Wireless capsule endoscopy(WCE)has the potential to fully replace conventional wired counterparts for its low invasiveness.Recent studies have attempted to expand the functions of capsules toward this goal.However,lim...Wireless capsule endoscopy(WCE)has the potential to fully replace conventional wired counterparts for its low invasiveness.Recent studies have attempted to expand the functions of capsules toward this goal.However,limitations in space and energy supply have resulted in the inability to perform multiple diagnostic and treatment tasks using a single capsule.In this study,we developed a dual-functional capsule robot(DFCR)for drug delivery and tissue biopsy based on magnetic torsion spring technology.The delivery module was shown to rotate the push rod with a thrust of 894 mN to release approximately 0.3 mL of semisolid drug.The biopsy module used a built-in blade to cut tissue with a shear stress of 22.87 MPa,producing a sample of approximately 1.8 mm3.Additionally,a five-degree-of-freedom permanent magnet drive system was developed.By adjusting the strength of the unidirectional magnetic field generated by an external magnet,the capsule can be wirelessly controlled to sequentially trigger the two functions.Ex vivo tests on porcine stomachs confirmed the feasibility of the prototype capsule(12 mm in diameter and 45 mm in length)in active movement,medication,and tissue biopsy.The newly developed DFCR further expands the clinical application prospects of WCE robots in minimally invasive surgery.展开更多
Photocatalytic water splitting is a promising way to produce H_(2),a green and clean energy source.However,efficient H_(2) production typically relies on the addition of electron donors,such as alcohols and acids,whic...Photocatalytic water splitting is a promising way to produce H_(2),a green and clean energy source.However,efficient H_(2) production typically relies on the addition of electron donors,such as alcohols and acids,which are neither environmentally friendly nor cost-effective.Recently,we have witnessed a surge of studies in coupling photocatalytic H_(2) evolution with organic pollutant oxidation,which significantly promotes charge separation and improves the overall photocatalytic efficiency.It is thus an opportune time to critically assess the recent literature concerning dual-functional photocatalytic systems and provide perspectives for its future development.In this minireview,we begin with the working principles and requirements for synergistic photocatalytic systems.We then summarize and critically discuss the recent advances in photocatalytic H_(2) production and the degradation of various organic pollutants,including antibiotics,dyes,and phenols.Finally,we discuss the current challenges and suggest future directions for this field.展开更多
Dual-function communication radar systems use common Radio Frequency(RF)signals are used for both communication and detection.For better compatibility with existing communication systems,we adopt Multiple-Input Multip...Dual-function communication radar systems use common Radio Frequency(RF)signals are used for both communication and detection.For better compatibility with existing communication systems,we adopt Multiple-Input Multiple-Output(MIMO)Orthogonal Frequency Division Multiplexing(OFDM)signals as integrated signals and investigate the estimation performance of MIMO-OFDM signals.First,we analyze the Cramer-Rao Lower Bound(CRLB)of parameter estimation.Then,the transmit powers over different subcarriers are optimized to achieve the best tradeoff between the transmission rate and the estimation performance.Finally,we propose a more accurate estimation method that uses Canonical Polyadic Decomposition(CPD)of the third-order tensor to obtain the parameter matrices.Due to the characteristic of the column structure of the parameter matrices,we only need to use DFT/IDFT to recover the parameters of multiple targets.The simulation results show that tensor-based estimation method can achieve a performance close to CRLB,and the estimation performance can be improved by optimizing the transmit powers.展开更多
Binders could play crucial or even decisive roles in the fabrication of low-cost, stable and high-capacity electrodes. This is especially the case for the silicon (Si) anodes and sulfur (S) cathodes that undergo large...Binders could play crucial or even decisive roles in the fabrication of low-cost, stable and high-capacity electrodes. This is especially the case for the silicon (Si) anodes and sulfur (S) cathodes that undergo large volume change and active material loss in lithium-ion batteries during prolonged cycles. Herein, a hydrophilic polymer poly(methyl vinyl ether-alt-maleic acid) (PMVEMA) was explored as a dual-functional aqueous binder for the preparation of high-performance silicon anode and sulfur cathode. Benefiting from the dual functions of PMVEMA, i.e., the excellent dispersion ability and strong binding forces, the as-prepared electrodes exhibit improved capacity, rate capability and long-term cycling performance. In particular, the as-prepared Si electrode delivers a high initial discharge capacity of 1346.5 mAh g^(−1) at a high rate of 8.4 A/g and maintains 834.5 mAh g^(−1) after 300 cycles at 4.2 A/g, while the as-prepared S cathode exhibits enhanced cycling performance with high remaining discharge capacities of 663.4 mAh g^(−1) after 100 cycles at 0.2 C and 487.07 mAh g^(−1) after 300 cycles at 1 C, respectively. These encouraging results suggest that PMVEMA could be a universal binder to facilitate the green manufacture of both anode and cathode for high-capacity energy storage systems.展开更多
Although extremely challenging,it is highly desirable to develop self-healing materials that exhibit high efficiency under environmental conditions for marine protection applications.In this work,polyurethane elastome...Although extremely challenging,it is highly desirable to develop self-healing materials that exhibit high efficiency under environmental conditions for marine protection applications.In this work,polyurethane elastomers with hydrogen bond and dimethylglyoxime-urethane(DOU)coordination complex were combined with in-situ dual-functional BiOI@Bi_(2)S_(3) to synthesize high-efficiency photothermal cyclic self-healing antibacterial coating.The photothermal efficiency of BiOI@Bi_(2)S_(3) is improved by 38% through interfacial regulation.BiOI@Bi_(2)S_(3)/PU rapidly rises by 50.2℃ within 300 s under near-infrared(NIR)light,which can trigger the hydrogen bond of polyurethane coating and recover the barrier properties of the coating through self-healing.Density functional theory was used to simulate and analyze the generation of multiple electron transfer paths after the vulcanization of BiOI,which improves the interfacial mobility of photogenerated carriers and generates more heat.Importantly,molecular dynamics verified the self-healing mechanism of hydrogen bond and the photothermal lifting mechanism of the coating.After 5th scratches and self-healing cycle tests,the coating has a self-healing efficiency of more than 80%,which can ensure the self-healing and anticorrosion protection performance of the coating for multiple cycles.The photocatalytic and photothermal properties of BiOI@Bi_(2)S_(3) enhance the antibacterial rate of the coating up to 99%.This work provides heuristic perspectives for the design of coatings with anti-corrosion,antibacterial and self-healing properties.展开更多
