Aqueous organic redox flow batteries(AORFBs),which exploit the reversible electrochemical reactions of water-soluble organic electrolytes to store electricity,have emerged as an efficient electrochemical energy storag...Aqueous organic redox flow batteries(AORFBs),which exploit the reversible electrochemical reactions of water-soluble organic electrolytes to store electricity,have emerged as an efficient electrochemical energy storage technology for the grid-scale integration of renewable electricity.pH-neutral AORFBs that feature high safety,low corrosivity,and environmental benignity are particularly promising,and their battery performance is significantly impacted by redox-active molecules and ion-exchange membranes(IEMs).Here,representative anolytes and catholytes engineered for use in pH-neutral AORFBs are outlined and summarized,as well as their side reactions that cause irreversible battery capacity fading.In addition,the recent achievements of IEMs for pH-neutral AORFBs are discussed,with a focus on the construction and tuning of ion transport channels.Finally,the critical challenges and potential research opportunities for developing practically relevant pH-neutral AORFBs are presented.展开更多
This work focuses on the development of high temperature polymer electrolyte membranes(HT-PEMs)as key materials for HT-PEM fuel cells(HT-PEMFCs).Recognizing the challenges associated with the phosphoric acid(PA) doped...This work focuses on the development of high temperature polymer electrolyte membranes(HT-PEMs)as key materials for HT-PEM fuel cells(HT-PEMFCs).Recognizing the challenges associated with the phosphoric acid(PA) doped polybenzimidazole(PBI) membranes,including the use of carcinogenic monomers and complex synthesis procedures,this study aims to develop more cost-effective,readily synthesized,and high-performance alternatives.A series of superacid-catalyzed polyhydroxyalkylation reactions have been carefully designed between p-terphenyl and aldehydes bearing imidazole moieties,resulting in a new class of HT-PEMs.It is found that the chemical structure of aldehyde-substituted N-heterocycles significantly impacts the polymerization reaction.Specifically,the use of 1-methyl-2-imidazole-formaldehyde and 1 H-imidazole-4-formaldehyde monomers leads to the formation of high-viscosity,rigid,and ether-free polymers,denoted as PTIm-a and PTIm-b.Membranes fabricated from these polymers,due to their pendent imidazole groups,exhibit an exceptional capacity for PA absorption.Notably,PTIm-a,carrying methylimidazole moieties,demonstrates a superior chemical stability by maintaining morphology and structural stability during 350 h of Fenton testing.After being immersed in 75 wt% PA at 40℃,the PTIm-a membrane reaches a PA content of 152%,maintains a good tensile strength of 13.6 MPa,and exhibits a moderate conductivity of 50.2 mS cm^(-1) at 180℃.Under H_(2)/O_(2) operational conditions,a single cell based on the PTIm-a membrane attains a peak power density of 732 mW cm^(-2) at 180℃ without backpressure.Furthermore,the membrane demonstrates stable cycle stability over 173 h within 18 days at a current density of 200 mA cm^(-2),indicating its potential for practical application in HT-PEMFCs.This work highlights innovative strategies for the synthesis of advanced HT-PEMs,offering significant improvements in membrane properties and fuel cell performance,thus expanding the horizons of HT-PEMFC technology.展开更多
Sustainable agriculture plays a crucial role in meeting the growing global demand for food while minimizing adverse environmental impacts from the overuse of synthetic pesticides and conventional fertilizers.In this c...Sustainable agriculture plays a crucial role in meeting the growing global demand for food while minimizing adverse environmental impacts from the overuse of synthetic pesticides and conventional fertilizers.In this context,renewable biopolymers being more sustainable offer a viable solution to improve agricultural sustainability and production.Nano/micro-structural supramolecular biopolymers are among these innovative biopolymers that are much sought after for their unique features.These biomaterials have complex hierarchical structures,great stability,adjustable mechanical strength,stimuli-responsiveness,and self-healing attributes.Functional molecules may be added to their flexible structure,for enabling novel agricultural uses.This overview scrutinizes how nano/micro-structural supramolecular biopolymers may radically alter farming practices and solve lingering problems in agricultural sector namely improve agricultural production,soil health,and resource efficiency.Controlled bioactive ingredient released from biopolymers allows the tailored administration of agrochemicals,bioactive agents,and biostimulators as they enhance nutrient absorption,moisture retention,and root growth.Nano/micro-structural supramolecular biopolymers may protect crops by appending antimicrobials and biosensing entities while their eco-friendliness supports sustainable agriculture.Despite their potential,further studies are warranted to understand and optimize their usage in agricultural domain.This effort seeks to bridge the knowledge gap by investigating their applications,challenges,and future prospects in the agricultural sector.Through experimental investigations and theoretical modeling,this overview aims to provide valuable insights into the practical implementation and optimization of supramolecular biopolymers in sustainable agriculture,ultimately contributing to the development of innovative and eco-friendly solutions to enhance agricultural productivity while minimizing environmental impact.展开更多
