Skin-attachable electronics have garnered considerable research attention in health monitoring and artificial intelligence domains,whereas susceptibility to elec-tromagnetic interference(EMI),heat accumulation issues,...Skin-attachable electronics have garnered considerable research attention in health monitoring and artificial intelligence domains,whereas susceptibility to elec-tromagnetic interference(EMI),heat accumulation issues,and ultraviolet(UV)-induced aging problems pose significant constraints on their potential applications.Here,an ultra-elas-tic,highly breathable,and thermal-comfortable epidermal sensor with exceptional UV-EMI shielding performance and remarkable thermal conductivity is developed for high-fidelity monitoring of multiple human electrophysiological signals.Via filling the elastomeric microfibers with thermally conductive boron nitride nanoparticles and bridging the insulating fiber interfaces by plating Ag nanoparticles(NPs),an interwoven thermal con-ducting fiber network(0.72 W m^(-1) K^(-1))is constructed benefiting from the seamless thermal interfaces,facilitating unimpeded heat dissipation for comfort skin wearing.More excitingly,the elastomeric fiber substrates simultaneously achieve outstanding UV protection(UPF=143.1)and EMI shielding(SET>65,X-band)capabilities owing to the high electrical conductivity and surface plasmon resonance of Ag NPs.Furthermore,an electronic textile prepared by printing liquid metal on the UV-EMI shielding and thermally conductive nonwoven textile is finally utilized as an advanced epidermal sensor,which succeeds in monitoring different electrophysiological signals under vigorous electromagnetic interference.This research paves the way for developing protective and environmentally adaptive epidermal electronics for next-generation health regulation.展开更多
The poor reversibility of Zn anodes induced by dendrite growth,surface passivation,and corrosion,severely hinders the practical applicability of Zn metal batteries.To address these issues,a plasmaassisted aerogel(PAG)...The poor reversibility of Zn anodes induced by dendrite growth,surface passivation,and corrosion,severely hinders the practical applicability of Zn metal batteries.To address these issues,a plasmaassisted aerogel(PAG)interface engineering was proposed as efficient ion transport modulator that can simultaneously regulate uniform Zn^(2+)flux and desolvation behavior during battery operation.The PAG with ordered mesopores acted as an ion sieve to homogenize Zn deposition and accelerate Zn^(2+)flux,which is favorable for corrosion resistance and dendrite suppression.Importantly,the plasma-assisted aerogel with abundant hydrophilic groups can facilitate the desolvation kinetics of Zn^(2+)due to the multiple hydrogen-bonding interaction with the activated water molecules,thus accelerating the Zn^(2+)migration kinetics.Consequently,the Zn/Zn cell assembled with PAG-modified separator demonstrates stable plating and stripping behavior(over 1400 h at 1 mA cm^(-2))and high Coulombic efficiency(99.8%at1 mA cm^(-2)after 1100 cycles),and the Zn‖MnO_(2)full cell shows excellent long-term cycling stability and maintains a high capacity of 154.9 mA h g^(-1)after 1000 cycles at 1 A g^(-1).This study provides a feasible approach for the large-scale fabrication of aerogel functionalized separators to realize ultra-stable Zn metal batteries.展开更多
Photocatalytic water splitting based on semiconductor photocatalysts is a promising approach for producing carbon‐neutral,sustainable,and clean H_(2) fuel.Cocatalyst loading,which is an appealing strategy,has been ex...Photocatalytic water splitting based on semiconductor photocatalysts is a promising approach for producing carbon‐neutral,sustainable,and clean H_(2) fuel.Cocatalyst loading,which is an appealing strategy,has been extensively employed to improve the photocatalytic efficiency semiconductors.In view of the high cost and rare preservation of noble metal cocatalysts that significantly hinder their utilization for large‐scale energy production,various cocatalysts comprising earth‐abundant ele‐ments have been developed as noble‐metal‐free candidates using different methods to boost pho‐tocatalytic water splitting.Among these preparation strategies,photodeposition has attracted tre‐mendous attention in the deposition of earth‐abundant cocatalysts owing to its simplicity and mod‐erate availability,improved interfacial charge separation and transfer,and abundant active sites on the surface.In this review,we first summarize the deposition principles,deposition advantages,categories of cocatalysts,roles of cocatalysts,influencing factors,modification strategies,and design considerations in the photodeposition of earth‐abundant cocatalysts.The photodeposited earth‐abundant cocatalysts for the photocatalytic H_(2) evolution half reaction,photocatalytic O_(2) evo‐lution half reaction,and overall photocatalytic water splitting are discussed.Finally,some perspec‐tives on the challenges and possible future directions for the photodeposition of earth‐abundant cocatalysts in photocatalytic water splitting are presented.展开更多
Sodium iron hexacyanoferrate(FeHCF)is one of the most promising cathode materials for sodium-ion batteries(SIBs)due to its low cost theoretical capacity.However,the low electrochemical activity of Fe^(LS)(C)in FeHCF d...Sodium iron hexacyanoferrate(FeHCF)is one of the most promising cathode materials for sodium-ion batteries(SIBs)due to its low cost theoretical capacity.However,the low electrochemical activity of Fe^(LS)(C)in FeHCF drags down its practical capacity and potential plateau.Herein,FeHCF with high Fe^(LS)(C)electrochemical activity(C-FeHCF)is synthesized via a facile citric acid-assisted solvothermal method.As the cathode of SIBs,C-FeHCF shows superior cycling stability(ca.87.3%capacity retention for 1000 cycles at 10 C)and outstanding rate performance(ca.68.5%capacity retention at 50 C).Importantly,the contribution of Fe^(LS)(C)to the whole capacity was quantitatively analyzed via combining dQ/dV and discharge curve for the first time,and the index reaches 44.53%for C-FeHCF,close to the theoretical value.In-situ X-ray diffraction proves the structure stability of C-FeHCF during charge-discharge process,ensuring its superior cycling performance.Furthermore,the application feasibility of the C-FeHCF cathode in quasi-solid SIBs is also evaluated.The quasi-solid SIBs with the C-FeHCF cathode exhibit excellent electrochemical performance,delivering an initial discharge capacity of 106.5 mAh g^(−1) at 5 C and high capacity retention of 89.8%over 1200 cycles.This work opens new insights into the design and development of advanced cathode materials for SIBs and the beyond.展开更多
