Carbon peaking and carbon neutralization trigger a technical revolution in energy&environment related fields.Development of new technologies for green energy production and storage,industrial energy saving and eff...Carbon peaking and carbon neutralization trigger a technical revolution in energy&environment related fields.Development of new technologies for green energy production and storage,industrial energy saving and efficiency reinforcement,carbon capture,and pollutant gas treatment is in highly imperious demand.The emerging porous framework materials such as metal–organic frameworks(MOFs),covalent organic frameworks(COFs)and hydrogen-bonded organic frameworks(HOFs),owing to the permanent porosity,tremendous specific surface area,designable structure and customizable functionality,have shown great potential in major energy-consuming industrial processes,including sustainable energy gas catalytic conversion,energy-efficient industrial gas separation and storage.Herein,this manuscript presents a systematic review of porous framework materials for global and comprehensive energy&environment related applications,from a macroscopic and application perspective.展开更多
Biomass conversion offers an efficient approach to alleviate the energy and environmental issues.Electrochemical oxidation of 5-hydroxymethylfurfural(HMF)has attracted tremendous attention in the latest few years for ...Biomass conversion offers an efficient approach to alleviate the energy and environmental issues.Electrochemical oxidation of 5-hydroxymethylfurfural(HMF)has attracted tremendous attention in the latest few years for the mild synthesis conditions and high conversion efficiency to obtain 2,5-furan dicarboxylic acid(FDCA),but there still remain problems such as limited yield,short cycle life,and ambiguous reaction mechanism.Despite many reviews highlighting a variety of electrocatalysts for electrochemical oxidation of HMF,a detailed discussion of the structural modulation of catalyst and the underlying catalytic mechanism is still lacking.We herein provide a comprehensive summary of the recent development of electrochemical oxidation of HMF to FDCA,particularly focusing on the mechanism studies as well as the advanced strategies developed to regulate the structure and optimize the performance of the electrocatalysts,including heterointerface construction,defect engineering,single-atom engineering,and in situ reconstruction.Experimental characterization techniques and theoretical calculation methods for mechanism and active site studies are elaborated,and challenges and future directions of electrochemical oxidation of HMF are also prospected.This review will provide guidance for designing advanced catalysts and deepening the understanding of the reaction mechanism beneath electrochemical oxidation of HMF to FDCA.展开更多
The continuous increase of global atmospheric CO_(2) concentrations brutally damages our environment. A series of methods have been developed to convert CO_(2) to valuable fuels and value-added chemicals to maintain t...The continuous increase of global atmospheric CO_(2) concentrations brutally damages our environment. A series of methods have been developed to convert CO_(2) to valuable fuels and value-added chemicals to maintain the equilibrium of carbon cycles. The electrochemical CO_(2) reduction reaction(CO_(2)RR) is one of the promising methods to produce fuels and chemicals, and it could offer sustainable paths to decrease carbon intensity and support renewable energy. Thus, significant research efforts and highly efficient catalysts are essential for converting CO_(2) into other valuable chemicals and fuels. Transition metal-based single atoms catalysts(TM-SACs) have recently received much attention and offer outstanding electrochemical applications with high activity and selectivity opportunities. By taking advantage of both heterogeneous and homogeneous catalysts, TM-SACs are the new rising star for electrochemical conversion of CO_(2) to the value-added product with high selectivity. In recent years, enormous research effort has been made to synthesize different TM-SACs with different M–Nxsites and study the electrochemical conversion of CO_(2) to CO. This review has discussed the development and characterization of different TMSACs with various catalytic sites, fundamental understanding of the electrochemical process in CO_(2) RR,intrinsic catalytic activity, and molecular strategics of SACs responsible for CO_(2)RR. Furthermore, we extensively review previous studies on 1 st-row transition metals TM-SACs(Ni, Co, Fe, Cu, Zn, Sn) and dual-atom catalysts(DACs) utilized for electrochemical CO_(2) conversions and highlight the opportunities and challenges.展开更多
A novel Ag@nitrogen-doped porous carbon(Ag-NPC) composite was synthesized via a facile hydrothermal method and applied as an anode material in lithium-ion batteries(LIBs). Using this method, Ag nanoparticles(Ag NPs) w...A novel Ag@nitrogen-doped porous carbon(Ag-NPC) composite was synthesized via a facile hydrothermal method and applied as an anode material in lithium-ion batteries(LIBs). Using this method, Ag nanoparticles(Ag NPs) were embedded in NPC through thermal decomposition of Ag NO_3 in the pores of NPC. The reversible capacity of Ag-NPC remained at 852 m Ah g^(-1)after 200 cycles at a current density of 0.1 A g^(-1), showing its remarkable cycling stability. The enhancement of the electrochemical properties such as cycling performance,reversible capacity and rate performance of Ag-NPC compared to the NPC contributed to the synergistic effects between Ag NPs and NPC.展开更多
Traditional synthetic methodologies are confronted with great challenges to fabricate complex nanomaterials with delicate design,high efficiency and excellent sustainability.During the past decade,bio-inspired synthes...Traditional synthetic methodologies are confronted with great challenges to fabricate complex nanomaterials with delicate design,high efficiency and excellent sustainability.During the past decade,bio-inspired synthesis has been extensively applied as an effective and efficient strategy for the fabrication of nanomaterials and nanostructures.Mimicking electrode materials at nanoscale in the aspect of either structure or functionality has been receiving surging interest because of their incomparable advantages and outperforming properties.In this review,we summarize the recent progresses on bio-inspired synthesis of nanomaterials and smart structures in the field of energy storage and conversion.Firstly,an overall introduction of bio-inspired synthetic strategies will be presented,with focus on the biotemplates and bio-resources.Following that,a library of complex mimicking structures featured by high-order,hierarchical porosity,or bionic function are introduced,with discussion on their chemical and physical properties associated with the structure.The enhanced electrochemical properties such as energy density,cycling stability,etc.in different electrochemical systems will be also discussed.At last,we will expand the perspectives regarding the advantages and limitations of bioinspired strategy and possible solutions in the future.展开更多
