Excessive Fe^(3+) ion concentrations in wastewater pose a long-standing threat to human health.Achieving low-cost,high-efficiency quantification of Fe^(3+) ion concentration in unknown solutions can guide environmenta...Excessive Fe^(3+) ion concentrations in wastewater pose a long-standing threat to human health.Achieving low-cost,high-efficiency quantification of Fe^(3+) ion concentration in unknown solutions can guide environmental management decisions and optimize water treatment processes.In this study,by leveraging the rapid,real-time detection capabilities of nanopores and the specific chemical binding affinity of tannic acid to Fe^(3+),a linear relationship between the ion current and Fe^(3+) ion concentration was established.Utilizing this linear relationship,quantification of Fe^(3+) ion concentration in unknown solutions was achieved.Furthermore,ethylenediaminetetraacetic acid disodium salt was employed to displace Fe^(3+) from the nanopores,allowing them to be restored to their initial conditions and reused for Fe^(3+) ion quantification.The reusable bioinspired nanopores remain functional over 330 days of storage.This recycling capability and the long-term stability of the nanopores contribute to a significant reduction in costs.This study provides a strategy for the quantification of unknown Fe^(3+) concentration using nanopores,with potential applications in environmental assessment,health monitoring,and so forth.展开更多
Flexible zinc-ion batteries(FZIBs)have been acknowledged as a potential cornerstone for the future development of flexible energy storage,yet conventional FZIBs still encounter challenges,particularly concerning perfo...Flexible zinc-ion batteries(FZIBs)have been acknowledged as a potential cornerstone for the future development of flexible energy storage,yet conventional FZIBs still encounter challenges,particularly concerning performance failure at low temperatures.To address these challenges,a novel anti-freezing leather gel electrolyte(AFLGE-30)is designed,incorporating ethanol as a hydrogen bonding acceptor.The AFLGE-30 demonstrates exceptional frost resistance while maintaining favorable flexibility even at-30℃;accordingly,the battery can achieve a high specific capacity of about 70 m Ah/g.Cu//Zn battery exhibits remarkable stability at room temperature,retaining~96%efficiency after 120 plating/stripping cycles at1 m A/cm^(2).Concurrently,the Zn//Zn symmetric batteries demonstrate a lifespan of 4100 h at room temperature,which is attributed to the enhancement of Zn^(2+)deposition kinetics,restraining the formation of zinc dendrites.Furthermore,FZIBs exhibit minimal capacity loss even after bending,impacting,or burning.This work provides a promising strategy for designing low-temperature-resistant FZIBs.展开更多
Post-earthquake rescue missions are full of challenges due to the unstable structure of ruins and successive aftershocks.Most of the current rescue robots lack the ability to interact with environments,leading to low ...Post-earthquake rescue missions are full of challenges due to the unstable structure of ruins and successive aftershocks.Most of the current rescue robots lack the ability to interact with environments,leading to low rescue efficiency.The multimodal electronic skin(e-skin)proposed not only reproduces the pressure,temperature,and humidity sensing capabilities of natural skin but also develops sensing functions beyond it—perceiving object proximity and NO2 gas.Its multilayer stacked structure based on Ecoflex and organohydrogel endows the e-skin with mechanical properties similar to natural skin.Rescue robots integrated with multimodal e-skin and artificial intelligence(AI)algorithms show strong environmental perception capabilities and can accurately distinguish objects and identify human limbs through grasping,laying the foundation for automated post-earthquake rescue.Besides,the combination of e-skin and NO2 wireless alarm circuits allows robots to sense toxic gases in the environment in real time,thereby adopting appropriate measures to protect trapped people from the toxic environment.Multimodal e-skin powered by AI algorithms and hardware circuits exhibits powerful environmental perception and information processing capabilities,which,as an interface for interaction with the physical world,dramatically expands intelligent robots’application scenarios.展开更多
Electrocatalytic nitrogen reduction reaction(NRR)is considered as an attractive approach for ammonia synthesis under mild conditions.A bottleneck of NRR is the exploration of efficient catalysts for accelerating react...Electrocatalytic nitrogen reduction reaction(NRR)is considered as an attractive approach for ammonia synthesis under mild conditions.A bottleneck of NRR is the exploration of efficient catalysts for accelerating reaction kinetics,among which heterogeneous structures possessing distinct atomic arrangement could modify electronic structure,and therefore altering their NRR activity.Here,we report a facile strategy for fabricating hetero-phase metal oxides derived from metal organic framework that are further integrated with Au nanoparticles as NRR catalysts.The phase composition of zirconia can be easily adjusted by simply changing the reaction temperature,where the monoclinic and tetragonal phases with the roughly close proportions have a distinct interface,leading to a strong interaction between Au and ZrO_(2).The enhanced interaction renders Au to be more electropositive and facilitates stronger binding to N_(2).As a result,a remarkable ammonia yield of 22.32μg h^(-1)mg_(cat.)^(-1) and a Faradaic efficiency of 31.92%can be achieved at low overpotential.This work is expected to pave the way for the design of heterogeneous structures and the exploration of hetero-phase nanostructures in boosting the electrocatalytic NRR.展开更多
Au is considered as one of the most promising catalysts for nitrogen reduction reaction(NRR),however maximizing the activity utilization rate of Au and understanding the synergistic effects between Au and carriers pos...Au is considered as one of the most promising catalysts for nitrogen reduction reaction(NRR),however maximizing the activity utilization rate of Au and understanding the synergistic effects between Au and carriers pose ongoing challenges.Herein,we systematically explore the synergistic catalytic effect of incorporating Au with boron clusters for accelerating NRR kinetics.An in-situ abinitio strategy is employed to construct B-doped Au nanoparticles(2-6 nm in diameter)loaded on BO_(x) substrates(AuBO_(x)),in which B not only modulates the surface electronic structure of Au but also forms strong coupling interactions to stabilize the nanoparticles.The electrochemical results show that Au-BO_(x) possesses excellent NRR activity(NH_(3) yield of 48.52μg h^(-1)mg_(cat)^(-1),Faraday efficiency of 56.18%),and exhibits high stability and reproducibility throughout the electrocatalytic NRR process.Theoretical calculations reveal that the introduction of B induces the formation of both Au dangling bond and Au-B coupling bond.which considerably facilitates the hydrogenation of~*N_(2)^(-)~*NH_(3).The present work provides a new avenue for the preparation of metal-boron materials achieved by one-step reduction and doping process,utilizing boron clusters as reducing and stabilizing agents.展开更多
