ABSTRACT Rationally designing broad-spectrum photocatalysts to harvest whole visible-light region photons and enhance solar energy conversion is a“holy grail”for researchers,but is still a challenging issue.Herein,b...ABSTRACT Rationally designing broad-spectrum photocatalysts to harvest whole visible-light region photons and enhance solar energy conversion is a“holy grail”for researchers,but is still a challenging issue.Herein,based on the common polymeric carbon nitride(PCN),a hybrid co-catalysts system comprising plasmonic Au nanoparticles(NPs)and atomically dispersed Pt single atoms(PtSAs)with different functions was constructed to address this challenge.For the dual co-catalysts decorated PCN(PtSAs–Au_(2.5)/PCN),the PCN is photoexcited to generate electrons under UV and short-wavelength visible light,and the synergetic Au NPs and PtSAs not only accelerate charge separation and transfer though Schottky junctions and metal-support bond but also act as the co-catalysts for H_(2) evolution.Furthermore,the Au NPs absorb long-wavelength visible light owing to its localized surface plasmon resonance,and the adjacent PtSAs trap the plasmonic hot-electrons for H_(2) evolution via direct electron transfer effect.Consequently,the PtSAs–Au_(2.5)/PCN exhibits excellent broad-spectrum photocatalytic H_(2) evolution activity with the H_(2) evolution rate of 8.8 mmol g^(−1) h^(−1) at 420 nm and 264μmol g^(−1) h^(−1) at 550 nm,much higher than that of Au_(2.5)/PCN and PtSAs–PCN,respectively.This work provides a new strategy to design broad-spectrum photocatalysts for energy conversion reaction.展开更多
Proton-exchange membrane water electrolysis(PEM WE)is a particularly promising technology for renewable hydrogen produc-tion.However,the excessive passivation of the gas diffusion layer(GDL)will seriously affect the h...Proton-exchange membrane water electrolysis(PEM WE)is a particularly promising technology for renewable hydrogen produc-tion.However,the excessive passivation of the gas diffusion layer(GDL)will seriously affect the high surface-contact resistance and result in energy losses.Thus,a mechanism for improving the conductivity and interface stability of the GDL is an urgent issue.In this work,we have prepared a hydrophilic and corrosion resistant conductive composite protective coating.The polydopamine(PDA)film on the Ti surface,which was obtained via the solution oxidation method,ensured that neither micropores nor pinholes existed in the final hybrid coatings.In-situ reduced gold nanoparticles(AuNPs)improved the conductivity to achieve the desired interfacial contact resistance and further enhanced the corrosion resistance.The surface composition of the treated samples was investigated using scanning electron microscopy(SEM),transmis-sion electron microscopy(TEM),X-ray diffraction(XRD),and Fourier transform infrared spectroscopy(FTIR).The results indicated that the optimized reaction conditions included a pH value of 3 of HAuCl_(4) solution with PDA deposition(48 h)on papers and revealed the lowest con-tact resistance(0.5 mΩ·cm^(2))and corrosion resistance(0.001μA·cm^(−2))in a 0.5 M H_(2)SO_(4)+2 ppm F−solution(1.7 V vs.RHE)among all the modified specimens,where RHE represents reversible hydrogen electrode.These findings indicated that the Au-PDA coating is very appropriate for the modification of Ti GDLs in PEM WE systems.展开更多
Highly ordered TiO2 nanotube array (TNA) films are fabricated by using an anodic oxidation method. Au nanoparticles (NPs) films are decorated onto the top of TNA films with the aid of ion-sputtering and thermal an...Highly ordered TiO2 nanotube array (TNA) films are fabricated by using an anodic oxidation method. Au nanoparticles (NPs) films are decorated onto the top of TNA films with the aid of ion-sputtering and thermal annealing. An enhanced photocatalytic activity under ultraviolet C (UVC, 266 nm) light irradiation is obtained compared with that of the pristine TNA, which is shown by the steady-state photoluminescence (PL) spectra. Furthermore, a distinct blue shift in the nanosecond time-resolved transient photoluminescence (NTRT-PL) spectra is observed. Such a phenomenon could be well explained by considering the competition between the surface photocatalytic process and the recombination of the photo-generated carriers. The enhanced UV photocatalytic activities of the Au-TNA composite are evaluated through photo-degradation of methyl orange (MO) in an aqueous solution with ultraviolet-visible absorption spectrometry. Our current work may provide a simple strategy to synthesize defect-related composite photocatalytic devices.展开更多
Au nanoparticles (NPs) mixed with a majority of bone-like, rod, and cube shapes and a minority of irregu- lar spheres, which can generate a wide absorption spectrum of 400 nm-1000 nm and three localized surface plas...Au nanoparticles (NPs) mixed with a majority of bone-like, rod, and cube shapes and a minority of irregu- lar spheres, which can generate a wide absorption spectrum of 400 nm-1000 nm and three localized surface plas- mon resonance peaks, respectively, at 525, 575, and 775 nrn, are introduced into the hole extraction layer poly(3,4- ethylenedioxythiophene):poly(4-styrenesulfonate) (PEDOT:PSS) to improve optical-to-electrical conversion performances in polymer photovoltaic ceils. With the doping concentration of Au NPs optimized, the cell performance is significantly improved: the short-circuit current density and power conversion efficiency of the poly(3-hexylthiophene): [6,6]-phenyl- C60-butyric acid methyl ester cell are increased by 20.54% and 21.2%, reaching 11.15 mA.cm-2 and 4.23%. The variations of optical, electrical, and morphology with the incorporation of Au NPs in the cells are analyzed in detail, and our results demonstrate that the cell performance improvement can be attributed to a synergistic reaction, including: 1) both the local- ized surface plasmon resonanceand scattering-induced absorption enhancement of the active layer, 2) Au doping-induced hole transport/extraction ability enhancement, and 3) large interface roughness-induced efficient exciton dissociation and hole collection.展开更多
The Au nanoparticles has been prepared by microwave high-pressure procedure with alcohol as the reducing agent. The color of colloidal Au nanoparticles is blue-violet. The maximum absorption spectrum of colloidal Au i...The Au nanoparticles has been prepared by microwave high-pressure procedure with alcohol as the reducing agent. The color of colloidal Au nanoparticles is blue-violet. The maximum absorption spectrum of colloidal Au is at 580 nm, and the resonance scattering peak is at 580 nm. Using this method, the colloidal Au of long-time stability can be prepared Simply and quickly.展开更多