In order to prepare the polyethylene materials with controlling properties,we developed two kinds of controllable cross-linking polyethylene foaming system.2,5-dimethyl-2,5-bis (tert-butyl peroxy) hexane was used as c...In order to prepare the polyethylene materials with controlling properties,we developed two kinds of controllable cross-linking polyethylene foaming system.2,5-dimethyl-2,5-bis (tert-butyl peroxy) hexane was used as cross-linking agent and TEMPO as cross-linking inhibitor,azodicarbonamide (AC) was used as foaming agent and citric acid as foaming promoter.The density,expansion ratio,cellular structure and mechanical property of these two kinds of controllable materials were studied.Experimental results show that,properties of these two kinds of materials appear similar trend:cellular size and expansion ratio are enlarged with the amount of cross-linking inhibitor or foaming promoter increasing,while density and mechanical strength appear decreasing trend.Through comparing those two material systems’ properties,cross-linking polyethelene foaming system with citric acid as foaming promoter has better properties.展开更多
Engineering the electronic structure of surface active sites at the atomic level can be an efficient way to modulate the reactivity of catalysts.Herein,we report the rational tuning of surface electronic structure of ...Engineering the electronic structure of surface active sites at the atomic level can be an efficient way to modulate the reactivity of catalysts.Herein,we report the rational tuning of surface electronic structure of FePS_(3) nanosheets(NSs)by anchoring atomically dispersed metal atom.Theoretical calculations predict that the strong electronic coupling effect in single-atom Ni-FePS_(3) facilitates electron aggregation from Fe atom to the nearby Ni-S bond and enhances the electron-transfer of Ni and S sites,which balances the oxygen species adsorption capacity,reinforces water adsorption and dissociation process to accelerate corresponding oxygen evolution reaction(OER)and hydrogen evolution reaction(HER).The optimal Ni-FePS_(3)NSs/C exhibits outstanding electrochemical water-splitting activities,delivering an overpotential of 287 mV at the current density of 10 mA cm^(-2) and a Tafel slope of 41.1 mV dec^(-1) for OER;as well as an overpotential decrease of 219 mV for HER compared with pure FePS_(3)NSs/C.The concept of electronic coupling interaction between the substrate and implanted single active species offers an additional method for catalyst design and beyond.展开更多
In this study,Ag/γ-Al_(2)O_(3)catalysts were synthesized by an Ar dielectric barrier discharge plasma using silver nitrate as the Ag source andγ-alumina(γ-Al_(2)O_(3))as the support.It is revealed that plasma can r...In this study,Ag/γ-Al_(2)O_(3)catalysts were synthesized by an Ar dielectric barrier discharge plasma using silver nitrate as the Ag source andγ-alumina(γ-Al_(2)O_(3))as the support.It is revealed that plasma can reduce silver ions to generate crystalline silver nanoparticles(Ag NPs)of good dispersion and uniformity on the alumina surface,leading to the formation of Ag/γ-Al_(2)O_(3)catalysts in a green manner without traditional chemical reductants.Ag/γ-Al_(2)O_(3)exhibited good catalytic activity and stability in CO oxidation reactions,and the activity increased with increase in the Ag content.For catalysts with more than 2 wt%Ag,100%CO conversion can be achieved at 300°C.The catalytic activity of the Ag/γ-Al_(2)O_(3)catalysts is also closely related to the size of theγ-alumina,where Ag/nano-γ-Al_(2)O_(3)catalysts demonstrate better performance than Ag/micro-γ-Al_(2)O_(3)catalysts with the same Ag content.In addition,the catalytic properties of plasma-generated Ag/nano-γ-Al_(2)O_(3)(Ag/γ-Al_(2)O_(3)-P)catalysts were compared with those of Ag/nano-γ-Al_(2)O_(3)catalysts prepared by the traditional calcination approach(Ag/γ-Al_(2)O_(3)-C),with the plasma-generated samples demonstrating better overall performance.This simple,rapid and green plasma process is considered to be applicable for the synthesis of diverse noble metal-based catalysts.展开更多
The demand for highly porous yet transparent aerogels with mechanical flexibility and solar-thermal dual-regulation for energy-saving windows is significant but challenging.Herein,a delaminated aerogel film(DAF)is fab...The demand for highly porous yet transparent aerogels with mechanical flexibility and solar-thermal dual-regulation for energy-saving windows is significant but challenging.Herein,a delaminated aerogel film(DAF)is fabricated through filtration-induced delaminated gelation and ambient drying.The delaminated gelation process involves the assembly of fluorinated cellulose nanofiber(FCNF)at the solid-liquid interface between the filter and the filtrate during filtration,resulting in the formation of lamellar FCNF hydrogels with strong intra-plane and weak interlayer hydrogen bonding.By exchanging the solvents from water to hexane,the hydrogen bonding in the FCNF hydrogel is further enhanced,enabling the formation of the DAF with intra-layer mesopores upon ambient drying.The resulting aerogel film is lightweight and ultra-flexible,which pos-sesses desirable properties of high visible-light transmittance(91.0%),low thermal conductivity(33 mW m^(-1) K^(-1)),and high atmospheric-window emissivity(90.1%).Furthermore,the DAF exhibits reduced surface energy and exceptional hydrophobicity due to the presence of fluorine-containing groups,enhancing its durability and UV resistance.Consequently,the DAF has demonstrated its potential as solar-thermal regulatory cooling window materials capable of simultaneously providing indoor lighting,thermal insulation,and daytime radiative cooling under direct sunlight.Significantly,the enclosed space protected by the DAF exhibits a temperature reduction of 2.6℃ compared to that shielded by conventional architectural glass.展开更多
Copper-based metal-organic frameworks(Cu-MOFs)are a promising multiphase catalyst for catalyzing C-S coupling reactions by virtue of their diverse structures and functions.However,the unpleasant odor and instability o...Copper-based metal-organic frameworks(Cu-MOFs)are a promising multiphase catalyst for catalyzing C-S coupling reactions by virtue of their diverse structures and functions.However,the unpleasant odor and instability of the organosulfur,as well as the mass-transfer resistance that exists in multiphase catalysis,have often limited the catalytic application of Cu-MOFs in C-S coupling reactions.In this paper,a Cu-MOFs catalyst modified by cetyltrimethylammonium bromide(CTAB)was designed to enhance mass transfer by increasing the adsorption of organic substrates using the long alkanes of CTAB.Concurrently,elemental sulfur was used to replace organosulfur to achieve a highly efficient and atom-economical multicomponent C-S coupling reaction.展开更多