Lithium-sulfur battery(Li-S)is considered as one of the new-generation rechargeable batteries with high performance because of its extremely high theoretical capacity,energy density,environmental harmony and low cost....Lithium-sulfur battery(Li-S)is considered as one of the new-generation rechargeable batteries with high performance because of its extremely high theoretical capacity,energy density,environmental harmony and low cost.However,low electrical and ionic conductivity of sulfur,safety concerns and parasitic reaction generated by the dissolved polysulfide species in electrolyte hinder the commercialization of Li-S battery.Herein,we report a polyhedral porous structure comprising of carbon coating metal selenide nanoparticles(CoSe2/C),which could not only host sulfur for Li-S battery owing to its porous and conductive structure,but also mitigate the shuttle phenomenon by polysulfides adsorption and catalytic acceleration of redox kinetics.As a result,a performance enhanced CoSe2/C-S electrode for Li-S battery is achieved.展开更多
Carbon materials derived from biomass waste are considered as potential electrocatalysts for applications in zinc-air batteries(ZABs)due to their low cost and good catalytic activity.Here,we reported the preparation o...Carbon materials derived from biomass waste are considered as potential electrocatalysts for applications in zinc-air batteries(ZABs)due to their low cost and good catalytic activity.Here,we reported the preparation of gel-based catalysts through utilizing hydrolyzed waste leather powder cross-linked with metallic salt solutions.After calcination,iron-nickel alloy anchored in nitrogen-doped porous carbon catalysts(Fe Ni@NDC)was achieved.Compared with commercial Pt/C catalyst,Fe Ni@NDC-800 exhibited lower E_(1/2)(0.77 V)and better durability.More importantly,the resulting Fe Ni@NDC-800-based alkaline ZABs achieved power density of 93.01 m W/cm^(2) and open circuit voltage of 1.45 V,which the Fe Ni@NDC-800-based neutral ZAB displayed a charge/discharge cycle stability of 275 h.This work opens up the possibility of rational design and preparation of low-cost and high-performance electrocatalysts from recyclable leather waste.展开更多
As an effective and competitive supplement to the commercialized lithium ion batteries(LIBs),sodium ion batteries(SIBs)have been receiving increasing attention in recent years due to lower cost,richer content,and broa...As an effective and competitive supplement to the commercialized lithium ion batteries(LIBs),sodium ion batteries(SIBs)have been receiving increasing attention in recent years due to lower cost,richer content,and broader distribution of sodium[1–7].Sodium has similar electrochemical properties to lithium,and thus the concepts for the preparation of electrode materials for SIBs can be borrowed from LIBs[8,9].展开更多
Compared with solid alkali metal anodes(Li, Na, K), liquid metal anodes(LMAs) could enable high-energy batteries due to their unique advantages, such as self-healing property and no dendrites. Among LMAs,liquid Na-K a...Compared with solid alkali metal anodes(Li, Na, K), liquid metal anodes(LMAs) could enable high-energy batteries due to their unique advantages, such as self-healing property and no dendrites. Among LMAs,liquid Na-K alloy anode has become a hotspot due to its high theoretical capacity, low redox potential and formation at room temperature(RT). However, it is challenging to utilize liquid Na-K alloy directly and independently as an electrode;and the high surface tension makes it more difficult to immerse into porous current collectors at RT. Herein, an amorphous hollow carbon film(AHCF) consisting of hollow spheres with significant surface defects has been designed to quickly infiltrate Na-K liquid alloy into the hollow carbon film at RT, forming a composite electrode(Na-K@AHCF). The symmetric cell with Na-K@AHCF could exhibit a cycle lifespan up to 400 h at 0.1 m A/cm^(2) and achieve stable stripping/deposition even at 5 mA/cm^(2). When matching with cathode material of sulfurized polyacrylonitrile(SPAN), the obtained K-S full cell exhibits good cycle stability and rate performance.展开更多
The integration of organic and inorganic materials has been widely used in various applications to generate novel functional nanomaterials characterized by unique properties.Functional crystalline framework nanosheets...The integration of organic and inorganic materials has been widely used in various applications to generate novel functional nanomaterials characterized by unique properties.Functional crystalline framework nanosheets and their synergistic effects have been studied recently for possessing the advantages of functional species as well as crystalline framework nanosheets.Hence,we have focused on the preparation methods and applications of functional crystalline framework nanosheets in this review.We introduced crystalline framework nanosheets and discussed the importance of integrating functional species with nanosheets to form functional crystalline framework nanosheets.Then,two aspects of the preparation methods of functional crystalline framework nanosheets were reviewed:in situ synthesis and post-synthesis modification.Subsequently,we discussed the properties of the crystalline framework nanosheets combined with various functional species and summarized their applications in catalysis,sensing,separation,and energy storage.Finally,we have shared our insights on the challenges of functional crystalline framework nanosheets,hoping to contribute to the knowledge base for optimizing the preparation methods,expanding categories,improving stability,and exploring potential applications.展开更多
Metal-organic frameworks(MOFs)have been widely considered as ideal platforms for the preparation of biomimetic catalysts,but it remains challenging to fabricate MOF-based enzyme-like catalysts with optimal activity.He...Metal-organic frameworks(MOFs)have been widely considered as ideal platforms for the preparation of biomimetic catalysts,but it remains challenging to fabricate MOF-based enzyme-like catalysts with optimal activity.Here,we leverage the inherent flexibility of MOFs and propose a novel trans-functionalization strategy to construct a carbonic anhydrase(CA)mimic by the structural transformation from ZIF-L to ZIF-8.Theoretical and experimental results reveal that during the structural transformation,the hydroxyl group will preferentially coordinate with the interlayer Zn clusters to form the CA-like active center Zn-N3-OH.Therefore,more accessible active centers are generated on the as-prepared ZIF-8-OH,resulting in substantially enhanced catalytic activity in the hydrolysis of para-nitrophenyl acetate.展开更多