With plenty of popular and effective ternary organic solar cells(OSCs)construction strategies proposed and applied,its power conversion efficiencies(PCEs)have come to a new level of over 19%in single-junction devices....With plenty of popular and effective ternary organic solar cells(OSCs)construction strategies proposed and applied,its power conversion efficiencies(PCEs)have come to a new level of over 19%in single-junction devices.However,previous studies are heavily based in chloroform(CF)leaving behind substantial knowledge deficiencies in understanding the influence of solvent choice when introducing a third component.Herein,we present a case where a newly designed asymmetric small molecular acceptor using fluoro-methoxylated end-group modification strategy,named BTP-BO-3FO with enlarged bandgap,brings different morphological evolution and performance improvement effect on host system PM6:BTP-eC9,processed by CF and ortho-xylene(o-XY).With detailed analyses supported by a series of experiments,the best PCE of 19.24%for green solvent-processed OSCs is found to be a fruit of finely tuned crystalline ordering and general aggregation motif,which furthermore nourishes a favorable charge generation and recombination behavior.Likewise,over 19%PCE can be achieved by replacing spin-coating with blade coating for active layer deposition.This work focuses on understanding the commonly met yet frequently ignored issues when building ternary blends to demonstrate cutting-edge device performance,hence,will be instructive to other ternary OSC works in the future.展开更多
The Nano-Micro Letters(2024)16:193,article by Shangguan et al.,entitled“Making the Complicated Simple:A Minimizing Carrier Strategy on Innovative Nanopesticides”(Nano-Micro Lett.https://doi.org/10.1007/s40820-024-01...The Nano-Micro Letters(2024)16:193,article by Shangguan et al.,entitled“Making the Complicated Simple:A Minimizing Carrier Strategy on Innovative Nanopesticides”(Nano-Micro Lett.https://doi.org/10.1007/s40820-024-01413-5),was published online on 14 May,2024,with errors.The structural formulas and captions of the three acyl chlorides in Fig.3A were wrong.They should be as shown below.展开更多
The lithium metal anode is hailed as the desired "holy grail" for the forthcoming generation of highenergy-density batteries,given its astounding theoretical capacity and low potential.Nonetheless,the format...The lithium metal anode is hailed as the desired "holy grail" for the forthcoming generation of highenergy-density batteries,given its astounding theoretical capacity and low potential.Nonetheless,the formation and growth of dendrites seriously compromise battery life and safety.Herein,an yttriastabilized bismuth oxide(YSB) layer is fabricated on the polypropylene(PP) separator,where YSB reacts with Li anode in-situ in the cell to form a multi-component composite interlayer consisting of Li_(3)Bi,Li_(2)O,and Y_(2)O_(3).The interlayer can function not only as a redistributor to regulate Li^(+) distribution but also as an anion adsorber to increase the Li^(+) transference number from 0.37 to 0.79 for suppressing dendrite nucleation and growth.Consequently,compared with the cell with a baseline separator,those with modified separators exhibit prolonged lifespan in both Li/Li symmetrical cells and Li/Cu half-cells.Notably,the full cells coupled with ultrahigh-loading LiFePO_(4) display an excellent cycling performance of 1700 cycles with a high capacity retention of ~80% at 1 C,exhibiting great potential for practical applications.This work provides a feasible and effective new strategy for separator modification towards building a much-anticipated dendrite-free Li anode and realizing long-lifespan lithium metal batteries.展开更多
The development of low-cost,abundant,and efficient non-metal catalysts has always been a research focus on photocatalytic hydrogen evolution reactions.Boron nitride nanosheet(BNNS),which is a promising non-metallic tw...The development of low-cost,abundant,and efficient non-metal catalysts has always been a research focus on photocatalytic hydrogen evolution reactions.Boron nitride nanosheet(BNNS),which is a promising non-metallic two-dimensional material,possesses remarkable properties.However,its inherently wide bandgap significantly limits their potential for visible-light-responsive catalysis,and conventional chemical methods struggle to overcome this limitation.In this study,we employed high-energy ionizing radiation to precisely regulate defect formation in BNNS at ambient temperature and pressure.The results showed that gamma-ray radiation markedly enhanced the efficiency of photocatalytic hydrogen production of the irradiated BNNS with increasing absorbed dose.The maximum hydrogen production rate of the samples reached 1033.7μmol/(g·h),which represents an increase of almost two orders of magnitude compared to commercial BNNS.The structural characterization also confirmed that the introduction of three-boron-center defects results in forming intermediate energy levels and improving the charge carrier separation efficiency of BNNS.This transformation converts BNNS from a wide bandgap semiconductor to a visible-light-responsive catalyst.This work not only provides a novel approach for the application of BNNS in visible-light photocatalysis,but also demonstrates the unique role of radiation technology in quantitatively regulating defects and improving catalytic activity.展开更多
