Realizing the hydrogen economy by water electrolysis is an attractive approach for hydrogen production,while the efficient and stable bifunctional catalysts under high current densities are the bottleneck that limits ...Realizing the hydrogen economy by water electrolysis is an attractive approach for hydrogen production,while the efficient and stable bifunctional catalysts under high current densities are the bottleneck that limits the half-cell reactions of water splitting.Here,we propose an approach of hydrothermal and thermal annealing methods for robust MoO_(2)/MoNi_(4)@Ru/RuO_(2) heterogeneous cuboid array electrocatalyst with multiplying surface-active sites by depositing a monolayer amount of Ru.Benefiting from abundant MoO_(2)/MoNi_(4)@Ru/RuO_(2)heterointerfaces,MoO_(2)/MoNi_(4)@Ru/RuO_(2) heterogeneous cuboid array electrocatalysts effectively drive the alkaline water splitting with superior hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)performances.The synthesized MoO_(2)/MoNi_(4)@Ru/RuO_(2) has high HER activity,which realizes the working overpotentials of 48 mV at 50 mA·cm^(-2),further achieving overpotentials of 230 mv for industry-level 1000 mA·cm^(-2) in alkaline water electrolysis.Moreover,it also showed an enhanced OER activity than commercial RuO_(2) with a small overpotential of 280 mV at 200 mA·cm^(-2) in alkaline media.When building an electrolyzer with electrodes of(-)MoO_(2)/MoNi_(4)@Ru/RuO_(2)IIMo02/MoNig@Ru/RuO_(2)(+),a cell voltage of 1.63 V and 1.75 V is just required to support the current density of 200 mA·cm^(-2) and 500 mA-cm^(-2) in alkaline water electrolysis,much lower than that of the electrolyzer of(-)Pt/CIIRuO_(2)(+).This work demonstrates that MoO_(2)/MoNig@Ru/RuO_(2) heterogeneous nanosheet arrays are promising candidates for industrial water electrolysis applications,providing a possibility for the exploration of water electrolysis with a large currentdensity.展开更多
Urea and oxalic acid are critical component in various chemical manufacturing industries.However,achieving simultaneous generation of urea and oxalic acid in a continuous-flow electrolyzer is a challenge.Herein,we rep...Urea and oxalic acid are critical component in various chemical manufacturing industries.However,achieving simultaneous generation of urea and oxalic acid in a continuous-flow electrolyzer is a challenge.Herein,we report a continuous-flow electrolyzer equipped with 9-square centime-ter-effective area gas diffusion electrodes(GDE)which can simultaneously catalyze the glycerol oxidation reaction in the anode region and the reduction reaction of CO_(2) and nitrate in the cathode region,producing oxalic acid and urea at both the anode and cathode,respectively.The current density at low cell voltage(0.9 V)remained above 18.7 mA cm^(-2) for 10 consecutive electrolysis cycles(120 h in total),and the Faraday efficiency of oxalic acid(67.1%) and urea(70.9%)did not decay.Experimental and theoretical studies show that in terms of the formation of C-N bond at the cathode,Pd-sites can provide protons for the hydrogenation process of CO_(2) and NO_(3)^(-),Cu-sites can promote the generation of *COOH and Bi-sites can stabilize *COOH.In addition,in terms of glycerol oxidation,the introduction of Cu and Bi into Pd metallene promotes the oxidation of hydroxyl groups and the cleavage of C-C bond in glycerol molecules,respectively.展开更多
The electrolysis of water powered by renewable energy sources offers a promising method of"green hydrogen"production,which is considered to be at the heart of future carbon-neutral energy systems.In the past...The electrolysis of water powered by renewable energy sources offers a promising method of"green hydrogen"production,which is considered to be at the heart of future carbon-neutral energy systems.In the past decades,researchers have reported a number of hydrogen evolution reaction(HER)electrocatalysts with activity comparable to that of commercial Pt/C,but most of them are tested within a small current density range,typically no more than 500 mA cm^(-2).To realize the industrial application of hydrogen production from water electrolysis,it is essential to develop high-efficiency HER electrocatalysts at high current density(HCD≥500 mA cm^(-2)).Nevertheless,it remains challenging and significant to rational design HCD electrocatalysts for HER.In this paper,the design strategy of HCD electrocatalysts is discussed,and some HCD electrocatalysts for HER are reviewed in seven categories(alloy,metal oxide,metal hydroxide,metal sulfide/selenide,metal nitride,metal phosphide and other derived electrocatalysts).At the end of this article,we also pro-pose some viewpoints and prospects for the future development and research directions of HCD electrocatalysts for HER.展开更多