With rapid development of 5G communication technologies,electromagnetic interference(EMI)shielding for electronic devices has become an urgent demand in recent years,where the development of corresponding EMI shieldin...With rapid development of 5G communication technologies,electromagnetic interference(EMI)shielding for electronic devices has become an urgent demand in recent years,where the development of corresponding EMI shielding materials against detrimental electromagnetic radiation plays an essential role.Meanwhile,the EMI shielding materials with high flexibility and functional integrity are highly demanded for emerging shielding applications.Hitherto,a variety of flexible EMI shielding materials with lightweight and multifunctionalities have been developed.In this review,we not only introduce the recent development of flexible EMI shielding materials,but also elaborate the EMI shielding mechanisms and the index for"green EMI shielding"performance.In addition,the construction strategies for sophisticated multifunctionalities of flexible shielding materials are summarized.Finally,we propose several possible research directions for flexible EMI shielding materials in near future,which could be inspirational to the fast-growing next-generation flexible electronic devices with reliable and multipurpose protections as offered by EMI shielding materials.展开更多
Non-precious metal nitrogen-doped carbonaceous materials have attracted tremendous attention in the field of electrochemical energy storage and conversion.Herein,we report the designed synthesis of a novel series of C...Non-precious metal nitrogen-doped carbonaceous materials have attracted tremendous attention in the field of electrochemical energy storage and conversion.Herein,we report the designed synthesis of a novel series of Co-N-C nanocomposites and their evaluation of electrochemical properties.Novel yolkshell structured Co nanoparticles@polymer materials are fabricated from the facile coating polymer strategy on the surface of ZIF-67.After calcination in nitrogen atmosphere,the Co–N–C nanocomposites in which cobalt metal nanoparticles are embedded in the highly porous and graphitic carbon matrix are successfully achieved.The cobalt nanoparticles containing cobalt metal crystallites with an oxidized shell and/or smaller(or amorphous)cobalt-oxide deposits appear on the surface of graphitic carbons.The prepared Co–N–C nanoparticles showed favorable electrocatalytic activity for oxygen reduction reactions,which is attributed to its high graphitic degree,large surface area and the large amount existence of Co–N active sites.展开更多
Metal–organic gel(MOG)derived composites are promising multi-functional materials due to their alterable composition,identifiable chemical homogeneity,tunable shape,and porous structure.Herein,stable metal–organic h...Metal–organic gel(MOG)derived composites are promising multi-functional materials due to their alterable composition,identifiable chemical homogeneity,tunable shape,and porous structure.Herein,stable metal–organic hydrogels are prepared by regulating the complexation effect,solution polarity and curing speed.Meanwhile,collagen peptide is used to facilitate the fabrication of a porous aerogel with excellent physical properties as well as the homogeneous dispersion of magnetic particles during calcination.Subsequently,two kinds of heterometallic magnetic coupling systems are obtained through the application of Kirkendall effect.FeCo/nitrogen-doped carbon(NC)aerogel demonstrates an ultra-strong microwave absorption of−85 dB at an ultra-low loading of 5%.After reducing the time taken by atom shifting,a FeCo/Fe3O4/NC aerogel containing virus-shaped particles is obtained,which achieves an ultra-broad absorption of 7.44 GHz at an ultra-thin thickness of 1.59 mm due to the coupling effect offered by dual-soft-magnetic particles.Furthermore,both aerogels show excellent thermal insulation property,and their outstanding radar stealth performances in J-20 aircraft are confirmed by computer simulation technology.The formation mechanism of MOG is also discussed along with the thermal insulation and electromagnetic wave absorption mechanism of the aerogels,which will enable the development and application of novel and lightweight stealth coatings.展开更多
Flexible sensors based on MXene-polymer composites are highly prospective for next-generation wearable electronics used in human-machine interfaces.One of the motivating factors behind the progress of flexible sensors...Flexible sensors based on MXene-polymer composites are highly prospective for next-generation wearable electronics used in human-machine interfaces.One of the motivating factors behind the progress of flexible sensors is the steady arrival of new conductive materials.MXenes,a new family of 2D nanomaterials,have been draw-ing attention since the last decade due to their high electronic conduc-tivity,processability,mechanical robustness and chemical tunability.In this review,we encompass the fabrication of MXene-based polymeric nanocomposites,their structure-property relationship,and applications in the flexible sensor domain.Moreover,our discussion is not only lim-ited to sensor design,their mechanism,and various modes of sensing platform,but also their future perspective and market throughout the world.With our article,we intend to fortify the bond between flexible matrices and MXenes thus promoting the swift advancement of flexible MXene-sensors for wearable technologies.展开更多
Polyolefins such as polyethylene(PE)are one of the largest-scale synthetic plastics and play a key role in modern society.However,polyethylene is extremely inert to chemical recycling owing to its lack of chemical fun...Polyolefins such as polyethylene(PE)are one of the largest-scale synthetic plastics and play a key role in modern society.However,polyethylene is extremely inert to chemical recycling owing to its lack of chemical functionality and low polarity,making it one of the most challenging environmental hazards globally.Herein,we developed a phosphorylated CeO_(2)catalyst by an organophosphate precursor and featured efficient photocatalysis of low-density polyethylene(LDPE)without the acid or alkaline pre-treatment.Compared to pristine CeO_(2),the surface phosphorylation allows to introduce Brønsted acid sites,which facilitate to form carbonium ions on LDPE via protonation.In addition,the suitable band structure of the phosphorylated CeO_(2)catalyst enables efficient photoabsorption and generates reactive oxygen species,leading to the C–C bond cleavage of LDPE.As a result,the phosphorylated CeO_(2)catalyst exhibited an outstanding carbon conversion rate of>94%after 48 h of photocatalysis under 50 mW/cm^(2)of simulated sunlight,with a high CO_(2)product selectivity of>99%.Furthermore,the PE microparticles with sizes larger than 10μm released from LDPE plastic wrap were directly and completely degraded by photocatalysis within 12 h,suggesting an attractive and environmentally benign strategy of utilizing solar energy-based photocatalysis for reducing potential hazards of LDPE plastic trashes.展开更多