Developing sulfur cathodes with high catalytic activity on accelerating the sluggish redox kinetics of lithium polysulfides(Li PSs) and unveiling their mechanisms are pivotal for advanced lithium–sulfur(Li–S)batteri...Developing sulfur cathodes with high catalytic activity on accelerating the sluggish redox kinetics of lithium polysulfides(Li PSs) and unveiling their mechanisms are pivotal for advanced lithium–sulfur(Li–S)batteries. Herein, MoS2 is verified to reduce the Gibbs free energy for rate-limiting step of sulfur reduction and the dissociation energy of lithium sulfide(Li2 S) for the first time employing theoretical calculations. The Mo S2 nanosheets coated on mesoporous hollow carbon spheres(MHCS) are then reasonably designed as a sulfur host for high-capacity and long-life Li–S battery, in which MHCS can guarantee the high sulfur loading and fast electron/ion transfer. It is revealed that the shuttle effect is efficiently inhibited because of the boosted conversion of Li PSs. As a result, the coin cell based on the MHCS@Mo S2-S cathode exhibits stable cycling performance maintaining 735.7 mAh g^(-1) after 500 cycles at 1.0 C. More importantly, the pouch cell employing the MHCS@Mo S2-S cathodes achieves high specific capacity of1353.2 m Ah g^(-1) and prominent cycle stability that remaining 960.0 m Ah g^(-1) with extraordinary capacity retention of 79.8% at 0.1 C after 170 cycles. Therefore, this work paves a new avenue for developing practical high specific energy and long-life pouch-type Li–S batteries.展开更多
Photocatalytic dual-functional reaction under visible light irradiation represents a sustainable development strategy.In detail,H2production coupled with benzylamine oxidation can remarkably lower the cost by replacin...Photocatalytic dual-functional reaction under visible light irradiation represents a sustainable development strategy.In detail,H2production coupled with benzylamine oxidation can remarkably lower the cost by replacing sacrificial agents.In this work,Cd S quantum dots(Cd S QDs)were successfully loaded onto the surface of a porphyrinic metal-organic framework(Pd-PCN-222)by the electrostatic selfassembly at room temperature.The consequent Pd-PCN-222/CdS heterojunction composites displayed superb photocatalytic activity under visible light irradiation,achieving a H2production and benzylamine oxidation rate of 5069 and 3717μmol g^(-1)h^(-1)with>99%selectivity in 3 h.There is no noticeable loss of catalytic capability during three successive runs.Mechanistic studies by in situ electron spin resonance and X-ray photoelectron spectroscopy disclosed that CdS QDs injected photoexcited electrons to Pd-PCN-222 and then Zr6clusters under visible-light irradiation,and thus Cd S QDs and Zr6clusters behave as the photocatalytic oxidation and reduction centers,respectively.展开更多
Marine biofouling is a worldwide challenge that needs to be solved urgently.Poly(dimethylsiloxane)(PDMS)-based fouling release coatings with low surface free energy(SFE)could effectively inhibit bio-fouling.Neverthele...Marine biofouling is a worldwide challenge that needs to be solved urgently.Poly(dimethylsiloxane)(PDMS)-based fouling release coatings with low surface free energy(SFE)could effectively inhibit bio-fouling.Nevertheless,their poor mechanical durability,adhesive strength,and antifouling performance under static conditions significantly limit their applications.Herein,a novel mechanically robust Al_(2)O_(3)-PDMS-Cu composite coating with strong adhesive strength and remarkable antifouling performance was developed.The Al_(2)O_(3)-PDMS-Cu coating loaded with a small amount of Cu was fabricated by infiltrating PDMS into plasma-sprayed micro/nano-scaled porous Al_(2)O_(3)-Cu coating.Results showed that the fabri-cation of this Al_(2)O_(3)-PDMS-Cu coating did not alter the surface hydrophobicity and SFE of PDMS signif-icantly,thus presenting little influence on its inherent fouling release property.After rigorous abrasion test,the Al_(2)O_(3)-PDMS-Cu coating presented remarkably improved surface hydrophobicity due to the ex-posure of micro/nano structure,rather than falling offas that of PDMS coating.The combination of excel-lent abrasion resistance and one order of magnitude higher adhesive strength and hardness than PDMS coating contributed to the outstanding mechanical robustness of Al_(2)O_(3)-PDMS-Cu coating.Additionally,the antifouling assays against marine bacteria adhesion(95%reduction rate for Escherichia coli.(E.coli))and algae attachment(96%and 94%reduction rates for Chlorella and Phaeodactylum tricornutum(P.tricor-nutum),respectively after 21 days of incubation)demonstrated the superior antifouling performance of the Al_(2)O_(3)-PDMS-Cu coating.Thus,a high-performance Al_(2)O_(3)-PDMS-Cu antifouling coating with excellent mechanical robustness and long-term antifouling performance was achieved via the combination of me-chanical durability of Al_(2)O_(3)skeleton and the dual-functional antifouling strategy,i.e.,the fouling release property of PDMS and fouling resistance of Cu.展开更多
The commercial viability of lithium-sulfur batteries is still challenged by the notorious lithium polysulfides(Li PSs)shuttle effect on the sulfur cathode and uncontrollable Li dendrites growth on the Li anode.Herein,...The commercial viability of lithium-sulfur batteries is still challenged by the notorious lithium polysulfides(Li PSs)shuttle effect on the sulfur cathode and uncontrollable Li dendrites growth on the Li anode.Herein,a bi-service host with Co-Fe binary-metal selenide quantum dots embedded in three-dimensional inverse opal structured nitrogen-doped carbon skeleton(3DIO FCSe-QDs@NC)is elaborately designed for both sulfur cathode and Li metal anode.The highly dispersed FCSe-QDs with superb adsorptive-catalytic properties can effectively immobilize the soluble Li PSs and improve diffusion-conversion kinetics to mitigate the polysulfide-shutting behaviors.Simultaneously,the 3D-ordered porous networks integrated with abundant lithophilic sites can accomplish uniform Li deposition and homogeneous Li-ion flux for suppressing the growth of dendrites.Taking advantage of these merits,the assembled Li-S full batteries with 3DIO FCSe-QDs@NC host exhibit excellent rate performance and stable cycling ability(a low decay rate of 0.014%over 2,000 cycles at 2C).Remarkably,a promising areal capacity of 8.41 mAh cm^(-2)can be achieved at the sulfur loading up to 8.50 mg cm^(-2)with an ultra-low electrolyte/sulfur ratio of 4.1μL mg^(-1).This work paves the bi-serve host design from systematic experimental and theoretical analysis,which provides a viable avenue to solve the challenges of both sulfur and Li electrodes for practical Li-S full batteries.展开更多
Hydrogen,as a green and clean next-generation fuel,is a key to achieving the goal of carbon neutrality.Constructing an electrocatalyst with bifunctional hydrogen evolution and oxygen evolution activity in the same ele...Hydrogen,as a green and clean next-generation fuel,is a key to achieving the goal of carbon neutrality.Constructing an electrocatalyst with bifunctional hydrogen evolution and oxygen evolution activity in the same electrolyte is a key technology for producing hydrogen via water splitting.Herein,a bimetallic active site catalyst,which possessed an edge-riched MoS_(2)nanoflakes array vertically growing on cubic CoS_(2),forming a nuclear-shell heterogeneous configuration,termed CSC-Mo S_(2)@Co S_(2).was reported The optimal CSC-Mo S_(2)@Co S_(2)-24 possessed good dualfunctional electrocatalytic activity(hydrogen evolution(HER),10 m A·cm^(-2)@241.5 m V and oxygen evolution(OER),10 m A·cm^(-2)@350 m V).Especially,CSC-Mo S_(2)@CoS_(2)-24 exhibited an extremely high mass activity for HER,and only required an overpotential of~550 m V when reaching a large current density of 1422 m A·mg^(-1),which was20.6-fold that of the bulk CoS_(2)(69 m A·mg^(-1)),as well as exhibiting stability of up to 100 h.The good electrocatalytic performance was attributed to the nuclear-shell heterostructure of Mo S_(2)@CoS_(2)hybrid could bring critical synergies,improving efficient mass transfer and electron transfer processes between Co S_(2)and Mo S_(2),which collaboratively promoted the electrocatalytic kinetics.It is foreseeable that the method proposed in this work will have guiding value for the preparation of dual-functional electrocatalysts with multi-interface heterostructures by assembling layered sulfides on cubic sulfides.展开更多