Electrochemical reduction of CO_(2)(CO_(2)RR)has become a research hot spot in recent years in the context of carbon neutrality.HCOOH is one of the most promising products obtained by electrochemical reduction of CO_(...Electrochemical reduction of CO_(2)(CO_(2)RR)has become a research hot spot in recent years in the context of carbon neutrality.HCOOH is one of the most promising products obtained by electrochemical reduction of CO_(2) due to its high energy value as estimated by market price per energy unit and wide application in chemical industry.Biomass is the most abundant renewable resource in the natural world.Coupling biomass oxidative conversion with CO_(2)RR driven by renewable electricity would well achieve carbon negativity.In this work,we comprehensively reviewed the current research progress on CO_(2)RR to produce HCOOH and coupled system for conversion of biomass and its derivatives to produce value-added products.Sn-and Bi-based electrocatalysts are discussed for CO_(2)RR with regards to the structure of the catalyst and reaction mechanisms.Electro-oxidation reactions of biomass derived sugars,alcohols,furan aldehydes and even polymeric components of lignocellulose were reviewed as alternatives to replace oxygen evolution reaction(OER)in the conventional electrolysis process.It was recommended that to further improve the efficiency of the coupled system,future work should be focused on the development of more efficient and stable catalysts,careful design of the electrolytic cells for improving the mass transfer and development of environment-friendly processes for recovering the formed formate and biomass oxidation products.展开更多
Soft actuators have garnered substantial attention in current years in view of their potential appliances in diverse domains like robotics,biomedical devices,and biomimetic systems.These actuators mimic the natural mo...Soft actuators have garnered substantial attention in current years in view of their potential appliances in diverse domains like robotics,biomedical devices,and biomimetic systems.These actuators mimic the natural movements of living organisms,aiming to attain enhanced flexibility,adaptability,and versatility.On the other hand,angle-independent structural color has been achieved through innovative design strategies and engineering approaches.By carefully controlling the size,shape,and arrangement of nanostructures,researchers have been able to create materials exhibiting consistent colors regardless of the viewing angle.One promising class of materials that holds great potential for bioinspired soft actuators is MXenes in view of their exceptional mechanical,electrical,and optical properties.The integration of MXenes for bioinspired soft actuators with angle-independent structural color offers exciting possibilities.Overcoming material compatibility issues,improving color reproducibility,scalability,durability,power supply efficiency,and cost-effectiveness will play vital roles in advancing these technologies.This perspective appraises the development of bioinspired MXene-centered soft actuators with angleindependent structural color in soft robotics.展开更多
Highly-efficient oxidation of 5-hydroxymethylfurtural(HMF) to 2,5-furandicarboxylic acid(FDCA) at low temperature with air as the oxidant is still challenging.Herein,inspired by the respirato ry electron transport cha...Highly-efficient oxidation of 5-hydroxymethylfurtural(HMF) to 2,5-furandicarboxylic acid(FDCA) at low temperature with air as the oxidant is still challenging.Herein,inspired by the respirato ry electron transport chain(ETC) of living cells mediated by electron carriers,we constructed artificial ETCs and transformed liquid flow fuel cells(LFFCs) to flexible reactors for efficient oxidation of HMF to produce FDCA under mild conditions.This LFFC reactor employed an electrodeposition modified nickel foam as an anode to promote HMF oxidation and(VO_(2))_(2)SO_(4) as a cathode electron carrier to facilitate the electron transfer to air.The reaction rate could be easily controlled by selecting the anode catalyst,adjusting the external loading and changing the cathodic electron carrier or oxidants.A maximal power density of 44.9 mW cm^(-2) at room temperature was achieved,while for FDCA production,short-circuit condition was preferred to achieve quick transfer of electrons.For a single batch operation with 0.1 M initial HMF,FDCA yield reached 97.1%.By fed-batch operation,FDCA concentration reached 144.5 g L^(-1) with a total yield of 96%.Ni^(2+)/Ni^(3+) redox couple was the active species mediating the electron transfer,while both experimental and DFT calculation results indicated that HMFCA pathway was the preferred reaction mechanism.展开更多
