Nitrogenous compounds(i.e.,amines,amides,nitriles,oximes,amino acids and nitrogen-heterocycles derivatives)are important building blocks for synthetic chemistry,pharmaceuticals,and functional materials.Conventional sy...Nitrogenous compounds(i.e.,amines,amides,nitriles,oximes,amino acids and nitrogen-heterocycles derivatives)are important building blocks for synthetic chemistry,pharmaceuticals,and functional materials.Conventional synthetic strategies involve the use of toxic organic nitrogenous precursors or expensive heterogeneous catalysts under elevated temperatures and pressurized oxygen.Heterogeneous electrocatalysis can initiate the activation of inorganic N sources(i.e.,NH_(3)and NO^(-)_(x))under ambient reactions in liquid phase by applying a small bias,thus allowing the synthesis of value?added nitrogenous compounds from carbonyls,alkenes,keto acids,and even carbon dioxide in a sustainable manner without the use of oxidants/reductants.This review outlines recent de-velopments in electrosynthesis of nitrogenous compounds using inorganic N sources,focusing on reaction mechanisms understanding,the design and optimization of efficient electrocatalysts,and the advances in cell configurations for various C‒N coupling reactions.The limitations and challenges in applications are also discussed.展开更多
The effects of seemingly inert alkali metal(AM)cations on the electrocatalytic activity of electrode materials towards reactions essential for energy provision have become the emphasis of substantial research efforts ...The effects of seemingly inert alkali metal(AM)cations on the electrocatalytic activity of electrode materials towards reactions essential for energy provision have become the emphasis of substantial research efforts in recent years.The hydrogen and oxygen evolution reactions during alkaline water electrolysis and the oxygen electro-reduction taking place in fuel cells are of particular importance.There is no universal theory explaining all the details of the AM cation effect in electrocatalysis.For example,it remains unclear how“spectator”AM-cations can change the kinetics of electrocatalytic reactions often more significantly than the modifications of the elec-trode structure and composition.This situation originates partly from a lack of systematic experimental and theoretical studies of this phenomenon.The present work exploits impedance spectroscopy to investigate the influence of the AM cations on the mechanism of the hydrogen evolution reaction at Pt microelectrodes.The activity follows the trend:Li^(+)≥Na^(+)≥K^(+)≥Cs^(+),where the highest activity corresponds to 0.1 M LiOH electrolytes at low overpotentials.We demonstrate that the nature of the AM cations also changes the relative contribution of the Volmer–Heyrovsky and Volmer–Tafel mechanisms to the overall reaction,with the former being more important for LiOH electrolytes.Our density functional theory-based thermodynamics and molecular dynamics calculations support these findings.展开更多
Coating microdefects and localized corrosion in coating/metal system are inevitable,accelerating the degradation of metal infrastructure.Early evaluating coating microdefects and detecting corrosion sites are urgent y...Coating microdefects and localized corrosion in coating/metal system are inevitable,accelerating the degradation of metal infrastructure.Early evaluating coating microdefects and detecting corrosion sites are urgent yet remain challenge to achieve.Herein,we propose a robust,universal and efficient fluorescence-based strategy for hierarchical warning of coating damage and metal corrosion by introducing the concepts of damage-induced fluorescence enhancement effect(DIE)and ionic-recognition induced quenching effect(RIQ).The coatings with dualresponsiveness for coating defect and steel corrosion are constructed by incorporating synthesized nanoprobes composed of metal organic frameworks(Ni–Zn-MOFs)loaded with Rhodamine B(RhB@MOFs).The initial damage to the coating causes an immediate intensification of fluorescence,while the specific ionic-recognition characteristic of RhB with Fe3t results in an evident fluorescence quenching,enabling the detection of coating damage and corrosion.Importantly,this nanoprobes are insensitive to the coating matrix and exhibit stable corrosion warning capability across various coating systems.Meanwhile,electrochemical investigations indicate that the impedance values of RM/EP maintain above 10^(8)Ωcm^(2)even after 60 days of immersion.Therefore,the incorporation of fluorescent nanoprobes greatly inhibits the intrusion of electrolytes into polymer and improves the corrosion protection performance of the coating.This powerful strategy towards dual-level damage warning provides insights for the development of long-term smart protective materials.展开更多
The continuous depletion of fossil fuels and the effects of climate change have encouraged prompt action to attain carbon neutrality.Technologies that transform and store renewable energy are crucial for creating a su...The continuous depletion of fossil fuels and the effects of climate change have encouraged prompt action to attain carbon neutrality.Technologies that transform and store renewable energy are crucial for creating a sustainable society,which is independent of fossil fuels.In this regard,electrochemical water splitting based on the oxygen evolution reaction(OER)and hydrogen evolution reaction(HER)is an attractive technique for producing carbon-free hydrogen fuels.Additionally,rechargeable metal–air batteries(MABs)are another intriguing way for renewable energy storage through reversible oxygen reactions(OER and the oxygen reduction reaction,ORR).Herein,we comprehensively review bifunctional electrocatalysts for water splitting(HER and OER)and MABs(OER and ORR),particularly 2D carbon material-derived heterostructures.The synthesis and properties of 2D carbon materials and their energy conversion and storage mechanisms are discussed to highlight the bifunc-tionality of the heterostructures.Recent studies on bifunctional electrocatalysts based on 2D carbon-derived heterostructures are also reviewed.Finally,perspectives for future studies and multifunctional catalysts are presented.展开更多
Electrochemical CO_(2)reduction has been considered a promising approach to neutralizing the global CO_(2)level.As an intriguing technique,metal-CO_(2)battery devices can not only capture CO_(2)into valuable carbonace...Electrochemical CO_(2)reduction has been considered a promising approach to neutralizing the global CO_(2)level.As an intriguing technique,metal-CO_(2)battery devices can not only capture CO_(2)into valuable carbonaceous chem-icals and reduce the CO_(2)concentration in the atmosphere but enable energy conversion.Among metal-CO_(2)batteries,aqueous Zn–CO_(2)batteries,especially rechargeable systems,exhibit flexible CO_(2)electrochemistry in terms of multi-carbon chemicals,which are gaseous or water-soluble,in favor of rechargeability and cycling durability of aqueous battery systems.Despite the increasing number of publications on Zn–CO_(2)batteries in the past three years,this field is still in its beginning stage and facing many challenges considering the capability of CO_(2)fixation and battery performance.Herein,we present a timely and overall summary of the recent progress in Zn–CO_(2)batteries,including fundamental mechanisms,affecting factors on electrochemical performance,catalyst cathodes,and electrolytes(catholytes and anolytes).Besides,we assess the application potential of Zn–CO_(2)batteries and compare this with those of alkali metal-CO_(2)batteries based on CO_(2)fixation and battery perfor-mance.Finally,we point out some current challenges for the further development of Zn–CO_(2)batteries and put forward perspectives of the research directions for practical applications of Zn–CO_(2)batteries in the future.展开更多