The rapid quantification of hydroxyl radical (·OH) in real samples is a great challenge due to its highly reactive nature and the potential interferences from other coexisting reactive oxygen species (ROS). Herei...The rapid quantification of hydroxyl radical (·OH) in real samples is a great challenge due to its highly reactive nature and the potential interferences from other coexisting reactive oxygen species (ROS). Herein, a chemiluminescence (CL) probe (ox-CDs) was rationally developed for the detection of ·OH through controlled oxidation treatment of original CDs (o-CDs) with H_(2)O_(2). Post-oxidation of CDs can reduce the surface defects or functional groups on the CDs, exposing reactive sites capable of effectively reacting with ·OH. The chemical energy generated from redox reaction between ·OH and the ox-CDs can be efficiently utilized to generate strong and selective CL responses to ·OH without interferences from other ROS. Thus, a highly selective and sensitive CL method with a linear range from 0.01 to 150 μM and a detection limit of 3 nM was developed, which was successfully applied for monitoring the ·OH production from cigarette and mosquito coil smoke.展开更多
It is of great significance to synthesize carbon dots(CDs)with desirable hydrophilicity for the ever-growing application of CDs in different fields.In this study,the hydrophilic and hydrophobic CDs were facilely prepa...It is of great significance to synthesize carbon dots(CDs)with desirable hydrophilicity for the ever-growing application of CDs in different fields.In this study,the hydrophilic and hydrophobic CDs were facilely prepared by solvothermal treatment of o-dihydroxybenzene and urea in N,N-dimethylformamide(DMF).Optimization experiments revealed that the solvothermal temperature has a great impact on the surface states of the CDs.The hydrophobic CDs with a contact angle of 110.7°was obtained at 200℃.The structural and optical characterizations,along with theoretical calculations elucidated that the lipophilic nature of the CDs was resulting from the formation of polymer chains.The presence of extended conjugated sp^(2)-domains and amino groups contributed to the red emission of the CDs synthesized at low reaction temperatures(160-200℃).With the further increase of solvothermal temperature,the hydrophobic CDs were gradually transformed to the hydrophilic state accompanying the blue shift of the fluorescence of the CDs.The highly hydrophilic CDs with a contact angle of 25.9°were obtained at 240℃ due to the increased formation of hydrophilic functional groups on the surface of CDs.The red emissive CDs exhibited a sensitive color and fluorescence response to ethanol content while the fluorescence of the blue emissive CDs remained constant.By combining the two kinds of CDs,a dual-emission sensor was constructed,which was successfully applied for the evaluation of the alcoholic strength in commercial Baijiu commodities in both fluorometric and colorimetric modes.展开更多
The d-d orbital coupling induced by crystal-phase engineering can effectively adjust the electronic structure of electrocatalysts,thus showing significant catalytic performance,while it has been rarely explored in ele...The d-d orbital coupling induced by crystal-phase engineering can effectively adjust the electronic structure of electrocatalysts,thus showing significant catalytic performance,while it has been rarely explored in electrochemical acetonitrile reduction reaction(ARR)to date.Herein,we successfully realize the structural transformation of Pd Cu metallic aerogels(MAs)from face-centered cubic(FCC)to body-centered cubic(BCC)through annealing treatment.Specifically,the BCC Pd Cu MAs exhibit excellent ARR performance with high ethylamine selectivity of 90.91%,Faradaic efficiency of 88.60%,yield rate of 316.0 mmol h^(-1)g^(-1)_(Pd+Cu)and long-term stability for consecutive electrolysis within 20 h at-0.55 V vs.reversible hydrogen electrode,outperforming than those of FCC Pd Cu MAs.Under the membrane electrode assembly system,BCC Pd Cu MAs also demonstrate excellent ethylamine yield rate of 389.5 mmol h^(-1)g^(-1)_(Pd+Cu).Density functional theory calculation reveals that the d-d orbital coupling in BCC Pd Cu MAs results in an evident correlation effect for the interaction of Pd and Cu sites,which boosts up the Cu sites electronic activities to enhance ARR performance.Our work opens a new route to develop efficient ARR electrocatalysts from the perspective of crystalline structure transformation.展开更多
Negatively thermo-responsive 2D membranes,which mimic the stomatal opening/closing of plants,have drawn substantial interest for tunable molecular separation processes.However,these membranes are still restricted sign...Negatively thermo-responsive 2D membranes,which mimic the stomatal opening/closing of plants,have drawn substantial interest for tunable molecular separation processes.However,these membranes are still restricted significantly on account of low water permeability and poor dynamic tunability of 2D nanochannels under temperature stimulation.Here,we present a biomimetic negatively thermo-responsive MXene membrane by covalently grafting poly(N-isopropylacrylamide)(PNIPAm)onto MXene nanosheets.The uniformly grafted PNIPAm polymer chains can enlarge the interlayer spacings for increasing water permeability while also allowing more tunability of 2D nanochannels for enhancing the capability of gradually separating multiple molecules of different sizes.As expected,the constructed membrane exhibits ultrahigh water permeance of 95.6 L m^(-2) h^(-1) bar^(-1) at 25℃,which is eight-fold higher than the state-of-the-art negatively thermoresponsive 2D membranes.Moreover,the highly temperature-tunable 2D nanochannels enable the constructed membrane to perform excellent graded molecular sieving for dye-and antibiotic-based ternary mixtures.This strategy provides new perspectives in engineering smart 2D membrane and expands the scope of temperature-responsive membranes,showing promising applications in micro/nanofluidics and molecular separation.展开更多
Personal daytime radiative cooling(PDRC)materials have high sunlight reflection and high selective emis-sivity to outer space in the main atmospheric window,demonstrating huge potential in energy-saving for sustainabl...Personal daytime radiative cooling(PDRC)materials have high sunlight reflection and high selective emis-sivity to outer space in the main atmospheric window,demonstrating huge potential in energy-saving for sustainable development.Recently,polymer-based membranes for radiative cooling have been widely re-ported,due to their easy processing,low cost,and unique optical performance.However,the desired high sunlight reflectance of PDRC materials is easily dampened by environmental aging,high temperature,and ultraviolet(UV)irradiation,resulting in reduced cooling performance for most polymers,adverse to large-scale practical applications.In this work,we demonstrate a novel polyimide nanofiber(PINF)membrane with a fluorine-containing structure via typical electrospinning technology.The resultant PINF membrane exhibits high sunlight reflectance,UV resistance,and excellent thermal stability,rendering anti-aging day-time radiative cooling.The sunlight reflectance of PINF membranes could maintain constant in the aging test for continuous 720 h under outdoor solar irradiation,exhibiting durable and long-term personal day-time radiative cooling performance.展开更多