The performance of organic electrochemical transistors(OECTs)relies on the interaction between organic semiconductors and ions.Consequently,hydrophilic ethylene glycol(EG)side chains are incorporated into organic semi...The performance of organic electrochemical transistors(OECTs)relies on the interaction between organic semiconductors and ions.Consequently,hydrophilic ethylene glycol(EG)side chains are incorporated into organic semiconductors to improve the channel’s capacity to absorb ions.However,the EG substituted organic semiconductors tend to swell when immersed in aqueous electrolytes and exhibit microstructural changes induced by dopant ions.In our research,we introduce an alkyl spacer to create distance between the fullerene and EG chain.This approach is designed to reduce the negative effects of swelling and balance the ion and electron conduction.We conducted an analysis of OECTs using four fullerene derivatives:no alkyl spacer,butyl,hexyl,and octyl spacers.The OECTs based on fullerene derivatives with butyl and hexyl spacers exhibit enhanced transconductance(g_(m)=11.8 and 19.4 mS)compared to the ones without alkyl spacers.It has also been observed that the butyl and hexyl spacers lead to a more than tenfold increase in volumetric capacitance.Further increasing the alkyl spacer(octyl group)leads to no transistor behavior.Our study uncovers the relationship between alkyl spacers and the performance of OECTs based on fullerene derivatives.This will serve as a guideline for designing n-type small molecules for OECTs.Finally,we showcased the potential of utilizing OECTs based on these fullerene derivatives in cation sensing,which is promising for developing sweat sensors.展开更多
Metal nanoparticle@porous material composites have attracted increasing attention due to their excellent synergistic catalytic performance.However,it is a challenge to introduce metal nanoparticles into cavities of po...Metal nanoparticle@porous material composites have attracted increasing attention due to their excellent synergistic catalytic performance.However,it is a challenge to introduce metal nanoparticles into cavities of porous materials without agglomeration on the exterior.Despite the progress achieved,a universal approach that can integrate different kinds of metal nanoparticles and porous materials is still highly desirable.Here we report a facile and general approach to fabricating metal nanoparticle@porous materials by microwave-triggered selective heating.The microwave can pass through the non-polar solvent and act on the polar solvent in the porous materials,causing the polar solvent to be heated,vaporized,and away from the pores of porous materials.The local void produced by the escape of polar solvent facilitates non-polar solvent containing metallic precursor to be dragged into the narrow pores,followed by further reduction,resulting in the complete encapsulation of nanoparticles.A series of metal nanoparticles@porous materials,ranging from metal-organic frameworks(MOFs)to zeolites,are successfully prepared by this method and show excellent size selectivity in catalytic reactions.展开更多
The light-driven material-microorganism biohybrid system has the potential to transfer solar energy for chemical production.However,few studies have reported the construction of biohybrid systems using light-responsiv...The light-driven material-microorganism biohybrid system has the potential to transfer solar energy for chemical production.However,few studies have reported the construction of biohybrid systems using light-responsive materials with nonmodel strains that have been widely used in practical industrial production for value-added chemicals,especially with regard to the mechanism of action of photogenerated charges in the cytoplasm,probably due to the complexity of their anabolic pathways.Herein,a biohybrid system as a research mode was constructed by electrostatically self-assembling a highly efficient light-harvesting material of graphite-phase nitrided carbon(g-C_(3)N_(4))nanosheets with nonmodel strains(Phaffia rhodozyma)for synthesis of nutritional chemical astaxanthin.The biohybrid interface enabled efficient separation,transfer,and transport of photogenerated charges from g-C_(3)N_(4) into the interior of P.rhodozyma,which improved the substance metabolism and the energy metabolism of P.rhodozyma.Notably,photogenerated charges can significantly promote the accumulation of precursors along the astaxanthin anabolic pathway and enhance the cytoplasmic redox environment and ATP levels in the interior of P.rhodozyma,even under adverse conditions(such as enzyme inhibitors),thus increasing the yield of astaxanthin compared to the traditional culture of P.rhodozyma.This study not only provides new ideas for converting solar energy into value-added chemicals,but it also provides guidance for regulating microbial synthesis plants.展开更多
Metal-organic framework(MOF)nanosheets and covalent organic framework(COF)nanosheets as emerging porous materials nanosheets have captured increasing attention owing to their attractive properties originating from the...Metal-organic framework(MOF)nanosheets and covalent organic framework(COF)nanosheets as emerging porous materials nanosheets have captured increasing attention owing to their attractive properties originating from the advantages of large lateral size,ultrathin thickness,tailorable physiochemical environment,flexibility and highly accessible active sites on surface,and the applications of them have been explored in a wide range of fields.Although MOF and COF nanosheets own many similar properties,their applications in various fields show significant differences,probably due to their different compositions and bonding modes.Hence,we summarize the recent progress of MOF and COF nanosheets by comparative analysis on their advantages and limitations in synthesis and applications,providing a more profound and full-scale perspective for researchers or beginners to understand this field.Herein,the categories of preparation methods of MOF and COF nanosheets are firstly discussed,including top-down and bottom-up methods.Secondly,the applications of MOF and COF nanosheets for separation,catalysis,sensing and energy storage are summarized.Finally,based on current achievements,we put forward our personal insights into the challenges and outlooks on the synthesis,characterizations,and promising applications for future research of MOF and COF nanosheets.展开更多