In recent years,the demand for high-performance rechargeable lithium batteries has increased significantly,and many efforts have been made to boost the use of advanced electrode materials.Since graphene was first isol...In recent years,the demand for high-performance rechargeable lithium batteries has increased significantly,and many efforts have been made to boost the use of advanced electrode materials.Since graphene was first isolated by Novoselov et al.,graphene/graphene-based materials have become an active area of research and are considered to be promising high-performance electrode materials.Graphene is a two-dimensional single-atom carbon-packed material that possesses fascinating properties,including a large surface area,remarkable electrical conductivity,extraordinary intrinsic electron mobility,high Young's modulus,superior mechanical strength,optical transmittance,catalytic performance,and stability.Therefore,graphene is considered an attractive ma-terial for rechargeable lithium-ion batteries(LIBs),lithium-sulfur batteries(LSBs),and lithium-oxygen batteries(LOBs).In this comprehensive review,we emphasise the recent progress in the controllable synthesis,func-tionalisation,and role of graphene in rechargeable lithium batteries.Finally,in this review,we aim to address the most promising results,benefits,challenges,critical issues,research directions,and perspectives to explain the developmental directions of graphene for batteries.展开更多
Owing to the outstanding optoelectronic properties of perovskite materials,perovskite solar cells(PSCs)have been widely studied by academic organizations and industry corporations,with great potential to become the ne...Owing to the outstanding optoelectronic properties of perovskite materials,perovskite solar cells(PSCs)have been widely studied by academic organizations and industry corporations,with great potential to become the next-generation commercial solar cells.However,critical challenges remain in preserving high efficiency practical large-scale commercialized PSCs:a)the long-term stability of the cell materials and devices,b)lead leakage,and c)methods to scale the cells for larger area applications.This paper summarizes the prior-art strategies to address the above challenges,including the latest studies on the traditional glass-glass and thin-film encapsulation methods to better improve the reliability of PSCs,new technologies for preventing lead leakage,and geometric improvement strategies to enhance the reliability,efficiency,and performance of perovskite solar modules(PSMs).Through these strategies,the device achieved enhanced performance in long-term stability tests.The encapsulation resulted in a high lead leakage inhibition rate of up to 99%,and the PSMs possessed a geometric fill factor of 99.6%and a power conversion efficiency(PCE)of 20.7%.The dramatic improvement of efficiency and reliability of perovskite solar cells and modules indicate the great potential for mass production and commer-cialization of perovskite solar applications in the near future.展开更多
Nanocrystals have emerged as cutting-edge functional materials benefiting from the increased surface and enhanced coupling of electronic states.High-resolution imaging in transmission electron microscope can provide i...Nanocrystals have emerged as cutting-edge functional materials benefiting from the increased surface and enhanced coupling of electronic states.High-resolution imaging in transmission electron microscope can provide invaluable structural information of crystalline materials,albeit it remains greatly challenging to nanocrystals due to the arduousness of accurate zone axis adjustment.Herein,a homemade software package,called SmartAxis,is developed for rapid yet accurate zone axis alignment of nanocrystals.Incident electron beam tilt is employed as an eccentric goniometer to measure the angular deviation of a crystal to a zone axis,and then serves as a linkage to calculate theαandβtilts of goniometer based on an accurate quantitative relationship.In this way,high-resolution imaging of one identical small Au nanocrystal,as well as electron beam-sensitive MIL-101 metal-organic framework crystals,along multiple zone axes,was performed successfully by using this accurate,time-and electron dose-saving zone axis alignment software package.展开更多
To accelerate the development of lithium-ion batteries(LIBs),researchers should urgently exploit next-generation electrodes with high specific capacity,long cycle stability,and excellent rate performance,such as TMOs,...To accelerate the development of lithium-ion batteries(LIBs),researchers should urgently exploit next-generation electrodes with high specific capacity,long cycle stability,and excellent rate performance,such as TMOs,silicon-based materials,and alloys.Among all the modification measures,hierarchical micro-nano structure and yolk–shell structure are considered suitable and effective ways to improve the electrochemical performance of those novel materials.Herein,a facile glucose-assisted solvothermal method combined with heat treatment was implemented to synthesize hierarchical micro-nano yolk–shell V_(2)O_(3).The special-structured material exhibited higher specific capacity,better structure stability,and faster electrochemical kinetics compared with nanosheet-structured and micro-nano-cluster-structured V_(2)O_(3).When used as an anode for LIB,mnYS-V_(2)O_(3)delivered high specific capacity of 650.1 mA h g^(-1)after over 500 cycles at a current density of 100 mA g^(-1),with a retention of 93.4%.Moreover,the morphology evolution mechanism of micro-nano structure and yolk–shell structure was investigated in this work,which is beneficial to the design of other mnYS-structured TMOs.展开更多
The preparation of red,green,and blue quantum dot(QD)pixelated arrays with high precision,resolution,and brightness poses a significant challenge on the development of advanced micro-displays for virtual,augmented,and...The preparation of red,green,and blue quantum dot(QD)pixelated arrays with high precision,resolution,and brightness poses a significant challenge on the development of advanced micro-displays for virtual,augmented,and mixed reality applications.Alongside the controlled synthesis of high-performance QDs,a reliable QD patterning technology is crucial in overcoming this challenge.Among the various methods available,photolithography-based patterning technologies show great potentials in producing ultra-fine QD patterns at micron scale.This review article presents the recent advancements in the field of QD patterning using photolithography techniques and explores their applications in micro-display technology.Firstly,we discuss QD patterning through photolithography techniques employing photoresist(PR),which falls into two categories:PRassisted photolithography and photolithography of QDPR.Subsequently,direct photolithography techniques based on photo-induced crosslinking of photosensitive groups and photo-induced ligand cleavage mechanisms are thoroughly reviewed.Meanwhile,we assess the performance of QD arrays fabricated using these photolithography techniques and their integration into QD light emitting diode display devices as well as color conversionbased micro light emitting diode display devices.Lastly,we summarize the most recent developments in this field and outline future prospects.展开更多