A launching system with a filter cartridge structure was proposed to improve the muzzle velocity of the projectile.The combustion chamber of the launching system is divided into two fixed chambers,one is located in th...A launching system with a filter cartridge structure was proposed to improve the muzzle velocity of the projectile.The combustion chamber of the launching system is divided into two fixed chambers,one is located in the breech chamber,and the other is arranged in the barrel.The breech chamber charge was ignited first,and the charges in the auxiliary chambers were ignited by the high-temperature,highpressure combustible gas trailing the projectile.In this way,the combustible gas in the auxiliary chambers could compensate for the pressure drop caused by the movement of the projectile.The proposed device features the advantage of launching a projectile with high muzzle velocity without exceeding the maximum pressure in the chamber.In order to obtain some internal ballistic characteristics of the launch system,some critical structure,such as the length of the filter cartridge auxiliary charge,the combustion degree of the propellant in the chamber,and the length of the barrel,are discussed.The experimental results show that with the increased auxiliary charge length,a pressure plateau or even a secondary peak pressure can be formed,which is less than the peak pressure.The projectile velocity increased by 23.57%,14.64%,and 7.65%when the diaphragm thickness was 0 mm,1 mm,and2 mm,respectively.The muzzle velocity of the projectile can be increased by 13.42%by increasing the length of the barrel.Under the same charge condition,with the increase of barrel length,the energy utilization rate of propellant increases by 28.64%.展开更多
Operando monitoring of internal and local electrochemical processes within lithium-ion batteries(LIBs)is crucial,necessitating a range of non-invasive,real-time imaging characterization techniques including nuclear ma...Operando monitoring of internal and local electrochemical processes within lithium-ion batteries(LIBs)is crucial,necessitating a range of non-invasive,real-time imaging characterization techniques including nuclear magnetic resonance(NMR)techniques.This review provides a comprehensive overview of the recent applications and advancements of non-invasive magnetic resonance imaging(MRI)techniques in LIBs.It initially introduces the principles and hardware of MRI,followed by a detailed summary and comparison of MRI techniques used for characterizing liquid/solid electrolytes,electrodes and commercial batteries.This encompasses the determination of electrolytes'transport properties,acquisition of ion distribution profile,and diagnosis of battery defects.By focusing on experimental parameters and optimization strategies,our goal is to explore MRI methods suitable to a variety of research subjects,aiming to enhance imaging quality across diverse scenarios and offer critical physical/chemical insights into the ongoing operation processes of LIBs.展开更多
Lithium metal is considered as the ultimate anode material for the next generation of high-energy density batteries.However,non-uniform lithium dendrite growth,serious electrolyte consumption,and significant volume ch...Lithium metal is considered as the ultimate anode material for the next generation of high-energy density batteries.However,non-uniform lithium dendrite growth,serious electrolyte consumption,and significant volume changes during lithium deposition/stripping processes lead to sustained accumulation of inactive lithium and poor cycling reversibility.Quantifying the formation and evolution of inactive lithium under different conditions and fully evaluating the complex failure modes are the key issues in this challenging field.This article comprehensively reviews recent research progress on the quantification of formation and evolution of inactive lithium detected by different quantitative techniques in rechargeable lithium metal batteries.The key research challenges such as failure mechanism,modification strategies and operando characterization of lithium metal anodes are systematically summarized and prospected.This review provides a new angle of view to understand failure mechanism of lithium metal anodes and inspiration and guidance for the future development of rechargeable lithium metal batteries.展开更多
Lithium–oxygen battery with ultrahigh theoretical energy density is considered a highly competitive next-generation energy storage device,but its practical application is severely hindered by issues such as difficult...Lithium–oxygen battery with ultrahigh theoretical energy density is considered a highly competitive next-generation energy storage device,but its practical application is severely hindered by issues such as difficult decomposition of discharge products at present.Here,we have developed N-doped carbon anchored atomically dispersed Ru sites cathode catalyst with open hollow structure(h-RuNC)for Lithium–oxygen battery.On one hand,the abundance of atomically dispersed Ru sites can effectively catalyze the formation and decomposition of discharge products,thereby greatly enhancing the redox kinetics.On the other hand,the open hollow structure not only enhances the mass activity of atomically dispersed Ru sites but also improves the diffusion efficiency of catalytic molecules.Therefore,the excellent activity from atomically dispersed Ru sites and the enhanced diffusion from open hollow structure respectively improve the redox kinetics and cycling stability,ultimately achieving a high-performance lithium–oxygen battery.展开更多
Here we propose a new concept of"molecule aging":with some special treatment,a molecule could be"aged"by losing some unknown tiny particles or pieces from atoms in the molecule,Such"aging"...Here we propose a new concept of"molecule aging":with some special treatment,a molecule could be"aged"by losing some unknown tiny particles or pieces from atoms in the molecule,Such"aging"or loss of unknown tiny particles does not change apparently its molecular structure or chemical composition,but some physicochemical properties could be changed irreversibly.We further confirm such"molecule aging"via a long-term electron attacking to age water(H_(2)O)molecules.The IR spectra show no structural difference between the fresh water and the aged one,while the NMR spectra show that the electron attacking can decrease the size of water clusters.Such facts indicate that the electron attacking indeed can"affect"the structure of water molecule slightly but without damaging to its basic molecule frame.Further exploration reveals that the hydrogen evolution reaction(HER)activity of the aged water molecule is lower than the fresh water on the same Pt/C electrocatalyst.The density functional theory calculations indicate that the shortened O-H bond in H_(2)O indeed can present lower HER activity,so the observed size decrease of water clusters from NMR probably could be attributed to the shortening of O-H bond in water molecules.Such results indicate significantly that the molecule aging can produce materials with new functions for new possible applications.展开更多