Chiral nanomaterials have distinct chiroptical properties of preferential interactions to circularly polarized lights.Chirality-based biosensors have emerged for detection of biomolecules,ions and cells in recent year...Chiral nanomaterials have distinct chiroptical properties of preferential interactions to circularly polarized lights.Chirality-based biosensors have emerged for detection of biomolecules,ions and cells in recent years.This review provides an extensive overview of biosensors based on chiral nanomaterials,starting with approaches to chiral nanomaterials construction in terms of fabrication strategies.Fabrication of chiral nanomaterials and their biosensor applications is presented for different material types,with special emphasis on the role and importance of material properties and signal generation in detection.We assessed the technological prospects of the emerging fields of chiral construction,circularly polarized luminescence,Raman optical activity and so on along with their current challenges.Prospective venues for future research on chiral nanomaterials in fabrication,biosensing,disease diagnosis and treatment are also presented in the review.展开更多
Tianxi Liu was missed to be denoted as a corresponding author in the article.Both Chao Zhang and Tianxi Liu are the corresponding authors of this article.The original article has been corrected.Open Access This articl...Tianxi Liu was missed to be denoted as a corresponding author in the article.Both Chao Zhang and Tianxi Liu are the corresponding authors of this article.The original article has been corrected.Open Access This article is licensed under a Creative Commons Attribution 4.0 International License,which permits use,sharing,adaptation,distribution,and reproduction in any medium or format,as long as you give appropriate credit to the original author(s)and the source,provide a link to the Creative Commons licence,and indicate if changes were made.The images or other third-party material in this article are included in the article’s Creative Commons licence,unless indicated otherwise in a credit line to the material.If material is not included in the article’s Creative Commons licence and your intended use is not permitted by statutory regulation or exceeds the permitted use,you will need to obtain permission directly from the copyright holder.展开更多
Fluorescent nanomaterials have attracted much attention,due to their unique luminescent properties and promis-ing applications in biomedical areas.In this study,lignin basedfluorescent nanoparticles(LFNP)with high yiel...Fluorescent nanomaterials have attracted much attention,due to their unique luminescent properties and promis-ing applications in biomedical areas.In this study,lignin basedfluorescent nanoparticles(LFNP)with high yield(up to 32.4%)were prepared from lignin nanoparticles(LNP)by one-pot hydrothermal method with ethylene-diamine(EDA)and citric acid.Morphology and chemical structure of LFNP were investigated by SEM,FT-IR,and zeta potential,and it was found that the structure of LFNP changed with the increase of citric acid addition.LFNP showed the highestfluorescence intensity under UV excitation at wavelengths of 375–385 nm,with emis-sion wavelengths between 454–465 nm,and exhibited strong photoluminescence behavior.Meanwhile,with the increase of citric acid content,the energy gap(ΔE)gradually decreased from 3.87 to 3.14 eV,which corresponds to the gradual enhancement offluorescence performance.LFNP also exhibited excellent antioxidant activity,with DPPH free radical scavenging rate increased from 80.8%for LNP up to 96.7%for LFNP,confirming the great potential of these materials for application in biomedicine and cosmetic health care.展开更多
Conversion of methane into value-added chemicals is of significance for methane utilization and industrial demand of primary chemical products.The barrier associated with the nonpolar structure of methane and the high...Conversion of methane into value-added chemicals is of significance for methane utilization and industrial demand of primary chemical products.The barrier associated with the nonpolar structure of methane and the high bond energy C-H bond(4.57 eV)makes it difficult to realize methane conversion and activation under mild conditions.The photothermal synergetic strategy by combining photon energy and thermo energy provides an advanced philosophy to achieve efficient methane conversion.In this review,we overview the current pioneering studies of photothermal methane indirect conversion and present the methane direct conversion by the way of photocatalysis and thermocatalysis to provide a fundamental understanding of methane activation.Finally,we end this review with a discussion on the remaining challenges and perspectives of methane direct conversion over single-atom catalysts via photothermal synergetic strategy.展开更多
Membrane separation technology has been taken up for use in diverse applications such as water treatment,pharmaceutical,petroleum,and energy-related industries.Compared with the design of membrane materials,the innova...Membrane separation technology has been taken up for use in diverse applications such as water treatment,pharmaceutical,petroleum,and energy-related industries.Compared with the design of membrane materials,the innovation of membrane preparation technique is more urgent for the development of membrane separation technology,because it not only affects physicochemical properties and separation performance of the fabricated membranes,but also determines their potential in industrialized application.Among the various membrane preparation methods,spray technique has recently gained increasing attention because of its low cost,rapidity,scalability,minimum of environmental burden,and viability for nearly unlimited range of materials.In this Review article,we summarized and discussed the recent developments in separation membranes using the spray technique,including the fundamentals,important features and applications.The present challenges and future considerations have been touched to provide inspired insights for developing the sprayed separation membranes.展开更多
In order to develop functional energy storage device,it is necessary to improve the energy and power density.As a potential candidate that can synergistically harmonize energy and power density,lithium ion capacitor(L...In order to develop functional energy storage device,it is necessary to improve the energy and power density.As a potential candidate that can synergistically harmonize energy and power density,lithium ion capacitor(LIC)has shown exciting promises in recent years.However,in the recent years,alternative metal has been explored to replace lithium in such metal-ion capacitor system.Hence,in this work we present zinc ion capacitor(ZIC)in which zinc acts as negative electrode and Metal Organic framework(MOF)derived carbon as positive electrode.The assembled ZIC was able to demonstrate exceptional power density of 85.5 kW kg^-1 and a maximal energy density of 36.4W h kg^-1,together with 99%capacitance retention after cycling for 20000 cycles.展开更多
基金financially supported by the National Natural Science Foundation of China(52373079,52161135302,52233006)the China Postdoctoral Science Foundation(2022M711355)the Natural Science Foundation of Jiangsu Province(BK20221540).