Carbon nanodots(CDs) based fluorescent nanoprobes have recently drawn much attention in chemo-/bio-sensing and bioimaging.However,it is still challenging to integrate the colorimetric and fluorometric dual readouts in...Carbon nanodots(CDs) based fluorescent nanoprobes have recently drawn much attention in chemo-/bio-sensing and bioimaging.However,it is still challenging to integrate the colorimetric and fluorometric dual readouts into a single CD.Herein,novel hybrid CDs(HCDs) are prepared by a simple microwave-assisted reaction of citric acid(CA),branched polyethyleneimine(BPEI) and potassium thiocyanate(KSCN).As-prepared HCDs show extraordinary properties,including excitation-dependent emission,satisfactory fluorescence quantum yield(46.8%),excellent biocompatibility and optical stability.Significantly,the fluorescence intensity at 450 nm exhibits linear correlation over the Fe^(3+)concentration from 1 mmol/L to 150 mmol/L with a detection limit(LOD) of 52 nmol/L.Meanwhile,the solution color changes from colorless to orange,and the absorbance at 460 nm increased linearly with Fe^(3+)concentration ranging from 0.02 mmol/L to 5 mmol/L(LOD:3.4 mmol/L).All the evidence illustrates that the HCDs can be conditioned for specific Fe^(3+)sensing with colorimetric and fluorometric dual readouts,which has also been verified with paper-based microchips.The possible mechanism is attributed to the specific interactions between surface functional groups on the HCDs and Fe^(3+).Additionally,the HCDs are successfully applied in sensing Fe^(3+)in wastewater and living cells,demonstrating its potential applications in future environment monitoring and disease diagnosis.展开更多
The terahertz technology has attracted considerable attention because of its potential applications in various fields.However,the research of functional devices,including polarization converters,remains a major demand...The terahertz technology has attracted considerable attention because of its potential applications in various fields.However,the research of functional devices,including polarization converters,remains a major demand for practical applications.In this work,a reflective dual-functional terahertz metadevice is presented,which combines two different polarization conversions through using a switchable metasurface.Different functions can be achieved because of the insulator-to-metal transition of vanadium dioxide(VO_(2)).At room temperature,the metadevice can be regarded as a linear-to-linear polarization convertor containing a gold circular split-ring resonator(CSRR),first polyimide(PI)spacer,continuous VO_(2) film,second PI spacer,and gold substrate.The converter possesses a polarization conversion ratio higher than 0.9 and a bandwidth ratio of 81%in a range from 0.912 THz to 2.146 THz.When the temperature is above the insulator-to-metal transition temperature(approximately 68℃)and VO_(2) becomes a metal,the metasurface transforms into a wideband linear-to-circular polarization converter composed of the gold CSRR,first PI layer,and continuous VO_(2) film.The ellipticity is close to-1,while the axis ratio is lower than 3 dB in a range of 1.07 THz-1.67 THz.The metadevice also achieves a large angle tolerance and large manufacturing tolerance.展开更多
The intrinsic poor electrical conductivity,severe dissolution of K x S y intermediates,and inferior conversion reaction reversibility extremely impede the practical application of the transition-metal chalcogenides(TM...The intrinsic poor electrical conductivity,severe dissolution of K x S y intermediates,and inferior conversion reaction reversibility extremely impede the practical application of the transition-metal chalcogenides(TMDs)anode for potassium-ion batteries(PIBs).Herein,a rationally designed Cu_(9)S_(5)/MoS_(2)/C heterostruc-ture hollow nanocage was synthesized with assistance from metal-organic frameworks(MOFs)precursor.During the K-storage process,the homogeneously distributed the sulfiphilic nature of Cu 0 reaction prod-uct could act as a dual-functional catalyst,not only facilitating the rapid charge transfer but also effec-tively anchoring(K x S y)polysulfides,thus boosting K-storage reactions reversibility during the conversion reaction process.When applied as an anode for PIBs,the as-prepared heterostructure exhibits excellent reversible capacity and long cycle lifespan(350.5 mAh g^(-1)at 0.1 A g^(-1)and 0.04%per cycle capacity de-cay at 1 A g^(-1)after 1000 cycles).Additionally,the potassium storage mechanism is distinctly revealed by in-situ characterizations.The nanoarchitecture designing strategy for the advanced electrode in this work could provide vital guidance for relevant energy storage materials.展开更多
The design and synthesis of non-precious metal dual-functional electrocatalysts through the modulation of electronic structure are important for the development of renewable hydrogen energy.Herein,MnS_(2)/MnO_(2)-CC h...The design and synthesis of non-precious metal dual-functional electrocatalysts through the modulation of electronic structure are important for the development of renewable hydrogen energy.Herein,MnS_(2)/MnO_(2)-CC heterostructure dual-functional catalysts with ultrathin nanosheets were prepared by a twostep electrodeposition method for efficient acidic hydrogen evolution reaction(HER) and degradation of organic wastewater(such as methylene blue(MB)).The electronic structure of Mn atoms at the MnS_(2)/MnO_(2)-CC heterostructure interface is reconfigured under the joint action of S and O atoms.Theoretical calculations show that the Mn d-band electron distribution in MnS_(2)/MnO_(2)-CC catalyst has higher occupied states near the Fermi level compared to the MnO_(2) and MnS_(2) catalysts,which indicates that MnS_(2)/MnO_(2)-CC catalyst has better electron transfer capability and catalytic activity.The MnS_(2)/MnO_(2)-CC catalysts require overpotential of only 66 and 116 mV to reach current density of 10 and 100 mA cm^(-2)in MB/H_(2)SO_(4) media.The MnS_(2)/MnO_(2)-CC catalyst also has a low Tafel slope(26.72 mV dec^(-1)) and excellent stability(the performance does not decay after 20 h of testing).In addition,the MB removal efficiency of the MnS_(2)/MnO_(2)-CC catalyst with a better kinetic rate(0.0226) can reach 97.76%,which is much higher than that of the MnO_(x)-CC catalyst(72.10%).This strategy provides a new way to develop efficient and stable non-precious metal dual-functional electrocatalysts for HER and organic wastewater degradation.展开更多
Bisphenol A （BPA） was one of the environmental hormones that would cause endocrine and metabolic disorders in human or wildlife. This paper proposed a method to detect the trace amounts of BPA in water samples by fu...Bisphenol A （BPA） was one of the environmental hormones that would cause endocrine and metabolic disorders in human or wildlife. This paper proposed a method to detect the trace amounts of BPA in water samples by fully utilizing the enrichment and resonance amplification functions of a new dual-functional membrane. In this work, gold nanoparticles （AuNPs） modified by 3-amino-5-mercapto-1,2,4-triazole （AMT） were embedded in nylon66 membrane to produce a dual-functional membrane which could carry out sample enrichment by capturing BPA molecules from water and achieve resonance amplification by connecting BPA to the surfaces of AuNPs. By designing an automatic sampler for large-volume enrichment, the SERS enhancement factor （EF） of the method was further improved to 1.2 × 105. The present method had been successfully applied to detect BPA in drinking water and environmental water by SERS with the detection limit of 0.012 μg/L. It had the potential for on-site detecting of BPA in various water samples.展开更多
The joint beamforming design challenge for dual-functional radar-communication systems is addressed in this paper.The base station in these systems is tasked with simultaneously sending shared signals for both multi-u...The joint beamforming design challenge for dual-functional radar-communication systems is addressed in this paper.The base station in these systems is tasked with simultaneously sending shared signals for both multi-user communication and target sensing.The primary objective is to maximize the sum rate of multi-user communication,while also ensuring sufficient beampattern gain at particular angles that are of interest for sensing,all within the constraints of the transmit power budget.To tackle this complex non-convex problem,an effective algorithm that iteratively optimizes the joint beamformers is developed.This algorithm leverages the techniques of fractional programming and semidefinite relaxation to achieve its goals.The numerical results confirm the effectiveness of the proposed algorithm.展开更多