Flexible electronics are playing an increasingly important role in human health monitoring and healthcare diagnosis.Strong adhesion on human tissue would be ideal for reducing interface resistance and motion artifacts...Flexible electronics are playing an increasingly important role in human health monitoring and healthcare diagnosis.Strong adhesion on human tissue would be ideal for reducing interface resistance and motion artifacts,but arising problems such as skin irritation,rubefaction,and pain upon device removal have hampered their utility.Here,inspired by the temperature reversibility of hydrogen bonding,a skin-friendly conductive hydrogel with multiple-hydrogen bonds was designed by using biocompatible poly(vinyl alcohol)(PVA),phytic acid(PA),and gelatin(Gel).The obtained PVA/PA/Gel(PPG)hydrogel with temperature-triggered tunable mechanic could reliably adhere to skin and detect electrophysiological signals under a hot compress while be readily removed under a cool compress.Furthermore,the additional advantages of transparency,breathability,and antimicrobial activity of the PPG hydrogel ensure its long-time wearable value on the skin.It is both environmentally friendly and cost saving for the waste PPG hydrogel during production can be recycled based on their reversible physical bonding.The PPG hydrogel sensor is expected to have good application prospects to record electrophysiological signals in human health monitoring.展开更多
The development of artificial enzyme mimics has been rapidly growing in recent years, and it is attracting increasing attention owing to their remarkable advantages over natural enzymes. Herein, we developed a general...The development of artificial enzyme mimics has been rapidly growing in recent years, and it is attracting increasing attention owing to their remarkable advantages over natural enzymes. Herein, we developed a general and facile method to fabricate efficient glutathione peroxidase （GPx） mimics by grafting selenium-containing molecules （phenylselenylbromide, PhSeBr） to a Zr（W）-based UiO-66-NH2 framework. In the presence of glutathione （GSH） serving as substrate, the fabricated UiO-66-Se catalysts can catalyze the reduction of hydroperoxides. The as-prepared UiO-66-Se systems show good catalytic activity over three cycles. These high-efficiency GPx mimic metal-organic frameworks （MOFs） are endowed with excellent thermal and structural stability, providing a promising avenue for the development of artificial enzyme mimics.展开更多
A facile encapsulation strategy for the preparation of metal layer/metal-organic framework （metal/MOF） hybrid thin films, by alternately growing MOF thin films and sputter-coating metal layers, is reported. The cont...A facile encapsulation strategy for the preparation of metal layer/metal-organic framework （metal/MOF） hybrid thin films, by alternately growing MOF thin films and sputter-coating metal layers, is reported. The controlled species of the MOF thin films and metal layers, as well as the designed thickness of MOF thin films, endow the resulting hybrid thin films with improved functional and design flexibility. Importantly, the metaL/MOF hybrid thin films, with well-defined sandwich structures, exhibit excellent selective catalytic activity, derived from MOFs acting as molecular sieves and the metal layers providing active sites.展开更多
Sweat contains a broad range of critical biomarkers including ions,small molecules,and macromolecules that may indirectly or directly reflect the health status of the human body and thereby help track disease progress...Sweat contains a broad range of critical biomarkers including ions,small molecules,and macromolecules that may indirectly or directly reflect the health status of the human body and thereby help track disease progression.Wearable sweat biosensors enable the collection and analysis of sweat in situ,achieving real-time,continuous,and noninvasive monitoring of human biochemical parameters at the molecular level.This review summarizes the physiological/pathological information of sweat and wearable sweat biosensors.First,the production of sweat pertaining to various electrolytes,metabolites,and proteins is described.Then,the compositions of the wearable sweat biosensors are summarized,and the design of each subsystem is introduced in detail.The latest applications of wearable sweat biosensors for outdoor,hospital,and family monitoring are highlighted.Finally,the review provides a summary and an outlook on the future developments and challenges of wearable sweat biosensors with the aim of advancing the field of wearable sweat monitoring technology.展开更多
Sweat is a biofluid with rich information that can reflect an individual’s state of health or activity.But the real-time in situ sweat sensors lack the ability of long-term monitoring.Against this background,this art...Sweat is a biofluid with rich information that can reflect an individual’s state of health or activity.But the real-time in situ sweat sensors lack the ability of long-term monitoring.Against this background,this article provides a holistic review on the necessary process and methods for sweat sensing,including sweat collection,composition analysis,energy supply,and data processing.The impacts of the environment in stimulating sweat production,providing energy supply,and intelligent health monitoring are discussed.Based on the review of previous endeavors,the future development in material,structure and artificial intelligence application of long-term sweat monitoring is envisioned.展开更多
基金supported by the National Natural Science Foundation of China(Nos.52303380,52025132,52273305,22205185,21621091,22021001,and 22121001)Fundamental Research Funds for the Central Universities(No.20720240041)+3 种基金the 111 Project(Nos.B17027 and B16029)the National Science Foundation of Fujian Province of China(No.2022J02059)the Science and Technology Projects of Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province(No.RD2022070601)the New Cornerstone Science Foundation through the XPLORER PRIZE。
文摘Excessive Fe^(3+) ion concentrations in wastewater pose a long-standing threat to human health.Achieving low-cost,high-efficiency quantification of Fe^(3+) ion concentration in unknown solutions can guide environmental management decisions and optimize water treatment processes.In this study,by leveraging the rapid,real-time detection capabilities of nanopores and the specific chemical binding affinity of tannic acid to Fe^(3+),a linear relationship between the ion current and Fe^(3+) ion concentration was established.Utilizing this linear relationship,quantification of Fe^(3+) ion concentration in unknown solutions was achieved.Furthermore,ethylenediaminetetraacetic acid disodium salt was employed to displace Fe^(3+) from the nanopores,allowing them to be restored to their initial conditions and reused for Fe^(3+) ion quantification.The reusable bioinspired nanopores remain functional over 330 days of storage.This recycling capability and the long-term stability of the nanopores contribute to a significant reduction in costs.This study provides a strategy for the quantification of unknown Fe^(3+) concentration using nanopores,with potential applications in environmental assessment,health monitoring,and so forth.