Motivated by the recent discovery of unconventional superconductivity around a magnetic quantum critical point in pressurized CeSb_(2),here we present a high-pressure study of an isostructural antiferromagnetic(AFM) S...Motivated by the recent discovery of unconventional superconductivity around a magnetic quantum critical point in pressurized CeSb_(2),here we present a high-pressure study of an isostructural antiferromagnetic(AFM) SmSb_(2) through electrical transport and synchrotron x-ray diffraction measurements.At P_(C)~2.5 GPa,we found a pressure-induced magnetic phase transition accompanied by a Cmca→P4/nmm structural phase transition.In the pristine AFM phase below P_(C),the AFM transition temperature of SmSb_(2) is insensitive to pressure;in the emergent magnetic phase above P_(C),however,the magnetic critical temperature increases rapidly with increasing pressure.In addition,at ambient pressure,the magnetoresistivity(MR) of SmSb_(2) increases suddenly upon cooling below the AFM transition temperature and presents linear nonsaturating behavior under high field at 2 K.With increasing pressure above P_(C),the MR behavior remains similar to that observed at ambient pressure,both in terms of temperature-and field-dependent MR.This leads us to argue an AFM-like state for SmSb_(2) above P_(C).Within the investigated pressure of up to 45.3 GPa and the temperature of down to 1.8 K,we found no signature of superconductivity in SmSb_(2).展开更多
Phase transitions involving oxygen ion extraction within the framework of the crystallographic relevance have been widely exploited for sake of superconductivity,ferromagnetism,and ion conductivity in perovskiterelate...Phase transitions involving oxygen ion extraction within the framework of the crystallographic relevance have been widely exploited for sake of superconductivity,ferromagnetism,and ion conductivity in perovskiterelated oxides.However,atomic-scale pathways of phase transitions and ion extraction threshold are inadequately understood.Here we investigate the atomic structure evolution of LaCoO_(3) films upon oxygen extraction and subsequent Co migration,focusing on the key role of epitaxial strain.The brownmillerite to Ruddlesden-Popper phase transitions are discovered to stabilize at distinct crystal orientations in compressive-and tensile-strained cobaltites,which could be attributed to in-plane and out-of-plane Ruddlesden-Popper stacking faults,respectively.A two-stage process from exterior to interior phase transition is evidenced in compressive-strained LaCoO_(2.5),while a single-step nucleation process leaving bottom layer unchanged in tensile-strained situation.Strain analyses reveal that the former process is initiated by an expansion in Co layer at boundary,whereas the latter one is associated with an edge dislocation combined with antiphase boundary.These findings provide a chemomechanical perspective on the structure regulation of perovskite oxides and enrich insights into strain-dependent phase diagram in epitaxial oxides films.展开更多
Two-dimensional(2D)van der Waals magnetic materials have promising and versatile electronic and magnetic properties in the 2D limit,indicating a considerable potential to advance spintronic applications.Theoretical pr...Two-dimensional(2D)van der Waals magnetic materials have promising and versatile electronic and magnetic properties in the 2D limit,indicating a considerable potential to advance spintronic applications.Theoretical predictions thus far have not ascertained whether monolayer VCl_(3) is a ferromagnetic(FM)or anti-FM monolayer;this also remains to be experimentally verified.We theoretically investigate the influence of potential factors,including C_(3) symmetry breaking,orbital ordering,epitaxial strain,and charge doping,on the magnetic ground state.Utilizing first-principles calculations,we predict a collinear type-Ⅲ FM ground state in monolayer VCl_(3) with a broken C_(3) symmetry,wherein only the former two of three t_(2g)orbitals(a_(1g),e_(g2)^(π)and e_(g1)^(π))are occupied.The atomic layer thickness and bond angles of monolayer VCl_(3) undergo abrupt changes driven by an orbital ordering switch,resulting in concomitant structural and magnetic phase transitions.Introducing doping to the underlying Cl atoms of monolayer VCl_(3) without C_(3) symmetry simultaneously induces in-and out-of-plane polarizations.This can achieve a multiferroic phase transition if combined with the discovered adjustments of magnetic ground state and polarization magnitude under strain.The establishment of an orbital-ordering driven regulatory mechanism can facilitate deeper exploration and comprehension of magnetic properties of strongly correlated systems in monolayer VCl_(3).展开更多
Although the performance of perovskite solar cells(PSCs)has been dramatically increased in recent years,stability is still the main obstacle preventing the PSCs from being commercial.PSC device instability can be caus...Although the performance of perovskite solar cells(PSCs)has been dramatically increased in recent years,stability is still the main obstacle preventing the PSCs from being commercial.PSC device instability can be caused by a variety of reasons,including ions diffusion,surface and grain boundary defects,etc.In this work,the cross-linkable tannic acid(TA)is introduced to modify perovskite film through post-treatment method.The numerous organic functional groups(–OH and C=O)in TA can interact with the uncoordinated Pb^(2+)and I^(-)ions in perovskite,thus passivating defects and inhibiting ions diffusion.In addition,the formed TA network can absorb a small amount of the residual moisture inside the device to protect the perovskite layer.Furthermore,TA modification regulates the energy level of perovskite,and reduces interfacial charge recombination.Ultimately,following TA treatment,the device efficiency is increased significantly from 21.31%to 23.11%,with a decreased hysteresis effect.Notably,the treated device shows excellent air,thermal,and operational stability.In light of this,the readily available,inexpensive TA has the potential to operate as a multipurpose interfacial modifier to increase device efficiency while also enhancing device stability.展开更多
基金the financial support from the National Natural Science Foundation of China(22090062,21922810,21825802,22138003,22108083,and 21725603)the Guangdong Pearl River Talents Program(2021QN02C8)+3 种基金the Science and Technology Program of Guangzhou(202201010118)Zhejiang Provincial Natural Science Foundation of China(LR20B060001)National Science Fund for Excellent Young Scholars(22122811)China Postdoctoral Science Foundation(2022M710123)。
文摘Carbon peaking and carbon neutralization trigger a technical revolution in energy&environment related fields.Development of new technologies for green energy production and storage,industrial energy saving and efficiency reinforcement,carbon capture,and pollutant gas treatment is in highly imperious demand.The emerging porous framework materials such as metal–organic frameworks(MOFs),covalent organic frameworks(COFs)and hydrogen-bonded organic frameworks(HOFs),owing to the permanent porosity,tremendous specific surface area,designable structure and customizable functionality,have shown great potential in major energy-consuming industrial processes,including sustainable energy gas catalytic conversion,energy-efficient industrial gas separation and storage.Herein,this manuscript presents a systematic review of porous framework materials for global and comprehensive energy&environment related applications,from a macroscopic and application perspective.