BiOBr/ZnO composite photocatalysts were prepared by a simple hydrothermal method. The as-prepared samples were characterized by X-ray diffraction(XRD), scanning electron microscopy(SEM), transmission electron microsco...BiOBr/ZnO composite photocatalysts were prepared by a simple hydrothermal method. The as-prepared samples were characterized by X-ray diffraction(XRD), scanning electron microscopy(SEM), transmission electron microscopy(TEM), high-resolution transmission electron microscopy(HRTEM), UV–Vis diffusion reflectance spectroscopy(DRS) and photoluminescence(PL) spectroscopy, respectively. The photocatalytic activities were evaluated by the degradation of methyl blue(MB) under the simulated sunlight irradiation. Among all the samples, the BiOBr/ZnO composite with a mole ratio of 3:1(Bi:Zn) exhibited the best photocatalytic activity. The improvement of photocatalytic activity was mainly attributed to the low recombination ratio of photo-induced electron-hole pairs. The possible photocatalytic mechanism was discussed on the basis of the band structures of BiOBr and ZnO.展开更多
Direct electrochemical reduction ofp-nitrophenol (PNP) was investigated on a room temperature ionic liquid N-butylpyridinium hexafluorophosphate (BPPF6) modified carbon paste electrode (CILE). The cathodic peak ...Direct electrochemical reduction ofp-nitrophenol (PNP) was investigated on a room temperature ionic liquid N-butylpyridinium hexafluorophosphate (BPPF6) modified carbon paste electrode (CILE). The cathodic peak potential was positively shifted and the peak currents were increased compared to that obtained on traditional carbon paste electrode (CPE). The results indicated that the presence of ionic liquid BPPF6 on the electrode surface showed excellent catalytic ability to the electrochemical reduction of PNP. The electrochemical behaviors of PNP on the CILE were investigated by cyclic voltammetry and the conditions such as the scan rate, the buffer pH, the substrate concentration were optimized. The electrochemical parameters were further calculated with the results of the electron transfer number (n), the charge-transfer coefficient (α) and the surface concentration (Гr) as 1.76, 0.37 and 2.47 × 10^-9 mol/cm^2, respectively, for the selected reductive peak. The results indicated that PNP showed an irreversible adsorption-controlled electrode process on the CILE.展开更多
Among the sustainable energy sources,hydrogen is the one most promising for alleviating the pollution issues related to the usage of conventional fuels,as it can be produced in an efficient and eco-friendly way via el...Among the sustainable energy sources,hydrogen is the one most promising for alleviating the pollution issues related to the usage of conventional fuels,as it can be produced in an efficient and eco-friendly way via electrocatalytic water splitting.The hydrogen evolution reaction(HER,a half-reaction of water splitting)plays a pivotal role in decreasing the price and increasing the catalytic efficiency of hydrogen production and is efficiently promoted by metal phosphides in different electrolytes.Herein,we summarize the recent advances in the development of metal phosphides as HER electrocatalysts,focus on their synthesis(post-treatment,in situ generation,and electrodeposition methods)and the enhancement of their electrocatalytic activity(via elemental doping,interface and vacancy engineering,construction of specific supports and nanostructures,and the design of bior polymetallic phosphides),and highlight the crucial issues and challenges of future development.展开更多
The hydrogen energy generated by the electrocatalytic water splitting reaction has been established as a renewable and clean energy carrier with ultra-high energy density,which can well make up for shortcomings of con...The hydrogen energy generated by the electrocatalytic water splitting reaction has been established as a renewable and clean energy carrier with ultra-high energy density,which can well make up for shortcomings of conventional renewable energy sources,such as geographical limitations,climatic depen-dence,and energy wastage.Notably,the introduction of electrocatalysts can enhance the efficiency of the water splitting process to generate hydrogen.Particularly,the heterostructure electrocatalysts constructed by coupling mul-tiple components(or phases)have emerged as the most promising option for water splitting due to the well-known electronic and synergistic effects.The existing reviews on