文摘Skin-attachable electronics have garnered considerable research attention in health monitoring and artificial intelligence domains,whereas susceptibility to elec-tromagnetic interference(EMI),heat accumulation issues,and ultraviolet(UV)-induced aging problems pose significant constraints on their potential applications.Here,an ultra-elas-tic,highly breathable,and thermal-comfortable epidermal sensor with exceptional UV-EMI shielding performance and remarkable thermal conductivity is developed for high-fidelity monitoring of multiple human electrophysiological signals.Via filling the elastomeric microfibers with thermally conductive boron nitride nanoparticles and bridging the insulating fiber interfaces by plating Ag nanoparticles(NPs),an interwoven thermal con-ducting fiber network(0.72 W m^(-1) K^(-1))is constructed benefiting from the seamless thermal interfaces,facilitating unimpeded heat dissipation for comfort skin wearing.More excitingly,the elastomeric fiber substrates simultaneously achieve outstanding UV protection(UPF=143.1)and EMI shielding(SET>65,X-band)capabilities owing to the high electrical conductivity and surface plasmon resonance of Ag NPs.Furthermore,an electronic textile prepared by printing liquid metal on the UV-EMI shielding and thermally conductive nonwoven textile is finally utilized as an advanced epidermal sensor,which succeeds in monitoring different electrophysiological signals under vigorous electromagnetic interference.This research paves the way for developing protective and environmentally adaptive epidermal electronics for next-generation health regulation.
基金financially supported by the National Natural Science Foundation of China(NSFC)(52203261)Natural Science Foundation of Jiangsu Province(BK20210474)the project of research on the industrial application of"controllable synthesis of nanocarbon-based polymer composites and their application in new energy”(N0.CJGJZD20210408092400002).
文摘The poor reversibility of Zn anodes induced by dendrite growth,surface passivation,and corrosion,severely hinders the practical applicability of Zn metal batteries.To address these issues,a plasmaassisted aerogel(PAG)interface engineering was proposed as efficient ion transport modulator that can simultaneously regulate uniform Zn^(2+)flux and desolvation behavior during battery operation.The PAG with ordered mesopores acted as an ion sieve to homogenize Zn deposition and accelerate Zn^(2+)flux,which is favorable for corrosion resistance and dendrite suppression.Importantly,the plasma-assisted aerogel with abundant hydrophilic groups can facilitate the desolvation kinetics of Zn^(2+)due to the multiple hydrogen-bonding interaction with the activated water molecules,thus accelerating the Zn^(2+)migration kinetics.Consequently,the Zn/Zn cell assembled with PAG-modified separator demonstrates stable plating and stripping behavior(over 1400 h at 1 mA cm^(-2))and high Coulombic efficiency(99.8%at1 mA cm^(-2)after 1100 cycles),and the Zn‖MnO_(2)full cell shows excellent long-term cycling stability and maintains a high capacity of 154.9 mA h g^(-1)after 1000 cycles at 1 A g^(-1).This study provides a feasible approach for the large-scale fabrication of aerogel functionalized separators to realize ultra-stable Zn metal batteries.
文摘Photocatalytic water splitting based on semiconductor photocatalysts is a promising approach for producing carbon‐neutral,sustainable,and clean H_(2) fuel.Cocatalyst loading,which is an appealing strategy,has been extensively employed to improve the photocatalytic efficiency semiconductors.In view of the high cost and rare preservation of noble metal cocatalysts that significantly hinder their utilization for large‐scale energy production,various cocatalysts comprising earth‐abundant ele‐ments have been developed as noble‐metal‐free candidates using different methods to boost pho‐tocatalytic water splitting.Among these preparation strategies,photodeposition has attracted tre‐mendous attention in the deposition of earth‐abundant cocatalysts owing to its simplicity and mod‐erate availability,improved interfacial charge separation and transfer,and abundant active sites on the surface.In this review,we first summarize the deposition principles,deposition advantages,categories of cocatalysts,roles of cocatalysts,influencing factors,modification strategies,and design considerations in the photodeposition of earth‐abundant cocatalysts.The photodeposited earth‐abundant cocatalysts for the photocatalytic H_(2) evolution half reaction,photocatalytic O_(2) evo‐lution half reaction,and overall photocatalytic water splitting are discussed.Finally,some perspec‐tives on the challenges and possible future directions for the photodeposition of earth‐abundant cocatalysts in photocatalytic water splitting are presented.
基金supported by the Natural Science Foundation of Jiangsu Province (No.BK20210474)the National Natural Science Foundation of China (No.21938005)the Fundamental Research Funds for the Central Universities (No.JUSRP122013).
文摘Sodium iron hexacyanoferrate(FeHCF)is one of the most promising cathode materials for sodium-ion batteries(SIBs)due to its low cost theoretical capacity.However,the low electrochemical activity of Fe^(LS)(C)in FeHCF drags down its practical capacity and potential plateau.Herein,FeHCF with high Fe^(LS)(C)electrochemical activity(C-FeHCF)is synthesized via a facile citric acid-assisted solvothermal method.As the cathode of SIBs,C-FeHCF shows superior cycling stability(ca.87.3%capacity retention for 1000 cycles at 10 C)and outstanding rate performance(ca.68.5%capacity retention at 50 C).Importantly,the contribution of Fe^(LS)(C)to the whole capacity was quantitatively analyzed via combining dQ/dV and discharge curve for the first time,and the index reaches 44.53%for C-FeHCF,close to the theoretical value.In-situ X-ray diffraction proves the structure stability of C-FeHCF during charge-discharge process,ensuring its superior cycling performance.Furthermore,the application feasibility of the C-FeHCF cathode in quasi-solid SIBs is also evaluated.The quasi-solid SIBs with the C-FeHCF cathode exhibit excellent electrochemical performance,delivering an initial discharge capacity of 106.5 mAh g^(−1) at 5 C and high capacity retention of 89.8%over 1200 cycles.This work opens new insights into the design and development of advanced cathode materials for SIBs and the beyond.
基金Funded by National Natural Science Foundation of China (No.21975108)Fundamental Research Funds for the Central Universities of China (No.JUSRP121033)。
文摘In order to prepare the polyethylene materials with controlling properties,we developed two kinds of controllable cross-linking polyethylene foaming system.2,5-dimethyl-2,5-bis (tert-butyl peroxy) hexane was used as cross-linking agent and TEMPO as cross-linking inhibitor,azodicarbonamide (AC) was used as foaming agent and citric acid as foaming promoter.The density,expansion ratio,cellular structure and mechanical property of these two kinds of controllable materials were studied.Experimental results show that,properties of these two kinds of materials appear similar trend:cellular size and expansion ratio are enlarged with the amount of cross-linking inhibitor or foaming promoter increasing,while density and mechanical strength appear decreasing trend.Through comparing those two material systems’ properties,cross-linking polyethelene foaming system with citric acid as foaming promoter has better properties.