基金National Natural Science Foundation of China(22272150,22302177)Major Program of Zhejiang Provincial Natural Science Foundation of China(LD22B030002)+2 种基金Zhejiang Provincial Ten Thousand Talent Program(2021R51009)Public Technology Application Project of Jinhua City(2022-4-067)Self Designed Scientific Research of Zhejiang Normal University(2021ZS0604)。
文摘Biomass conversion offers an efficient approach to alleviate the energy and environmental issues.Electrochemical oxidation of 5-hydroxymethylfurfural(HMF)has attracted tremendous attention in the latest few years for the mild synthesis conditions and high conversion efficiency to obtain 2,5-furan dicarboxylic acid(FDCA),but there still remain problems such as limited yield,short cycle life,and ambiguous reaction mechanism.Despite many reviews highlighting a variety of electrocatalysts for electrochemical oxidation of HMF,a detailed discussion of the structural modulation of catalyst and the underlying catalytic mechanism is still lacking.We herein provide a comprehensive summary of the recent development of electrochemical oxidation of HMF to FDCA,particularly focusing on the mechanism studies as well as the advanced strategies developed to regulate the structure and optimize the performance of the electrocatalysts,including heterointerface construction,defect engineering,single-atom engineering,and in situ reconstruction.Experimental characterization techniques and theoretical calculation methods for mechanism and active site studies are elaborated,and challenges and future directions of electrochemical oxidation of HMF are also prospected.This review will provide guidance for designing advanced catalysts and deepening the understanding of the reaction mechanism beneath electrochemical oxidation of HMF to FDCA.
基金BRNS,Mumbai,India(No-2013/37P/67/BRNS),MNRE,New Delhi,India(No-102/87/2011-NT),and CSIR,New Delhi,India{YSP-02(P-81-113),OLP-95}for the financial supportUGC,New Delhi,for a fellowship。
文摘The continuous increase of global atmospheric CO_(2) concentrations brutally damages our environment. A series of methods have been developed to convert CO_(2) to valuable fuels and value-added chemicals to maintain the equilibrium of carbon cycles. The electrochemical CO_(2) reduction reaction(CO_(2)RR) is one of the promising methods to produce fuels and chemicals, and it could offer sustainable paths to decrease carbon intensity and support renewable energy. Thus, significant research efforts and highly efficient catalysts are essential for converting CO_(2) into other valuable chemicals and fuels. Transition metal-based single atoms catalysts(TM-SACs) have recently received much attention and offer outstanding electrochemical applications with high activity and selectivity opportunities. By taking advantage of both heterogeneous and homogeneous catalysts, TM-SACs are the new rising star for electrochemical conversion of CO_(2) to the value-added product with high selectivity. In recent years, enormous research effort has been made to synthesize different TM-SACs with different M–Nxsites and study the electrochemical conversion of CO_(2) to CO. This review has discussed the development and characterization of different TMSACs with various catalytic sites, fundamental understanding of the electrochemical process in CO_(2) RR,intrinsic catalytic activity, and molecular strategics of SACs responsible for CO_(2)RR. Furthermore, we extensively review previous studies on 1 st-row transition metals TM-SACs(Ni, Co, Fe, Cu, Zn, Sn) and dual-atom catalysts(DACs) utilized for electrochemical CO_(2) conversions and highlight the opportunities and challenges.
基金supported by the Scientific and Technological Innovation Platform of Fujian Province(2006L2003)
文摘A novel Ag@nitrogen-doped porous carbon(Ag-NPC) composite was synthesized via a facile hydrothermal method and applied as an anode material in lithium-ion batteries(LIBs). Using this method, Ag nanoparticles(Ag NPs) were embedded in NPC through thermal decomposition of Ag NO_3 in the pores of NPC. The reversible capacity of Ag-NPC remained at 852 m Ah g^(-1)after 200 cycles at a current density of 0.1 A g^(-1), showing its remarkable cycling stability. The enhancement of the electrochemical properties such as cycling performance,reversible capacity and rate performance of Ag-NPC compared to the NPC contributed to the synergistic effects between Ag NPs and NPC.
基金the 100 Talented Team of Hunan Province(XiangZu[2016]91)the“Huxiang high-level talents”program(no.2018RS3077,no.2019RS1007).
文摘Traditional synthetic methodologies are confronted with great challenges to fabricate complex nanomaterials with delicate design,high efficiency and excellent sustainability.During the past decade,bio-inspired synthesis has been extensively applied as an effective and efficient strategy for the fabrication of nanomaterials and nanostructures.Mimicking electrode materials at nanoscale in the aspect of either structure or functionality has been receiving surging interest because of their incomparable advantages and outperforming properties.In this review,we summarize the recent progresses on bio-inspired synthesis of nanomaterials and smart structures in the field of energy storage and conversion.Firstly,an overall introduction of bio-inspired synthetic strategies will be presented,with focus on the biotemplates and bio-resources.Following that,a library of complex mimicking structures featured by high-order,hierarchical porosity,or bionic function are introduced,with discussion on their chemical and physical properties associated with the structure.The enhanced electrochemical properties such as energy density,cycling stability,etc.in different electrochemical systems will be also discussed.At last,we will expand the perspectives regarding the advantages and limitations of bioinspired strategy and possible solutions in the future.
基金This work was financially supported by the National Natural Science Foundation of China(51725101,11727807,51672050,61790581,52102368,52101213)the Ministry of Science and Technology of China(973 Project No.2018YFA0209102)+6 种基金University Development Fund(UDF0100152)the Program for Guangdong Introducing Innovative and Entrepreneurial Teams(Grant No.2017ZT07C291)Shenzhen Science and Technology Program(Grant No.KQTD20170810141424366)China Postdoctoral Science Foundation(Grant No.2020M680085)Regional Joint Fund for Basic Research and Applied Basic Research of Guangdong Province(No.2020SA001515110905)Science and Technology Department of Jiangsu Province of China(Grant No.BK20210261)Open access funding provided by Shanghai Jiao Tong University
文摘With rapid development of 5G communication technologies,electromagnetic interference(EMI)shielding for electronic devices has become an urgent demand in recent years,where the development of corresponding EMI shielding materials against detrimental electromagnetic radiation plays an essential role.Meanwhile,the EMI shielding materials with high flexibility and functional integrity are highly demanded for emerging shielding applications.Hitherto,a variety of flexible EMI shielding materials with lightweight and multifunctionalities have been developed.In this review,we not only introduce the recent development of flexible EMI shielding materials,but also elaborate the EMI shielding mechanisms and the index for"green EMI shielding"performance.In addition,the construction strategies for sophisticated multifunctionalities of flexible shielding materials are summarized.Finally,we propose several possible research directions for flexible EMI shielding materials in near future,which could be inspirational to the fast-growing next-generation flexible electronic devices with reliable and multipurpose protections as offered by EMI shielding materials.