A novel hydrogen-bonded organic frameworks(HOFs)FJU-200 has been constructed from N,N’-bis(5-isophthalic acid)naphthalimide(H_(4)L).FJU-200 has a good dual-function of aniline and ultraviolet detection.FJU-200 is the...A novel hydrogen-bonded organic frameworks(HOFs)FJU-200 has been constructed from N,N’-bis(5-isophthalic acid)naphthalimide(H_(4)L).FJU-200 has a good dual-function of aniline and ultraviolet detection.FJU-200 is the first case of HOF with dual sensing of visual color changes and photoluminescence quenching for aniline detection,and the detection limit of aniline can reach5.5 x 10^(-4)mol/L.Under ultraviolet FJU-200 will rapidly change from light yellow to rustic brown,which makes it possible to use FJU-200 to achieve minute-level ultraviolet detection.Moreover,for more convenient use,FJU-200 test papers are prepared.Using them,convenient and fast aniline or ultraviolet detection can be realized.The single-crystal X-ray structures show that compared with the original FJU-200,both PhNH_(2)@FJU-200 and UV-FJU-200 have larger pore sizes,and the dihedral angles of the H_(2)L^(2-)in framework has been changed.展开更多
The rational fabrication of photocatalysts with dual functions upon visible light, such as photocatalytic radioactive U(Ⅵ)reduction and value-added organic oxidation, is highly desirable but remains huge challenge. H...The rational fabrication of photocatalysts with dual functions upon visible light, such as photocatalytic radioactive U(Ⅵ)reduction and value-added organic oxidation, is highly desirable but remains huge challenge. Here, we couple the photocatalytic U(Ⅵ) reduction with the oxidative organic synthesis to one system using novel extended π-conjugated framework(Cu@ThTCPP) without the expense of sacrificial reagents. Noticeably, the as-prepared Cu@Th-TCPP linked by tetratopic tetrakis(4-carboxyphenyl)porphyrin(TCPP) ligand and unique Th(μ-O)(HCOO)(HO)secondary building unit(SBU) exhibits significantly enhanced activity when the photocatalytic U(Ⅵ) reduction and thioanisole oxidation were integrated to one system.Further experimental characterizations demonstrate that the highly conjugated framework of Cu@Th-TCPP is good for the charge transfer and separation, while incorporating Cusite further accelerates the charge-carrier dynamics, thus giving rise to the dual-functional property. Apparently, this strategy conforms to atomic economy, opens a new horizon to address radioactive environmental pollution in natural water systems and soils, and simultaneously produces valuable chemicals.展开更多
IntegratingH_(2)O_(2)evolution with oxidative organic synthesis in a semiconductordriven photoredox reaction is highly attractive since H_(2)O_(2)and high-value chemicals can be concurrently produced using solar light...IntegratingH_(2)O_(2)evolution with oxidative organic synthesis in a semiconductordriven photoredox reaction is highly attractive since H_(2)O_(2)and high-value chemicals can be concurrently produced using solar light as the only energy input.The dual-functional photocatalytic approach,free from sacrificial agents,enables simultaneous production of H_(2)O_(2)and high-value organic chemicals.This strategy promises a green and sustainable organic synthesis with minimal greenhouse gas emissions.In this review,we first elucidate the fundamental principles of cooperative photoredox integration of H_(2)O_(2)synthesis and selective organic oxidation with simultaneous utilization of photoexcited electrons and holes over semiconductor-based photocatalysts.Afterwards,a thorough review on the recent advancements of cooperative photoredox synthesis of H_(2)O_(2)and value-added chemicals is presented.Notably,in-depth discussions and insights into the techniques for unravelling the photoredox reaction mechanisms are elucidated.Finally,critical challenges and prospects in this thriving field are comprehensively discussed.It is envisioned that this review will serve as a pivotal guidance on the rational design of such dual-functional photocatalytic system,thereby further stimulating the development of economical and environmentally benignH_(2)O_(2)and high-value chemicals production.展开更多
The development of an efficient dual-function catalytic-sorption system,which seamlessly integrates reaction and separation into a single step for extractant-free systems,represents a transformative advancement in oxi...The development of an efficient dual-function catalytic-sorption system,which seamlessly integrates reaction and separation into a single step for extractant-free systems,represents a transformative advancement in oxidative desulfurization(ODS)process.In this work,we introduce a novel dualfunction amphiphilic biochar(Mo/CBC)catalyst,functionalized with MoO_(3-x)featuring abundant oxygen vacancies,for highly effective extractant-free ODS.The polarity of the biochar was precisely tailored by varying the amount of KOH,leading to the creation of amphiphilic carriers.Subsequent ball milling facilitated the successful loading of MoO_(3-x)onto the biochar surface via an impregnation-calcination route leveraging carbon reduction,resulting in the synthesis of amphiphilic Mo/CBC catalysts.The amphiphilic nature of these catalysts ensures their stable dispersion within the oil phase,while also facilitating their interaction with the oxidant H2O2 and the adsorption of sulfur-containing oxidation products.Characterization techniques,including EPR,XPS,and in situ XRD,verified the existence of abundant oxygen vacancies obtained by carbon reduction on the amphiphilic Mo/CBC catalysts,which significantly boosted their activity in an extractant-free ODs system.Remarkably,the amphiphilic Mo/CBC catalyst displayed exceptional catalytic performance,achieving a desulfurization efficiency of 99.6%in just 10 min without extraction solvent.DFT theoretical calculations further revealed that H_(2)O_(2)readily dissociates into two OH radicals on the O_(vac)-MoO_(3),overcoming a low energy barrier.This process was identified as a key contributor to the catalyst's outstanding ODS performance.Furthermore,other biochar sources,such as rice straw,bamboo,rapeseed oil cake,and walnut oil cake,were investigated to produce Mo-based amphiphilic biochar catalysts,which all showed excellent desulfurization performance.This work establishes a versatile and highly efficient dual-function catalytic-sorption system by designing amphiphilic biochar catalysts enriched with oxygen vacancies,paving the way for the development of universally applicable ODS catalysts for industrial applications.展开更多
基金supported by the National Natural Science Foundation of China(No.52105072)Zhejiang Provincial Natural Science Foundation of China(No.LZ24E050004)+2 种基金Jiangsu Provincial Outstanding Youth Program(No.BK20230072)a grant from Suzhou Industrial Foresight and Key Core Technology Project(No.SYC2022044)grants from Jiangsu Qinglan Project and Jiangsu 333 High-level Talents.
文摘Wireless capsule endoscopy(WCE)has the potential to fully replace conventional wired counterparts for its low invasiveness.Recent studies have attempted to expand the functions of capsules toward this goal.However,limitations in space and energy supply have resulted in the inability to perform multiple diagnostic and treatment tasks using a single capsule.In this study,we developed a dual-functional capsule robot(DFCR)for drug delivery and tissue biopsy based on magnetic torsion spring technology.The delivery module was shown to rotate the push rod with a thrust of 894 mN to release approximately 0.3 mL of semisolid drug.The biopsy module used a built-in blade to cut tissue with a shear stress of 22.87 MPa,producing a sample of approximately 1.8 mm3.Additionally,a five-degree-of-freedom permanent magnet drive system was developed.By adjusting the strength of the unidirectional magnetic field generated by an external magnet,the capsule can be wirelessly controlled to sequentially trigger the two functions.Ex vivo tests on porcine stomachs confirmed the feasibility of the prototype capsule(12 mm in diameter and 45 mm in length)in active movement,medication,and tissue biopsy.The newly developed DFCR further expands the clinical application prospects of WCE robots in minimally invasive surgery.