Polystyrene crosslinked microspheres were prepared by soap-free emulsion polymerization using styrene (St) and divinylbenzene (DVB) as monomers;then,the microporous structure was knitted by the Friedel-Crafts alkylati...Polystyrene crosslinked microspheres were prepared by soap-free emulsion polymerization using styrene (St) and divinylbenzene (DVB) as monomers;then,the microporous structure was knitted by the Friedel-Crafts alkylation reaction,and the Au nanoparticles (AuNPs) were loaded into the pores through thermal reduction,to obtain AuNPs/ hyper-crosslinked microporous polymer composite microspheres.SEM and particle-size test results show that the microspheres show good monodispersity.The micropore analysis indicates that the specific surface area and the pore volume of the microporous polymer microspheres decrease with increasing DVB content,and when the DVB content is 0.1%,the specific surface area reaches a maximum of 1 174.6 m2/g.After loading AuNPs,the specific surface area and the amount of micropores of the composite microspheres decrease obviously.The results of XRD and XPS analyses suggest that HAuCl4 is reduced to AuNPs.The composite microspheres show a good catalytic performance for the reduction catalyst of 4-nitrophenol.展开更多
Flower-liked SnO_2 nanorods were prepared by a hydrothermal method.The sensors were fabricated using SnO_2 nanorods adsorption of Au nanoparticles through sputtering deposition.We found that the loading of a small amo...Flower-liked SnO_2 nanorods were prepared by a hydrothermal method.The sensors were fabricated using SnO_2 nanorods adsorption of Au nanoparticles through sputtering deposition.We found that the loading of a small amount of Au nanoparticles on the surface of SnO_2 nanorods can effectively enhance and functionalize the gas sensing performance of SnO_2 nanorods,which due to the Au adsorption make the surface-depletion effect more pronounced.Such enhanced surface depletion increases the sensitivity,lowers the operation temperature and decreases the response time.展开更多
Biosynthesizing Au nanoparticles(AuNPs)from gold-bearing scraps provides a sustainable method to meet the urgent demand for AuNPs.However,it remains challenging to efficiently biosynthesize AuNPs of which the diameter...Biosynthesizing Au nanoparticles(AuNPs)from gold-bearing scraps provides a sustainable method to meet the urgent demand for AuNPs.However,it remains challenging to efficiently biosynthesize AuNPs of which the diameter is less than 10 nm from a trace amount of Au^(3+)concentration at the level of tens ppm.Here,we constructed an exoelectrogenic cell(eCell)-conductive reduced-graphene-oxide aero-gel(rGA)biohybrid by assembling Shewanella sp.S1(SS1)as living biocatalyst and rGA as conductive ad-sorbent,in which Au^(3+)at trace concentrations would be enriched by the adsorption of rGA and reduced to AuNPs through the extracellular electron transfer(EET)of SS1.To regulate the size of the synthe-sized AuNPs to 10 nm,the strain SS1 was engineered to enhance its EET,resulting in strain RS2(pYYD-P tac-ribADEHC&pHG13-P_(bad)-omcC in SS1).Strain RS2 was further assembled with rGA to construct the RS2-rGA biohybrid,which could synthesize AuNPs with the size of 7.62±2.82 nm from 60 ppm Au^(3+)so-lution.The eCell-rGA biohybrid integrated Au^(3+)adsorption and reduction,which enabled AuNPs biosyn-thesis from a trace amount of Au^(3+).Thus,the required Au^(3+)ions concentration was reduced by one or two orders of magnitude compared with conventional methods of AuNPs biosynthesis.Our work devel-oped an AuNPs size regulation technology via engineering eCell’s EET with synthetic biology methods,providing a feasible approach to synthesize AuNPs with controllable size from trace level of gold ions.展开更多
Targeted construction of new covalent organic frameworks(COFs)with specific purposes and rationalities to build colorimetric assay platform for environmental pollutant monitoring have attracted increasing interest.How...Targeted construction of new covalent organic frameworks(COFs)with specific purposes and rationalities to build colorimetric assay platform for environmental pollutant monitoring have attracted increasing interest.However,it is still challenging due to lack of available coordination sites inside COFs pores and only a slight bonding ability for anchoring metal.In this work,a two-dimensional(2D)COFs(termed as Tz-COF)with high crystallinity,excellent chemical stability,and abundant sulfur coordination in its skeletons was synthesized and used for the confined growth of Au NPs.It was found that the Au NPs showed significant dispersibility for the support of Tz-COF.The proposed Tz-COF@Au NPs possessed outstanding Hg^(2+)-activated peroxidase-like activity benefited from physicochemical properties of gold amalgam and synergistic effect between COFs and Au NPs to oxidize chromogenic substrate.Based on highly efficient activity and distinctive color evolution,the strategy for detecting Hg^(2+)was developed and successfully applied to determine the content of Hg^(2+)in real environmental samples.This work manifests that a potential strategy to establish a colorimetric assay platform for environmental pollutant monitoring based on the targeted manufacturing of novel COFs with specific functions.展开更多
Hematite(α-Fe_(2)O_(3)) based photoanodes have been extensively studied due to various intriguing features that make them viable candidates for a photoelectrochemical(PEC) water splitting photoanode.Herein,we propose...Hematite(α-Fe_(2)O_(3)) based photoanodes have been extensively studied due to various intriguing features that make them viable candidates for a photoelectrochemical(PEC) water splitting photoanode.Herein,we propose a Zr-doped Fe_(2)O_(3) photoanode decorated with facilely spin-coated Au nanoparticles(NPs) and microwave-assisted attached Si co-doping in conjunction with a SiO_(x) overlayer that displayed a remarkable photocurrent density of 2.01 mA/cm^(2) at 1.23 V vs.RHE.The kinetic dynamics at the photoelectrode/-electrolyte interface was examined by employing systematic electrochemical investigations.The Au NPs played a dual role in increasing PEC water splitting.First,the Schottky interface that was formed between Au NPs and Zr-Fe_(2)O_(3) lectrode ensured the prevention of electron flow from the photoanode to the metal,increasing the number of available charges as well as suppressing surface charge recombination.Second,Au extracted photoholes from the bulk of the Zr-Fe_(2)O_(3) and transported them to the outer SiO_(x) overlayer,while the SiO_(x) overlayer efficiently collected the photoholes and promoted the hole injection into the electrolyte.Further,Si co-doping enhanced bulk conductivity by reducing bulk charge transfer resistance and improving charge carrier density.This study outlines a technique to design a metallic charge transfer path with an overlayer for solar energy conversion.展开更多