Aqueous-electrolyte-based zinc-ion batteries(ZIBs),which have significant advantages over other batteries,including low cost,high safety,high ionic conductivity,and a natural abundance of zinc,have been regarded as a ...Aqueous-electrolyte-based zinc-ion batteries(ZIBs),which have significant advantages over other batteries,including low cost,high safety,high ionic conductivity,and a natural abundance of zinc,have been regarded as a potential alternative to lithium-ion batteries(LIBs).ZIBs still face some critical challenges,however,especially for building a reversible zinc anode.To address the reversibility of zinc anode,great efforts have been made on intrinsic anode engineering and anode interface modification.Less attention has been devoted to the electrolyte additives,however,which could not only significantly improve the reversibility of zinc anode,but also determine the viability and overall performance of ZIBs.This review aims to provide an overview of the two main functions of electrolyte additives,followed by details on six reasons why additives might improve the performance of ZIBs from the perspectives of creating new layers and regulating current plating/stripping processes.Furthermore,the remaining difficulties and potential directions for additives in aqueous ZIBs are also highlighted.展开更多
ArticlenArticle types Articles commonly fall into one of three main categories:Fulllength articles,Review articles and Short communications.Full-length articles are original,unpublished primary research.Extensions of ...ArticlenArticle types Articles commonly fall into one of three main categories:Fulllength articles,Review articles and Short communications.Full-length articles are original,unpublished primary research.Extensions of work that has been published previously in short form such as a Communication are usually acceptable.Short communications must contain original and highly significant work whose high novelty warrants rapid publication.Review articles may be an authoritative overview of a field,a comprehensive literature reviews,or tutorial-style reference materials.Reviews are usually invited by the editor,but a topic may be proposed by an author via the editorial office.展开更多
The mass discarding face masks has caused severe environmental problems during and after the COVID-19 pandemic.To reduce waste and minimize environmental impact,we present a new face mask featuring selfcharging extend...The mass discarding face masks has caused severe environmental problems during and after the COVID-19 pandemic.To reduce waste and minimize environmental impact,we present a new face mask featuring selfcharging extended service time and fully biodegradable materials.To extend the effective service time,we need to supplement the lost electric charge of the electret layer of face masks,for which task we propose to use the piezoelectric effect and generate electricity from breathing motions.However,existing piezoelectric materials are either toxic,impermeable,rigid,costly,or non-degradable.We synthesize a fully biodegradable piezoelectric membrane composed of polyvinyl alcohol(PVA)and glycine(GLY)via the electrospinning process.Parameters are accurately controlled to ensure that glycine crystallizes into a highly piezoelectricβphase during electrospinning and enables piezoelectric responses of the filter membrane.Tested with the standard 0.3μm particles,face masks made of the PVA-GLY membrane show an outstanding filtration efficiency of 97%,which remains stable over at least 10 h of high-concentration continuous filtration.Furthermore,we demonstrated the biodegradability of PVA-GLY masks,which can degrade completely within a few weeks,compared to commonly used surgical masks requiring over thirty years to be decomposed.展开更多
Excessive emissions of greenhouse gases such as carbon dioxide have led to global climate change,which poses one of the greatest threats to human survival in the 21st century.The urgent need to achieve carbon neutrali...Excessive emissions of greenhouse gases such as carbon dioxide have led to global climate change,which poses one of the greatest threats to human survival in the 21st century.The urgent need to achieve carbon neutrality to mitigate climatic issues has stimulated the rapid development of advanced materials and technologies for clean energy conversion and efficient storage.In recent years,a series of remarkable advances have emerged,revealing innovative materials and strategies that significantly accelerate the transition toward sus-tainable energy solutions.In this context,this special issue presents ten high-quality contributions,including seven comprehensive reviews and three original research articles[1-10],focusing on the latest ad-vances and frontier research in advanced materials and technologies toward carbon neutrality.Collectively,these works highlight the latest progress in catalytic energy conversion,photovoltaic technologies,and electrochemical energy storage,providing valuable insights to guide future efforts in the design of carbon-neutral materials and sustainable energy systems.展开更多
Two-dimensional(2D)materials have attracted considerable research interest due to their precisely defined properties and versatile applications.In this realm,borophene-a single atomic sheet of boron atoms arranged in ...Two-dimensional(2D)materials have attracted considerable research interest due to their precisely defined properties and versatile applications.In this realm,borophene-a single atomic sheet of boron atoms arranged in a honeycomb lattice-has emerged as a promising candidate.While borophenes were theoretically predicted to have unique structural,optical,and electronic properties,the experimental synthesis of crystalline borophene sheets was first demonstrated on metal substrates in 2015,marking a crucial milestone.Since then,research efforts have focused on controlling the synthesis of semiconducting borophene polymorphs and exploring their novel physical characteristics.This review aims to explore the potential of 2D materials,specifically borophene,in various technological fields such as batteries,supercapacitors,fuel cells,and more.The analysis emphasises meticulous scrutiny of synthesis techniques due to their fundamental importance in realising borophene's properties.Specifically,the high carrier mobilities,tuneable bandgaps,and exceptional thermal conductivity of borophene are highlighted.By providing a comprehensive outlook on the significance of borophene in advancing materials science and technologies,this review contributes to shaping the landscape of 2D material research.展开更多