基金supported by the National Natural Science Foundation of China(Nos.22075139 and 62288102)。
文摘Flexible zinc-ion batteries(FZIBs)have been acknowledged as a potential cornerstone for the future development of flexible energy storage,yet conventional FZIBs still encounter challenges,particularly concerning performance failure at low temperatures.To address these challenges,a novel anti-freezing leather gel electrolyte(AFLGE-30)is designed,incorporating ethanol as a hydrogen bonding acceptor.The AFLGE-30 demonstrates exceptional frost resistance while maintaining favorable flexibility even at-30℃;accordingly,the battery can achieve a high specific capacity of about 70 m Ah/g.Cu//Zn battery exhibits remarkable stability at room temperature,retaining~96%efficiency after 120 plating/stripping cycles at1 m A/cm^(2).Concurrently,the Zn//Zn symmetric batteries demonstrate a lifespan of 4100 h at room temperature,which is attributed to the enhancement of Zn^(2+)deposition kinetics,restraining the formation of zinc dendrites.Furthermore,FZIBs exhibit minimal capacity loss even after bending,impacting,or burning.This work provides a promising strategy for designing low-temperature-resistant FZIBs.
基金supports from the National Natural Science Foundation of China(61801525)the independent fund of the State Key Laboratory of Optoelectronic Materials and Technologies(Sun Yat-sen University)under grant No.OEMT-2022-ZRC-05+3 种基金the Opening Project of State Key Laboratory of Polymer Materials Engineering(Sichuan University)(Grant No.sklpme2023-3-5))the Foundation of the state key Laboratory of Transducer Technology(No.SKT2301),Shenzhen Science and Technology Program(JCYJ20220530161809020&JCYJ20220818100415033)the Young Top Talent of Fujian Young Eagle Program of Fujian Province and Natural Science Foundation of Fujian Province(2023J02013)National Key R&D Program of China(2022YFB2802051).
文摘Post-earthquake rescue missions are full of challenges due to the unstable structure of ruins and successive aftershocks.Most of the current rescue robots lack the ability to interact with environments,leading to low rescue efficiency.The multimodal electronic skin(e-skin)proposed not only reproduces the pressure,temperature,and humidity sensing capabilities of natural skin but also develops sensing functions beyond it—perceiving object proximity and NO2 gas.Its multilayer stacked structure based on Ecoflex and organohydrogel endows the e-skin with mechanical properties similar to natural skin.Rescue robots integrated with multimodal e-skin and artificial intelligence(AI)algorithms show strong environmental perception capabilities and can accurately distinguish objects and identify human limbs through grasping,laying the foundation for automated post-earthquake rescue.Besides,the combination of e-skin and NO2 wireless alarm circuits allows robots to sense toxic gases in the environment in real time,thereby adopting appropriate measures to protect trapped people from the toxic environment.Multimodal e-skin powered by AI algorithms and hardware circuits exhibits powerful environmental perception and information processing capabilities,which,as an interface for interaction with the physical world,dramatically expands intelligent robots’application scenarios.
基金supported by the National Natural Science Foundation(Nos.22075133 and 21701086)。
文摘Electrocatalytic nitrogen reduction reaction(NRR)is considered as an attractive approach for ammonia synthesis under mild conditions.A bottleneck of NRR is the exploration of efficient catalysts for accelerating reaction kinetics,among which heterogeneous structures possessing distinct atomic arrangement could modify electronic structure,and therefore altering their NRR activity.Here,we report a facile strategy for fabricating hetero-phase metal oxides derived from metal organic framework that are further integrated with Au nanoparticles as NRR catalysts.The phase composition of zirconia can be easily adjusted by simply changing the reaction temperature,where the monoclinic and tetragonal phases with the roughly close proportions have a distinct interface,leading to a strong interaction between Au and ZrO_(2).The enhanced interaction renders Au to be more electropositive and facilitates stronger binding to N_(2).As a result,a remarkable ammonia yield of 22.32μg h^(-1)mg_(cat.)^(-1) and a Faradaic efficiency of 31.92%can be achieved at low overpotential.This work is expected to pave the way for the design of heterogeneous structures and the exploration of hetero-phase nanostructures in boosting the electrocatalytic NRR.
基金supported by the National Natural Science Foundation of China(22075133,62288102,22375091,21971114,and 21701086)the Jiangsu Provincial Funds(BX2022013)。
文摘Au is considered as one of the most promising catalysts for nitrogen reduction reaction(NRR),however maximizing the activity utilization rate of Au and understanding the synergistic effects between Au and carriers pose ongoing challenges.Herein,we systematically explore the synergistic catalytic effect of incorporating Au with boron clusters for accelerating NRR kinetics.An in-situ abinitio strategy is employed to construct B-doped Au nanoparticles(2-6 nm in diameter)loaded on BO_(x) substrates(AuBO_(x)),in which B not only modulates the surface electronic structure of Au but also forms strong coupling interactions to stabilize the nanoparticles.The electrochemical results show that Au-BO_(x) possesses excellent NRR activity(NH_(3) yield of 48.52μg h^(-1)mg_(cat)^(-1),Faraday efficiency of 56.18%),and exhibits high stability and reproducibility throughout the electrocatalytic NRR process.Theoretical calculations reveal that the introduction of B induces the formation of both Au dangling bond and Au-B coupling bond.which considerably facilitates the hydrogenation of~*N_(2)^(-)~*NH_(3).The present work provides a new avenue for the preparation of metal-boron materials achieved by one-step reduction and doping process,utilizing boron clusters as reducing and stabilizing agents.
