A gold catalyst of Au/pyrenyl‑graphdiyne(Pyr‑GDY)was prepared by anchoring small size of gold nanoparticles(Au NPs)on the surface of Pyr‑GDY for electrocatalytic nitrogen reduction reaction(eNRR),in which Au NPs with ...A gold catalyst of Au/pyrenyl‑graphdiyne(Pyr‑GDY)was prepared by anchoring small size of gold nanoparticles(Au NPs)on the surface of Pyr‑GDY for electrocatalytic nitrogen reduction reaction(eNRR),in which Au NPs with a size of approximately 3.69 nm was evenly distributed on spongy‑like porous Pyr‑GDY.The catalyst exhibited a good electrocatalytic activity for N_(2)reduction in a nitrogen‑saturated electrolyte,with an ammonia yield of 32.1μg·h^(-1)·mg_(cat)^(-1)at-0.3 V(vs RHE),3.5 times higher than that of Au/C(Au NPs anchored on carbon black).In addition,Au/Pyr‑GDY showed a Faraday efficiency(FE)of 26.9%for eNRR,and a good catalysis durability for over 22 h.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
Iron oxide supported Au nanomaterials are one of the most studied catalysts for low-temperature CO oxidation.Catalytic performance not only critically depends on the size of the supported Au nanoparticles(NPs)but also...Iron oxide supported Au nanomaterials are one of the most studied catalysts for low-temperature CO oxidation.Catalytic performance not only critically depends on the size of the supported Au nanoparticles(NPs)but also strongly on the chemical nature of the iron oxide.In this study,Au NPs supported on iron oxide nanorods with different surface properties throughβ-FeOOH annealing,at varying temperatures,were synthesized,and applied in the CO oxidation.Detailed characterizations of the interactions between Au NPs and iron oxides were obtained by X-ray diffraction,transmission electron microscopy(TEM),and X-ray photoelectron spectroscopy.The results indicate that the surface hydroxyl group on the Au/FeOOH catalyst,before calcination(Au/FeOOH-fresh),could facilitate the oxygen adsorption and dissociation on positively charged Au,thereby contributing to the low-temperature CO oxidation reactivity.After calcination at 200℃,under air exposure,the chemical state of the supported Au NP on varied iron oxides partly changed from metal cation to Au0,along with the disappearance of the surface OH species.Au/FeOOH with the highest Au0 content exhibits the highest activity in CO oxidation,among the as-synthesized catalysts.Furthermore,good durability in CO oxidation was achieved over the Au/FeOOH catalyst for 12 h without observable deactivation.In addition,the advanced identical-location TEM method was applied to the gas phase reaction to probe the structure evolution of the Au/iron oxide series of the catalysts and support structure.A Au NP size-dependent Ostwald ripening process mediated by the transport of Au(CO)x mobile species under certain reaction conditions is proposed,which offers a new insight into the validity of the structure-performance relationship.展开更多
Chemical modification(CM)and deposition-precipitation(DP)methods were used for the dispersion of active Au nanoparticles on mesoporous silica materials in this work.XRD,TEM,N2 adsorption isotherms and UV-Vis absorptio...Chemical modification(CM)and deposition-precipitation(DP)methods were used for the dispersion of active Au nanoparticles on mesoporous silica materials in this work.XRD,TEM,N2 adsorption isotherms and UV-Vis absorption spectra were used to characterize in detail Au-SBA-15 materials prepared by the two methods. The analysis results showed that high loading(1.7%,by mass)and uniform Au nanoparticles(approximately 3 nm) were dispersed in the channels of mesoporous SBA-15 by the CM method.While for the DP method,most of Au nanoparticles with the size of 10—15nm were aggregated outside of the channels of SBA-15 and the actual loading of Au was only 0.38%(by mass).展开更多