interface engineering for electrocatalyst design mostly focus on the relationship between the heterostructures and specific electrocatalytic reactions.However,a comprehensive overview of the integra-tion of model building,directional synthesis,and electrocatalytic mechanism has been rarely reported.To this end,in this review,the development of heterostructure catalysts is systematically introduced from the perspective of interface classification,interface growth and synthesis,and regulation of electrocatalytic performance based on the interfacial microenvironment(bonding,electronic configuration,lattice strain,etc.),thereby offering useful insights on the design and construction of interfacial models.Besides,com-bined with the current development and applications of interface engineering strategies,the challenges of future heterostructure catalysts are discussed and relevant solutions are proposed.Overall,this review can serve as a useful theo-retical reference for the integration of interfacial model building,directional synthesis,and electrocatalytic mechanism,which can further promote the development of hydrogen production technologies with low energy consump-tion and high yield.展开更多
To accelerate the kinetics of the oxygen reduction reaction(ORR)in proton exchange membrane fuel cells,ultrafine Pt nanoparticles modified with trace amounts of cobalt were fabricated and decorated on carbon black thr...To accelerate the kinetics of the oxygen reduction reaction(ORR)in proton exchange membrane fuel cells,ultrafine Pt nanoparticles modified with trace amounts of cobalt were fabricated and decorated on carbon black through a strategy involving modified glycol reduction and chemical etching.The obtained Pt36Co/C catalyst exhibits a much larger electrochemical surface area(ECSA)and an improved ORR electrocatalytic activity compared to commercial Pt/C.Moreover,an electrode prepared with Pt36Co/C was further evaluated under H2-air single cell test conditions,and exhibited a maximum specific power density of 10.27 W mgPt^-1,which is 1.61 times higher than that of a conventional Pt/C electrode and also competitive with most state-of-the-art Pt-based architectures.In addition,the changes in ECSA,power density,and reacting resistance during the accelerated degradation process further demonstrate the enhanced durability of the Pt36Co/C electrode.The superior performance observed in this work can be attributed to the synergy between the ultrasmall size and homogeneous distribution of catalyst nanoparticles,bimetallic ligand and electronic effects,and the dissolution of unstable Co with the rearrangement of surface structure brought about by acid etching.Furthermore,the accessible raw materials and simplified operating procedures involved in the fabrication process would result in great cost-effectiveness for practical applications of PEMFCs.展开更多
Three-dimensional(3D)ordered porous carbon is generally believed to be a promising electromagnetic wave(EMW)absorbing material.However,most research works targeted performance improvement of 3D ordered porous carbon,a...Three-dimensional(3D)ordered porous carbon is generally believed to be a promising electromagnetic wave(EMW)absorbing material.However,most research works targeted performance improvement of 3D ordered porous carbon,and the specific attenuation mechanism is still ambiguous.Therefore,in this work,a novel ultra-light egg-derived porous carbon foam(EDCF)structure has been successfully constructed by a simple carbonization combined with the silica microsphere template-etching process.Based on an equivalent substitute strategy,the influence of pore volume and specific surface area on the electromagnetic parameters and EMW absorption properties of the EDCF products was confirmed respectively by adjusting the addition content and diameter of silica microspheres.As a primary attenuation mode,the dielectric loss originates from the comprehensive effect of conduction loss and polarization loss in S-band and C band,and the value is dominated by polarization loss in X band and Ku band,which is obviously greater than that of conduction loss.Furthermore,in all samples,the largest effective absorption bandwidth of EDCF-3 is 7.12 GHz under the thickness of 2.13 mm with the filling content of approximately 5 wt%,covering the whole Ku band.Meanwhile,the EDCF-7 sample with optimized pore volume and specific surface area achieves minimum reflection loss(RL_(min))of−58.08 dB at 16.86 GHz while the thickness is 1.27 mm.The outstanding research results not only provide a novel insight into enhancement of EMW absorption properties but also clarify the dominant dissipation mechanism for the porous carbon-based absorber from the perspective of objective experiments.展开更多