In recent years,water evaporation-induced electricity has attracted a great deal of attention as an emerging green and renewable energy harvesting technology.Although abundant materials have been developed to fabricat...In recent years,water evaporation-induced electricity has attracted a great deal of attention as an emerging green and renewable energy harvesting technology.Although abundant materials have been developed to fabricate hydrovoltaic devices,the limitations of high costs,inconvenient storage and transport,low environmental benefits,and unadaptable shape have restricted their wide applications.Here,an electricity generator driven by water evaporation has been engineered based on natural biomass leather with inherent properties of good moisture permeability,excellent wettability,physicochemical stability,flexibility,and biocompatibility.Including numerous nano/microchannels together with rich oxygen-bearing functional groups,the natural leather-based water evaporator,Leather_(Emblic-NPs-SA/CB),could continuously produce electricity even staying outside,achieving a maximum output voltage of∼3 V with six-series connection.Furthermore,the leather-based water evaporator has enormous potential for use as a flexible self-powered electronic floor and seawater demineralizer due to its sensitive pressure sensing ability as well as its excellent photothermal conversion efficiency(96.3%)and thus fast water evaporation rate(2.65 kg m^(−2)h^(−1)).This work offers a new and functional material for the construction of hydrovoltaic devices to harvest the sustained green energy from water evaporation in arbitrary ambient environments,which shows great promise in their widespread applications.展开更多
The flourishing progress in nanotechnology offers boundless opportunities for agriculture,particularly in the realm of nanopesticides research and development.However,concerns have been raised regarding the human and ...The flourishing progress in nanotechnology offers boundless opportunities for agriculture,particularly in the realm of nanopesticides research and development.However,concerns have been raised regarding the human and environmental safety issues stemming from the unrestrained use of non-therapeutic nanomaterials in nanopesticides.It is also important to consider whether the current development strategy of nanopesticides based on nanocarriers can strike a balance between investment and return,and if the complex material composition genuinely improves the efficiency,safety,and circularity of nanopesticides.Herein,we introduced the concept of nanopesticides with minimizing carriers(NMC)prepared through prodrug design and molecular self-assembly emerging as practical tools to address the current limitations,and compared it with nanopesticides employing non-therapeutic nanomaterials as carriers(NNC).We further summarized the current development strategy of NMC and examined potential challenges in its preparation,performance,and production.Overall,we asserted that the development of NMC systems can serve as the innovative driving force catalyzing a green and efficient revolution in nanopesticides,offering a way out of the current predicament.展开更多
Dialysis plays a crucial role in the purification of nanomaterials but its impact on the structural properties of carbon nanomaterials was never investigated.Herein,a carbon-based nanomaterial generated electrochemica...Dialysis plays a crucial role in the purification of nanomaterials but its impact on the structural properties of carbon nanomaterials was never investigated.Herein,a carbon-based nanomaterial generated electrochemically in potassium phosphate buffer,was characterized before and after dialysis against pure water.It is shown that dialysis affects the size of the carbon domains,structural organization,surface functionalization,oxidation degree of carbon,and grade of amorphicity.Accordingly,dialysis drives the nanomaterial organization from discrete roundish carbon domains,with sizes ranging from 70 to 160 nm,towards linear stacking structures of small nanoparticles(<15 nm).In parallel,alcohol and ether(epoxide)surface groups evolve into more oxidized carbon groups(e.g.,ketone and ester groups).Investigation of the as-prepared nanomaterial by electron paramagnetic resonance(EPR)revealed a resonance signal consistent with carbon-oxygen centred radicals.Additionally,this study brings to light the selective affinity of the carbon nanomaterial under study to capture Na^(+)ions,a property greatly enhanced by the dialysis process,and its high ability to trap oxygen,particularly before dialysis.These findings open new perspectives for the application of carbon-based nanomaterials and raise awareness of the importance of structural changes that can occur during the purification of carbon-based nanomaterials.展开更多
基金funded by the National Key Research and Development Program of China(Nos.2022YFB3805303,2022YFB3805304)the National Natural Science Foundation of China(Grant/Award Numbers:22308345,U20A20127)+1 种基金the Anhui Provincial Natural Science Foundation(No.2308085QB68)the Fundamental Research Funds for the Central Universities(No.WK2060000059).
文摘Aqueous organic redox flow batteries(AORFBs),which exploit the reversible electrochemical reactions of water-soluble organic electrolytes to store electricity,have emerged as an efficient electrochemical energy storage technology for the grid-scale integration of renewable electricity.pH-neutral AORFBs that feature high safety,low corrosivity,and environmental benignity are particularly promising,and their battery performance is significantly impacted by redox-active molecules and ion-exchange membranes(IEMs).Here,representative anolytes and catholytes engineered for use in pH-neutral AORFBs are outlined and summarized,as well as their side reactions that cause irreversible battery capacity fading.In addition,the recent achievements of IEMs for pH-neutral AORFBs are discussed,with a focus on the construction and tuning of ion transport channels.Finally,the critical challenges and potential research opportunities for developing practically relevant pH-neutral AORFBs are presented.