The BiOCl(BOC)synthesized by the water bath heating method was treated with sodium borohydride(NaBH_(4))to introduce oxygen vacancies(OVs).At the same time,Au nanoparticles were loaded to prepare a series of Au/BiOCl ...The BiOCl(BOC)synthesized by the water bath heating method was treated with sodium borohydride(NaBH_(4))to introduce oxygen vacancies(OVs).At the same time,Au nanoparticles were loaded to prepare a series of Au/BiOCl samples with different ratios.OVs and Au nanoparticles can promote the light absorption of host photocatalyst in the visible region.The calculated work function of BiOCl and Au can verify the existence of Ohmic contact between the interface of them,which is conducive to the separation of charge carriers.Through a series of photoelectric tests,it was verified experimentally that the separation of charge carriers is indeed enhanced.The high-energy hot electrons produced by Au under the surface plasmon resonance(SPR)effect can increase the counts of electrons to participate in the CO_(2)reduction reaction.Especially for 1.0%-Au/BOC,the yields of CO can reach 43.16μmol g^(−1)h^(−1),which is 6.6 times more than that of BOC.Therefore,loading precious metal on semiconductors is an effective strategy to promote the photocatalytic performance of CO_(2)reduction reactions.展开更多
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
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
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 capped by hexadecanethiol and dodecanethiol were chemically synthesized. The characteristics of electrical conductivity for the capped nanoparticles dissolved in chloroform and toluene solvents were i...Au nanoparticles capped by hexadecanethiol and dodecanethiol were chemically synthesized. The characteristics of electrical conductivity for the capped nanoparticles dissolved in chloroform and toluene solvents were investigated. The electrical conductivity of the samples is conspicuously Au nanoparticle concentration dependent. The results show that a rapid conductivity increases when the nanoparticle concentration increases from low value to a moderate value of 5.47 g/L and 11.22 g/L, which is capped by hexadecanethiol and dodecanethiol in chloroform solvent, and 2.77 g/L and 7.88 g/L in toluene solvent. The room-temperature dc conductivity σ dc of Au nanoparticle capped by hexadecanethiol is smaller than that capped by dodecanethiol in the whole range of Au nanoparticle concentrations. The conductivity of Au nanoparticle suspensions increases almost linearly in the temperature range in above two solvents.展开更多
The Au nanoparticles decorated graphene（AuNPs@Gr）/nickel foam（Gr/NiF） nanocomposite（AuNPs@Gr/NiF） was prepared by chemical vapor deposition followed by electrophoretic deposition of AuNPs on Gr/NiF. The morpholo...The Au nanoparticles decorated graphene（AuNPs@Gr）/nickel foam（Gr/NiF） nanocomposite（AuNPs@Gr/NiF） was prepared by chemical vapor deposition followed by electrophoretic deposition of AuNPs on Gr/NiF. The morphology, microstructure and sensing performance of the as-prepared AuNPs@Gr/NiF nanocomposite were characterized and measured, respectively by scanning electron microscope, transmission electron microscope, ultraviolet visible spectroscopy and chemical workstation. The asprepared AuNPs@Gr/NiF nanocomposite was used as the electrode to construct a chemical sensor for the detection of hydrogen peroxide（H2O2）. The results showed that the AuNPs distributed homogenously and stably on the surface of Gr/NiF. The chemical sensor exhibits a sensitive and selective performance to the detection of H2O2.展开更多
A remarkable solvent effect in a single-phase synthesis of monodisperse amine-capped Au nanoparticles is demonstrated.Oleylamine-capped Au nanoparticles were prepared via the reduction of HAuCU by an amine-borane comp...A remarkable solvent effect in a single-phase synthesis of monodisperse amine-capped Au nanoparticles is demonstrated.Oleylamine-capped Au nanoparticles were prepared via the reduction of HAuCU by an amine-borane complex in the presence of oleylamine in an organic solvent.When linear or planar hydrocarbon（e.g.,n-hexane,n-octane,1-octadecylene,benzene,and toluene） was used as the solvent, high-quality monodisperse Au nanoparticles with tunable sizes were obtained.However,Au nanoparticles with poor size dispersity were obtained when tetralin,chloroform or cyclohexane was used as the solvent.The revealed solvent effect allows the controlled synthesis of monodisperse Au nanoparticles with tunable size of 3-10 nm.展开更多