基金supported by the National Natural Science Foundation of China(51702155,51902036)the National Science Foundation for Distinguished Young Scholars(21625401)+3 种基金the Jiangsu Provincial Founds for Natural Science Foundation(BK20170975)the Natural Science Fund for Colleges and Universities in Jiangsu Province(17KJB480007)the National Key R&D Program of China(Grant No.2017YFA0207202 and 2017YFA0207201)the Natural Science Foundation of Chongqing Science&Technology Commission(No.cstc2019jcyj-msxm X0144)。
文摘Lithium-sulfur battery(Li-S)is considered as one of the new-generation rechargeable batteries with high performance because of its extremely high theoretical capacity,energy density,environmental harmony and low cost.However,low electrical and ionic conductivity of sulfur,safety concerns and parasitic reaction generated by the dissolved polysulfide species in electrolyte hinder the commercialization of Li-S battery.Herein,we report a polyhedral porous structure comprising of carbon coating metal selenide nanoparticles(CoSe2/C),which could not only host sulfur for Li-S battery owing to its porous and conductive structure,but also mitigate the shuttle phenomenon by polysulfides adsorption and catalytic acceleration of redox kinetics.As a result,a performance enhanced CoSe2/C-S electrode for Li-S battery is achieved.
基金supported by National Natural Science Foundation of China(No.22075139)。
文摘Carbon materials derived from biomass waste are considered as potential electrocatalysts for applications in zinc-air batteries(ZABs)due to their low cost and good catalytic activity.Here,we reported the preparation of gel-based catalysts through utilizing hydrolyzed waste leather powder cross-linked with metallic salt solutions.After calcination,iron-nickel alloy anchored in nitrogen-doped porous carbon catalysts(Fe Ni@NDC)was achieved.Compared with commercial Pt/C catalyst,Fe Ni@NDC-800 exhibited lower E_(1/2)(0.77 V)and better durability.More importantly,the resulting Fe Ni@NDC-800-based alkaline ZABs achieved power density of 93.01 m W/cm^(2) and open circuit voltage of 1.45 V,which the Fe Ni@NDC-800-based neutral ZAB displayed a charge/discharge cycle stability of 275 h.This work opens up the possibility of rational design and preparation of low-cost and high-performance electrocatalysts from recyclable leather waste.
基金supported by the National Key R&D Program of China(Grant No.2017YFA0207202)Postgraduate Research&Practice Innovation Program of Jiangsu Province(KYCX20_1058)。
文摘As an effective and competitive supplement to the commercialized lithium ion batteries(LIBs),sodium ion batteries(SIBs)have been receiving increasing attention in recent years due to lower cost,richer content,and broader distribution of sodium[1–7].Sodium has similar electrochemical properties to lithium,and thus the concepts for the preparation of electrode materials for SIBs can be borrowed from LIBs[8,9].
基金financially supported by the National Natural Science Foundation of China (No. 51702155)。
文摘Compared with solid alkali metal anodes(Li, Na, K), liquid metal anodes(LMAs) could enable high-energy batteries due to their unique advantages, such as self-healing property and no dendrites. Among LMAs,liquid Na-K alloy anode has become a hotspot due to its high theoretical capacity, low redox potential and formation at room temperature(RT). However, it is challenging to utilize liquid Na-K alloy directly and independently as an electrode;and the high surface tension makes it more difficult to immerse into porous current collectors at RT. Herein, an amorphous hollow carbon film(AHCF) consisting of hollow spheres with significant surface defects has been designed to quickly infiltrate Na-K liquid alloy into the hollow carbon film at RT, forming a composite electrode(Na-K@AHCF). The symmetric cell with Na-K@AHCF could exhibit a cycle lifespan up to 400 h at 0.1 m A/cm^(2) and achieve stable stripping/deposition even at 5 mA/cm^(2). When matching with cathode material of sulfurized polyacrylonitrile(SPAN), the obtained K-S full cell exhibits good cycle stability and rate performance.
基金financially supported by the National Natural Science Foundation of China (Nos.21727808,21971114,21908105,and 22205100)the Jiangsu Provincial Funds for Natural Science Foundation (No.BK20200090)。
文摘The integration of organic and inorganic materials has been widely used in various applications to generate novel functional nanomaterials characterized by unique properties.Functional crystalline framework nanosheets and their synergistic effects have been studied recently for possessing the advantages of functional species as well as crystalline framework nanosheets.Hence,we have focused on the preparation methods and applications of functional crystalline framework nanosheets in this review.We introduced crystalline framework nanosheets and discussed the importance of integrating functional species with nanosheets to form functional crystalline framework nanosheets.Then,two aspects of the preparation methods of functional crystalline framework nanosheets were reviewed:in situ synthesis and post-synthesis modification.Subsequently,we discussed the properties of the crystalline framework nanosheets combined with various functional species and summarized their applications in catalysis,sensing,separation,and energy storage.Finally,we have shared our insights on the challenges of functional crystalline framework nanosheets,hoping to contribute to the knowledge base for optimizing the preparation methods,expanding categories,improving stability,and exploring potential applications.
基金supported by the National Natural Science Foundation of China(62288102,22305116,21908105,21727808,and 21971114)the Jiangsu Provincial Funds for Natural Science Foundation(BK20230308 and BK20200090).