基金the National Natural Science Foundation of China(12025503,U1867215,11875211,U1932134)Hubei Provincial Natural Science Foundation(2019CFA036)the Fundamental Research Funds for the Central Universities(2042020kf0211)。
文摘Engineering the electronic structure of surface active sites at the atomic level can be an efficient way to modulate the reactivity of catalysts.Herein,we report the rational tuning of surface electronic structure of FePS_(3) nanosheets(NSs)by anchoring atomically dispersed metal atom.Theoretical calculations predict that the strong electronic coupling effect in single-atom Ni-FePS_(3) facilitates electron aggregation from Fe atom to the nearby Ni-S bond and enhances the electron-transfer of Ni and S sites,which balances the oxygen species adsorption capacity,reinforces water adsorption and dissociation process to accelerate corresponding oxygen evolution reaction(OER)and hydrogen evolution reaction(HER).The optimal Ni-FePS_(3)NSs/C exhibits outstanding electrochemical water-splitting activities,delivering an overpotential of 287 mV at the current density of 10 mA cm^(-2) and a Tafel slope of 41.1 mV dec^(-1) for OER;as well as an overpotential decrease of 219 mV for HER compared with pure FePS_(3)NSs/C.The concept of electronic coupling interaction between the substrate and implanted single active species offers an additional method for catalyst design and beyond.
基金financial support from National Natural Science Foundation of China(Nos.52004102 and 22078125)Postdoctoral Science Foundation of China(No.2021M690068)+2 种基金Fundamental Research Funds for the Central Universities(Nos.JUSRP221018 and JUSRP622038)Key Laboratory of Green Cleaning Technology and Detergent of Zhejiang Province(No.Q202204)Open Project of Key Laboratory of Green Chemical Engineering Process of Ministry of Education(No.GCP202112)。
文摘In this study,Ag/γ-Al_(2)O_(3)catalysts were synthesized by an Ar dielectric barrier discharge plasma using silver nitrate as the Ag source andγ-alumina(γ-Al_(2)O_(3))as the support.It is revealed that plasma can reduce silver ions to generate crystalline silver nanoparticles(Ag NPs)of good dispersion and uniformity on the alumina surface,leading to the formation of Ag/γ-Al_(2)O_(3)catalysts in a green manner without traditional chemical reductants.Ag/γ-Al_(2)O_(3)exhibited good catalytic activity and stability in CO oxidation reactions,and the activity increased with increase in the Ag content.For catalysts with more than 2 wt%Ag,100%CO conversion can be achieved at 300°C.The catalytic activity of the Ag/γ-Al_(2)O_(3)catalysts is also closely related to the size of theγ-alumina,where Ag/nano-γ-Al_(2)O_(3)catalysts demonstrate better performance than Ag/micro-γ-Al_(2)O_(3)catalysts with the same Ag content.In addition,the catalytic properties of plasma-generated Ag/nano-γ-Al_(2)O_(3)(Ag/γ-Al_(2)O_(3)-P)catalysts were compared with those of Ag/nano-γ-Al_(2)O_(3)catalysts prepared by the traditional calcination approach(Ag/γ-Al_(2)O_(3)-C),with the plasma-generated samples demonstrating better overall performance.This simple,rapid and green plasma process is considered to be applicable for the synthesis of diverse noble metal-based catalysts.
基金The authors are grateful for the financial support from the National Natural Science Foundation of China(Grant Nos.52273067,52122303,52233006)the Fundamental Research Funds for the Central Universities(Grant No.2232023A-03)the Shuguang Program of Shanghai Education Development Foundation and Shanghai Municipal Education Commission(23SG29).
文摘The demand for highly porous yet transparent aerogels with mechanical flexibility and solar-thermal dual-regulation for energy-saving windows is significant but challenging.Herein,a delaminated aerogel film(DAF)is fabricated through filtration-induced delaminated gelation and ambient drying.The delaminated gelation process involves the assembly of fluorinated cellulose nanofiber(FCNF)at the solid-liquid interface between the filter and the filtrate during filtration,resulting in the formation of lamellar FCNF hydrogels with strong intra-plane and weak interlayer hydrogen bonding.By exchanging the solvents from water to hexane,the hydrogen bonding in the FCNF hydrogel is further enhanced,enabling the formation of the DAF with intra-layer mesopores upon ambient drying.The resulting aerogel film is lightweight and ultra-flexible,which pos-sesses desirable properties of high visible-light transmittance(91.0%),low thermal conductivity(33 mW m^(-1) K^(-1)),and high atmospheric-window emissivity(90.1%).Furthermore,the DAF exhibits reduced surface energy and exceptional hydrophobicity due to the presence of fluorine-containing groups,enhancing its durability and UV resistance.Consequently,the DAF has demonstrated its potential as solar-thermal regulatory cooling window materials capable of simultaneously providing indoor lighting,thermal insulation,and daytime radiative cooling under direct sunlight.Significantly,the enclosed space protected by the DAF exhibits a temperature reduction of 2.6℃ compared to that shielded by conventional architectural glass.
基金support from the National Natural Science Foundation of China(22078130)the Fundamental Research Funds for the Central Universities(1042050205225990/010)Starting Research Fund of Qingyuan Innovation Laboratory(00523001).
文摘Copper-based metal-organic frameworks(Cu-MOFs)are a promising multiphase catalyst for catalyzing C-S coupling reactions by virtue of their diverse structures and functions.However,the unpleasant odor and instability of the organosulfur,as well as the mass-transfer resistance that exists in multiphase catalysis,have often limited the catalytic application of Cu-MOFs in C-S coupling reactions.In this paper,a Cu-MOFs catalyst modified by cetyltrimethylammonium bromide(CTAB)was designed to enhance mass transfer by increasing the adsorption of organic substrates using the long alkanes of CTAB.Concurrently,elemental sulfur was used to replace organosulfur to achieve a highly efficient and atom-economical multicomponent C-S coupling reaction.
基金supported by the National Natural Science Foundation of China(Nos.51973083 and 22376081).