Gold nanoparticles(Au NPs)are nanoscale sources of light and electrons,which are highly relevant for their extensive applications in the field of photocatalysis.Although a number of research works have been carried ou...Gold nanoparticles(Au NPs)are nanoscale sources of light and electrons,which are highly relevant for their extensive applications in the field of photocatalysis.Although a number of research works have been carried out on chemical reactions accelerated by the energetic hot electrons/holes,the possibility of reaction pathway change on the plasmonic Au surfaces has not been reported so far.In this proof-ofconcept study,we find that Au NPs change the reaction pathway in photooxidation of alkyne under visible light irradiation.This reaction produces benzil(—CO—CO—)without the presence of Au NPs.In contrast,as indicated by surface-enhanced Raman spectroscopic(SERS)results,the C—C triple bonds(—C≡C—)adsorbed on Au NPs are converted into carboxyl(—COOH)and acyl chloride(—COCl)groups.The plasmonic Au NPs not only provide energetic charge carriers but also activate the reactant molecules as conventional heterogeneous catalysts.This study discloses the second role of plasmonic NPs in photocatalysis and bridges the gap between plasmon-driven and conventional heterogeneous catalysis.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
We report the hierarchical assembly of Au nanoparticles on carboxylized carbon nanotubes（c-CNTs）through Cu^（2＋） coordination. This route is facile and green, and can easily control the loading density of Au nanop...We report the hierarchical assembly of Au nanoparticles on carboxylized carbon nanotubes（c-CNTs）through Cu^（2＋） coordination. This route is facile and green, and can easily control the loading density of Au nanoparticles. The c-CNT matrix ensures uniform distribution of Au nanoparticles, which is particularly important for the enrichment of hot spots while preventing their serious agglomeration. Moreover, the cCNT matrix also contributes to the electromagnetic enhancement due to its surface plasmon resonance,and the chemical enhancement due to the adsorption of the target molecules. The resulting Au@c-CNT nanohybrids exhibit a remarkable synergy in SERS compared to neat Au nanoparticles.展开更多
To facilitate real-time monitoring and recording of humidity in the environment and to satisfy the requirement for strain performance in certain applications(such as wearable devices),this paper proposes an in-situ me...To facilitate real-time monitoring and recording of humidity in the environment and to satisfy the requirement for strain performance in certain applications(such as wearable devices),this paper proposes an in-situ method for synthesising Au nanoparticles on ZIF-67.In this study,an Au@ZIF-67 composite humidity-sensitive material was combined with flexible polyethylene terephthalate interdigitated electrodes to create an Au@ZIF-67 flexible humidity sensor.The prepared samples were characterised using X-ray diffraction,X-ray photoelectron spectroscopy,and transmission electron microscopy.The humidity-sensitive properties of the sensor were investigated,and its monitoring capabilities in applications involving respiration,gestures,skin,and baby diapers were tested.The experimental results indicate that compared with a pure ZIF-67 humidity sensor,the Au@ZIF-67(0.1Au@Z)flexible humidity sensor exhibits a 158.07%decrease in baseline resistance and a 51.66%increase in sensitivity to 95%relative humidity,and the hysteresis,response time,and recovery time are significantly reduced.Furthermore,the sensor exhibits excellent characteristics such as high resolution,repeatability,and stability.The obtained results regarding the material properties,humidity sensitivity,and practical application of non-contact humidity monitoring demonstrate that the prepared sensors exhibit excellent and comprehensive performance,indicating their broad prospects in wearable medical devices,wireless Internet of Things,humidity detection in complex environments,and intelligent integrated systems.展开更多
文摘A gold catalyst of Au/pyrenyl‑graphdiyne(Pyr‑GDY)was prepared by anchoring small size of gold nanoparticles(Au NPs)on the surface of Pyr‑GDY for electrocatalytic nitrogen reduction reaction(eNRR),in which Au NPs with a size of approximately 3.69 nm was evenly distributed on spongy‑like porous Pyr‑GDY.The catalyst exhibited a good electrocatalytic activity for N_(2)reduction in a nitrogen‑saturated electrolyte,with an ammonia yield of 32.1μg·h^(-1)·mg_(cat)^(-1)at-0.3 V(vs RHE),3.5 times higher than that of Au/C(Au NPs anchored on carbon black).In addition,Au/Pyr‑GDY showed a Faraday efficiency(FE)of 26.9%for eNRR,and a good catalysis durability for over 22 h.