基金the support of Chinese Government 1000 young talent planthe support of Curtin Strategic International Research Scholarship+8 种基金Curtin University Mobility ScholarshipChinese Government Award for Outstanding Self-Financed Students Abroadthe support from ATN Seed fundARC Future Fellowship (FT180100705)Discovery Project (DP180102297)the facilities, scientific and technical assistance of the Curtin University Electron Microscope Laboratories, a facility partially funded by the University, State and Commonwealth GovernmentsThe use of equipment, scientific and technical assistance of the WA X-Ray Surface Analysis Facility, funded by the Australian Research Council LIEF grant LE120100026the facilities, and the scientific and technical assistance of the Australian Microscopy & Microanalysis Research Facility at the Centre for Microscopy, Characterization & Analysis (CMCA), the University of Western Australia (UWA), a facility funded by the University, State and Commonwealth Governmentsthe support from the Australian Research Council Future Fellowship (FT12100178)
文摘Non-precious metal nitrogen-doped carbonaceous materials have attracted tremendous attention in the field of electrochemical energy storage and conversion.Herein,we report the designed synthesis of a novel series of Co-N-C nanocomposites and their evaluation of electrochemical properties.Novel yolkshell structured Co nanoparticles@polymer materials are fabricated from the facile coating polymer strategy on the surface of ZIF-67.After calcination in nitrogen atmosphere,the Co–N–C nanocomposites in which cobalt metal nanoparticles are embedded in the highly porous and graphitic carbon matrix are successfully achieved.The cobalt nanoparticles containing cobalt metal crystallites with an oxidized shell and/or smaller(or amorphous)cobalt-oxide deposits appear on the surface of graphitic carbons.The prepared Co–N–C nanoparticles showed favorable electrocatalytic activity for oxygen reduction reactions,which is attributed to its high graphitic degree,large surface area and the large amount existence of Co–N active sites.
基金the National Natural Science Foundation of China(22265021)the Aeronautical Science Foundation of China(2020Z056056003).
文摘Metal–organic gel(MOG)derived composites are promising multi-functional materials due to their alterable composition,identifiable chemical homogeneity,tunable shape,and porous structure.Herein,stable metal–organic hydrogels are prepared by regulating the complexation effect,solution polarity and curing speed.Meanwhile,collagen peptide is used to facilitate the fabrication of a porous aerogel with excellent physical properties as well as the homogeneous dispersion of magnetic particles during calcination.Subsequently,two kinds of heterometallic magnetic coupling systems are obtained through the application of Kirkendall effect.FeCo/nitrogen-doped carbon(NC)aerogel demonstrates an ultra-strong microwave absorption of−85 dB at an ultra-low loading of 5%.After reducing the time taken by atom shifting,a FeCo/Fe3O4/NC aerogel containing virus-shaped particles is obtained,which achieves an ultra-broad absorption of 7.44 GHz at an ultra-thin thickness of 1.59 mm due to the coupling effect offered by dual-soft-magnetic particles.Furthermore,both aerogels show excellent thermal insulation property,and their outstanding radar stealth performances in J-20 aircraft are confirmed by computer simulation technology.The formation mechanism of MOG is also discussed along with the thermal insulation and electromagnetic wave absorption mechanism of the aerogels,which will enable the development and application of novel and lightweight stealth coatings.
基金The authors would like to acknowledge the support from the Natural Sciences and Engineering Research Council of Canada in the form of Discovery Grants to ARR and SS(RGPIN-2019-07246 and RGPIN-2022-04988).A.Rosenkranz greatly acknowledges the financial support given by ANID-Chile within the project Fondecyt Regular 1220331 and Fondequip EQM190057.B.Wang gratefully acknowledges the financial support given by the Alexander von Humboldt Foundation.
文摘Flexible sensors based on MXene-polymer composites are highly prospective for next-generation wearable electronics used in human-machine interfaces.One of the motivating factors behind the progress of flexible sensors is the steady arrival of new conductive materials.MXenes,a new family of 2D nanomaterials,have been draw-ing attention since the last decade due to their high electronic conduc-tivity,processability,mechanical robustness and chemical tunability.In this review,we encompass the fabrication of MXene-based polymeric nanocomposites,their structure-property relationship,and applications in the flexible sensor domain.Moreover,our discussion is not only lim-ited to sensor design,their mechanism,and various modes of sensing platform,but also their future perspective and market throughout the world.With our article,we intend to fortify the bond between flexible matrices and MXenes thus promoting the swift advancement of flexible MXene-sensors for wearable technologies.
基金the following funding agencies for supporting this work: the National Natural Science Foundation of China (22025502, U23A20552, 22379026, 22222901, 22175022)the Natural Science Foundation of Shanghai (23ZR1407000)the Science and Technology Commission of Shanghai Municipality (21DZ1206800)
文摘Polyolefins such as polyethylene(PE)are one of the largest-scale synthetic plastics and play a key role in modern society.However,polyethylene is extremely inert to chemical recycling owing to its lack of chemical functionality and low polarity,making it one of the most challenging environmental hazards globally.Herein,we developed a phosphorylated CeO_(2)catalyst by an organophosphate precursor and featured efficient photocatalysis of low-density polyethylene(LDPE)without the acid or alkaline pre-treatment.Compared to pristine CeO_(2),the surface phosphorylation allows to introduce Brønsted acid sites,which facilitate to form carbonium ions on LDPE via protonation.In addition,the suitable band structure of the phosphorylated CeO_(2)catalyst enables efficient photoabsorption and generates reactive oxygen species,leading to the C–C bond cleavage of LDPE.As a result,the phosphorylated CeO_(2)catalyst exhibited an outstanding carbon conversion rate of>94%after 48 h of photocatalysis under 50 mW/cm^(2)of simulated sunlight,with a high CO_(2)product selectivity of>99%.Furthermore,the PE microparticles with sizes larger than 10μm released from LDPE plastic wrap were directly and completely degraded by photocatalysis within 12 h,suggesting an attractive and environmentally benign strategy of utilizing solar energy-based photocatalysis for reducing potential hazards of LDPE plastic trashes.