基金supported by the National Natural Science Foundation of China(Nos.22206113 and 22376124)the Outstanding Youth Science Fund(Overseas)of Shandong Provincial Natural Science Foundation(No.2022HWYQ-015)+4 种基金the Taishan Scholars Project Special Fund(No.tsqn202211039)the Guangdong Basic and Applied Basic Research Foundation(No.2021A1515111137)Qilu Youth Talent Program of Shandong University(No.61440082163171)the Natural Sciences and Engineering Research Council of Canadale Fonds de recherche du Quebec-Nature et technologies.
文摘Photocatalytic water splitting is a promising way to produce H_(2),a green and clean energy source.However,efficient H_(2) production typically relies on the addition of electron donors,such as alcohols and acids,which are neither environmentally friendly nor cost-effective.Recently,we have witnessed a surge of studies in coupling photocatalytic H_(2) evolution with organic pollutant oxidation,which significantly promotes charge separation and improves the overall photocatalytic efficiency.It is thus an opportune time to critically assess the recent literature concerning dual-functional photocatalytic systems and provide perspectives for its future development.In this minireview,we begin with the working principles and requirements for synergistic photocatalytic systems.We then summarize and critically discuss the recent advances in photocatalytic H_(2) production and the degradation of various organic pollutants,including antibiotics,dyes,and phenols.Finally,we discuss the current challenges and suggest future directions for this field.
基金supported by the National Natural Science Foundation of China under grants 62072229,U1936201,62071220,61976113joint project of China Mobile Research Institute&X-NET。
文摘Dual-function communication radar systems use common Radio Frequency(RF)signals are used for both communication and detection.For better compatibility with existing communication systems,we adopt Multiple-Input Multiple-Output(MIMO)Orthogonal Frequency Division Multiplexing(OFDM)signals as integrated signals and investigate the estimation performance of MIMO-OFDM signals.First,we analyze the Cramer-Rao Lower Bound(CRLB)of parameter estimation.Then,the transmit powers over different subcarriers are optimized to achieve the best tradeoff between the transmission rate and the estimation performance.Finally,we propose a more accurate estimation method that uses Canonical Polyadic Decomposition(CPD)of the third-order tensor to obtain the parameter matrices.Due to the characteristic of the column structure of the parameter matrices,we only need to use DFT/IDFT to recover the parameters of multiple targets.The simulation results show that tensor-based estimation method can achieve a performance close to CRLB,and the estimation performance can be improved by optimizing the transmit powers.
基金This work was financially supported by the Australian Research Council(ARC)Discovery Projects(DP210103266 and DPI 701048343)the Griffith University Ph.D.Scholarships.
文摘Binders could play crucial or even decisive roles in the fabrication of low-cost, stable and high-capacity electrodes. This is especially the case for the silicon (Si) anodes and sulfur (S) cathodes that undergo large volume change and active material loss in lithium-ion batteries during prolonged cycles. Herein, a hydrophilic polymer poly(methyl vinyl ether-alt-maleic acid) (PMVEMA) was explored as a dual-functional aqueous binder for the preparation of high-performance silicon anode and sulfur cathode. Benefiting from the dual functions of PMVEMA, i.e., the excellent dispersion ability and strong binding forces, the as-prepared electrodes exhibit improved capacity, rate capability and long-term cycling performance. In particular, the as-prepared Si electrode delivers a high initial discharge capacity of 1346.5 mAh g^(−1) at a high rate of 8.4 A/g and maintains 834.5 mAh g^(−1) after 300 cycles at 4.2 A/g, while the as-prepared S cathode exhibits enhanced cycling performance with high remaining discharge capacities of 663.4 mAh g^(−1) after 100 cycles at 0.2 C and 487.07 mAh g^(−1) after 300 cycles at 1 C, respectively. These encouraging results suggest that PMVEMA could be a universal binder to facilitate the green manufacture of both anode and cathode for high-capacity energy storage systems.
基金financially supported by the National Natural Science Foundation of China(Nos.52371081,U2106226)the Key Research and Development Program of Shandong province(No.2020CXGC010703)the Foundation of Key Laboratory of National Defense Science and Technology(No.JS220406).
文摘Although extremely challenging,it is highly desirable to develop self-healing materials that exhibit high efficiency under environmental conditions for marine protection applications.In this work,polyurethane elastomers with hydrogen bond and dimethylglyoxime-urethane(DOU)coordination complex were combined with in-situ dual-functional BiOI@Bi_(2)S_(3) to synthesize high-efficiency photothermal cyclic self-healing antibacterial coating.The photothermal efficiency of BiOI@Bi_(2)S_(3) is improved by 38% through interfacial regulation.BiOI@Bi_(2)S_(3)/PU rapidly rises by 50.2℃ within 300 s under near-infrared(NIR)light,which can trigger the hydrogen bond of polyurethane coating and recover the barrier properties of the coating through self-healing.Density functional theory was used to simulate and analyze the generation of multiple electron transfer paths after the vulcanization of BiOI,which improves the interfacial mobility of photogenerated carriers and generates more heat.Importantly,molecular dynamics verified the self-healing mechanism of hydrogen bond and the photothermal lifting mechanism of the coating.After 5th scratches and self-healing cycle tests,the coating has a self-healing efficiency of more than 80%,which can ensure the self-healing and anticorrosion protection performance of the coating for multiple cycles.The photocatalytic and photothermal properties of BiOI@Bi_(2)S_(3) enhance the antibacterial rate of the coating up to 99%.This work provides heuristic perspectives for the design of coatings with anti-corrosion,antibacterial and self-healing properties.
基金supported by the funding from the Strategy Priority Research Program of Chinese Academy of Science (Grant No. XDA17020404)DICP&QIBEBT (DICP&QIBEBT UN201702)+8 种基金R&D Projects in Key Areas of Guangdong Province (2019B090908001)Science and Technology Innovation Foundation of Dalian (2018J11CY020)Defense Industrial Technology Development Program (JCKY2018130C107)National Natural Science Foundation of China (Grants 51872283)Liao Ning Revitalization Talents Program (Grant XLYC1807153)Natural Science Foundation of Liaoning Province (Grant 20180510038)DICP (DICP ZZBS201708, DICP ZZBS201802)DNL Cooperation FundCAS (DNL180310, DNL180308, DNL201912, and DNL201915)。
文摘Developing sulfur cathodes with high catalytic activity on accelerating the sluggish redox kinetics of lithium polysulfides(Li PSs) and unveiling their mechanisms are pivotal for advanced lithium–sulfur(Li–S)batteries. Herein, MoS2 is verified to reduce the Gibbs free energy for rate-limiting step of sulfur reduction and the dissociation energy of lithium sulfide(Li2 S) for the first time employing theoretical calculations. The Mo S2 nanosheets coated on mesoporous hollow carbon spheres(MHCS) are then reasonably designed as a sulfur host for high-capacity and long-life Li–S battery, in which MHCS can guarantee the high sulfur loading and fast electron/ion transfer. It is revealed that the shuttle effect is efficiently inhibited because of the boosted conversion of Li PSs. As a result, the coin cell based on the MHCS@Mo S2-S cathode exhibits stable cycling performance maintaining 735.7 mAh g^(-1) after 500 cycles at 1.0 C. More importantly, the pouch cell employing the MHCS@Mo S2-S cathodes achieves high specific capacity of1353.2 m Ah g^(-1) and prominent cycle stability that remaining 960.0 m Ah g^(-1) with extraordinary capacity retention of 79.8% at 0.1 C after 170 cycles. Therefore, this work paves a new avenue for developing practical high specific energy and long-life pouch-type Li–S batteries.