文摘The rapid quantification of hydroxyl radical (·OH) in real samples is a great challenge due to its highly reactive nature and the potential interferences from other coexisting reactive oxygen species (ROS). Herein, a chemiluminescence (CL) probe (ox-CDs) was rationally developed for the detection of ·OH through controlled oxidation treatment of original CDs (o-CDs) with H_(2)O_(2). Post-oxidation of CDs can reduce the surface defects or functional groups on the CDs, exposing reactive sites capable of effectively reacting with ·OH. The chemical energy generated from redox reaction between ·OH and the ox-CDs can be efficiently utilized to generate strong and selective CL responses to ·OH without interferences from other ROS. Thus, a highly selective and sensitive CL method with a linear range from 0.01 to 150 μM and a detection limit of 3 nM was developed, which was successfully applied for monitoring the ·OH production from cigarette and mosquito coil smoke.
基金supported by the National Natural Science Foundation of China(Nos.51973083,22376081)the Fundamental Research Funds for the Central Universities(No.JUSRP22027).
文摘It is of great significance to synthesize carbon dots(CDs)with desirable hydrophilicity for the ever-growing application of CDs in different fields.In this study,the hydrophilic and hydrophobic CDs were facilely prepared by solvothermal treatment of o-dihydroxybenzene and urea in N,N-dimethylformamide(DMF).Optimization experiments revealed that the solvothermal temperature has a great impact on the surface states of the CDs.The hydrophobic CDs with a contact angle of 110.7°was obtained at 200℃.The structural and optical characterizations,along with theoretical calculations elucidated that the lipophilic nature of the CDs was resulting from the formation of polymer chains.The presence of extended conjugated sp^(2)-domains and amino groups contributed to the red emission of the CDs synthesized at low reaction temperatures(160-200℃).With the further increase of solvothermal temperature,the hydrophobic CDs were gradually transformed to the hydrophilic state accompanying the blue shift of the fluorescence of the CDs.The highly hydrophilic CDs with a contact angle of 25.9°were obtained at 240℃ due to the increased formation of hydrophilic functional groups on the surface of CDs.The red emissive CDs exhibited a sensitive color and fluorescence response to ethanol content while the fluorescence of the blue emissive CDs remained constant.By combining the two kinds of CDs,a dual-emission sensor was constructed,which was successfully applied for the evaluation of the alcoholic strength in commercial Baijiu commodities in both fluorometric and colorimetric modes.
基金financially supported by the National Natural Science Foundation of China(Grant Nos.52161135302,22105087)the Postdoctoral Research Foundation of China(Grant No.2022M721360)the Natural Science Foundation of Jiangsu Province(Grant No.BK20210446)。
文摘The d-d orbital coupling induced by crystal-phase engineering can effectively adjust the electronic structure of electrocatalysts,thus showing significant catalytic performance,while it has been rarely explored in electrochemical acetonitrile reduction reaction(ARR)to date.Herein,we successfully realize the structural transformation of Pd Cu metallic aerogels(MAs)from face-centered cubic(FCC)to body-centered cubic(BCC)through annealing treatment.Specifically,the BCC Pd Cu MAs exhibit excellent ARR performance with high ethylamine selectivity of 90.91%,Faradaic efficiency of 88.60%,yield rate of 316.0 mmol h^(-1)g^(-1)_(Pd+Cu)and long-term stability for consecutive electrolysis within 20 h at-0.55 V vs.reversible hydrogen electrode,outperforming than those of FCC Pd Cu MAs.Under the membrane electrode assembly system,BCC Pd Cu MAs also demonstrate excellent ethylamine yield rate of 389.5 mmol h^(-1)g^(-1)_(Pd+Cu).Density functional theory calculation reveals that the d-d orbital coupling in BCC Pd Cu MAs results in an evident correlation effect for the interaction of Pd and Cu sites,which boosts up the Cu sites electronic activities to enhance ARR performance.Our work opens a new route to develop efficient ARR electrocatalysts from the perspective of crystalline structure transformation.
基金supported by the National Nature Science Foundation of China(No.22278179,U23A20688)the National Key Research and Development Program of China(2021YFB3802600)+3 种基金the Fundamental Research Funds for the Central Universities(JUSRP622035)National First-Class Discipline Program of Light Industry Technology and Engineering(LIFE2018-19)MOE&SAFEA for the 111 Project(B13025)Natural Science Foundation of Xinjiang Uygur Autonomous Region(2022D01D030).
文摘Negatively thermo-responsive 2D membranes,which mimic the stomatal opening/closing of plants,have drawn substantial interest for tunable molecular separation processes.However,these membranes are still restricted significantly on account of low water permeability and poor dynamic tunability of 2D nanochannels under temperature stimulation.Here,we present a biomimetic negatively thermo-responsive MXene membrane by covalently grafting poly(N-isopropylacrylamide)(PNIPAm)onto MXene nanosheets.The uniformly grafted PNIPAm polymer chains can enlarge the interlayer spacings for increasing water permeability while also allowing more tunability of 2D nanochannels for enhancing the capability of gradually separating multiple molecules of different sizes.As expected,the constructed membrane exhibits ultrahigh water permeance of 95.6 L m^(-2) h^(-1) bar^(-1) at 25℃,which is eight-fold higher than the state-of-the-art negatively thermoresponsive 2D membranes.Moreover,the highly temperature-tunable 2D nanochannels enable the constructed membrane to perform excellent graded molecular sieving for dye-and antibiotic-based ternary mixtures.This strategy provides new perspectives in engineering smart 2D membrane and expands the scope of temperature-responsive membranes,showing promising applications in micro/nanofluidics and molecular separation.
基金National Natural Science Foundation of China(No.52073053)Young Elite Scientists Sponsorship Program by CAST(No.2021QNRC001)+2 种基金Shanghai Rising-Star Program(No.21QA1400300)Innovation Program of Shanghai Municipal Education Commission(No.2021–01–07–00–03-E00108)Fundamental Research Funds for the Central Universities(No.JUSRP123014).