基金financially supported by the National Natural Science Foundation of China under Project No.51874267 and No.12272374the Fundamental Research Funds for the Central Universities under Project Nos.WK2480000008,WK2480000007,and WK2320000049。
文摘A launching system with a filter cartridge structure was proposed to improve the muzzle velocity of the projectile.The combustion chamber of the launching system is divided into two fixed chambers,one is located in the breech chamber,and the other is arranged in the barrel.The breech chamber charge was ignited first,and the charges in the auxiliary chambers were ignited by the high-temperature,highpressure combustible gas trailing the projectile.In this way,the combustible gas in the auxiliary chambers could compensate for the pressure drop caused by the movement of the projectile.The proposed device features the advantage of launching a projectile with high muzzle velocity without exceeding the maximum pressure in the chamber.In order to obtain some internal ballistic characteristics of the launch system,some critical structure,such as the length of the filter cartridge auxiliary charge,the combustion degree of the propellant in the chamber,and the length of the barrel,are discussed.The experimental results show that with the increased auxiliary charge length,a pressure plateau or even a secondary peak pressure can be formed,which is less than the peak pressure.The projectile velocity increased by 23.57%,14.64%,and 7.65%when the diaphragm thickness was 0 mm,1 mm,and2 mm,respectively.The muzzle velocity of the projectile can be increased by 13.42%by increasing the length of the barrel.Under the same charge condition,with the increase of barrel length,the energy utilization rate of propellant increases by 28.64%.
基金supported by the National Key R&D Program of China,Grant No.2021YFB2401800。
文摘Operando monitoring of internal and local electrochemical processes within lithium-ion batteries(LIBs)is crucial,necessitating a range of non-invasive,real-time imaging characterization techniques including nuclear magnetic resonance(NMR)techniques.This review provides a comprehensive overview of the recent applications and advancements of non-invasive magnetic resonance imaging(MRI)techniques in LIBs.It initially introduces the principles and hardware of MRI,followed by a detailed summary and comparison of MRI techniques used for characterizing liquid/solid electrolytes,electrodes and commercial batteries.This encompasses the determination of electrolytes'transport properties,acquisition of ion distribution profile,and diagnosis of battery defects.By focusing on experimental parameters and optimization strategies,our goal is to explore MRI methods suitable to a variety of research subjects,aiming to enhance imaging quality across diverse scenarios and offer critical physical/chemical insights into the ongoing operation processes of LIBs.
基金financially supported by the National Key R&D Program of China, Grant No. 2021YFB2401800
文摘Lithium metal is considered as the ultimate anode material for the next generation of high-energy density batteries.However,non-uniform lithium dendrite growth,serious electrolyte consumption,and significant volume changes during lithium deposition/stripping processes lead to sustained accumulation of inactive lithium and poor cycling reversibility.Quantifying the formation and evolution of inactive lithium under different conditions and fully evaluating the complex failure modes are the key issues in this challenging field.This article comprehensively reviews recent research progress on the quantification of formation and evolution of inactive lithium detected by different quantitative techniques in rechargeable lithium metal batteries.The key research challenges such as failure mechanism,modification strategies and operando characterization of lithium metal anodes are systematically summarized and prospected.This review provides a new angle of view to understand failure mechanism of lithium metal anodes and inspiration and guidance for the future development of rechargeable lithium metal batteries.
基金This work was supported by National Key R&D Program of China(2021YFF0500503)National Natural Science Foundation of China(21925202,U22B2071)International Joint Mission on Climate Change and Carbon Neutrality.
文摘Lithium–oxygen battery with ultrahigh theoretical energy density is considered a highly competitive next-generation energy storage device,but its practical application is severely hindered by issues such as difficult decomposition of discharge products at present.Here,we have developed N-doped carbon anchored atomically dispersed Ru sites cathode catalyst with open hollow structure(h-RuNC)for Lithium–oxygen battery.On one hand,the abundance of atomically dispersed Ru sites can effectively catalyze the formation and decomposition of discharge products,thereby greatly enhancing the redox kinetics.On the other hand,the open hollow structure not only enhances the mass activity of atomically dispersed Ru sites but also improves the diffusion efficiency of catalytic molecules.Therefore,the excellent activity from atomically dispersed Ru sites and the enhanced diffusion from open hollow structure respectively improve the redox kinetics and cycling stability,ultimately achieving a high-performance lithium–oxygen battery.
基金funded by the Key Research and Development Program sponsored by the Ministry of Science and Technology(MOST)(2022YFA1203400)National Natural Science Foundation of China(21925205,22072145,21372155,22005294,and 22102172)。
文摘Here we propose a new concept of"molecule aging":with some special treatment,a molecule could be"aged"by losing some unknown tiny particles or pieces from atoms in the molecule,Such"aging"or loss of unknown tiny particles does not change apparently its molecular structure or chemical composition,but some physicochemical properties could be changed irreversibly.We further confirm such"molecule aging"via a long-term electron attacking to age water(H_(2)O)molecules.The IR spectra show no structural difference between the fresh water and the aged one,while the NMR spectra show that the electron attacking can decrease the size of water clusters.Such facts indicate that the electron attacking indeed can"affect"the structure of water molecule slightly but without damaging to its basic molecule frame.Further exploration reveals that the hydrogen evolution reaction(HER)activity of the aged water molecule is lower than the fresh water on the same Pt/C electrocatalyst.The density functional theory calculations indicate that the shortened O-H bond in H_(2)O indeed can present lower HER activity,so the observed size decrease of water clusters from NMR probably could be attributed to the shortening of O-H bond in water molecules.Such results indicate significantly that the molecule aging can produce materials with new functions for new possible applications.