Enhancing both the number of active sites available and the intrinsic activity of Co-based electrocatalysts simultaneously is a desirable goal.Herein,a ZIF-67-derived hierarchical porous cobalt sulfide decorated by Au...Enhancing both the number of active sites available and the intrinsic activity of Co-based electrocatalysts simultaneously is a desirable goal.Herein,a ZIF-67-derived hierarchical porous cobalt sulfide decorated by Au nanoparticles(NPs)(denoted as HP-Au@CoxSy@ZIF-67)hybrid is synthesized by low-temperature sulfuration treatment.The well-defined macroporous-mesoporous-microporous structure is obtained based on the combination of polystyrene spheres,as-formed CoxSy nanosheets,and ZIF-67 frameworks.This novel three-dimensional hierarchical structure significantly enlarges the three-phase interfaces,accelerating the mass transfer and exposing the active centers for oxygen evolution reaction.The electronic structure of Co is modulated by Au through charge transfer,and a series of experiments,together with theoretical analysis,is performed to ascertain the electronic modulation of Co by Au.Meanwhile,HP-Au@CoxSy@ZIF-67 catalysts with different amounts of Au were synthesized,wherein Au and NaBH4 reductant result in an interesting“competition effect”to regulate the relative ratio of Co^(2+)/Co^(3+),and moderate Au assists the electrochemical performance to reach the highest value.Consequently,the optimized HP-Au@CoxSy@ZIF-67 exhibits a low overpotential of 340 mV at 10 mA cm^(-2)and a Tafel slope of 42 mV dec-1 for OER in 0.1 M aqueous KOH,enabling efficient water splitting and Zn-air battery performance.The work here highlights the pivotal roles of both microstructural and electronic modulation in enhancing electrocatalytic activity and presents a feasible strategy for designing and optimizing advanced electrocatalysts.展开更多
Reactive oxygen species(ROS)plays important roles in living organisms.While ROS is a double-edged sword,which can eliminate drug-resistant bacteria,but excessive levels can cause oxidative damage to cells.A core–shel...Reactive oxygen species(ROS)plays important roles in living organisms.While ROS is a double-edged sword,which can eliminate drug-resistant bacteria,but excessive levels can cause oxidative damage to cells.A core–shell nanozyme,Ce O_(2)@ZIF-8/Au,has been crafted,spontaneously activating both ROS generating and scavenging functions,achieving the multifaceted functions of eliminating bacteria,reducing inflammation,and promoting wound healing.The Au Nanoparticles(NPs)on the shell exhibit high-efficiency peroxidase-like activity,producing ROS to kill bacteria.Meanwhile,the encapsulation of Ce O_(2) core within ZIF-8 provides a seal for temporarily limiting the superoxide dismutase and catalase-like activities of Ce O_(2) nanoparticles.Subsequently,as the ZIF-8 structure decomposes in the acidic microenvironment,the Ce O_(2) core is gradually released,exerting its ROS scavenging activity to eliminate excess ROS produced by the Au NPs.These two functions automatically and continuously regulate the balance of ROS levels,ultimately achieving the function of killing bacteria,reducing inflammation,and promoting wound healing.Such innovative ROS spontaneous regulators hold immense potential for revolutionizing the field of antibacterial agents and therapies.展开更多
Monodisperse Au nanoparticles(NPs)have been synthesized at room temperature via a burst nucleation of Au upon injection of the reducing agent t-butylamine-borane complex into a 1,2,3,4-tetrahydronaphthalene solution o...Monodisperse Au nanoparticles(NPs)have been synthesized at room temperature via a burst nucleation of Au upon injection of the reducing agent t-butylamine-borane complex into a 1,2,3,4-tetrahydronaphthalene solution of HAuCl4·3H2O in the presence of oleylamine.The as-synthesized Au NPs show size-dependent surface plasmonic properties between 520 and 530 nm.They adopt an icosahedral shape and are polycrystalline with multiple-twinned structures.When deposited on a graphitized porous carbon support,the NPs are highly active for CO oxidation,showing 100%CO conversion at-45°C.展开更多
A strategy of intensifying the visible light harvesting ability of anatase Ti02 hollow spheres(HSs)was developed,in which both sides of Ti02 HSs were utilised for stabilising Au nanoparticles(NPs)through the sacrifici...A strategy of intensifying the visible light harvesting ability of anatase Ti02 hollow spheres(HSs)was developed,in which both sides of Ti02 HSs were utilised for stabilising Au nanoparticles(NPs)through the sacrificial templating method and convex surface-induced confinement.The composite structure of single Au NP yolk-Ti02 shell-Au NPs,denoted as Au@Au(Ti02,was rendered and confirmed by the transmission electron microscopy analysis.Au@Au(Ti02 showed enhanced photocatalytic activity in the degradation of methylene blue and phenol in aqueous phase under visible light surpassing that of other reference materials such as Au(Ti02 by 77%and Au@P25 by 52%,respectively,in phenol degradation.展开更多
The surface enhanced fluorescence effect of acridine orange fluorophore in the proximity of Au nanoparticles has been investigated experimentally in the system of aqueous solution.Significant enhancement of the fluore...The surface enhanced fluorescence effect of acridine orange fluorophore in the proximity of Au nanoparticles has been investigated experimentally in the system of aqueous solution.Significant enhancement of the fluorescence intensity was observed when the system was excited with 532 nm or 442 nm CW lasers.The influence of the distances between neighboring Au particles as well as that between the fluorophore molecules and the Au surface were explored experimentally.The results demonstrated that a compact distribution of metallic particles was able to produce stronger fluorescence enhancement.Proper separation between the fluorophore molecules and the metal surface was favorable for a better enhancement.展开更多