Photodynamic therapy(PDT)has been established as one of the most promising novel cancer therapies with fewer side-effects and enhanced efficacy compared to the currently available conventional treatments.However,its a...Photodynamic therapy(PDT)has been established as one of the most promising novel cancer therapies with fewer side-effects and enhanced efficacy compared to the currently available conventional treatments.However,its application has been hindered by the limitations that photosensitizers(PS)have.The combination of PS with metallic nanoparticles like platinum nanoparticles(PtNPs),can help to overcome these intrinsic drawbacks.In this work,the combination of PtNPs and the natural photosensitizer riboflavin(RF)is proposed.PtNPs are synthesized using RF(Pt@RF)as reducing and stabilizing agent in a one-step method,obtaining nanoparticles with mesoporous structure for UV triggered PDT.In view of possible future UV irradiation treatments,the degradation products of RF,ribitol(RB)and lumichrome(LC),this last being a photosensitizing byproduct,are also employed for the synthesis of porous PtNPs,obtaining Pt@LC and Pt@RB.When administered in vitro to lung cancer cells,all the samples elicit a strong decrease of cell viability and a decrease of intracellular ATP levels.The antitumoral effect of both Pt@RF and Pt@LC is triggered by UV-A irradiation.This antitumoral activity is caused by the induction of oxidative stress,shown in our study by the decrease in intracellular glutathione and increased expression of antioxidant enzymes.展开更多
Cancer treatment often requires a multimodal approach,such as combining chemotherapy and gene therapy.However,challenges such as low therapeutic efficacy and off-target effects hinder the effectiveness of these treatm...Cancer treatment often requires a multimodal approach,such as combining chemotherapy and gene therapy.However,challenges such as low therapeutic efficacy and off-target effects hinder the effectiveness of these treatments.In this study,the use of calcium-doped metal-organic frameworks Cu_(2)(BDC)_(2)(DABCO)as a nanocarrier platform for the co-delivery of doxorubicin(DOX)and plasmid CRISPR(pCRISPR)proposed to enhance anticancer efficiency.We demonstrated that Ca-doped MOF nanocarriers significantly improved the uptake of DOX and pCRISPR by in cancer cells.The co-delivery of DOX and pCRISPR with Ca-doped MOF nanocarriers resulted in a significant rise in cell death and decreased targeted gene expression.展开更多
Article ■Article types Articles commonly fall into one of three main categories:Fulllength articles,Review articles and Short communications.Full-length articles are original,unpublished primary research.Extensions o...Article ■Article types Articles commonly fall into one of three main categories:Fulllength articles,Review articles and Short communications.Full-length articles are original,unpublished primary research.Extensions of work that has been published previously in short form such as a Communication are usually acceptable.展开更多
Metal-organic frameworks(MOFs)have been considered as great contender and promising electrode materials for supercapacitors.However,their low capacity,aggregation,and poor porosity have necessitated the exploration of...Metal-organic frameworks(MOFs)have been considered as great contender and promising electrode materials for supercapacitors.However,their low capacity,aggregation,and poor porosity have necessitated the exploration of new approaches to enhance the performance of these active materials.In this study,sphere-like MOF were in-situ grown and it subsequently burst,transformed into a desired metal oxide heterostructure comprising n-type ZnO and p-type NiO(ZnO/NiO-350).The resulting optimized flower-like structure,composed of interlaced nanoflakes derived from MOFs,greatly improved the active sites,porosity,and functionality of the electrode materials.The ZnO/NiO-350 electrode exhibited superior electrochemical activities for supercapacitors,compared to the parent MOF,bare n-type,and p-type counterparts.The specific capacitance can reach to 543 F g^(-1) at a current density of 1 A g^(-1).Theoretical modeling and simulations were employed to gain insights into the atomic-scale properties of the materials.Furthermore,an assembled hybrid device using active carbon and ZnO/NiO-350 as electrodes demonstrated excellent energy density of 44 Wh kg^(-1) at a power density of 1.6 Kw kg^(-1).After 5000 cycles at 10 A g^(-1),the cycling stability remained excellent 80%of the initial capacitance.Overall,such evaluation of unique electrode with superior properties may be useful for the next generation supercapacitor electrode.展开更多
The endocrine-disrupting chemicals(EDCs)and antibiotics are causing negative effects on human beings and animals by disrupting the endocrine system and spreading antimicrobial resistance.The current need is to eradica...The endocrine-disrupting chemicals(EDCs)and antibiotics are causing negative effects on human beings and animals by disrupting the endocrine system and spreading antimicrobial resistance.The current need is to eradicate pharmaceutical waste from water bodies using advanced catalytic systems with high efficiency.Novel ternary carbon quantum dots(CQDs)decorated Z-Scheme WS_(2)-PANI nanocomposite was prepared by a green synthesis assisted in-situ polymerization for the photodegradation and detection of Estradiol(EST)and Nitrofurantoin(NFT).HRTEM micrographs revealed the formation of CQDs with a mean size of 4nm anchored on the surface of WS_(2)/PANI(width:PANI~20-30nm).The ternary nanocomposite showed excellent photocatalytic activity,degraded NFT(95.7%in 60min),and EST(96.6%in 60min).The rate kinetics study confirms the reaction followed pseudo first-order model.This heterostructure exhibited enhanced performances by modulating the energy level configuration,enhancing the absorption of visible light(2.4eV),and significantly improving the charge separation,three times higher than pristine WS_(2).These are highly favorable for increasing the generation of photoinduced charges and enhancing the overall performance of the catalyst.Further,the electrochemical sensor was prepared using CQDs@WS_(2)/PANI nanocomposite on a paper-based electrode.The CQDs@WS_(2)/PANI exhibit a linear response of 0.1-100nM,with a limit of detection of 13nM.This synergistic interfacial interaction resulted in the significantly improved electrochemical performance of the modified electrode.The proposed Z-scheme was justified by electron paramagnetic resonance(EPR)and scavenger experiment.An intermediate degradation pathway was also proposed.The synthesized materials were characterized using FESEM,HRTEM,XRD,FTIR,XPS,UV-visible spectroscopy,PL,and TRPL.Therefore,this study provides a direct approach to fabricate a heterojunction that combines two-dimensional,one dimensional,and zero-dimensional properties,enabling control over the energy level configuration and subsequent improvements in photocatalytic and electrocatalytic efficiency.展开更多
基金the NSFC(No.22472112)the Suzhou Foreign Academician Workstation(No.SWY2022001)for financial supportsthe Soochow Municipal Laboratory for Low Carbon Technologies and Industries.