基金Natural Science Foundation of China (51603031)Liaoning Provincial Natural Science Foundation of China (2020-MS-087)China Scholarship Council(202306080157)。
文摘This work focuses on the development of high temperature polymer electrolyte membranes(HT-PEMs)as key materials for HT-PEM fuel cells(HT-PEMFCs).Recognizing the challenges associated with the phosphoric acid(PA) doped polybenzimidazole(PBI) membranes,including the use of carcinogenic monomers and complex synthesis procedures,this study aims to develop more cost-effective,readily synthesized,and high-performance alternatives.A series of superacid-catalyzed polyhydroxyalkylation reactions have been carefully designed between p-terphenyl and aldehydes bearing imidazole moieties,resulting in a new class of HT-PEMs.It is found that the chemical structure of aldehyde-substituted N-heterocycles significantly impacts the polymerization reaction.Specifically,the use of 1-methyl-2-imidazole-formaldehyde and 1 H-imidazole-4-formaldehyde monomers leads to the formation of high-viscosity,rigid,and ether-free polymers,denoted as PTIm-a and PTIm-b.Membranes fabricated from these polymers,due to their pendent imidazole groups,exhibit an exceptional capacity for PA absorption.Notably,PTIm-a,carrying methylimidazole moieties,demonstrates a superior chemical stability by maintaining morphology and structural stability during 350 h of Fenton testing.After being immersed in 75 wt% PA at 40℃,the PTIm-a membrane reaches a PA content of 152%,maintains a good tensile strength of 13.6 MPa,and exhibits a moderate conductivity of 50.2 mS cm^(-1) at 180℃.Under H_(2)/O_(2) operational conditions,a single cell based on the PTIm-a membrane attains a peak power density of 732 mW cm^(-2) at 180℃ without backpressure.Furthermore,the membrane demonstrates stable cycle stability over 173 h within 18 days at a current density of 200 mA cm^(-2),indicating its potential for practical application in HT-PEMFCs.This work highlights innovative strategies for the synthesis of advanced HT-PEMs,offering significant improvements in membrane properties and fuel cell performance,thus expanding the horizons of HT-PEMFC technology.
基金support provided by the UKRI via Grant No.EP/T024607/1Royal Society via grant number IES\R2\222208.
文摘Sustainable agriculture plays a crucial role in meeting the growing global demand for food while minimizing adverse environmental impacts from the overuse of synthetic pesticides and conventional fertilizers.In this context,renewable biopolymers being more sustainable offer a viable solution to improve agricultural sustainability and production.Nano/micro-structural supramolecular biopolymers are among these innovative biopolymers that are much sought after for their unique features.These biomaterials have complex hierarchical structures,great stability,adjustable mechanical strength,stimuli-responsiveness,and self-healing attributes.Functional molecules may be added to their flexible structure,for enabling novel agricultural uses.This overview scrutinizes how nano/micro-structural supramolecular biopolymers may radically alter farming practices and solve lingering problems in agricultural sector namely improve agricultural production,soil health,and resource efficiency.Controlled bioactive ingredient released from biopolymers allows the tailored administration of agrochemicals,bioactive agents,and biostimulators as they enhance nutrient absorption,moisture retention,and root growth.Nano/micro-structural supramolecular biopolymers may protect crops by appending antimicrobials and biosensing entities while their eco-friendliness supports sustainable agriculture.Despite their potential,further studies are warranted to understand and optimize their usage in agricultural domain.This effort seeks to bridge the knowledge gap by investigating their applications,challenges,and future prospects in the agricultural sector.Through experimental investigations and theoretical modeling,this overview aims to provide valuable insights into the practical implementation and optimization of supramolecular biopolymers in sustainable agriculture,ultimately contributing to the development of innovative and eco-friendly solutions to enhance agricultural productivity while minimizing environmental impact.