Ti O2-supported Pd Au bimetallic nanoparticles(NPs) with small size and good dispersity were prepared by the room-temperature ionic liquid-assisted bimetal sputtering, which is simple, environmentally friendly, and fr...Ti O2-supported Pd Au bimetallic nanoparticles(NPs) with small size and good dispersity were prepared by the room-temperature ionic liquid-assisted bimetal sputtering, which is simple, environmentally friendly, and free of additives and byproducts. Pd/Au atomic ratio can be tuned by controlling the sputtering conditions simply. High catalytic activity was found in Pd Au–NPs–Ti O2 hybrids for solvent-free selective oxidation of 1-phenylethanol using O2 as the oxidant at the low temperature of 50 °C and low pressure of 1 atm. It was found that Pd/Au ratio strongly affected the catalytical activity, and the highest conversion of about 35 % and turnover frequency of about 421 h-1were achieved at 1:1 of Pd/Au atomic ratio. The synergistic effect in Pd Au NPs was also discussed based on the comprehensive characterization results.The present approach may offer an alternative platform for future development of green-chemistry compatible bimetallic nanocatalysts.展开更多
This work demonstrated the feasibility of detecting hydrocortisone in cosmetics using a novel CdSe/CdS quan- tum dots-based competitive fluoroimmunoassay with magnetic core/shell Fe3Oa/Au nanoparticles (MCFN) as sol...This work demonstrated the feasibility of detecting hydrocortisone in cosmetics using a novel CdSe/CdS quan- tum dots-based competitive fluoroimmunoassay with magnetic core/shell Fe3Oa/Au nanoparticles (MCFN) as solid carriers. Hydrocortisone antigen was labeled with the synthesized core/shell CdSe/CdS quantum dots (QDs) to form the antigen-QDs conjugate. Meanwhile, hydrocortisone antibody was incubated with MCFN and the immobilized antibody was obtained. The immobilized antibody was then mixed sequentially with hydrocortisone and a slightly excess amount of the QDs-labeled hydrocortisone antigen, allowing their competition for binding with the antibody immobilized on MCFN. The bound hydrocortisone and the antigen-QDs conjugates on MCFN were removed subsequently after the mixture was applied to a magnetic force. The analyte concentration was obtained by measuring the fluorescence intensity of the unbound hydrocortisone antigen-QDs conjugates. The proposed method was characterized by simplicity, rapidity, and high sensitivity with a wide linear working range of 0.5 to 15000 pg·mL^-1 and a low detection limit of 0.5 pg.mL^- 1. The proposed method was successfully applied to the determination of hydrocortisone in cosmetics with satisfactory results.展开更多
An electrochemical sensor for determination of hydroquinone (HQ) and catechol (CC) was developed using Au nanoparticles (AuNPs) fabricated on reduced graphene oxide/polyimide (PIIRGO) film by electroless depos...An electrochemical sensor for determination of hydroquinone (HQ) and catechol (CC) was developed using Au nanoparticles (AuNPs) fabricated on reduced graphene oxide/polyimide (PIIRGO) film by electroless deposition. The electrochemical behaviors of HQ and CC at PIIRGO-AuNPs electrode were investigated by cyclic voltammetry (CV) and differential pulse voltammetry (DPV). Under the optimized condition, the current responses at PI/RGO-AuNPs electrode were linear over ranges from 1 to 654 mol/L for HQ and from 2 to 1289 mol/L for CC, with the detection limits of 0.09 and 0.2 mollL, respectively. The proposed electrode exhibited good reproducibility, stability and selectivity. In addition, the proposed electrode was successfully applied in the determination of HQ and CC in tap water and the Yellow River samples.展开更多
Fabrication of multifunctional nanoplatform to in situ monitor Fenton reaction is of vital importance to probe the underlying reaction process and design high-performance catalyst. Herein, a hybrid catalyst comprising...Fabrication of multifunctional nanoplatform to in situ monitor Fenton reaction is of vital importance to probe the underlying reaction process and design high-performance catalyst. Herein, a hybrid catalyst comprising of single-crystalline Au nanoparticles (SC Au NPs) on reduced graphene oxide (RGO) sheet was prepared, which not only exhibited an excellent ^(1)O_(2) mediated Fenton-like catalytic activity in promoting rhodamine 6G (R6G) degradation by activating H_(2)O_(2), but also displayed a sensitive surface-enhanced Raman spectroscopy (SERS) detection performance to R6G with a linear response range from 1.0×10^(-8) mol/L to 1.0×10^(-5) mol/L thus providing a powerful and versatile nanoplatform for in situ SERS monitoring Fenton-like catalytic reaction. The integration of catalytic and SERS activities into a single nanostructure are expected to provide great potentials for practical applications in environmental catalysis.展开更多
Controlled integration of ultrafine metal nanoparticles (MNPs) and metal- organic frameworks (MOFs) has drawn much attention due to their unique physical and chemical properties. However, the development of a one-...Controlled integration of ultrafine metal nanoparticles (MNPs) and metal- organic frameworks (MOFs) has drawn much attention due to their unique physical and chemical properties. However, the development of a one-step strategy for preparing ultrafine MNPs within MOFs still remains a great challenge. Herein, a facile synthetic approach toward the abovementioned composites was developed. In contrast to the conventional approach, these hybrids were prepared by the direct mixing of metal and MOF precursors in the reaction solution assisted by microwave irradiation. Impressively, the Au/MOF-199 composite with uniformly distributed ultrafine Au nanoparticles could be fabricated in only two minutes, and the Au loading could be increased up to a level of 5.13%. The multifunctional Au/MOF-199 catalysts exhibited high turnover numbers (TONs) and turnover frequencies (TOFs) in the three-component coupling reaction of formaldehyde, phenylacetylene, and piperidine (AB-coupling). Owing to the confinement effect of MOF-199, the 5.13%Au/MOF-199 catalyst could be recycled for five runs without serious loss of activity, with no obvious aggregation of Au NPs detected.展开更多
基金supported by the National Natural Science Foundation of China(Grant No.51871078 and 52071119)Interdisciplinary Research Foundation of HIT(Grant No.IR2021208)+1 种基金State Key Laboratory of Urban Water Resource and Environment(Harbin Institute of Technology)(No.2022TS38)Heilongjiang Science Foundation(No.LH2020B006).