基金Project supported by the National Key Research and Development Program of China (Grant Nos. 2023YFA1406102 and 2022YFA1602603)the National Natural Science Foundation of China (Grant Nos. 12374049 and 12174395)+2 种基金the China Postdoctoral Science Foundation (Grant No. 2023M743542)Hefei Institutes of Physical Science,Chinese Academy of Sciences the Director’s Fundation of (Grant No. YZJJ2024QN41)the Basic Research Program of the Chinese Academy of Sciences Based on Major Scientific Infrastructures (Grant No. JZHKYPT-2021-08)。
文摘Motivated by the recent discovery of unconventional superconductivity around a magnetic quantum critical point in pressurized CeSb_(2),here we present a high-pressure study of an isostructural antiferromagnetic(AFM) SmSb_(2) through electrical transport and synchrotron x-ray diffraction measurements.At P_(C)~2.5 GPa,we found a pressure-induced magnetic phase transition accompanied by a Cmca→P4/nmm structural phase transition.In the pristine AFM phase below P_(C),the AFM transition temperature of SmSb_(2) is insensitive to pressure;in the emergent magnetic phase above P_(C),however,the magnetic critical temperature increases rapidly with increasing pressure.In addition,at ambient pressure,the magnetoresistivity(MR) of SmSb_(2) increases suddenly upon cooling below the AFM transition temperature and presents linear nonsaturating behavior under high field at 2 K.With increasing pressure above P_(C),the MR behavior remains similar to that observed at ambient pressure,both in terms of temperature-and field-dependent MR.This leads us to argue an AFM-like state for SmSb_(2) above P_(C).Within the investigated pressure of up to 45.3 GPa and the temperature of down to 1.8 K,we found no signature of superconductivity in SmSb_(2).
基金supported by the National Natural Science Foundation of China(Grant Nos.52322212,52072400,52025025,and 52250402)。
文摘Phase transitions involving oxygen ion extraction within the framework of the crystallographic relevance have been widely exploited for sake of superconductivity,ferromagnetism,and ion conductivity in perovskiterelated oxides.However,atomic-scale pathways of phase transitions and ion extraction threshold are inadequately understood.Here we investigate the atomic structure evolution of LaCoO_(3) films upon oxygen extraction and subsequent Co migration,focusing on the key role of epitaxial strain.The brownmillerite to Ruddlesden-Popper phase transitions are discovered to stabilize at distinct crystal orientations in compressive-and tensile-strained cobaltites,which could be attributed to in-plane and out-of-plane Ruddlesden-Popper stacking faults,respectively.A two-stage process from exterior to interior phase transition is evidenced in compressive-strained LaCoO_(2.5),while a single-step nucleation process leaving bottom layer unchanged in tensile-strained situation.Strain analyses reveal that the former process is initiated by an expansion in Co layer at boundary,whereas the latter one is associated with an edge dislocation combined with antiphase boundary.These findings provide a chemomechanical perspective on the structure regulation of perovskite oxides and enrich insights into strain-dependent phase diagram in epitaxial oxides films.
基金supported by the National Key Research and Development Program of China(Grant Nos.2018YFE0202700 and 2023YFA1406500)the National Natural Science Foundation of China(Grant Nos.11974422 and 12104504)+2 种基金the Strategic Priority Research Program of the Chinese Academy of Sciences(Grant No.XDB30000000)Fundamental Research Funds for the Central Universities,and Research Funds of Renmin University,China(Grant No.22XNKJ30)supported by the Outstanding Innovative Talents Cultivation Funded Programs 2023 of Renmin University,China。
文摘Two-dimensional(2D)van der Waals magnetic materials have promising and versatile electronic and magnetic properties in the 2D limit,indicating a considerable potential to advance spintronic applications.Theoretical predictions thus far have not ascertained whether monolayer VCl_(3) is a ferromagnetic(FM)or anti-FM monolayer;this also remains to be experimentally verified.We theoretically investigate the influence of potential factors,including C_(3) symmetry breaking,orbital ordering,epitaxial strain,and charge doping,on the magnetic ground state.Utilizing first-principles calculations,we predict a collinear type-Ⅲ FM ground state in monolayer VCl_(3) with a broken C_(3) symmetry,wherein only the former two of three t_(2g)orbitals(a_(1g),e_(g2)^(π)and e_(g1)^(π))are occupied.The atomic layer thickness and bond angles of monolayer VCl_(3) undergo abrupt changes driven by an orbital ordering switch,resulting in concomitant structural and magnetic phase transitions.Introducing doping to the underlying Cl atoms of monolayer VCl_(3) without C_(3) symmetry simultaneously induces in-and out-of-plane polarizations.This can achieve a multiferroic phase transition if combined with the discovered adjustments of magnetic ground state and polarization magnitude under strain.The establishment of an orbital-ordering driven regulatory mechanism can facilitate deeper exploration and comprehension of magnetic properties of strongly correlated systems in monolayer VCl_(3).
基金supported by the General Program of Chongqing Natural Science Foundation(CSTB2022NSCQMSX1227 and CSTB2022NSCQ-MSX0459)the supports from the Fundamental Research Funds for the Central Universities(SWU-XDJH202314)。
文摘Although the performance of perovskite solar cells(PSCs)has been dramatically increased in recent years,stability is still the main obstacle preventing the PSCs from being commercial.PSC device instability can be caused by a variety of reasons,including ions diffusion,surface and grain boundary defects,etc.In this work,the cross-linkable tannic acid(TA)is introduced to modify perovskite film through post-treatment method.The numerous organic functional groups(–OH and C=O)in TA can interact with the uncoordinated Pb^(2+)and I^(-)ions in perovskite,thus passivating defects and inhibiting ions diffusion.In addition,the formed TA network can absorb a small amount of the residual moisture inside the device to protect the perovskite layer.Furthermore,TA modification regulates the energy level of perovskite,and reduces interfacial charge recombination.Ultimately,following TA treatment,the device efficiency is increased significantly from 21.31%to 23.11%,with a decreased hysteresis effect.Notably,the treated device shows excellent air,thermal,and operational stability.In light of this,the readily available,inexpensive TA has the potential to operate as a multipurpose interfacial modifier to increase device efficiency while also enhancing device stability.