基金R.Ma thanks the support from PolyU Distinguished Postdoc Fellowship(1-YW4C)Z.Luo thanks the National Natural Science Foundation of China(NSFC,No.22309119)+7 种基金J.Wu thanks the Guangdong government and the Guangzhou government for funding(2021QN02C110)the Guangzhou Municipal Science and Technology Project(No.2023A03J0097 and 2023A03J0003)H.Yan appreciates the support from the National Key Research and Development Program of China(No.2019YFA0705900)funded by MOST,the Basic and Applied Research Major Program of Guangdong Province(No.2019B030302007)the Shen Zhen Technology and Innovation Commission through(Shenzhen Fundamental Research Program,JCYJ20200109140801751)the Hong Kong Research Grants Council(research fellow scheme RFS2021-6S05,RIF project R6021-18,CRF project C6023‐19G,GRF project 16310019,16310020,16309221,and 16309822)Hong Kong Innovation and Technology Commission(ITC‐CNERC14SC01)Foshan‐HKUST(Project NO.FSUST19‐CAT0202)Zhongshan Municipal Bureau of Science and Technology(NO.ZSST20SC02)and Tencent Xplorer Prize。
文摘With plenty of popular and effective ternary organic solar cells(OSCs)construction strategies proposed and applied,its power conversion efficiencies(PCEs)have come to a new level of over 19%in single-junction devices.However,previous studies are heavily based in chloroform(CF)leaving behind substantial knowledge deficiencies in understanding the influence of solvent choice when introducing a third component.Herein,we present a case where a newly designed asymmetric small molecular acceptor using fluoro-methoxylated end-group modification strategy,named BTP-BO-3FO with enlarged bandgap,brings different morphological evolution and performance improvement effect on host system PM6:BTP-eC9,processed by CF and ortho-xylene(o-XY).With detailed analyses supported by a series of experiments,the best PCE of 19.24%for green solvent-processed OSCs is found to be a fruit of finely tuned crystalline ordering and general aggregation motif,which furthermore nourishes a favorable charge generation and recombination behavior.Likewise,over 19%PCE can be achieved by replacing spin-coating with blade coating for active layer deposition.This work focuses on understanding the commonly met yet frequently ignored issues when building ternary blends to demonstrate cutting-edge device performance,hence,will be instructive to other ternary OSC works in the future.
文摘The Nano-Micro Letters(2024)16:193,article by Shangguan et al.,entitled“Making the Complicated Simple:A Minimizing Carrier Strategy on Innovative Nanopesticides”(Nano-Micro Lett.https://doi.org/10.1007/s40820-024-01413-5),was published online on 14 May,2024,with errors.The structural formulas and captions of the three acyl chlorides in Fig.3A were wrong.They should be as shown below.
基金supported by the National Nature Science Foundation of China [52172247, 21875237]the National Key R&D Program of China [2018YFB0905400]。
文摘The lithium metal anode is hailed as the desired "holy grail" for the forthcoming generation of highenergy-density batteries,given its astounding theoretical capacity and low potential.Nonetheless,the formation and growth of dendrites seriously compromise battery life and safety.Herein,an yttriastabilized bismuth oxide(YSB) layer is fabricated on the polypropylene(PP) separator,where YSB reacts with Li anode in-situ in the cell to form a multi-component composite interlayer consisting of Li_(3)Bi,Li_(2)O,and Y_(2)O_(3).The interlayer can function not only as a redistributor to regulate Li^(+) distribution but also as an anion adsorber to increase the Li^(+) transference number from 0.37 to 0.79 for suppressing dendrite nucleation and growth.Consequently,compared with the cell with a baseline separator,those with modified separators exhibit prolonged lifespan in both Li/Li symmetrical cells and Li/Cu half-cells.Notably,the full cells coupled with ultrahigh-loading LiFePO_(4) display an excellent cycling performance of 1700 cycles with a high capacity retention of ~80% at 1 C,exhibiting great potential for practical applications.This work provides a feasible and effective new strategy for separator modification towards building a much-anticipated dendrite-free Li anode and realizing long-lifespan lithium metal batteries.
文摘The development of low-cost,abundant,and efficient non-metal catalysts has always been a research focus on photocatalytic hydrogen evolution reactions.Boron nitride nanosheet(BNNS),which is a promising non-metallic two-dimensional material,possesses remarkable properties.However,its inherently wide bandgap significantly limits their potential for visible-light-responsive catalysis,and conventional chemical methods struggle to overcome this limitation.In this study,we employed high-energy ionizing radiation to precisely regulate defect formation in BNNS at ambient temperature and pressure.The results showed that gamma-ray radiation markedly enhanced the efficiency of photocatalytic hydrogen production of the irradiated BNNS with increasing absorbed dose.The maximum hydrogen production rate of the samples reached 1033.7μmol/(g·h),which represents an increase of almost two orders of magnitude compared to commercial BNNS.The structural characterization also confirmed that the introduction of three-boron-center defects results in forming intermediate energy levels and improving the charge carrier separation efficiency of BNNS.This transformation converts BNNS from a wide bandgap semiconductor to a visible-light-responsive catalyst.This work not only provides a novel approach for the application of BNNS in visible-light photocatalysis,but also demonstrates the unique role of radiation technology in quantitatively regulating defects and improving catalytic activity.