文摘ABSTRACT Rationally designing broad-spectrum photocatalysts to harvest whole visible-light region photons and enhance solar energy conversion is a“holy grail”for researchers,but is still a challenging issue.Herein,based on the common polymeric carbon nitride(PCN),a hybrid co-catalysts system comprising plasmonic Au nanoparticles(NPs)and atomically dispersed Pt single atoms(PtSAs)with different functions was constructed to address this challenge.For the dual co-catalysts decorated PCN(PtSAs–Au_(2.5)/PCN),the PCN is photoexcited to generate electrons under UV and short-wavelength visible light,and the synergetic Au NPs and PtSAs not only accelerate charge separation and transfer though Schottky junctions and metal-support bond but also act as the co-catalysts for H_(2) evolution.Furthermore,the Au NPs absorb long-wavelength visible light owing to its localized surface plasmon resonance,and the adjacent PtSAs trap the plasmonic hot-electrons for H_(2) evolution via direct electron transfer effect.Consequently,the PtSAs–Au_(2.5)/PCN exhibits excellent broad-spectrum photocatalytic H_(2) evolution activity with the H_(2) evolution rate of 8.8 mmol g^(−1) h^(−1) at 420 nm and 264μmol g^(−1) h^(−1) at 550 nm,much higher than that of Au_(2.5)/PCN and PtSAs–PCN,respectively.This work provides a new strategy to design broad-spectrum photocatalysts for energy conversion reaction.
基金supported by the National Key Research and Development Program of China(No.2018 YFB1502403)。
文摘Proton-exchange membrane water electrolysis(PEM WE)is a particularly promising technology for renewable hydrogen produc-tion.However,the excessive passivation of the gas diffusion layer(GDL)will seriously affect the high surface-contact resistance and result in energy losses.Thus,a mechanism for improving the conductivity and interface stability of the GDL is an urgent issue.In this work,we have prepared a hydrophilic and corrosion resistant conductive composite protective coating.The polydopamine(PDA)film on the Ti surface,which was obtained via the solution oxidation method,ensured that neither micropores nor pinholes existed in the final hybrid coatings.In-situ reduced gold nanoparticles(AuNPs)improved the conductivity to achieve the desired interfacial contact resistance and further enhanced the corrosion resistance.The surface composition of the treated samples was investigated using scanning electron microscopy(SEM),transmis-sion electron microscopy(TEM),X-ray diffraction(XRD),and Fourier transform infrared spectroscopy(FTIR).The results indicated that the optimized reaction conditions included a pH value of 3 of HAuCl_(4) solution with PDA deposition(48 h)on papers and revealed the lowest con-tact resistance(0.5 mΩ·cm^(2))and corrosion resistance(0.001μA·cm^(−2))in a 0.5 M H_(2)SO_(4)+2 ppm F−solution(1.7 V vs.RHE)among all the modified specimens,where RHE represents reversible hydrogen electrode.These findings indicated that the Au-PDA coating is very appropriate for the modification of Ti GDLs in PEM WE systems.
基金supported by the National Natural Science Foundation of China(Grant No.11274082)the Shandong Excellent Young Scientist Research Award Fund Project,China(Grant No.BS2011CL002)
文摘Highly ordered TiO2 nanotube array (TNA) films are fabricated by using an anodic oxidation method. Au nanoparticles (NPs) films are decorated onto the top of TNA films with the aid of ion-sputtering and thermal annealing. An enhanced photocatalytic activity under ultraviolet C (UVC, 266 nm) light irradiation is obtained compared with that of the pristine TNA, which is shown by the steady-state photoluminescence (PL) spectra. Furthermore, a distinct blue shift in the nanosecond time-resolved transient photoluminescence (NTRT-PL) spectra is observed. Such a phenomenon could be well explained by considering the competition between the surface photocatalytic process and the recombination of the photo-generated carriers. The enhanced UV photocatalytic activities of the Au-TNA composite are evaluated through photo-degradation of methyl orange (MO) in an aqueous solution with ultraviolet-visible absorption spectrometry. Our current work may provide a simple strategy to synthesize defect-related composite photocatalytic devices.
基金Project supported by the National Basic Research Program of China(Grant Nos.2015CB932202 and 2012CB933301)the National Natural Science Foundation of China(Grant Nos.61274065,51173081,61136003,BZ2010043,51372119,and 51172110)+3 种基金the Science Fund from the Ministry of Education of China(Grant No.IRT1148)the Specialized Research Fund for the Doctoral Program of Higher Education of China(Grant No.20113223110005)the Priority Academic Program Development of Jiangsu Provincial Higher Education Institutions(Grant No.YX03001)the National Synergistic Innovation Center for Advanced Materials and the Synergetic Innovation Center for Organic Electronics and Information Displays,China
文摘Au nanoparticles (NPs) mixed with a majority of bone-like, rod, and cube shapes and a minority of irregu- lar spheres, which can generate a wide absorption spectrum of 400 nm-1000 nm and three localized surface plas- mon resonance peaks, respectively, at 525, 575, and 775 nrn, are introduced into the hole extraction layer poly(3,4- ethylenedioxythiophene):poly(4-styrenesulfonate) (PEDOT:PSS) to improve optical-to-electrical conversion performances in polymer photovoltaic ceils. With the doping concentration of Au NPs optimized, the cell performance is significantly improved: the short-circuit current density and power conversion efficiency of the poly(3-hexylthiophene): [6,6]-phenyl- C60-butyric acid methyl ester cell are increased by 20.54% and 21.2%, reaching 11.15 mA.cm-2 and 4.23%. The variations of optical, electrical, and morphology with the incorporation of Au NPs in the cells are analyzed in detail, and our results demonstrate that the cell performance improvement can be attributed to a synergistic reaction, including: 1) both the local- ized surface plasmon resonanceand scattering-induced absorption enhancement of the active layer, 2) Au doping-induced hole transport/extraction ability enhancement, and 3) large interface roughness-induced efficient exciton dissociation and hole collection.