文摘Nitrogenous compounds(i.e.,amines,amides,nitriles,oximes,amino acids and nitrogen-heterocycles derivatives)are important building blocks for synthetic chemistry,pharmaceuticals,and functional materials.Conventional synthetic strategies involve the use of toxic organic nitrogenous precursors or expensive heterogeneous catalysts under elevated temperatures and pressurized oxygen.Heterogeneous electrocatalysis can initiate the activation of inorganic N sources(i.e.,NH_(3)and NO^(-)_(x))under ambient reactions in liquid phase by applying a small bias,thus allowing the synthesis of value?added nitrogenous compounds from carbonyls,alkenes,keto acids,and even carbon dioxide in a sustainable manner without the use of oxidants/reductants.This review outlines recent de-velopments in electrosynthesis of nitrogenous compounds using inorganic N sources,focusing on reaction mechanisms understanding,the design and optimization of efficient electrocatalysts,and the advances in cell configurations for various C‒N coupling reactions.The limitations and challenges in applications are also discussed.
基金the German Research Foundation (DFG) under Germany's excellence strategy–EXC 2089/1–390776260, Germany's excellence cluster “e-conversion”the DFG project BA 5795/6-1+2 种基金funding from the European Union's Horizon 2020 research and innovation program under grant agreement HERMES No 952184the National Science Foundation (NSF) support through the NSF CAREER award (Grant No. CBET1941204)financial support from TUM Innovation Network for Artificial Intelligence powered Multifunctional Material Design (ARTEMIS).
文摘The effects of seemingly inert alkali metal(AM)cations on the electrocatalytic activity of electrode materials towards reactions essential for energy provision have become the emphasis of substantial research efforts in recent years.The hydrogen and oxygen evolution reactions during alkaline water electrolysis and the oxygen electro-reduction taking place in fuel cells are of particular importance.There is no universal theory explaining all the details of the AM cation effect in electrocatalysis.For example,it remains unclear how“spectator”AM-cations can change the kinetics of electrocatalytic reactions often more significantly than the modifications of the elec-trode structure and composition.This situation originates partly from a lack of systematic experimental and theoretical studies of this phenomenon.The present work exploits impedance spectroscopy to investigate the influence of the AM cations on the mechanism of the hydrogen evolution reaction at Pt microelectrodes.The activity follows the trend:Li^(+)≥Na^(+)≥K^(+)≥Cs^(+),where the highest activity corresponds to 0.1 M LiOH electrolytes at low overpotentials.We demonstrate that the nature of the AM cations also changes the relative contribution of the Volmer–Heyrovsky and Volmer–Tafel mechanisms to the overall reaction,with the former being more important for LiOH electrolytes.Our density functional theory-based thermodynamics and molecular dynamics calculations support these findings.
基金support by the National Natural Science Foundation of China(52201077)the Natural Science Foundation of Shandong Province(ZR2022QE191)+1 种基金Elite Scheme of Shandong University of Science and Technology(0104060541123)Talent introduction and Research Start-up Fund of Shandong University of Science and Technology(0104060510124).
文摘Coating microdefects and localized corrosion in coating/metal system are inevitable,accelerating the degradation of metal infrastructure.Early evaluating coating microdefects and detecting corrosion sites are urgent yet remain challenge to achieve.Herein,we propose a robust,universal and efficient fluorescence-based strategy for hierarchical warning of coating damage and metal corrosion by introducing the concepts of damage-induced fluorescence enhancement effect(DIE)and ionic-recognition induced quenching effect(RIQ).The coatings with dualresponsiveness for coating defect and steel corrosion are constructed by incorporating synthesized nanoprobes composed of metal organic frameworks(Ni–Zn-MOFs)loaded with Rhodamine B(RhB@MOFs).The initial damage to the coating causes an immediate intensification of fluorescence,while the specific ionic-recognition characteristic of RhB with Fe3t results in an evident fluorescence quenching,enabling the detection of coating damage and corrosion.Importantly,this nanoprobes are insensitive to the coating matrix and exhibit stable corrosion warning capability across various coating systems.Meanwhile,electrochemical investigations indicate that the impedance values of RM/EP maintain above 10^(8)Ωcm^(2)even after 60 days of immersion.Therefore,the incorporation of fluorescent nanoprobes greatly inhibits the intrusion of electrolytes into polymer and improves the corrosion protection performance of the coating.This powerful strategy towards dual-level damage warning provides insights for the development of long-term smart protective materials.
基金supported by National R&D Program through the National Research Foundation of Korea(NRF)funded by Ministry of Science and ICT(Nos.2022R1F1A1072420 and NRF-2020R1A3B2079803).
文摘The continuous depletion of fossil fuels and the effects of climate change have encouraged prompt action to attain carbon neutrality.Technologies that transform and store renewable energy are crucial for creating a sustainable society,which is independent of fossil fuels.In this regard,electrochemical water splitting based on the oxygen evolution reaction(OER)and hydrogen evolution reaction(HER)is an attractive technique for producing carbon-free hydrogen fuels.Additionally,rechargeable metal–air batteries(MABs)are another intriguing way for renewable energy storage through reversible oxygen reactions(OER and the oxygen reduction reaction,ORR).Herein,we comprehensively review bifunctional electrocatalysts for water splitting(HER and OER)and MABs(OER and ORR),particularly 2D carbon material-derived heterostructures.The synthesis and properties of 2D carbon materials and their energy conversion and storage mechanisms are discussed to highlight the bifunc-tionality of the heterostructures.Recent studies on bifunctional electrocatalysts based on 2D carbon-derived heterostructures are also reviewed.Finally,perspectives for future studies and multifunctional catalysts are presented.
基金supported by the National Key R&D Program of China under Project 2019YFA0705104GRF under Project CityU11212920.