基金support from the National Natural Science Foundation of China(Nos.21773314,21821003 and 21890382)the Guangdong Natural Science Funds for Distinguished Young Scholar(No.2019B151502017)。
文摘Photocatalytic dual-functional reaction under visible light irradiation represents a sustainable development strategy.In detail,H2production coupled with benzylamine oxidation can remarkably lower the cost by replacing sacrificial agents.In this work,Cd S quantum dots(Cd S QDs)were successfully loaded onto the surface of a porphyrinic metal-organic framework(Pd-PCN-222)by the electrostatic selfassembly at room temperature.The consequent Pd-PCN-222/CdS heterojunction composites displayed superb photocatalytic activity under visible light irradiation,achieving a H2production and benzylamine oxidation rate of 5069 and 3717μmol g^(-1)h^(-1)with>99%selectivity in 3 h.There is no noticeable loss of catalytic capability during three successive runs.Mechanistic studies by in situ electron spin resonance and X-ray photoelectron spectroscopy disclosed that CdS QDs injected photoexcited electrons to Pd-PCN-222 and then Zr6clusters under visible-light irradiation,and thus Cd S QDs and Zr6clusters behave as the photocatalytic oxidation and reduction centers,respectively.
基金the National Natural Science Foun-dation of China(No.52001280)the China Postdoctoral Science Foundation(No.2020M682339).
文摘Marine biofouling is a worldwide challenge that needs to be solved urgently.Poly(dimethylsiloxane)(PDMS)-based fouling release coatings with low surface free energy(SFE)could effectively inhibit bio-fouling.Nevertheless,their poor mechanical durability,adhesive strength,and antifouling performance under static conditions significantly limit their applications.Herein,a novel mechanically robust Al_(2)O_(3)-PDMS-Cu composite coating with strong adhesive strength and remarkable antifouling performance was developed.The Al_(2)O_(3)-PDMS-Cu coating loaded with a small amount of Cu was fabricated by infiltrating PDMS into plasma-sprayed micro/nano-scaled porous Al_(2)O_(3)-Cu coating.Results showed that the fabri-cation of this Al_(2)O_(3)-PDMS-Cu coating did not alter the surface hydrophobicity and SFE of PDMS signif-icantly,thus presenting little influence on its inherent fouling release property.After rigorous abrasion test,the Al_(2)O_(3)-PDMS-Cu coating presented remarkably improved surface hydrophobicity due to the ex-posure of micro/nano structure,rather than falling offas that of PDMS coating.The combination of excel-lent abrasion resistance and one order of magnitude higher adhesive strength and hardness than PDMS coating contributed to the outstanding mechanical robustness of Al_(2)O_(3)-PDMS-Cu coating.Additionally,the antifouling assays against marine bacteria adhesion(95%reduction rate for Escherichia coli.(E.coli))and algae attachment(96%and 94%reduction rates for Chlorella and Phaeodactylum tricornutum(P.tricor-nutum),respectively after 21 days of incubation)demonstrated the superior antifouling performance of the Al_(2)O_(3)-PDMS-Cu coating.Thus,a high-performance Al_(2)O_(3)-PDMS-Cu antifouling coating with excellent mechanical robustness and long-term antifouling performance was achieved via the combination of me-chanical durability of Al_(2)O_(3)skeleton and the dual-functional antifouling strategy,i.e.,the fouling release property of PDMS and fouling resistance of Cu.
基金financial support from the National Natural Science Foundation of China(Grant Nos.51871188 and 51931006)the Fundamental Research Funds for the Central Universities of China(Xiamen University:Nos.20720200068,20720190007 and 20720220074)+2 种基金Guangdong Basic and Applied Basic Research Foundation(No.2021A1515010139)Science and Technology Projects of Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province(HRTP-[2022]-22)the“Double-First Class”Foundation of Materials Intelligent Manufacturing Discipline of Xiamen University。
文摘The commercial viability of lithium-sulfur batteries is still challenged by the notorious lithium polysulfides(Li PSs)shuttle effect on the sulfur cathode and uncontrollable Li dendrites growth on the Li anode.Herein,a bi-service host with Co-Fe binary-metal selenide quantum dots embedded in three-dimensional inverse opal structured nitrogen-doped carbon skeleton(3DIO FCSe-QDs@NC)is elaborately designed for both sulfur cathode and Li metal anode.The highly dispersed FCSe-QDs with superb adsorptive-catalytic properties can effectively immobilize the soluble Li PSs and improve diffusion-conversion kinetics to mitigate the polysulfide-shutting behaviors.Simultaneously,the 3D-ordered porous networks integrated with abundant lithophilic sites can accomplish uniform Li deposition and homogeneous Li-ion flux for suppressing the growth of dendrites.Taking advantage of these merits,the assembled Li-S full batteries with 3DIO FCSe-QDs@NC host exhibit excellent rate performance and stable cycling ability(a low decay rate of 0.014%over 2,000 cycles at 2C).Remarkably,a promising areal capacity of 8.41 mAh cm^(-2)can be achieved at the sulfur loading up to 8.50 mg cm^(-2)with an ultra-low electrolyte/sulfur ratio of 4.1μL mg^(-1).This work paves the bi-serve host design from systematic experimental and theoretical analysis,which provides a viable avenue to solve the challenges of both sulfur and Li electrodes for practical Li-S full batteries.
基金financially supported by the National Science Foundation of China(Nos.52203314,52071226 and 51872193)the Natural Science Foundations of Jiangsu Province(No.BK20210847)+1 种基金Jiangsu Key Laboratory for Biomass Energy and Material(No.JSBEM-S-201805)the Natural Science Foundations of the Jiangsu Higher Education Institutions of China(No.21KJB430042)。
文摘Hydrogen,as a green and clean next-generation fuel,is a key to achieving the goal of carbon neutrality.Constructing an electrocatalyst with bifunctional hydrogen evolution and oxygen evolution activity in the same electrolyte is a key technology for producing hydrogen via water splitting.Herein,a bimetallic active site catalyst,which possessed an edge-riched MoS_(2)nanoflakes array vertically growing on cubic CoS_(2),forming a nuclear-shell heterogeneous configuration,termed CSC-Mo S_(2)@Co S_(2).was reported The optimal CSC-Mo S_(2)@Co S_(2)-24 possessed good dualfunctional electrocatalytic activity(hydrogen evolution(HER),10 m A·cm^(-2)@241.5 m V and oxygen evolution(OER),10 m A·cm^(-2)@350 m V).Especially,CSC-Mo S_(2)@CoS_(2)-24 exhibited an extremely high mass activity for HER,and only required an overpotential of~550 m V when reaching a large current density of 1422 m A·mg^(-1),which was20.6-fold that of the bulk CoS_(2)(69 m A·mg^(-1)),as well as exhibiting stability of up to 100 h.The good electrocatalytic performance was attributed to the nuclear-shell heterostructure of Mo S_(2)@CoS_(2)hybrid could bring critical synergies,improving efficient mass transfer and electron transfer processes between Co S_(2)and Mo S_(2),which collaboratively promoted the electrocatalytic kinetics.It is foreseeable that the method proposed in this work will have guiding value for the preparation of dual-functional electrocatalysts with multi-interface heterostructures by assembling layered sulfides on cubic sulfides.