文摘The Au nanoparticles has been prepared by microwave high-pressure procedure with alcohol as the reducing agent. The color of colloidal Au nanoparticles is blue-violet. The maximum absorption spectrum of colloidal Au is at 580 nm, and the resonance scattering peak is at 580 nm. Using this method, the colloidal Au of long-time stability can be prepared Simply and quickly.
基金the National Natural Science Foundation of China(No.51303049)。
文摘Polystyrene crosslinked microspheres were prepared by soap-free emulsion polymerization using styrene (St) and divinylbenzene (DVB) as monomers;then,the microporous structure was knitted by the Friedel-Crafts alkylation reaction,and the Au nanoparticles (AuNPs) were loaded into the pores through thermal reduction,to obtain AuNPs/ hyper-crosslinked microporous polymer composite microspheres.SEM and particle-size test results show that the microspheres show good monodispersity.The micropore analysis indicates that the specific surface area and the pore volume of the microporous polymer microspheres decrease with increasing DVB content,and when the DVB content is 0.1%,the specific surface area reaches a maximum of 1 174.6 m2/g.After loading AuNPs,the specific surface area and the amount of micropores of the composite microspheres decrease obviously.The results of XRD and XPS analyses suggest that HAuCl4 is reduced to AuNPs.The composite microspheres show a good catalytic performance for the reduction catalyst of 4-nitrophenol.
文摘Flower-liked SnO_2 nanorods were prepared by a hydrothermal method.The sensors were fabricated using SnO_2 nanorods adsorption of Au nanoparticles through sputtering deposition.We found that the loading of a small amount of Au nanoparticles on the surface of SnO_2 nanorods can effectively enhance and functionalize the gas sensing performance of SnO_2 nanorods,which due to the Au adsorption make the surface-depletion effect more pronounced.Such enhanced surface depletion increases the sensitivity,lowers the operation temperature and decreases the response time.
基金supported by the National Key Research and Development Program of China(No.2018YFA0901300)the Na-tional Natural Science Foundation of China(Nos.NSFC 32071411,NSFC 32001034,and NSFC 31701569)+1 种基金the Young Science and Tech-nology Talents Growth Project of Education Department of Guizhou Province(No.KY[2018]445)Key Laboratory of Wuliangye-flavor Liquor Solid-state Fermentation,China National Light Indus-try(No.2021JJ013).
文摘Biosynthesizing Au nanoparticles(AuNPs)from gold-bearing scraps provides a sustainable method to meet the urgent demand for AuNPs.However,it remains challenging to efficiently biosynthesize AuNPs of which the diameter is less than 10 nm from a trace amount of Au^(3+)concentration at the level of tens ppm.Here,we constructed an exoelectrogenic cell(eCell)-conductive reduced-graphene-oxide aero-gel(rGA)biohybrid by assembling Shewanella sp.S1(SS1)as living biocatalyst and rGA as conductive ad-sorbent,in which Au^(3+)at trace concentrations would be enriched by the adsorption of rGA and reduced to AuNPs through the extracellular electron transfer(EET)of SS1.To regulate the size of the synthe-sized AuNPs to 10 nm,the strain SS1 was engineered to enhance its EET,resulting in strain RS2(pYYD-P tac-ribADEHC&pHG13-P_(bad)-omcC in SS1).Strain RS2 was further assembled with rGA to construct the RS2-rGA biohybrid,which could synthesize AuNPs with the size of 7.62±2.82 nm from 60 ppm Au^(3+)so-lution.The eCell-rGA biohybrid integrated Au^(3+)adsorption and reduction,which enabled AuNPs biosyn-thesis from a trace amount of Au^(3+).Thus,the required Au^(3+)ions concentration was reduced by one or two orders of magnitude compared with conventional methods of AuNPs biosynthesis.Our work devel-oped an AuNPs size regulation technology via engineering eCell’s EET with synthetic biology methods,providing a feasible approach to synthesize AuNPs with controllable size from trace level of gold ions.
基金supported by the National Natural Science Foundation of China(Nos.22274021,21974021 and 22036001).
文摘Targeted construction of new covalent organic frameworks(COFs)with specific purposes and rationalities to build colorimetric assay platform for environmental pollutant monitoring have attracted increasing interest.However,it is still challenging due to lack of available coordination sites inside COFs pores and only a slight bonding ability for anchoring metal.In this work,a two-dimensional(2D)COFs(termed as Tz-COF)with high crystallinity,excellent chemical stability,and abundant sulfur coordination in its skeletons was synthesized and used for the confined growth of Au NPs.It was found that the Au NPs showed significant dispersibility for the support of Tz-COF.The proposed Tz-COF@Au NPs possessed outstanding Hg^(2+)-activated peroxidase-like activity benefited from physicochemical properties of gold amalgam and synergistic effect between COFs and Au NPs to oxidize chromogenic substrate.Based on highly efficient activity and distinctive color evolution,the strategy for detecting Hg^(2+)was developed and successfully applied to determine the content of Hg^(2+)in real environmental samples.This work manifests that a potential strategy to establish a colorimetric assay platform for environmental pollutant monitoring based on the targeted manufacturing of novel COFs with specific functions.
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korean government(MSIT)(NRF-2021R1A2C1095669,NRF-2021R1F1A1049366 and NRF2023R1A2C1003088)supported by the GRDC(Global Research Development Center)Cooperative Hub Program through the National Research Foundation of Korea(NRF)funded by the Ministry of Science and ICT(MSIT)(RS-202300258911)。
文摘Hematite(α-Fe_(2)O_(3)) based photoanodes have been extensively studied due to various intriguing features that make them viable candidates for a photoelectrochemical(PEC) water splitting photoanode.Herein,we propose a Zr-doped Fe_(2)O_(3) photoanode decorated with facilely spin-coated Au nanoparticles(NPs) and microwave-assisted attached Si co-doping in conjunction with a SiO_(x) overlayer that displayed a remarkable photocurrent density of 2.01 mA/cm^(2) at 1.23 V vs.RHE.The kinetic dynamics at the photoelectrode/-electrolyte interface was examined by employing systematic electrochemical investigations.The Au NPs played a dual role in increasing PEC water splitting.First,the Schottky interface that was formed between Au NPs and Zr-Fe_(2)O_(3) lectrode ensured the prevention of electron flow from the photoanode to the metal,increasing the number of available charges as well as suppressing surface charge recombination.Second,Au extracted photoholes from the bulk of the Zr-Fe_(2)O_(3) and transported them to the outer SiO_(x) overlayer,while the SiO_(x) overlayer efficiently collected the photoholes and promoted the hole injection into the electrolyte.Further,Si co-doping enhanced bulk conductivity by reducing bulk charge transfer resistance and improving charge carrier density.This study outlines a technique to design a metallic charge transfer path with an overlayer for solar energy conversion.