基金supported by the National Key R&D Program of China(2022YFA2105900)the National Natural Science Foundation of China(No.22178197)。
文摘Electrochemical reduction of CO_(2)(CO_(2)RR)has become a research hot spot in recent years in the context of carbon neutrality.HCOOH is one of the most promising products obtained by electrochemical reduction of CO_(2) due to its high energy value as estimated by market price per energy unit and wide application in chemical industry.Biomass is the most abundant renewable resource in the natural world.Coupling biomass oxidative conversion with CO_(2)RR driven by renewable electricity would well achieve carbon negativity.In this work,we comprehensively reviewed the current research progress on CO_(2)RR to produce HCOOH and coupled system for conversion of biomass and its derivatives to produce value-added products.Sn-and Bi-based electrocatalysts are discussed for CO_(2)RR with regards to the structure of the catalyst and reaction mechanisms.Electro-oxidation reactions of biomass derived sugars,alcohols,furan aldehydes and even polymeric components of lignocellulose were reviewed as alternatives to replace oxygen evolution reaction(OER)in the conventional electrolysis process.It was recommended that to further improve the efficiency of the coupled system,future work should be focused on the development of more efficient and stable catalysts,careful design of the electrolytic cells for improving the mass transfer and development of environment-friendly processes for recovering the formed formate and biomass oxidation products.
文摘Soft actuators have garnered substantial attention in current years in view of their potential appliances in diverse domains like robotics,biomedical devices,and biomimetic systems.These actuators mimic the natural movements of living organisms,aiming to attain enhanced flexibility,adaptability,and versatility.On the other hand,angle-independent structural color has been achieved through innovative design strategies and engineering approaches.By carefully controlling the size,shape,and arrangement of nanostructures,researchers have been able to create materials exhibiting consistent colors regardless of the viewing angle.One promising class of materials that holds great potential for bioinspired soft actuators is MXenes in view of their exceptional mechanical,electrical,and optical properties.The integration of MXenes for bioinspired soft actuators with angle-independent structural color offers exciting possibilities.Overcoming material compatibility issues,improving color reproducibility,scalability,durability,power supply efficiency,and cost-effectiveness will play vital roles in advancing these technologies.This perspective appraises the development of bioinspired MXene-centered soft actuators with angleindependent structural color in soft robotics.
基金supported by the National Key R&D Program of China(2022YFA2105900)the National Natural Science Foundation of China(22178197)。
文摘Highly-efficient oxidation of 5-hydroxymethylfurtural(HMF) to 2,5-furandicarboxylic acid(FDCA) at low temperature with air as the oxidant is still challenging.Herein,inspired by the respirato ry electron transport chain(ETC) of living cells mediated by electron carriers,we constructed artificial ETCs and transformed liquid flow fuel cells(LFFCs) to flexible reactors for efficient oxidation of HMF to produce FDCA under mild conditions.This LFFC reactor employed an electrodeposition modified nickel foam as an anode to promote HMF oxidation and(VO_(2))_(2)SO_(4) as a cathode electron carrier to facilitate the electron transfer to air.The reaction rate could be easily controlled by selecting the anode catalyst,adjusting the external loading and changing the cathodic electron carrier or oxidants.A maximal power density of 44.9 mW cm^(-2) at room temperature was achieved,while for FDCA production,short-circuit condition was preferred to achieve quick transfer of electrons.For a single batch operation with 0.1 M initial HMF,FDCA yield reached 97.1%.By fed-batch operation,FDCA concentration reached 144.5 g L^(-1) with a total yield of 96%.Ni^(2+)/Ni^(3+) redox couple was the active species mediating the electron transfer,while both experimental and DFT calculation results indicated that HMFCA pathway was the preferred reaction mechanism.
基金supported by the National Natural Science Foundation of China(22308210)the Scientific Research Program Funded by Shaanxi Provincial Education Department(23JK0350)+3 种基金the Open Foundation of Key Laboratory of Auxiliary Chemistry and Technology for Chemical Industry,Ministry of Education,and Shaanxi Collaborative Innovation Center of Industrial Auxiliary Chemistry and Technology,Shaanxi University of Science and Technology(KFKT2021-12)the Opening Project of Key Laboratory of Leather Chemistry and Engineering(Sichuan University),Ministry of Education(2022)the RIKEN-MOST Project between the Ministry of Science and Technology of the People's Republic of China(MOST)and RIKEN,the China Scholarship Council(202108610127)the Natural Science Foundation of Shaanxi University of Science&Technology(2019BT-44).