文摘Metal-organic frameworks(MOFs)have been widely considered as ideal platforms for the preparation of biomimetic catalysts,but it remains challenging to fabricate MOF-based enzyme-like catalysts with optimal activity.Here,we leverage the inherent flexibility of MOFs and propose a novel trans-functionalization strategy to construct a carbonic anhydrase(CA)mimic by the structural transformation from ZIF-L to ZIF-8.Theoretical and experimental results reveal that during the structural transformation,the hydroxyl group will preferentially coordinate with the interlayer Zn clusters to form the CA-like active center Zn-N3-OH.Therefore,more accessible active centers are generated on the as-prepared ZIF-8-OH,resulting in substantially enhanced catalytic activity in the hydrolysis of para-nitrophenyl acetate.
基金We acknowledge funding from the National Natural Science Foundation of China(Nos.22303071 and 51962036).
文摘The performance of organic electrochemical transistors(OECTs)relies on the interaction between organic semiconductors and ions.Consequently,hydrophilic ethylene glycol(EG)side chains are incorporated into organic semiconductors to improve the channel’s capacity to absorb ions.However,the EG substituted organic semiconductors tend to swell when immersed in aqueous electrolytes and exhibit microstructural changes induced by dopant ions.In our research,we introduce an alkyl spacer to create distance between the fullerene and EG chain.This approach is designed to reduce the negative effects of swelling and balance the ion and electron conduction.We conducted an analysis of OECTs using four fullerene derivatives:no alkyl spacer,butyl,hexyl,and octyl spacers.The OECTs based on fullerene derivatives with butyl and hexyl spacers exhibit enhanced transconductance(g_(m)=11.8 and 19.4 mS)compared to the ones without alkyl spacers.It has also been observed that the butyl and hexyl spacers lead to a more than tenfold increase in volumetric capacitance.Further increasing the alkyl spacer(octyl group)leads to no transistor behavior.Our study uncovers the relationship between alkyl spacers and the performance of OECTs based on fullerene derivatives.This will serve as a guideline for designing n-type small molecules for OECTs.Finally,we showcased the potential of utilizing OECTs based on these fullerene derivatives in cation sensing,which is promising for developing sweat sensors.
基金supported by the National Natural Science Foundation of China(Nos.21908105,21971114 and 62288102)the Nanjing Municipal Science and Technology Innovation Project.
文摘Metal nanoparticle@porous material composites have attracted increasing attention due to their excellent synergistic catalytic performance.However,it is a challenge to introduce metal nanoparticles into cavities of porous materials without agglomeration on the exterior.Despite the progress achieved,a universal approach that can integrate different kinds of metal nanoparticles and porous materials is still highly desirable.Here we report a facile and general approach to fabricating metal nanoparticle@porous materials by microwave-triggered selective heating.The microwave can pass through the non-polar solvent and act on the polar solvent in the porous materials,causing the polar solvent to be heated,vaporized,and away from the pores of porous materials.The local void produced by the escape of polar solvent facilitates non-polar solvent containing metallic precursor to be dragged into the narrow pores,followed by further reduction,resulting in the complete encapsulation of nanoparticles.A series of metal nanoparticles@porous materials,ranging from metal-organic frameworks(MOFs)to zeolites,are successfully prepared by this method and show excellent size selectivity in catalytic reactions.
基金supported by the National Natural Science Foundation of China (grant nos.21727808,21971114,and 21908105)the Natural Science Foundation of Jiangsu Province (grant no.BK20200090)the National Science Fund for Distinguished Young Scholars (grant no.21625401).
文摘The light-driven material-microorganism biohybrid system has the potential to transfer solar energy for chemical production.However,few studies have reported the construction of biohybrid systems using light-responsive materials with nonmodel strains that have been widely used in practical industrial production for value-added chemicals,especially with regard to the mechanism of action of photogenerated charges in the cytoplasm,probably due to the complexity of their anabolic pathways.Herein,a biohybrid system as a research mode was constructed by electrostatically self-assembling a highly efficient light-harvesting material of graphite-phase nitrided carbon(g-C_(3)N_(4))nanosheets with nonmodel strains(Phaffia rhodozyma)for synthesis of nutritional chemical astaxanthin.The biohybrid interface enabled efficient separation,transfer,and transport of photogenerated charges from g-C_(3)N_(4) into the interior of P.rhodozyma,which improved the substance metabolism and the energy metabolism of P.rhodozyma.Notably,photogenerated charges can significantly promote the accumulation of precursors along the astaxanthin anabolic pathway and enhance the cytoplasmic redox environment and ATP levels in the interior of P.rhodozyma,even under adverse conditions(such as enzyme inhibitors),thus increasing the yield of astaxanthin compared to the traditional culture of P.rhodozyma.This study not only provides new ideas for converting solar energy into value-added chemicals,but it also provides guidance for regulating microbial synthesis plants.
基金the National Natural Science Foundation of China for Distinguished Young Scholars(No.21625401)the National Natural Science Foundation of China(Nos.21727808,21971114).
文摘Metal-organic framework(MOF)nanosheets and covalent organic framework(COF)nanosheets as emerging porous materials nanosheets have captured increasing attention owing to their attractive properties originating from the advantages of large lateral size,ultrathin thickness,tailorable physiochemical environment,flexibility and highly accessible active sites on surface,and the applications of them have been explored in a wide range of fields.Although MOF and COF nanosheets own many similar properties,their applications in various fields show significant differences,probably due to their different compositions and bonding modes.Hence,we summarize the recent progress of MOF and COF nanosheets by comparative analysis on their advantages and limitations in synthesis and applications,providing a more profound and full-scale perspective for researchers or beginners to understand this field.Herein,the categories of preparation methods of MOF and COF nanosheets are firstly discussed,including top-down and bottom-up methods.Secondly,the applications of MOF and COF nanosheets for separation,catalysis,sensing and energy storage are summarized.Finally,based on current achievements,we put forward our personal insights into the challenges and outlooks on the synthesis,characterizations,and promising applications for future research of MOF and COF nanosheets.