基金National Natural Science Foundation of China,Grant/Award Numbers:52102260,52171211,51972220,61903235,U22A20145Shandong Provincial Natural Science Foundation,Grant/Award Numbers:ZR2020QB069,ZR2022ME051+4 种基金National Key Research and Development Program of China,Grant/Award Number:2022YFB4002004Scientific and Technological Innovation Ability Improvement Project of Minor Enterprises in Shandong Province,Grant/Award Number:2022TSGC1021Announce the List and Take Charge Project in Jinan,Grant/Award Number:202214012Major innovation project for integrating science,education and industry of Qilu University of Technology (Shandong Academy of Sciences),Grant/Award Numbers:2022JBZ01-07,2022PY044China Postdoctoral Science Foundation,Grant/Award Number:2022M711545。
文摘Enhancing both the number of active sites available and the intrinsic activity of Co-based electrocatalysts simultaneously is a desirable goal.Herein,a ZIF-67-derived hierarchical porous cobalt sulfide decorated by Au nanoparticles(NPs)(denoted as HP-Au@CoxSy@ZIF-67)hybrid is synthesized by low-temperature sulfuration treatment.The well-defined macroporous-mesoporous-microporous structure is obtained based on the combination of polystyrene spheres,as-formed CoxSy nanosheets,and ZIF-67 frameworks.This novel three-dimensional hierarchical structure significantly enlarges the three-phase interfaces,accelerating the mass transfer and exposing the active centers for oxygen evolution reaction.The electronic structure of Co is modulated by Au through charge transfer,and a series of experiments,together with theoretical analysis,is performed to ascertain the electronic modulation of Co by Au.Meanwhile,HP-Au@CoxSy@ZIF-67 catalysts with different amounts of Au were synthesized,wherein Au and NaBH4 reductant result in an interesting“competition effect”to regulate the relative ratio of Co^(2+)/Co^(3+),and moderate Au assists the electrochemical performance to reach the highest value.Consequently,the optimized HP-Au@CoxSy@ZIF-67 exhibits a low overpotential of 340 mV at 10 mA cm^(-2)and a Tafel slope of 42 mV dec-1 for OER in 0.1 M aqueous KOH,enabling efficient water splitting and Zn-air battery performance.The work here highlights the pivotal roles of both microstructural and electronic modulation in enhancing electrocatalytic activity and presents a feasible strategy for designing and optimizing advanced electrocatalysts.
基金supported by the Natural Science Foundation of Fujian Province of China(No.2022J01043)China Scholarship Council(201806315005 and 201703170071).
文摘Reactive oxygen species(ROS)plays important roles in living organisms.While ROS is a double-edged sword,which can eliminate drug-resistant bacteria,but excessive levels can cause oxidative damage to cells.A core–shell nanozyme,Ce O_(2)@ZIF-8/Au,has been crafted,spontaneously activating both ROS generating and scavenging functions,achieving the multifaceted functions of eliminating bacteria,reducing inflammation,and promoting wound healing.The Au Nanoparticles(NPs)on the shell exhibit high-efficiency peroxidase-like activity,producing ROS to kill bacteria.Meanwhile,the encapsulation of Ce O_(2) core within ZIF-8 provides a seal for temporarily limiting the superoxide dismutase and catalase-like activities of Ce O_(2) nanoparticles.Subsequently,as the ZIF-8 structure decomposes in the acidic microenvironment,the Ce O_(2) core is gradually released,exerting its ROS scavenging activity to eliminate excess ROS produced by the Au NPs.These two functions automatically and continuously regulate the balance of ROS levels,ultimately achieving the function of killing bacteria,reducing inflammation,and promoting wound healing.Such innovative ROS spontaneous regulators hold immense potential for revolutionizing the field of antibacterial agents and therapies.
基金by NSF/DMR 0606264 and a GAANN fellowship(Y.Lee).
文摘Monodisperse Au nanoparticles(NPs)have been synthesized at room temperature via a burst nucleation of Au upon injection of the reducing agent t-butylamine-borane complex into a 1,2,3,4-tetrahydronaphthalene solution of HAuCl4·3H2O in the presence of oleylamine.The as-synthesized Au NPs show size-dependent surface plasmonic properties between 520 and 530 nm.They adopt an icosahedral shape and are polycrystalline with multiple-twinned structures.When deposited on a graphitized porous carbon support,the NPs are highly active for CO oxidation,showing 100%CO conversion at-45°C.
文摘A strategy of intensifying the visible light harvesting ability of anatase Ti02 hollow spheres(HSs)was developed,in which both sides of Ti02 HSs were utilised for stabilising Au nanoparticles(NPs)through the sacrificial templating method and convex surface-induced confinement.The composite structure of single Au NP yolk-Ti02 shell-Au NPs,denoted as Au@Au(Ti02,was rendered and confirmed by the transmission electron microscopy analysis.Au@Au(Ti02 showed enhanced photocatalytic activity in the degradation of methylene blue and phenol in aqueous phase under visible light surpassing that of other reference materials such as Au(Ti02 by 77%and Au@P25 by 52%,respectively,in phenol degradation.