基金Financial support for this work came from the Project of Henan Provincial Medical Science and Technology Research Plan (No.SBGJ202002086)Guangdong Provincial Key Laboratory of Sensing Technology and Biomedical Instruments (No.2020B1212060077)Natural Science Foundation of China (Nos.81901808,81701752, 81601470)。
文摘Carbon nanodots(CDs) based fluorescent nanoprobes have recently drawn much attention in chemo-/bio-sensing and bioimaging.However,it is still challenging to integrate the colorimetric and fluorometric dual readouts into a single CD.Herein,novel hybrid CDs(HCDs) are prepared by a simple microwave-assisted reaction of citric acid(CA),branched polyethyleneimine(BPEI) and potassium thiocyanate(KSCN).As-prepared HCDs show extraordinary properties,including excitation-dependent emission,satisfactory fluorescence quantum yield(46.8%),excellent biocompatibility and optical stability.Significantly,the fluorescence intensity at 450 nm exhibits linear correlation over the Fe^(3+)concentration from 1 mmol/L to 150 mmol/L with a detection limit(LOD) of 52 nmol/L.Meanwhile,the solution color changes from colorless to orange,and the absorbance at 460 nm increased linearly with Fe^(3+)concentration ranging from 0.02 mmol/L to 5 mmol/L(LOD:3.4 mmol/L).All the evidence illustrates that the HCDs can be conditioned for specific Fe^(3+)sensing with colorimetric and fluorometric dual readouts,which has also been verified with paper-based microchips.The possible mechanism is attributed to the specific interactions between surface functional groups on the HCDs and Fe^(3+).Additionally,the HCDs are successfully applied in sensing Fe^(3+)in wastewater and living cells,demonstrating its potential applications in future environment monitoring and disease diagnosis.
基金the National Natural Science Foundation of China(Grant No.62001444)the Natural Science Foundation of Zhejiang Province,China(Grant No.LQ20F010009)+1 种基金the Basic Public Welfare Research Project of Zhejiang Province,China(Grant No.LGF19F010003)the State Key Laboratory of Crystal Materials,Shandong University,China(Grant No.KF1909)。
文摘The terahertz technology has attracted considerable attention because of its potential applications in various fields.However,the research of functional devices,including polarization converters,remains a major demand for practical applications.In this work,a reflective dual-functional terahertz metadevice is presented,which combines two different polarization conversions through using a switchable metasurface.Different functions can be achieved because of the insulator-to-metal transition of vanadium dioxide(VO_(2)).At room temperature,the metadevice can be regarded as a linear-to-linear polarization convertor containing a gold circular split-ring resonator(CSRR),first polyimide(PI)spacer,continuous VO_(2) film,second PI spacer,and gold substrate.The converter possesses a polarization conversion ratio higher than 0.9 and a bandwidth ratio of 81%in a range from 0.912 THz to 2.146 THz.When the temperature is above the insulator-to-metal transition temperature(approximately 68℃)and VO_(2) becomes a metal,the metasurface transforms into a wideband linear-to-circular polarization converter composed of the gold CSRR,first PI layer,and continuous VO_(2) film.The ellipticity is close to-1,while the axis ratio is lower than 3 dB in a range of 1.07 THz-1.67 THz.The metadevice also achieves a large angle tolerance and large manufacturing tolerance.
基金financially supported by the National Natural Science Foundation of China (Nos.52070194,52073309,51902347,and 51908555)the Natural Science Foundation of Hunan Province (Nos.2022JJ20069 and 2020JJ5741).
文摘The intrinsic poor electrical conductivity,severe dissolution of K x S y intermediates,and inferior conversion reaction reversibility extremely impede the practical application of the transition-metal chalcogenides(TMDs)anode for potassium-ion batteries(PIBs).Herein,a rationally designed Cu_(9)S_(5)/MoS_(2)/C heterostruc-ture hollow nanocage was synthesized with assistance from metal-organic frameworks(MOFs)precursor.During the K-storage process,the homogeneously distributed the sulfiphilic nature of Cu 0 reaction prod-uct could act as a dual-functional catalyst,not only facilitating the rapid charge transfer but also effec-tively anchoring(K x S y)polysulfides,thus boosting K-storage reactions reversibility during the conversion reaction process.When applied as an anode for PIBs,the as-prepared heterostructure exhibits excellent reversible capacity and long cycle lifespan(350.5 mAh g^(-1)at 0.1 A g^(-1)and 0.04%per cycle capacity de-cay at 1 A g^(-1)after 1000 cycles).Additionally,the potassium storage mechanism is distinctly revealed by in-situ characterizations.The nanoarchitecture designing strategy for the advanced electrode in this work could provide vital guidance for relevant energy storage materials.
基金supported by The Key Laboratory of Advanced Functional Materials, Ministry of Education of China, Beijing University of Technologythe National Natural Science Foundation of China (NSFC, 52070006)。
文摘The design and synthesis of non-precious metal dual-functional electrocatalysts through the modulation of electronic structure are important for the development of renewable hydrogen energy.Herein,MnS_(2)/MnO_(2)-CC heterostructure dual-functional catalysts with ultrathin nanosheets were prepared by a twostep electrodeposition method for efficient acidic hydrogen evolution reaction(HER) and degradation of organic wastewater(such as methylene blue(MB)).The electronic structure of Mn atoms at the MnS_(2)/MnO_(2)-CC heterostructure interface is reconfigured under the joint action of S and O atoms.Theoretical calculations show that the Mn d-band electron distribution in MnS_(2)/MnO_(2)-CC catalyst has higher occupied states near the Fermi level compared to the MnO_(2) and MnS_(2) catalysts,which indicates that MnS_(2)/MnO_(2)-CC catalyst has better electron transfer capability and catalytic activity.The MnS_(2)/MnO_(2)-CC catalysts require overpotential of only 66 and 116 mV to reach current density of 10 and 100 mA cm^(-2)in MB/H_(2)SO_(4) media.The MnS_(2)/MnO_(2)-CC catalyst also has a low Tafel slope(26.72 mV dec^(-1)) and excellent stability(the performance does not decay after 20 h of testing).In addition,the MB removal efficiency of the MnS_(2)/MnO_(2)-CC catalyst with a better kinetic rate(0.0226) can reach 97.76%,which is much higher than that of the MnO_(x)-CC catalyst(72.10%).This strategy provides a new way to develop efficient and stable non-precious metal dual-functional electrocatalysts for HER and organic wastewater degradation.
基金supported by the National Natural Science Foundation of China(Nos. 21575168, 21475153,21575167 and 21675178)the Guangdong Provincial Natural Science Foundation of China(No. 2015A030311020)+1 种基金the Special Funds for Public Welfare Research and Capacity Building in Guangdong Province of China(No. 2015A030401036)the Guangzhou Science andTechnology Program of China(Nos.201604020165, 201704020040)
文摘Bisphenol A （BPA） was one of the environmental hormones that would cause endocrine and metabolic disorders in human or wildlife. This paper proposed a method to detect the trace amounts of BPA in water samples by fully utilizing the enrichment and resonance amplification functions of a new dual-functional membrane. In this work, gold nanoparticles （AuNPs） modified by 3-amino-5-mercapto-1,2,4-triazole （AMT） were embedded in nylon66 membrane to produce a dual-functional membrane which could carry out sample enrichment by capturing BPA molecules from water and achieve resonance amplification by connecting BPA to the surfaces of AuNPs. By designing an automatic sampler for large-volume enrichment, the SERS enhancement factor （EF） of the method was further improved to 1.2 × 105. The present method had been successfully applied to detect BPA in drinking water and environmental water by SERS with the detection limit of 0.012 μg/L. It had the potential for on-site detecting of BPA in various water samples.
基金supported in part by the National Natural Science Foundation of China under Grant No.62201266in part by the Natural Science Foundation of Jiangsu Province under Grant No.BK20210335.