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 Natural Science Foundation of China(21773269,21761132025,91545119,21703262)the Youth Innovation Promotion Association CAS(2015152)+1 种基金the Joint Foundation of Liaoning Province Natural Science FoundationShenyang National Laboratory for Materials Science(20180510047)~~
文摘Iron oxide supported Au nanomaterials are one of the most studied catalysts for low-temperature CO oxidation.Catalytic performance not only critically depends on the size of the supported Au nanoparticles(NPs)but also strongly on the chemical nature of the iron oxide.In this study,Au NPs supported on iron oxide nanorods with different surface properties throughβ-FeOOH annealing,at varying temperatures,were synthesized,and applied in the CO oxidation.Detailed characterizations of the interactions between Au NPs and iron oxides were obtained by X-ray diffraction,transmission electron microscopy(TEM),and X-ray photoelectron spectroscopy.The results indicate that the surface hydroxyl group on the Au/FeOOH catalyst,before calcination(Au/FeOOH-fresh),could facilitate the oxygen adsorption and dissociation on positively charged Au,thereby contributing to the low-temperature CO oxidation reactivity.After calcination at 200℃,under air exposure,the chemical state of the supported Au NP on varied iron oxides partly changed from metal cation to Au0,along with the disappearance of the surface OH species.Au/FeOOH with the highest Au0 content exhibits the highest activity in CO oxidation,among the as-synthesized catalysts.Furthermore,good durability in CO oxidation was achieved over the Au/FeOOH catalyst for 12 h without observable deactivation.In addition,the advanced identical-location TEM method was applied to the gas phase reaction to probe the structure evolution of the Au/iron oxide series of the catalysts and support structure.A Au NP size-dependent Ostwald ripening process mediated by the transport of Au(CO)x mobile species under certain reaction conditions is proposed,which offers a new insight into the validity of the structure-performance relationship.
基金Supported by the National Natural Science Foundation of China （No.20490204）, Shanghai Municipal Science and Technology Commission of China （No.05DJ 14002） and Shanghai Municipal Education Commission of China.
文摘Chemical modification(CM)and deposition-precipitation(DP)methods were used for the dispersion of active Au nanoparticles on mesoporous silica materials in this work.XRD,TEM,N2 adsorption isotherms and UV-Vis absorption spectra were used to characterize in detail Au-SBA-15 materials prepared by the two methods. The analysis results showed that high loading(1.7%,by mass)and uniform Au nanoparticles(approximately 3 nm) were dispersed in the channels of mesoporous SBA-15 by the CM method.While for the DP method,most of Au nanoparticles with the size of 10—15nm were aggregated outside of the channels of SBA-15 and the actual loading of Au was only 0.38%(by mass).