基金supported by the Foundation for the Key Project of the Chinese Ministry of Education (Grant No. 108118)the Fundamental Research Funds for the Central Universities (Grant No. GK200901022)
文摘The surface enhanced fluorescence effect of acridine orange fluorophore in the proximity of Au nanoparticles has been investigated experimentally in the system of aqueous solution.Significant enhancement of the fluorescence intensity was observed when the system was excited with 532 nm or 442 nm CW lasers.The influence of the distances between neighboring Au particles as well as that between the fluorophore molecules and the Au surface were explored experimentally.The results demonstrated that a compact distribution of metallic particles was able to produce stronger fluorescence enhancement.Proper separation between the fluorophore molecules and the metal surface was favorable for a better enhancement.
基金supported by the National Natural Science Foundation of China(No.61274019)the Collaborative Innovation Center of Suzhou Nano Science & Technologythe Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD)
文摘Ti O2-supported Pd Au bimetallic nanoparticles(NPs) with small size and good dispersity were prepared by the room-temperature ionic liquid-assisted bimetal sputtering, which is simple, environmentally friendly, and free of additives and byproducts. Pd/Au atomic ratio can be tuned by controlling the sputtering conditions simply. High catalytic activity was found in Pd Au–NPs–Ti O2 hybrids for solvent-free selective oxidation of 1-phenylethanol using O2 as the oxidant at the low temperature of 50 °C and low pressure of 1 atm. It was found that Pd/Au ratio strongly affected the catalytical activity, and the highest conversion of about 35 % and turnover frequency of about 421 h-1were achieved at 1:1 of Pd/Au atomic ratio. The synergistic effect in Pd Au NPs was also discussed based on the comprehensive characterization results.The present approach may offer an alternative platform for future development of green-chemistry compatible bimetallic nanocatalysts.
基金Project supported by the National Natural Science Foundation of China (Nos. 20345006 and 20575043).
文摘This work demonstrated the feasibility of detecting hydrocortisone in cosmetics using a novel CdSe/CdS quan- tum dots-based competitive fluoroimmunoassay with magnetic core/shell Fe3Oa/Au nanoparticles (MCFN) as solid carriers. Hydrocortisone antigen was labeled with the synthesized core/shell CdSe/CdS quantum dots (QDs) to form the antigen-QDs conjugate. Meanwhile, hydrocortisone antibody was incubated with MCFN and the immobilized antibody was obtained. The immobilized antibody was then mixed sequentially with hydrocortisone and a slightly excess amount of the QDs-labeled hydrocortisone antigen, allowing their competition for binding with the antibody immobilized on MCFN. The bound hydrocortisone and the antigen-QDs conjugates on MCFN were removed subsequently after the mixture was applied to a magnetic force. The analyte concentration was obtained by measuring the fluorescence intensity of the unbound hydrocortisone antigen-QDs conjugates. The proposed method was characterized by simplicity, rapidity, and high sensitivity with a wide linear working range of 0.5 to 15000 pg·mL^-1 and a low detection limit of 0.5 pg.mL^- 1. The proposed method was successfully applied to the determination of hydrocortisone in cosmetics with satisfactory results.
基金Acknowledgement This work was supported by the National Natural Science Foundation of China (Grant No. 51372106).
文摘An electrochemical sensor for determination of hydroquinone (HQ) and catechol (CC) was developed using Au nanoparticles (AuNPs) fabricated on reduced graphene oxide/polyimide (PIIRGO) film by electroless deposition. The electrochemical behaviors of HQ and CC at PIIRGO-AuNPs electrode were investigated by cyclic voltammetry (CV) and differential pulse voltammetry (DPV). Under the optimized condition, the current responses at PI/RGO-AuNPs electrode were linear over ranges from 1 to 654 mol/L for HQ and from 2 to 1289 mol/L for CC, with the detection limits of 0.09 and 0.2 mollL, respectively. The proposed electrode exhibited good reproducibility, stability and selectivity. In addition, the proposed electrode was successfully applied in the determination of HQ and CC in tap water and the Yellow River samples.
基金supported by the National Natural Science Foundation of China (Nos. 21577156, 21876184)the Fundamental Research Funds for the Central University (No. 310421124)。
文摘Fabrication of multifunctional nanoplatform to in situ monitor Fenton reaction is of vital importance to probe the underlying reaction process and design high-performance catalyst. Herein, a hybrid catalyst comprising of single-crystalline Au nanoparticles (SC Au NPs) on reduced graphene oxide (RGO) sheet was prepared, which not only exhibited an excellent ^(1)O_(2) mediated Fenton-like catalytic activity in promoting rhodamine 6G (R6G) degradation by activating H_(2)O_(2), but also displayed a sensitive surface-enhanced Raman spectroscopy (SERS) detection performance to R6G with a linear response range from 1.0×10^(-8) mol/L to 1.0×10^(-5) mol/L thus providing a powerful and versatile nanoplatform for in situ SERS monitoring Fenton-like catalytic reaction. The integration of catalytic and SERS activities into a single nanostructure are expected to provide great potentials for practical applications in environmental catalysis.
基金The authors acknowledge the financial support from the National Natural Science Foundation of China (Nos. 21573286, 21173269, and 21572688), Ministry ofScience and Technology of China (Nos. 2011BAK15B05 and 2015AA034603), Specialized Research Fund for the Doctoral Program of Higher Education (No. 20130007110003), and Science Foundation of China University of Petroleum, Beijing (No. 2462015YQ0304).
文摘Controlled integration of ultrafine metal nanoparticles (MNPs) and metal- organic frameworks (MOFs) has drawn much attention due to their unique physical and chemical properties. However, the development of a one-step strategy for preparing ultrafine MNPs within MOFs still remains a great challenge. Herein, a facile synthetic approach toward the abovementioned composites was developed. In contrast to the conventional approach, these hybrids were prepared by the direct mixing of metal and MOF precursors in the reaction solution assisted by microwave irradiation. Impressively, the Au/MOF-199 composite with uniformly distributed ultrafine Au nanoparticles could be fabricated in only two minutes, and the Au loading could be increased up to a level of 5.13%. The multifunctional Au/MOF-199 catalysts exhibited high turnover numbers (TONs) and turnover frequencies (TOFs) in the three-component coupling reaction of formaldehyde, phenylacetylene, and piperidine (AB-coupling). Owing to the confinement effect of MOF-199, the 5.13%Au/MOF-199 catalyst could be recycled for five runs without serious loss of activity, with no obvious aggregation of Au NPs detected.