文摘The joint beamforming design challenge for dual-functional radar-communication systems is addressed in this paper.The base station in these systems is tasked with simultaneously sending shared signals for both multi-user communication and target sensing.The primary objective is to maximize the sum rate of multi-user communication,while also ensuring sufficient beampattern gain at particular angles that are of interest for sensing,all within the constraints of the transmit power budget.To tackle this complex non-convex problem,an effective algorithm that iteratively optimizes the joint beamformers is developed.This algorithm leverages the techniques of fractional programming and semidefinite relaxation to achieve its goals.The numerical results confirm the effectiveness of the proposed algorithm.
基金supported by the National Natural Science Foundation of China(Nos.21673039,21573042,21805039,21975044,21971038 and 21922810)the Fujian Provincial Department of Science and Technology(Nos.2018J07001 and2019H6012)。
文摘A novel hydrogen-bonded organic frameworks(HOFs)FJU-200 has been constructed from N,N’-bis(5-isophthalic acid)naphthalimide(H_(4)L).FJU-200 has a good dual-function of aniline and ultraviolet detection.FJU-200 is the first case of HOF with dual sensing of visual color changes and photoluminescence quenching for aniline detection,and the detection limit of aniline can reach5.5 x 10^(-4)mol/L.Under ultraviolet FJU-200 will rapidly change from light yellow to rustic brown,which makes it possible to use FJU-200 to achieve minute-level ultraviolet detection.Moreover,for more convenient use,FJU-200 test papers are prepared.Using them,convenient and fast aniline or ultraviolet detection can be realized.The single-crystal X-ray structures show that compared with the original FJU-200,both PhNH_(2)@FJU-200 and UV-FJU-200 have larger pore sizes,and the dihedral angles of the H_(2)L^(2-)in framework has been changed.
基金supported by Jiangxi Province Key Laboratory of Synthetic Chemistry(JXSC202004)the Foundation of Jiangxi Educational Committee(GJJ200731)the Natural Science Foundation of Jiangxi Province of China(20192BAB213001)。
文摘The rational fabrication of photocatalysts with dual functions upon visible light, such as photocatalytic radioactive U(Ⅵ)reduction and value-added organic oxidation, is highly desirable but remains huge challenge. Here, we couple the photocatalytic U(Ⅵ) reduction with the oxidative organic synthesis to one system using novel extended π-conjugated framework(Cu@ThTCPP) without the expense of sacrificial reagents. Noticeably, the as-prepared Cu@Th-TCPP linked by tetratopic tetrakis(4-carboxyphenyl)porphyrin(TCPP) ligand and unique Th(μ-O)(HCOO)(HO)secondary building unit(SBU) exhibits significantly enhanced activity when the photocatalytic U(Ⅵ) reduction and thioanisole oxidation were integrated to one system.Further experimental characterizations demonstrate that the highly conjugated framework of Cu@Th-TCPP is good for the charge transfer and separation, while incorporating Cusite further accelerates the charge-carrier dynamics, thus giving rise to the dual-functional property. Apparently, this strategy conforms to atomic economy, opens a new horizon to address radioactive environmental pollution in natural water systems and soils, and simultaneously produces valuable chemicals.
基金financial support provided by the Ministry of Higher Education Malaysia under the Fundamental Research Grant Scheme(FRGS)(Ref no.FRGS/1/2020/TK0/XMU/02/1)The authors would like to thank the Ministry of Science,Technology and Innovation(MOSTI)Malaysia under the Strategic Research Fund(SRF)(S.22015)+6 种基金financial support provided by theNationalNatural Science Foundation of China(Ref no.22202168)the Guangdong Basic and Applied Basic Research Foundation(Ref no.2021A1515111019)supported by the Embassy of the People’s Republic of China in Malaysia(EENG/0045)financial support from the State Key Laboratory of Physical Chemistry of Solid Surfaces,Xiamen University(Ref no.2023X11)funded by the Xiamen University Malaysia Investigatorship Grant(grant no.IENG/0038)the Xiamen University Malaysia Research Fund(ICOE/0001 and XMUMRF/2021-C8/IENG/0041)the Hengyuan International Sdn Bhd(grant no.EENG/0003).
文摘IntegratingH_(2)O_(2)evolution with oxidative organic synthesis in a semiconductordriven photoredox reaction is highly attractive since H_(2)O_(2)and high-value chemicals can be concurrently produced using solar light as the only energy input.The dual-functional photocatalytic approach,free from sacrificial agents,enables simultaneous production of H_(2)O_(2)and high-value organic chemicals.This strategy promises a green and sustainable organic synthesis with minimal greenhouse gas emissions.In this review,we first elucidate the fundamental principles of cooperative photoredox integration of H_(2)O_(2)synthesis and selective organic oxidation with simultaneous utilization of photoexcited electrons and holes over semiconductor-based photocatalysts.Afterwards,a thorough review on the recent advancements of cooperative photoredox synthesis of H_(2)O_(2)and value-added chemicals is presented.Notably,in-depth discussions and insights into the techniques for unravelling the photoredox reaction mechanisms are elucidated.Finally,critical challenges and prospects in this thriving field are comprehensively discussed.It is envisioned that this review will serve as a pivotal guidance on the rational design of such dual-functional photocatalytic system,thereby further stimulating the development of economical and environmentally benignH_(2)O_(2)and high-value chemicals production.
基金supported by the National Natural Science Foundation of China(22162008)the Science and Technology Supporting Project of Guizhou Province([2022]208)+1 种基金the Guizhou Province Local Government Overseas Study Programthe open project of Guizhou Provincial Double Carbon and Renewable Energy Technology Innovation Research Institute.
文摘The development of an efficient dual-function catalytic-sorption system,which seamlessly integrates reaction and separation into a single step for extractant-free systems,represents a transformative advancement in oxidative desulfurization(ODS)process.In this work,we introduce a novel dualfunction amphiphilic biochar(Mo/CBC)catalyst,functionalized with MoO_(3-x)featuring abundant oxygen vacancies,for highly effective extractant-free ODS.The polarity of the biochar was precisely tailored by varying the amount of KOH,leading to the creation of amphiphilic carriers.Subsequent ball milling facilitated the successful loading of MoO_(3-x)onto the biochar surface via an impregnation-calcination route leveraging carbon reduction,resulting in the synthesis of amphiphilic Mo/CBC catalysts.The amphiphilic nature of these catalysts ensures their stable dispersion within the oil phase,while also facilitating their interaction with the oxidant H2O2 and the adsorption of sulfur-containing oxidation products.Characterization techniques,including EPR,XPS,and in situ XRD,verified the existence of abundant oxygen vacancies obtained by carbon reduction on the amphiphilic Mo/CBC catalysts,which significantly boosted their activity in an extractant-free ODs system.Remarkably,the amphiphilic Mo/CBC catalyst displayed exceptional catalytic performance,achieving a desulfurization efficiency of 99.6%in just 10 min without extraction solvent.DFT theoretical calculations further revealed that H_(2)O_(2)readily dissociates into two OH radicals on the O_(vac)-MoO_(3),overcoming a low energy barrier.This process was identified as a key contributor to the catalyst's outstanding ODS performance.Furthermore,other biochar sources,such as rice straw,bamboo,rapeseed oil cake,and walnut oil cake,were investigated to produce Mo-based amphiphilic biochar catalysts,which all showed excellent desulfurization performance.This work establishes a versatile and highly efficient dual-function catalytic-sorption system by designing amphiphilic biochar catalysts enriched with oxygen vacancies,paving the way for the development of universally applicable ODS catalysts for industrial applications.