文摘Electrochemical CO_(2)reduction has been considered a promising approach to neutralizing the global CO_(2)level.As an intriguing technique,metal-CO_(2)battery devices can not only capture CO_(2)into valuable carbonaceous chem-icals and reduce the CO_(2)concentration in the atmosphere but enable energy conversion.Among metal-CO_(2)batteries,aqueous Zn–CO_(2)batteries,especially rechargeable systems,exhibit flexible CO_(2)electrochemistry in terms of multi-carbon chemicals,which are gaseous or water-soluble,in favor of rechargeability and cycling durability of aqueous battery systems.Despite the increasing number of publications on Zn–CO_(2)batteries in the past three years,this field is still in its beginning stage and facing many challenges considering the capability of CO_(2)fixation and battery performance.Herein,we present a timely and overall summary of the recent progress in Zn–CO_(2)batteries,including fundamental mechanisms,affecting factors on electrochemical performance,catalyst cathodes,and electrolytes(catholytes and anolytes).Besides,we assess the application potential of Zn–CO_(2)batteries and compare this with those of alkali metal-CO_(2)batteries based on CO_(2)fixation and battery perfor-mance.Finally,we point out some current challenges for the further development of Zn–CO_(2)batteries and put forward perspectives of the research directions for practical applications of Zn–CO_(2)batteries in the future.
基金supported by the National Natural Science Foundation of China(No.51962002)Guangxi Natural Science Foundation(No.2022GXNSFAA035463).
文摘In recent years,the demand for high-performance rechargeable lithium batteries has increased significantly,and many efforts have been made to boost the use of advanced electrode materials.Since graphene was first isolated by Novoselov et al.,graphene/graphene-based materials have become an active area of research and are considered to be promising high-performance electrode materials.Graphene is a two-dimensional single-atom carbon-packed material that possesses fascinating properties,including a large surface area,remarkable electrical conductivity,extraordinary intrinsic electron mobility,high Young's modulus,superior mechanical strength,optical transmittance,catalytic performance,and stability.Therefore,graphene is considered an attractive ma-terial for rechargeable lithium-ion batteries(LIBs),lithium-sulfur batteries(LSBs),and lithium-oxygen batteries(LOBs).In this comprehensive review,we emphasise the recent progress in the controllable synthesis,func-tionalisation,and role of graphene in rechargeable lithium batteries.Finally,in this review,we aim to address the most promising results,benefits,challenges,critical issues,research directions,and perspectives to explain the developmental directions of graphene for batteries.
基金supported by the National Natural Science Foundation of China(No.62404041)the Natural Science Foundation of Jiangsu Province of China(No.BK20230830).
文摘Owing to the outstanding optoelectronic properties of perovskite materials,perovskite solar cells(PSCs)have been widely studied by academic organizations and industry corporations,with great potential to become the next-generation commercial solar cells.However,critical challenges remain in preserving high efficiency practical large-scale commercialized PSCs:a)the long-term stability of the cell materials and devices,b)lead leakage,and c)methods to scale the cells for larger area applications.This paper summarizes the prior-art strategies to address the above challenges,including the latest studies on the traditional glass-glass and thin-film encapsulation methods to better improve the reliability of PSCs,new technologies for preventing lead leakage,and geometric improvement strategies to enhance the reliability,efficiency,and performance of perovskite solar modules(PSMs).Through these strategies,the device achieved enhanced performance in long-term stability tests.The encapsulation resulted in a high lead leakage inhibition rate of up to 99%,and the PSMs possessed a geometric fill factor of 99.6%and a power conversion efficiency(PCE)of 20.7%.The dramatic improvement of efficiency and reliability of perovskite solar cells and modules indicate the great potential for mass production and commer-cialization of perovskite solar applications in the near future.
基金supported by the National Key R&D Program of China(No.2021YFA1501002)Thousand Talents Program for Distinguished Young Scholars.X.Li thanks the National Natural Science Foundation of China(No.22309021).
文摘Nanocrystals have emerged as cutting-edge functional materials benefiting from the increased surface and enhanced coupling of electronic states.High-resolution imaging in transmission electron microscope can provide invaluable structural information of crystalline materials,albeit it remains greatly challenging to nanocrystals due to the arduousness of accurate zone axis adjustment.Herein,a homemade software package,called SmartAxis,is developed for rapid yet accurate zone axis alignment of nanocrystals.Incident electron beam tilt is employed as an eccentric goniometer to measure the angular deviation of a crystal to a zone axis,and then serves as a linkage to calculate theαandβtilts of goniometer based on an accurate quantitative relationship.In this way,high-resolution imaging of one identical small Au nanocrystal,as well as electron beam-sensitive MIL-101 metal-organic framework crystals,along multiple zone axes,was performed successfully by using this accurate,time-and electron dose-saving zone axis alignment software package.
基金supported by the National Natural Science Foundation of China(NSFC No.52372200)the Postgraduate Research&Practice Innovation Program of Jiangsu Province(No.KYCX23_0360).
文摘To accelerate the development of lithium-ion batteries(LIBs),researchers should urgently exploit next-generation electrodes with high specific capacity,long cycle stability,and excellent rate performance,such as TMOs,silicon-based materials,and alloys.Among all the modification measures,hierarchical micro-nano structure and yolk–shell structure are considered suitable and effective ways to improve the electrochemical performance of those novel materials.Herein,a facile glucose-assisted solvothermal method combined with heat treatment was implemented to synthesize hierarchical micro-nano yolk–shell V_(2)O_(3).The special-structured material exhibited higher specific capacity,better structure stability,and faster electrochemical kinetics compared with nanosheet-structured and micro-nano-cluster-structured V_(2)O_(3).When used as an anode for LIB,mnYS-V_(2)O_(3)delivered high specific capacity of 650.1 mA h g^(-1)after over 500 cycles at a current density of 100 mA g^(-1),with a retention of 93.4%.Moreover,the morphology evolution mechanism of micro-nano structure and yolk–shell structure was investigated in this work,which is beneficial to the design of other mnYS-structured TMOs.