基金supported by the National Natural Science Foundation of China(Nos.51772183.52072230)the Yulin Science and Technology Project(No.CXY-2020-040)。
文摘The BiOCl(BOC)synthesized by the water bath heating method was treated with sodium borohydride(NaBH_(4))to introduce oxygen vacancies(OVs).At the same time,Au nanoparticles were loaded to prepare a series of Au/BiOCl samples with different ratios.OVs and Au nanoparticles can promote the light absorption of host photocatalyst in the visible region.The calculated work function of BiOCl and Au can verify the existence of Ohmic contact between the interface of them,which is conducive to the separation of charge carriers.Through a series of photoelectric tests,it was verified experimentally that the separation of charge carriers is indeed enhanced.The high-energy hot electrons produced by Au under the surface plasmon resonance(SPR)effect can increase the counts of electrons to participate in the CO_(2)reduction reaction.Especially for 1.0%-Au/BOC,the yields of CO can reach 43.16μmol g^(−1)h^(−1),which is 6.6 times more than that of BOC.Therefore,loading precious metal on semiconductors is an effective strategy to promote the photocatalytic performance of CO_(2)reduction reactions.
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 (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Youth Research F oundation fromShanghai Jiaotong U niv. and the Special Foundation for Cross-field Innovation Research Group from Shanghai Science Council
文摘Au nanoparticles capped by hexadecanethiol and dodecanethiol were chemically synthesized. The characteristics of electrical conductivity for the capped nanoparticles dissolved in chloroform and toluene solvents were investigated. The electrical conductivity of the samples is conspicuously Au nanoparticle concentration dependent. The results show that a rapid conductivity increases when the nanoparticle concentration increases from low value to a moderate value of 5.47 g/L and 11.22 g/L, which is capped by hexadecanethiol and dodecanethiol in chloroform solvent, and 2.77 g/L and 7.88 g/L in toluene solvent. The room-temperature dc conductivity σ dc of Au nanoparticle capped by hexadecanethiol is smaller than that capped by dodecanethiol in the whole range of Au nanoparticle concentrations. The conductivity of Au nanoparticle suspensions increases almost linearly in the temperature range in above two solvents.
基金supports by the National Natural Science Foundation of China (21173041 and 11472080)the Natural Science Foundation of Jiangsu Province of China (BK20141336)+1 种基金the Opening Project of SEU-JSRI Joint Research Center for the Applica-tion of Advanced Carbon Materials, Chinathe Opening Project of Jiangsu Key Laboratory of Advanced Metallic Materials, China
文摘The Au nanoparticles decorated graphene（AuNPs@Gr）/nickel foam（Gr/NiF） nanocomposite（AuNPs@Gr/NiF） was prepared by chemical vapor deposition followed by electrophoretic deposition of AuNPs on Gr/NiF. The morphology, microstructure and sensing performance of the as-prepared AuNPs@Gr/NiF nanocomposite were characterized and measured, respectively by scanning electron microscope, transmission electron microscope, ultraviolet visible spectroscopy and chemical workstation. The asprepared AuNPs@Gr/NiF nanocomposite was used as the electrode to construct a chemical sensor for the detection of hydrogen peroxide（H2O2）. The results showed that the AuNPs distributed homogenously and stably on the surface of Gr/NiF. The chemical sensor exhibits a sensitive and selective performance to the detection of H2O2.
基金the MOST of China(Nos.2011CB932403, 2009CB930703)the NSFC(Nos.21131005,21021061, 20925103,20923004)the Fok Ying Tung Education Foundation (No.121011) for the financial support
文摘A remarkable solvent effect in a single-phase synthesis of monodisperse amine-capped Au nanoparticles is demonstrated.Oleylamine-capped Au nanoparticles were prepared via the reduction of HAuCU by an amine-borane complex in the presence of oleylamine in an organic solvent.When linear or planar hydrocarbon（e.g.,n-hexane,n-octane,1-octadecylene,benzene,and toluene） was used as the solvent, high-quality monodisperse Au nanoparticles with tunable sizes were obtained.However,Au nanoparticles with poor size dispersity were obtained when tetralin,chloroform or cyclohexane was used as the solvent.The revealed solvent effect allows the controlled synthesis of monodisperse Au nanoparticles with tunable size of 3-10 nm.