文摘Personal daytime radiative cooling(PDRC)materials have high sunlight reflection and high selective emis-sivity to outer space in the main atmospheric window,demonstrating huge potential in energy-saving for sustainable development.Recently,polymer-based membranes for radiative cooling have been widely re-ported,due to their easy processing,low cost,and unique optical performance.However,the desired high sunlight reflectance of PDRC materials is easily dampened by environmental aging,high temperature,and ultraviolet(UV)irradiation,resulting in reduced cooling performance for most polymers,adverse to large-scale practical applications.In this work,we demonstrate a novel polyimide nanofiber(PINF)membrane with a fluorine-containing structure via typical electrospinning technology.The resultant PINF membrane exhibits high sunlight reflectance,UV resistance,and excellent thermal stability,rendering anti-aging day-time radiative cooling.The sunlight reflectance of PINF membranes could maintain constant in the aging test for continuous 720 h under outdoor solar irradiation,exhibiting durable and long-term personal day-time radiative cooling performance.
基金financially supported by the National Natural Science Foundation of China(No.22272065)the Natural Science Foundation of Jiangsu Province(No.BK20211530)+1 种基金the Fundamental Research Funds for the Central Universities(No.JUSRP622018)the Key Research and Development Special Project of Gao'an City,Jiangxi Province,China(No.2023ZDYFZX06)。
文摘Chiral nanomaterials have distinct chiroptical properties of preferential interactions to circularly polarized lights.Chirality-based biosensors have emerged for detection of biomolecules,ions and cells in recent years.This review provides an extensive overview of biosensors based on chiral nanomaterials,starting with approaches to chiral nanomaterials construction in terms of fabrication strategies.Fabrication of chiral nanomaterials and their biosensor applications is presented for different material types,with special emphasis on the role and importance of material properties and signal generation in detection.We assessed the technological prospects of the emerging fields of chiral construction,circularly polarized luminescence,Raman optical activity and so on along with their current challenges.Prospective venues for future research on chiral nanomaterials in fabrication,biosensing,disease diagnosis and treatment are also presented in the review.
文摘Tianxi Liu was missed to be denoted as a corresponding author in the article.Both Chao Zhang and Tianxi Liu are the corresponding authors of this article.The original article has been corrected.Open Access This article is licensed under a Creative Commons Attribution 4.0 International License,which permits use,sharing,adaptation,distribution,and reproduction in any medium or format,as long as you give appropriate credit to the original author(s)and the source,provide a link to the Creative Commons licence,and indicate if changes were made.The images or other third-party material in this article are included in the article’s Creative Commons licence,unless indicated otherwise in a credit line to the material.If material is not included in the article’s Creative Commons licence and your intended use is not permitted by statutory regulation or exceeds the permitted use,you will need to obtain permission directly from the copyright holder.
基金This work was financially supported by National Natural Science Foundation of China(51903106)State Administration of Foreign Experts Affairs(G2021144006L).
文摘Fluorescent nanomaterials have attracted much attention,due to their unique luminescent properties and promis-ing applications in biomedical areas.In this study,lignin basedfluorescent nanoparticles(LFNP)with high yield(up to 32.4%)were prepared from lignin nanoparticles(LNP)by one-pot hydrothermal method with ethylene-diamine(EDA)and citric acid.Morphology and chemical structure of LFNP were investigated by SEM,FT-IR,and zeta potential,and it was found that the structure of LFNP changed with the increase of citric acid addition.LFNP showed the highestfluorescence intensity under UV excitation at wavelengths of 375–385 nm,with emis-sion wavelengths between 454–465 nm,and exhibited strong photoluminescence behavior.Meanwhile,with the increase of citric acid content,the energy gap(ΔE)gradually decreased from 3.87 to 3.14 eV,which corresponds to the gradual enhancement offluorescence performance.LFNP also exhibited excellent antioxidant activity,with DPPH free radical scavenging rate increased from 80.8%for LNP up to 96.7%for LFNP,confirming the great potential of these materials for application in biomedicine and cosmetic health care.
基金This project was supported financially by the National Natural Science Foundation of China(21908079,21902009,21707052)Natural Science Foundation of Jiangsu Province(BK20201345)+3 种基金the State Key Laboratory of Fine Chemicals,Dalian University of Technology(KF2005)Startup Funding at Jiangnan University(1045210322190170,1045281602190010,1042050205204100)Jiangsu Agriculture Science and Technology Innovation Fund(CX(20)3108)Fundamental Research Funds for the Central Universities(JUSRP11905,JUSRP52004B).
文摘Conversion of methane into value-added chemicals is of significance for methane utilization and industrial demand of primary chemical products.The barrier associated with the nonpolar structure of methane and the high bond energy C-H bond(4.57 eV)makes it difficult to realize methane conversion and activation under mild conditions.The photothermal synergetic strategy by combining photon energy and thermo energy provides an advanced philosophy to achieve efficient methane conversion.In this review,we overview the current pioneering studies of photothermal methane indirect conversion and present the methane direct conversion by the way of photocatalysis and thermocatalysis to provide a fundamental understanding of methane activation.Finally,we end this review with a discussion on the remaining challenges and perspectives of methane direct conversion over single-atom catalysts via photothermal synergetic strategy.
基金supported by the National Key Research and Development Program of China(2021YF B3802600)National Key Research and Development Project of China(2018YFE0203500)the Natural Science Foundation of Jiangsu Province(BK20190603).
文摘Membrane separation technology has been taken up for use in diverse applications such as water treatment,pharmaceutical,petroleum,and energy-related industries.Compared with the design of membrane materials,the innovation of membrane preparation technique is more urgent for the development of membrane separation technology,because it not only affects physicochemical properties and separation performance of the fabricated membranes,but also determines their potential in industrialized application.Among the various membrane preparation methods,spray technique has recently gained increasing attention because of its low cost,rapidity,scalability,minimum of environmental burden,and viability for nearly unlimited range of materials.In this Review article,we summarized and discussed the recent developments in separation membranes using the spray technique,including the fundamentals,important features and applications.The present challenges and future considerations have been touched to provide inspired insights for developing the sprayed separation membranes.
文摘In order to develop functional energy storage device,it is necessary to improve the energy and power density.As a potential candidate that can synergistically harmonize energy and power density,lithium ion capacitor(LIC)has shown exciting promises in recent years.However,in the recent years,alternative metal has been explored to replace lithium in such metal-ion capacitor system.Hence,in this work we present zinc ion capacitor(ZIC)in which zinc acts as negative electrode and Metal Organic framework(MOF)derived carbon as positive electrode.The assembled ZIC was able to demonstrate exceptional power density of 85.5 kW kg^-1 and a maximal energy density of 36.4W h kg^-1,together with 99%capacitance retention after cycling for 20000 cycles.
