution and photoluminescence imaging to show that sulfur vacancies in monolayer MoS_(2)microflakes lead to significant spatial heterogeneity in the electrochemical hydrogen evolution reaction(HER)activity.Specifically,colocated multi-microscopy unveils that regions with superior HER activity are associated with sulfur vacancy defects.As the vacancy density increases,the triangular flakes display significantly enhanced and spatially uniformly distributed electrocatalytic activity.Our multi-microscopic imaging approach using SECCM convincingly highlights the spatial heterogeneity of electrocatalytic activity across monolayer MoS_(2)by sulfur vacancy engineering.
文摘Single-atom Fe catalysts show significant promise in the electrocatalytic reduction of CO_(2)(CO_(2)RR),while their performance remains inferior to that of precious metal catalysts due to the overly strong binding of^(*)CO intermediates.Although the introduction of heteroatoms or transition metal sites can modulate the binding strength of^(*)CO on Fe sites,these regulators often induce competitive hydrogen evolution reaction(HER)with reduced Faraday efficiency(FE).In this work,we employ HER-inert Sn as a regulator to tune the electronic structure of Fe,weakening^(*)CO adsorption and enhancing CO_(2)RR performance.Diatomic Fe-Sn pairs supported on N-doped carbon(Fe-Sn/NC)were synthesized,achieving FE for CO exceeding 90%over a broad potential range from−0.4 to−0.9 V versus the reversible hydrogen electrode.Fe-Sn/NC shows a high turnover frequency of 1.5×10^(4)h^(-1),much higher than that of Fe/NC.Characterization results and theoretical calculations demonstrate that bonding Sn site to Fe generates electron-rich Fe centers,effectively reducing the adsorption strength of^(*)CO without triggering HER.Additionally,Fe-Sn/NC exhibits exceptional activity in hydrazine oxidation performance(HzOR).The HzOR-assisted CO_(2)RR system using Fe-Sn/NC as electrodes reduces energy consumption by 38%compared with the conventional CO_(2)RR coupled oxygen evolution reaction system.
基金the financial support from the National Natural Science Foundation of China(NSFC,No.22308067)the Nature Science Foundation of Guangxi(2025GXNSFBA069166)+2 种基金the Guangxi“Universal Support for Young Talents”Scientific Research Project(ZX02080030424007)the Dean Project of Guangxi Key Laboratory of Petrochemical Resource Processing and Process Intensification Technology(2022Z009)the Innovation Project of Guangxi Graduate Education(YCSW2024131)。
文摘This study innovatively proposes a“chemical prelithiation/alloying-induced interfacial reconstruction”synergistic strategy that fundamentally improves the performance of Si-based anodes.Through a precisely controlled process leveraging orbital energetics and Lewis acid catalysis,we successfully engineer a Li-Al-F phase on the interface of SiO(denoted as Pre-SiO-Al)anodes via sequential chemical prelithiation and AlF_(3)-driven interfacial alloying reactions.This novel approach breaks through the ion transport limitations of traditional LiF-dominated solid electrolyte interphase(SEI)layers,while concurrently addressing the critical challenges of low initial Coulombic efficiency(ICE)and severe volume expansion.Mechanism studies reveal that the Li-Al-F offers an ultralow Li^(+)diffusion barrier(0.1 eV),significantly enhancing interfacial ion transport kinetics.Meanwhile,the high mechanical strength and dynamic stress dissipation capability of LiAl-F effectively suppress SEI fracture caused by volume expansion,enabling coordinated deformation compatibility between the electrode and the interfacial layer.The Pre-SiO-Al anode maintains a high capacity of 682.6 m A h g^(-1)after 2000 cycles at 1.0 A g^(-1)with near 100% capacity retention.When paired with LiFePO_(4)cathode,the Pre-SiO-Al||LFP full cell achieves impressive rate capability and cycling stability(93.8% capacity retention after 150 cycles at 0.5 C),demonstrating strong commercialization potential.
文摘The synthesis ofα-amino acid from imines with different carbonyl sources is attractive for both synthetic organic and medicinal chemistry communities.Imines,which were easily available from the corresponding ketones and amines,were employed as one of the most ideal precursors.Traditionally,cyanation and subsequent hydrolysis were required to install the carboxyl group^([1]).In these cases,the toxicity of the cyanation reagents limited its further synthetic applications in organic chemsitry.Besides,metal activation of imine substrates to make the organometallic intermediate and trap CO_(2) to give the desiredα-amino acid were also developed by many groups(Scheme 1A).The utilization of stoiochiometric amounts of metal reagents was required to realize the transformation.Recently,Yu reported a novel photocatalytic reductive carboxylation protocol for synthesis ofα-amino acid from imines with CO_(2)as the carbonyl source^([2]).
文摘Electrochemical synthesis of value-added chemicals represents a promising approach to address multidisciplinary demands.This technology establishes direct pathways for electricity-to-chemical conversion while significantly reducing the carbon footprint of chemical manufacturing.It simultaneously optimizes chemical energy storage and grid management,offering sustainable solutions for renewable energy utilization and overcoming geographical constraints in energy distribution.As a critical nexus between renewable energy and green chemistry,electrochemical synthesis serves dual roles in energy transformation and chemical production,emerging as a vital component in developing carbon-neutral circular economies.Focusing on key small molecules(H_(2)O,CO_(2),N_(2),O_(2)),this comment examines fundamental scientific challenges and practical barriers in electrocatalytic conversion processes,bridging laboratory innovations with industrial-scale implementation.
文摘Currently,chemical furnaces play an important role in the chemical industry.It is necessary to ensure their quality and operation performance,so as to guarantee the efficiency of chemical production.Compared with other furnaces,chemical furnaces have strong particularity,which puts forward higher requirements for the thermal shock resistance of the refractories of furnace linings.This paper studied the thermal shock resistance of the refractories for chemical furnace linings,and proposed measures for improvement,providing experience and technical support for the safe production of chemical enterprises.
基金supported by the National Key R&D Program of China(No.2022YFB4002202)the National Natural Science Foundation of China(Nos.52172199 and 52302334)+5 种基金the Young Elite Scientists Sponsorship Program by CAST(No.2022QNRC001)Hubei Province(No.2023BAB115)Jiangsu Province(Nos.BZ2022027 and BE2023092)Changzhou City(No.CZ20230010)supported by the State Key Laboratory of Materials Processing and Die&Mould Technology,Huazhong University of Science and Technology(No.P2023-025)Material Science and Engineering Discipline Guidance Fund of China University of Mining and Technology(No.CUMTMS202203).
文摘To enhance the electrochemical performance of the reversible solid oxide cell(RSOC),a facile way through adopting A-site deficient Pr_(0.94)PrBaCo_(1.5)Fe_(0.5)O_(5+δ)(PBCF94)as an air electrode for RSOC is reported.The designed A-site Pr-deficient air electrode is expected to provide abundant oxygen vacancies,macroscopic nanoparticle generation,excellent redox properties and oxygen mobility,which ultimately contribute to the enhanced electrocatalytic activity.The results confirm that the RSOC with an A-site deficient air electrode exhibits considerable peak power density up to 1.53 W·cm^(-2),and the desirable electrolysis current density reaches 2.29 A·cm^(-2)at 1.5 V and 800℃.Correspondingly,the RSOC exhibits remarkable long-term reversible stability of 200 h.Thus,the A-site deficient Pr_(0.94)PrBaCo_(1.5)Fe_(0.5)O_(5+δ)air electrode could be the potential one for RSOC application.