基金supported by the National Natural Science Foundation of China(62374142,12175189 and 11904302)External Cooperation Program of Fujian(2022I0004)+1 种基金Fundamental Research Funds for the Central Universities(20720190005 and 20720220085)Major Science and Technology Project of Xiamen in China(3502Z20191015).
文摘The preparation of red,green,and blue quantum dot(QD)pixelated arrays with high precision,resolution,and brightness poses a significant challenge on the development of advanced micro-displays for virtual,augmented,and mixed reality applications.Alongside the controlled synthesis of high-performance QDs,a reliable QD patterning technology is crucial in overcoming this challenge.Among the various methods available,photolithography-based patterning technologies show great potentials in producing ultra-fine QD patterns at micron scale.This review article presents the recent advancements in the field of QD patterning using photolithography techniques and explores their applications in micro-display technology.Firstly,we discuss QD patterning through photolithography techniques employing photoresist(PR),which falls into two categories:PRassisted photolithography and photolithography of QDPR.Subsequently,direct photolithography techniques based on photo-induced crosslinking of photosensitive groups and photo-induced ligand cleavage mechanisms are thoroughly reviewed.Meanwhile,we assess the performance of QD arrays fabricated using these photolithography techniques and their integration into QD light emitting diode display devices as well as color conversionbased micro light emitting diode display devices.Lastly,we summarize the most recent developments in this field and outline future prospects.
基金supported by a Discovery Early Career Researcher Award (DECRA,No.DE180101478) of the Australian Research CouncilNational Natural Science Foundation of China (Youth Program,No.52204378).
文摘Aqueous-electrolyte-based zinc-ion batteries(ZIBs),which have significant advantages over other batteries,including low cost,high safety,high ionic conductivity,and a natural abundance of zinc,have been regarded as a potential alternative to lithium-ion batteries(LIBs).ZIBs still face some critical challenges,however,especially for building a reversible zinc anode.To address the reversibility of zinc anode,great efforts have been made on intrinsic anode engineering and anode interface modification.Less attention has been devoted to the electrolyte additives,however,which could not only significantly improve the reversibility of zinc anode,but also determine the viability and overall performance of ZIBs.This review aims to provide an overview of the two main functions of electrolyte additives,followed by details on six reasons why additives might improve the performance of ZIBs from the perspectives of creating new layers and regulating current plating/stripping processes.Furthermore,the remaining difficulties and potential directions for additives in aqueous ZIBs are also highlighted.
文摘ArticlenArticle types Articles commonly fall into one of three main categories:Fulllength articles,Review articles and Short communications.Full-length articles are original,unpublished primary research.Extensions of work that has been published previously in short form such as a Communication are usually acceptable.Short communications must contain original and highly significant work whose high novelty warrants rapid publication.Review articles may be an authoritative overview of a field,a comprehensive literature reviews,or tutorial-style reference materials.Reviews are usually invited by the editor,but a topic may be proposed by an author via the editorial office.
基金supported by General Research Grants (GRF Project No. 11212021 and No. 11210822) from the Research Grants Council of the Hong Kong Special Administrative Regionthe Innovation and Technology Fund (Project No. ITS/065/20GHP/096/19SZ) from Innovation and Technology Commission of Hong Kong Special Administrative Region
文摘The mass discarding face masks has caused severe environmental problems during and after the COVID-19 pandemic.To reduce waste and minimize environmental impact,we present a new face mask featuring selfcharging extended service time and fully biodegradable materials.To extend the effective service time,we need to supplement the lost electric charge of the electret layer of face masks,for which task we propose to use the piezoelectric effect and generate electricity from breathing motions.However,existing piezoelectric materials are either toxic,impermeable,rigid,costly,or non-degradable.We synthesize a fully biodegradable piezoelectric membrane composed of polyvinyl alcohol(PVA)and glycine(GLY)via the electrospinning process.Parameters are accurately controlled to ensure that glycine crystallizes into a highly piezoelectricβphase during electrospinning and enables piezoelectric responses of the filter membrane.Tested with the standard 0.3μm particles,face masks made of the PVA-GLY membrane show an outstanding filtration efficiency of 97%,which remains stable over at least 10 h of high-concentration continuous filtration.Furthermore,we demonstrated the biodegradability of PVA-GLY masks,which can degrade completely within a few weeks,compared to commonly used surgical masks requiring over thirty years to be decomposed.
文摘Excessive emissions of greenhouse gases such as carbon dioxide have led to global climate change,which poses one of the greatest threats to human survival in the 21st century.The urgent need to achieve carbon neutrality to mitigate climatic issues has stimulated the rapid development of advanced materials and technologies for clean energy conversion and efficient storage.In recent years,a series of remarkable advances have emerged,revealing innovative materials and strategies that significantly accelerate the transition toward sus-tainable energy solutions.In this context,this special issue presents ten high-quality contributions,including seven comprehensive reviews and three original research articles[1-10],focusing on the latest ad-vances and frontier research in advanced materials and technologies toward carbon neutrality.Collectively,these works highlight the latest progress in catalytic energy conversion,photovoltaic technologies,and electrochemical energy storage,providing valuable insights to guide future efforts in the design of carbon-neutral materials and sustainable energy systems.
文摘Two-dimensional(2D)materials have attracted considerable research interest due to their precisely defined properties and versatile applications.In this realm,borophene-a single atomic sheet of boron atoms arranged in a honeycomb lattice-has emerged as a promising candidate.While borophenes were theoretically predicted to have unique structural,optical,and electronic properties,the experimental synthesis of crystalline borophene sheets was first demonstrated on metal substrates in 2015,marking a crucial milestone.Since then,research efforts have focused on controlling the synthesis of semiconducting borophene polymorphs and exploring their novel physical characteristics.This review aims to explore the potential of 2D materials,specifically borophene,in various technological fields such as batteries,supercapacitors,fuel cells,and more.The analysis emphasises meticulous scrutiny of synthesis techniques due to their fundamental importance in realising borophene's properties.Specifically,the high carrier mobilities,tuneable bandgaps,and exceptional thermal conductivity of borophene are highlighted.By providing a comprehensive outlook on the significance of borophene in advancing materials science and technologies,this review contributes to shaping the landscape of 2D material research.