The seawater desalination based on solardriven interfacial evaporation has emerged as a promising technique to alleviate the global crisis on freshwater shortage.However,achieving high desalination performance on actu...The seawater desalination based on solardriven interfacial evaporation has emerged as a promising technique to alleviate the global crisis on freshwater shortage.However,achieving high desalination performance on actual,oil-contaminated seawater remains a critical challenge,because the transport channels and evaporation interfaces of the current solar evaporators are easily blocked by the oil slicks,resulting in undermined evaporation rate and conversion efficiency.Herein,we propose a facile strategy for fabricating a modularized solar evaporator based on flexible MXene aerogels with arbitrarily tunable,highly ordered cellular/lamellar pore structures for high-efficiency oil interception and desalination.The core design is the creation of 1D fibrous MXenes with sufficiently large aspect ratios,whose superior flexibility and plentiful link forms lay the basis for controllable 3D assembly into more complicated pore structures.The cellular pore structure is responsible for effective contaminants rejection due to the multi-sieving effect achieved by the omnipresent,isotropic wall apertures together with underwater superhydrophobicity,while the lamellar pore structure is favorable for rapid evaporation due to the presence of continuous,large-area evaporation channels.The modularized solar evaporator delivers the best evaporation rate(1.48 kg m-2h-1)and conversion efficiency(92.08%)among all MXene-based desalination materials on oil-contaminated seawater.展开更多
Coordination engineering can enhance the activity and stability of the catalyst in heterogeneous catalysis.However,the axial coordination engineering between different groups on the carbon carrier and molecular cataly...Coordination engineering can enhance the activity and stability of the catalyst in heterogeneous catalysis.However,the axial coordination engineering between different groups on the carbon carrier and molecular catalysts in the electrocatalytic carbon dioxide reduction reaction(CO_(2)RR)has been studied rarely.Through coordination engineering strategy,a series of amino(NH_(2)),hydroxyl(OH),and carboxyl(COOH)groups functionalized carbon nanotubes(CNT)immobilized cobalt phthalocyanine(CoPc)catalysts are designed.Compared with no groups,OH groups and COOH groups,NH_(2)groups can effectively change the coordination environment of the central metal Co,thereby significantly increasing the turnover frequency(TOF)(31.4 s^(-1)at-0.6 V vs.RHE,CoPc/NH_(2)-CNT>CoPc/OH-CNT>CoPc/COOH-CN>CoPc/CNT).In the flow cell,the CoPc/NH_(2)-CNT catalyst has high carbon monoxide(CO)selectivity at high current density(~100%at-225 mA·cm^(-2),~96%at-351 mA·cm^(-2)).Importantly,the CoPc/NH_(2)-CNT catalyst can operate stably for 100 h at 225 mA·cm^(-2).Theoretical calculations reveal that CoPc/NH_(2)-CNT catalyst is beneficial to the formation of^(*)COOH and desorption of^(*)CO,thus promoting CO_(2)RR.This work provides an excellent platform for understanding the effect of coordination engineering on electrocatalytic performance and promotes a way to explore efficient and stable catalysts in other applications.展开更多
The purpose of this study is to comparatively investigate the plant uptake, accumulation and translocation behaviors of polycyclic aromatic hydrocarbons (PAHs) as priority pollutants in soil contaminated with oily slu...The purpose of this study is to comparatively investigate the plant uptake, accumulation and translocation behaviors of polycyclic aromatic hydrocarbons (PAHs) as priority pollutants in soil contaminated with oily sludge. The influence of different oily sludge application doses on the uptake of contaminants was studied together with the profile of individual PAH in roots, straws and leaves of winter wheat. Pot experiments were conducted using oily sludge application doses of 0, 5, 10, 15 and 20 percent, respectively. The total PAHs contents of control soil and oily sludge were 16.96 and 3504.66 μg/g, respectively. Analysis for the contents of the 16 PAHs was carried out with a HPLC-UV using plant tissue samples obtained at the 265th day of growth. The total PAHs contents in treated winter wheat were 9.02-334.81 ng/g for roots, 8.45-336.52 ng/g for straws and 10.70-406.32 ng/g for leaves. In addition to 5% of oily sludge dose, the total PAHs content in leaves was always highest under other doses of oily sludge application. With respect to individual PAH, the content did not show a significant plant tissue related trend. However, both the total content and individual content of PAHs in treated winter wheat tissues did increase with increasing oily sludge application dose. Another analysis for the control soil indicates that the degradation rate of PAHs was significantly enhanced by winter wheat after 265 days of growth based on the residual concentrations of PAHs in planted and unplanted soils.展开更多