文摘In recent years,water evaporation-induced electricity has attracted a great deal of attention as an emerging green and renewable energy harvesting technology.Although abundant materials have been developed to fabricate hydrovoltaic devices,the limitations of high costs,inconvenient storage and transport,low environmental benefits,and unadaptable shape have restricted their wide applications.Here,an electricity generator driven by water evaporation has been engineered based on natural biomass leather with inherent properties of good moisture permeability,excellent wettability,physicochemical stability,flexibility,and biocompatibility.Including numerous nano/microchannels together with rich oxygen-bearing functional groups,the natural leather-based water evaporator,Leather_(Emblic-NPs-SA/CB),could continuously produce electricity even staying outside,achieving a maximum output voltage of∼3 V with six-series connection.Furthermore,the leather-based water evaporator has enormous potential for use as a flexible self-powered electronic floor and seawater demineralizer due to its sensitive pressure sensing ability as well as its excellent photothermal conversion efficiency(96.3%)and thus fast water evaporation rate(2.65 kg m^(−2)h^(−1)).This work offers a new and functional material for the construction of hydrovoltaic devices to harvest the sustained green energy from water evaporation in arbitrary ambient environments,which shows great promise in their widespread applications.
基金funded by the National Key Research Development Program of China(2022YFD1700500)Beijing Natural Science Foundation(6232033).
文摘The flourishing progress in nanotechnology offers boundless opportunities for agriculture,particularly in the realm of nanopesticides research and development.However,concerns have been raised regarding the human and environmental safety issues stemming from the unrestrained use of non-therapeutic nanomaterials in nanopesticides.It is also important to consider whether the current development strategy of nanopesticides based on nanocarriers can strike a balance between investment and return,and if the complex material composition genuinely improves the efficiency,safety,and circularity of nanopesticides.Herein,we introduced the concept of nanopesticides with minimizing carriers(NMC)prepared through prodrug design and molecular self-assembly emerging as practical tools to address the current limitations,and compared it with nanopesticides employing non-therapeutic nanomaterials as carriers(NNC).We further summarized the current development strategy of NMC and examined potential challenges in its preparation,performance,and production.Overall,we asserted that the development of NMC systems can serve as the innovative driving force catalyzing a green and efficient revolution in nanopesticides,offering a way out of the current predicament.
基金FCT(Portugal's Foundation for Science and Technology)for financial support through the CQ-VR(UIDB/00616/2020,UIDP/00616/2020),CQE/Institute of Molecular Sciences(UIBD/00100/2020,UIPD/00100/2020 and LA/P/0056/2020),Institute for Bioengineering and Biosciences-iBB/Associate Laboratory Institute for Health and Bioeconomy-i4HB(UIDB/04565/2020,UIDP/04565/2020,and LA/P/0140/2020)FCT,MCTES,ESF,and EU through the individual research Ph.D.for the Ph.D.scholarship(SFRH/BD/138425/2018)+1 种基金FCT for funding through the Scientific Employment Stimulus—Institutional Call(Ref.CEECINST/00136/2021)the EPSRC funded National Research Facility(EP/W014521/1)。
文摘Dialysis plays a crucial role in the purification of nanomaterials but its impact on the structural properties of carbon nanomaterials was never investigated.Herein,a carbon-based nanomaterial generated electrochemically in potassium phosphate buffer,was characterized before and after dialysis against pure water.It is shown that dialysis affects the size of the carbon domains,structural organization,surface functionalization,oxidation degree of carbon,and grade of amorphicity.Accordingly,dialysis drives the nanomaterial organization from discrete roundish carbon domains,with sizes ranging from 70 to 160 nm,towards linear stacking structures of small nanoparticles(<15 nm).In parallel,alcohol and ether(epoxide)surface groups evolve into more oxidized carbon groups(e.g.,ketone and ester groups).Investigation of the as-prepared nanomaterial by electron paramagnetic resonance(EPR)revealed a resonance signal consistent with carbon-oxygen centred radicals.Additionally,this study brings to light the selective affinity of the carbon nanomaterial under study to capture Na^(+)ions,a property greatly enhanced by the dialysis process,and its high ability to trap oxygen,particularly before dialysis.These findings open new perspectives for the application of carbon-based nanomaterials and raise awareness of the importance of structural changes that can occur during the purification of carbon-based nanomaterials.
文摘基于脉冲激光沉积(PLD)技术在光寻址电位传感器(LAPS)表面上制备了Fe-Ge-Sb-Se硫系玻璃薄膜,合成的靶材成分为Fe1.2(Ge28Sb12Se60)98.8,在Si/SiO2基质上的金属层为Cr/Au,硫系玻璃薄膜对Fe3+敏感,显示了良好的重复性和稳定性.在1×10-5～1×10-2mol/L呈现线性,斜率为(56±2)mV/decade,检测下限为5×10mol/L,当浓度高于1×10-4mol/L时,响应时间不超过40 s;当低于此浓度时,响应时间不超过2 min.