基金funded by the Horizon Europe Project"PERSEUS"(No.101099423)financed by the Ministry of Universities under application 33.50.460A.752by the European Union NextGenerationEU/PRTR through a contract Margarita Salas from Universidade de Vigo.
文摘Photodynamic therapy(PDT)has been established as one of the most promising novel cancer therapies with fewer side-effects and enhanced efficacy compared to the currently available conventional treatments.However,its application has been hindered by the limitations that photosensitizers(PS)have.The combination of PS with metallic nanoparticles like platinum nanoparticles(PtNPs),can help to overcome these intrinsic drawbacks.In this work,the combination of PtNPs and the natural photosensitizer riboflavin(RF)is proposed.PtNPs are synthesized using RF(Pt@RF)as reducing and stabilizing agent in a one-step method,obtaining nanoparticles with mesoporous structure for UV triggered PDT.In view of possible future UV irradiation treatments,the degradation products of RF,ribitol(RB)and lumichrome(LC),this last being a photosensitizing byproduct,are also employed for the synthesis of porous PtNPs,obtaining Pt@LC and Pt@RB.When administered in vitro to lung cancer cells,all the samples elicit a strong decrease of cell viability and a decrease of intracellular ATP levels.The antitumoral effect of both Pt@RF and Pt@LC is triggered by UV-A irradiation.This antitumoral activity is caused by the induction of oxidative stress,shown in our study by the decrease in intracellular glutathione and increased expression of antioxidant enzymes.
文摘Cancer treatment often requires a multimodal approach,such as combining chemotherapy and gene therapy.However,challenges such as low therapeutic efficacy and off-target effects hinder the effectiveness of these treatments.In this study,the use of calcium-doped metal-organic frameworks Cu_(2)(BDC)_(2)(DABCO)as a nanocarrier platform for the co-delivery of doxorubicin(DOX)and plasmid CRISPR(pCRISPR)proposed to enhance anticancer efficiency.We demonstrated that Ca-doped MOF nanocarriers significantly improved the uptake of DOX and pCRISPR by in cancer cells.The co-delivery of DOX and pCRISPR with Ca-doped MOF nanocarriers resulted in a significant rise in cell death and decreased targeted gene expression.
文摘Article ■Article types Articles commonly fall into one of three main categories:Fulllength articles,Review articles and Short communications.Full-length articles are original,unpublished primary research.Extensions of work that has been published previously in short form such as a Communication are usually acceptable.
基金supported by the Hong Kong Research Grants Council(No.CityU 11201522).
文摘Metal-organic frameworks(MOFs)have been considered as great contender and promising electrode materials for supercapacitors.However,their low capacity,aggregation,and poor porosity have necessitated the exploration of new approaches to enhance the performance of these active materials.In this study,sphere-like MOF were in-situ grown and it subsequently burst,transformed into a desired metal oxide heterostructure comprising n-type ZnO and p-type NiO(ZnO/NiO-350).The resulting optimized flower-like structure,composed of interlaced nanoflakes derived from MOFs,greatly improved the active sites,porosity,and functionality of the electrode materials.The ZnO/NiO-350 electrode exhibited superior electrochemical activities for supercapacitors,compared to the parent MOF,bare n-type,and p-type counterparts.The specific capacitance can reach to 543 F g^(-1) at a current density of 1 A g^(-1).Theoretical modeling and simulations were employed to gain insights into the atomic-scale properties of the materials.Furthermore,an assembled hybrid device using active carbon and ZnO/NiO-350 as electrodes demonstrated excellent energy density of 44 Wh kg^(-1) at a power density of 1.6 Kw kg^(-1).After 5000 cycles at 10 A g^(-1),the cycling stability remained excellent 80%of the initial capacitance.Overall,such evaluation of unique electrode with superior properties may be useful for the next generation supercapacitor electrode.
基金supported by (Dr. Manika Khanuja, Nanomission, (DST)[DST/NM/NB/2018/203(G) (JMI)]UGC grant (No.F.4(201-FRP)/2015 (BSR))
文摘The endocrine-disrupting chemicals(EDCs)and antibiotics are causing negative effects on human beings and animals by disrupting the endocrine system and spreading antimicrobial resistance.The current need is to eradicate pharmaceutical waste from water bodies using advanced catalytic systems with high efficiency.Novel ternary carbon quantum dots(CQDs)decorated Z-Scheme WS_(2)-PANI nanocomposite was prepared by a green synthesis assisted in-situ polymerization for the photodegradation and detection of Estradiol(EST)and Nitrofurantoin(NFT).HRTEM micrographs revealed the formation of CQDs with a mean size of 4nm anchored on the surface of WS_(2)/PANI(width:PANI~20-30nm).The ternary nanocomposite showed excellent photocatalytic activity,degraded NFT(95.7%in 60min),and EST(96.6%in 60min).The rate kinetics study confirms the reaction followed pseudo first-order model.This heterostructure exhibited enhanced performances by modulating the energy level configuration,enhancing the absorption of visible light(2.4eV),and significantly improving the charge separation,three times higher than pristine WS_(2).These are highly favorable for increasing the generation of photoinduced charges and enhancing the overall performance of the catalyst.Further,the electrochemical sensor was prepared using CQDs@WS_(2)/PANI nanocomposite on a paper-based electrode.The CQDs@WS_(2)/PANI exhibit a linear response of 0.1-100nM,with a limit of detection of 13nM.This synergistic interfacial interaction resulted in the significantly improved electrochemical performance of the modified electrode.The proposed Z-scheme was justified by electron paramagnetic resonance(EPR)and scavenger experiment.An intermediate degradation pathway was also proposed.The synthesized materials were characterized using FESEM,HRTEM,XRD,FTIR,XPS,UV-visible spectroscopy,PL,and TRPL.Therefore,this study provides a direct approach to fabricate a heterojunction that combines two-dimensional,one dimensional,and zero-dimensional properties,enabling control over the energy level configuration and subsequent improvements in photocatalytic and electrocatalytic efficiency.