基金supported by the National Key R&D Program of China (2021YFB3200302)the National Natural Science Foundation of China (Nos.22078265,21838009,22075139,62101545,and 21908179)by the Shaanxi Provincial Science Foundation (Nos.2017SF-201).
文摘Flexible electronics are playing an increasingly important role in human health monitoring and healthcare diagnosis.Strong adhesion on human tissue would be ideal for reducing interface resistance and motion artifacts,but arising problems such as skin irritation,rubefaction,and pain upon device removal have hampered their utility.Here,inspired by the temperature reversibility of hydrogen bonding,a skin-friendly conductive hydrogel with multiple-hydrogen bonds was designed by using biocompatible poly(vinyl alcohol)(PVA),phytic acid(PA),and gelatin(Gel).The obtained PVA/PA/Gel(PPG)hydrogel with temperature-triggered tunable mechanic could reliably adhere to skin and detect electrophysiological signals under a hot compress while be readily removed under a cool compress.Furthermore,the additional advantages of transparency,breathability,and antimicrobial activity of the PPG hydrogel ensure its long-time wearable value on the skin.It is both environmentally friendly and cost saving for the waste PPG hydrogel during production can be recycled based on their reversible physical bonding.The PPG hydrogel sensor is expected to have good application prospects to record electrophysiological signals in human health monitoring.
基金The project was supported by the National Natural Science Foundation of China for Distinguished Young Scholars （Nos. 21425416 and 21625401）, the Foundation for Innovative Research Groups of the National Natural Science Foundation of China （No. 21421064）, the National Natural Science Foundation of China （Nos. 21574065, 21504043 and 21604038）, the Jiangsu Provincial Founds for Distinguished Young Scholars （No. BK20140044） and NSF （No. BK20160975）, the Program for Outstanding Young Scholars from the Organization Department of the CPC Central Committee, and the National Key Basic Research Program of China （Nos. 2013CB834502 and 2015CB932200）.
文摘The development of artificial enzyme mimics has been rapidly growing in recent years, and it is attracting increasing attention owing to their remarkable advantages over natural enzymes. Herein, we developed a general and facile method to fabricate efficient glutathione peroxidase （GPx） mimics by grafting selenium-containing molecules （phenylselenylbromide, PhSeBr） to a Zr（W）-based UiO-66-NH2 framework. In the presence of glutathione （GSH） serving as substrate, the fabricated UiO-66-Se catalysts can catalyze the reduction of hydroperoxides. The as-prepared UiO-66-Se systems show good catalytic activity over three cycles. These high-efficiency GPx mimic metal-organic frameworks （MOFs） are endowed with excellent thermal and structural stability, providing a promising avenue for the development of artificial enzyme mimics.
基金The project was supported by the Jiangsu Provincial Founds for Distringuished Young Scholars （No. 55135011）, start-up fund at Nanjing Tech University and the National Natural Science Foundation （Nos. 21574065 and 21504043）.
文摘A facile encapsulation strategy for the preparation of metal layer/metal-organic framework （metal/MOF） hybrid thin films, by alternately growing MOF thin films and sputter-coating metal layers, is reported. The controlled species of the MOF thin films and metal layers, as well as the designed thickness of MOF thin films, endow the resulting hybrid thin films with improved functional and design flexibility. Importantly, the metaL/MOF hybrid thin films, with well-defined sandwich structures, exhibit excellent selective catalytic activity, derived from MOFs acting as molecular sieves and the metal layers providing active sites.
基金supported by the National Key R&D Program of China(2020YFA0709900)the National Science Fund for Distinguished Young Scholars(21625401)+5 种基金the National Natural Science Foundation of China(22077101,21701086,21727808)the Joint Research Funds of Department of Science&Technology of Shaanxi Province and Northwestern Polytechnical University(2020GXLH-Z-008)the Open Project Program of Wuhan National Laboratory for Optoelectronics(No.2020WNLOKF023)the ChinaSweden Joint Mobility Project(51811530018)the Natural Science Basic Research Program of Shaanxi(Program No.2019JLZ-11)the Fundamental Research Funds for the Central Universities Postgraduate Research&Practice Innovation Program of Jiangsu Province(KYCX21_1100).
文摘Sweat contains a broad range of critical biomarkers including ions,small molecules,and macromolecules that may indirectly or directly reflect the health status of the human body and thereby help track disease progression.Wearable sweat biosensors enable the collection and analysis of sweat in situ,achieving real-time,continuous,and noninvasive monitoring of human biochemical parameters at the molecular level.This review summarizes the physiological/pathological information of sweat and wearable sweat biosensors.First,the production of sweat pertaining to various electrolytes,metabolites,and proteins is described.Then,the compositions of the wearable sweat biosensors are summarized,and the design of each subsystem is introduced in detail.The latest applications of wearable sweat biosensors for outdoor,hospital,and family monitoring are highlighted.Finally,the review provides a summary and an outlook on the future developments and challenges of wearable sweat biosensors with the aim of advancing the field of wearable sweat monitoring technology.
基金supported by the State Key Laboratory of Mechanical System and Vibration Project (Grant no.MSVZD202108)the open project of National Research Center for Translational Medicine,Shanghai (Project no.TMSK2021-146).
文摘Sweat is a biofluid with rich information that can reflect an individual’s state of health or activity.But the real-time in situ sweat sensors lack the ability of long-term monitoring.Against this background,this article provides a holistic review on the necessary process and methods for sweat sensing,including sweat collection,composition analysis,energy supply,and data processing.The impacts of the environment in stimulating sweat production,providing energy supply,and intelligent health monitoring are discussed.Based on the review of previous endeavors,the future development in material,structure and artificial intelligence application of long-term sweat monitoring is envisioned.