基金supported by the National Natural Science Foundation of China(Nos.22022406,21861132016 and 21775074)the Natural Science Foundation of Tianjin(Nos.20JCJQJC00110 and 20JCYBJC00590)+2 种基金the Fundamental Research Funds for the Central Universities-Nankai University(No.000082)the 111 project(No.B12015)the National Key R&D Program(Nos.2017YFA0206702 and 2016YFB0901502)。
文摘Gold nanoparticles(Au NPs)are nanoscale sources of light and electrons,which are highly relevant for their extensive applications in the field of photocatalysis.Although a number of research works have been carried out on chemical reactions accelerated by the energetic hot electrons/holes,the possibility of reaction pathway change on the plasmonic Au surfaces has not been reported so far.In this proof-ofconcept study,we find that Au NPs change the reaction pathway in photooxidation of alkyne under visible light irradiation.This reaction produces benzil(—CO—CO—)without the presence of Au NPs.In contrast,as indicated by surface-enhanced Raman spectroscopic(SERS)results,the C—C triple bonds(—C≡C—)adsorbed on Au NPs are converted into carboxyl(—COOH)and acyl chloride(—COCl)groups.The plasmonic Au NPs not only provide energetic charge carriers but also activate the reactant molecules as conventional heterogeneous catalysts.This study discloses the second role of plasmonic NPs in photocatalysis and bridges the gap between plasmon-driven and conventional heterogeneous catalysis.
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financially supported by the National Natural Science Foundation of China(No.21474058)
文摘We report the hierarchical assembly of Au nanoparticles on carboxylized carbon nanotubes（c-CNTs）through Cu^（2＋） coordination. This route is facile and green, and can easily control the loading density of Au nanoparticles. The c-CNT matrix ensures uniform distribution of Au nanoparticles, which is particularly important for the enrichment of hot spots while preventing their serious agglomeration. Moreover, the cCNT matrix also contributes to the electromagnetic enhancement due to its surface plasmon resonance,and the chemical enhancement due to the adsorption of the target molecules. The resulting Au@c-CNT nanohybrids exhibit a remarkable synergy in SERS compared to neat Au nanoparticles.
基金supported by the Natural Science Project of Zhengzhou Science and Technology Bureau(No.21ZZXTCX12)the Key Research and Development Program of Henan Province(No.221111220300)+1 种基金the Key Program of the National Natural Science Foundation of China(No.62333013)the Youth Backbone Teacher Training Program of Henan University of Technology(No.21420154).
文摘To facilitate real-time monitoring and recording of humidity in the environment and to satisfy the requirement for strain performance in certain applications(such as wearable devices),this paper proposes an in-situ method for synthesising Au nanoparticles on ZIF-67.In this study,an Au@ZIF-67 composite humidity-sensitive material was combined with flexible polyethylene terephthalate interdigitated electrodes to create an Au@ZIF-67 flexible humidity sensor.The prepared samples were characterised using X-ray diffraction,X-ray photoelectron spectroscopy,and transmission electron microscopy.The humidity-sensitive properties of the sensor were investigated,and its monitoring capabilities in applications involving respiration,gestures,skin,and baby diapers were tested.The experimental results indicate that compared with a pure ZIF-67 humidity sensor,the Au@ZIF-67(0.1Au@Z)flexible humidity sensor exhibits a 158.07%decrease in baseline resistance and a 51.66%increase in sensitivity to 95%relative humidity,and the hysteresis,response time,and recovery time are significantly reduced.Furthermore,the sensor exhibits excellent characteristics such as high resolution,repeatability,and stability.The obtained results regarding the material properties,humidity sensitivity,and practical application of non-contact humidity monitoring demonstrate that the prepared sensors exhibit excellent and comprehensive performance,indicating their broad prospects in wearable medical devices,wireless Internet of Things,humidity detection in complex environments,and intelligent integrated systems.