In this study,Ni_(2)P-Cd_(0.9)Zn_(0.1)S(NPCZS)composites were synthesized by coupling tetrapod bundle Cd_(0.9)Zn_(0.1)S(CZS)and coralline-like Ni_(2)P(NP)via a simple calcination method.CZS shows outstanding activity ...In this study,Ni_(2)P-Cd_(0.9)Zn_(0.1)S(NPCZS)composites were synthesized by coupling tetrapod bundle Cd_(0.9)Zn_(0.1)S(CZS)and coralline-like Ni_(2)P(NP)via a simple calcination method.CZS shows outstanding activity in photocatalytic hydrogen evolution(1.31 mmol h^(‒1)),owing to its unique morphology and heterophase homojunctions(ZB/WZ),which accelerate the separation and transfer of photogenerated charges.After coupling with NP,the photoactivity of NPCZS was enhanced,and the maximum hydrogen evolution rate of 1.88 mmol h^(‒1)was reached at a NP content of 12 wt%,which was 1.43 times higher than that of pure CZS.The experimental results of the photocatalytic activity,viz.photoluminescence spectra,surface photovoltage spectra,and electrochemical test showed that the enhanced photoactivity of NPCZS should be attributed to the synergistic effects of the novel tetrapod-bundle morphology,heterophase homojunctions,and decoration of the NP co-catalyst.Moreover,the as-prepared NPCZS composites exhibited excellent photostability and recyclability.Herein,we propose a possible mechanism for the enhanced photocatalytic activity.展开更多
The Br?nsted-acidic polyether ionic liquids(ILs)with different polymerization degrees(n value)were prepared via the reaction of tetramethylguanidine and epoxy ethane,followed by successive reactions with 1,3-propane s...The Br?nsted-acidic polyether ionic liquids(ILs)with different polymerization degrees(n value)were prepared via the reaction of tetramethylguanidine and epoxy ethane,followed by successive reactions with 1,3-propane sultone and trifluoromethanesulfonic acid(TfOH).The prepared ILs were characterized by infrared spectroscopy and 1H nuclear magnetic resonance spectroscopy,and their thermal stability was determined by thermal gravimetry.The synthesized polyether ILs coupled with TfOH were used to catalyze the alkylation reaction of isobutane and isobutene for the preparation of alkylate gasoline.The polyether ILs could improve the substrate dissolution and promote the separation of the catalyst from the products.The ideal IL(n=94)was determined.The optimized alkylation reaction conditions covered:a VTfOH/VIL ratio of 0.35,a reaction temperature of 40℃,a reaction time of 50 min,and a stirring speed of 800 r/min.The conversion of isobutene was 92.4%and the selectivity for the C8-product was 81.6%.Under optimal conditions,the catalyst life was determined and TfOH showed improved cyclic performance in the polyether ILs.After 8 operating cycles,the catalytic activity of the catalyst showed negligible decline.展开更多
Constructing heterojunction is a promising way to improve the charge transfer efficiency and can thus promote the electrochemical properties.Herein,a facile and effective epitaxial-like growth strategy is applied to N...Constructing heterojunction is a promising way to improve the charge transfer efficiency and can thus promote the electrochemical properties.Herein,a facile and effective epitaxial-like growth strategy is applied to NiSe2 nano-octahe-dra to fabricate the NiSe2-(100)/Ni(OH)2-(110)heterojunction.The heterojunction composite and Ni(OH)2(performing high electrochemical activity)is ideal high-rate battery-type supercapacitor electrode.The NiSe2/Ni(OH)2 electrode exhibits a high specific capacity of 909 C g^-1 at 1 A g^-1 and 597 C g^-1 at 20 A g^-1.The assembled asymmetric supercapacitor composed of the NiSe2/Ni(OH)2 cathode and p-phenylenediamine-functional reduced graphene oxide anode achieves an ultrahigh specific capacity of 303 C g^-1 at 1 A g^-1 and a superior energy density of 76.1 Wh kg^-1 at 906 W kg^-1,as well as an outstanding cycling stability of 82%retention for 8000 cycles at 10 A g^-1.To the best of our knowledge,this is the first example of NiSe2/Ni(OH)2 heterojunction exhibiting such remarkable supercapacitor performance.This work not only provides a promising candidate for next-generation energy storage device but also offers a possible universal strategy to fabricate metal selenides/metal hydroxides heterojunctions.展开更多
A 2 D-2 D titanium dioxide nanosheet-reduced graphene oxide(TNS-r GO)composite with better electronic conductivity and hydrophilicity was prepared by the hydrothermal method.The as-obtained TNS-r GO composite was furt...A 2 D-2 D titanium dioxide nanosheet-reduced graphene oxide(TNS-r GO)composite with better electronic conductivity and hydrophilicity was prepared by the hydrothermal method.The as-obtained TNS-r GO composite was further functionalized with 3-aminopropyltriethoxysilane(APTES)to provide a large amount of-NH2 groups on the surface for anchoring ultrafine Pd Ag alloy nanoparticles with an average particle size of 1.69 nm by a facile wet reduction approach.Benefiting from the combined effects of well-dispersed Pd Ag alloy nanoparticles,facilitated electron transfer from TNS-r GO to Pd,and increased electron density of active sites,the Pd8 Ag_(1)/NH_(2)-TNS-r GO catalyst exhibited excellent activity towards dehydrogenation of formic acid without adding any additives at 298 K,corresponding to an initial turn over frequency as high as 1090 h-1,which is much higher than that of most other state-of-theart catalysts.展开更多
Constructing highly-efficient electrocatalysts toward hydrogen evolution reaction(HER)/oxygen evolution reaction(OER)/oxygen reduction reaction(ORR)with excellent stability is quite important for the development of re...Constructing highly-efficient electrocatalysts toward hydrogen evolution reaction(HER)/oxygen evolution reaction(OER)/oxygen reduction reaction(ORR)with excellent stability is quite important for the development of renewable energy-related applications.Herein,Co-Ru based compounds supported on nitrogen doped two-dimensional(2D)carbon nanosheets(NCN)are developed via one step pyrolysis procedure(Co-Ru/NCN)for HER/ORR and following low-temperature oxidation process(Co-Ru@RuO_(x)/NCN)for OER.The specific 2D morphology guarantees abundant active sites exposure.Furthermore,the synergistic effects arising from the interaction between Co and Ru are crucial in enhancing the catalytic performance.Thus,the resulting Co-Ru/NCN shows remarkable electrocatalytic performance for HER(70 mV at 10 mA cm^(-2))in 1 M KOH and ORR(half-wave potential E_(1/2)=0.81 V)in 0.1 M KOH.Especially,the Co-Ru@RuO_(x)/NCN obtained by oxidation exhibits splendid OER performance in both acid(230 mV at 10 mA cm^(-2))and alkaline media(270 mV at 10 mA cm^(-2))coupled with excellent stability.Consequently,the fabricated two-electrode water-splitting device exhibits excellent performance in both acidic and alkaline environments.This research provides a promising avenue for the advancement of multifunctional nanomaterials.展开更多
Non-noble-metal-based electrocatalysts with superior oxygen reduction reaction(ORR)activity to platinum(Pt)are highly desirable but their fabrications are challenging and thus impeding their applications in metal-air ...Non-noble-metal-based electrocatalysts with superior oxygen reduction reaction(ORR)activity to platinum(Pt)are highly desirable but their fabrications are challenging and thus impeding their applications in metal-air batteries and fuel cells.Here,we report a facile molten salt assisted two-step pyrolysis strategy to construct carbon nanosheets matrix with uniformly dispersed Fe_(3) N/Fe nanoparticles and abundant nitrogen-coordinated Fe single atom moieties(Fe@Fe_(SA)-N-C).Thermal exfoliation and etching effect of molten salt contribute to the formation of carbon nanosheets with high porosity,large surface area and abundant uniformly immobilized active sites.Aberration-corrected high-angle annular dark-field scanning transmission electron microscopy(HAADF-STEM)image,X-ray absorption fine spectroscopy,and X-ray photoelectron spectroscopy indicate the generation of Fe(mainly Fe_(3) N/Fe)and Fe_(SA)-N-C moieties,which account for the catalytic activity for ORR.Further study on modulating the crystal structure and composition of Fe_(3) N/Fe nanoparticles reveals that proper chemical environment of Fe in Fe_(3) N/Fe notably optimizes the ORR activity.Consequently,the presence of abundant Fe_(SA)-N-C moieties,and potential synergies of Fe_(3) N/Fe nanoparticles and carbon shells,markedly promote the reaction kinetics.The as-developed Fe@Fe_(SA)-N-C-900 electrocatalyst displays superior ORR performance with a half-wave potential(E_(1/2))of 0.83 V versus reversible hydrogen electrode(RHE)and a diffusion limited current density of 5.6 mA cm^(-2).In addition,a rechargeable Zn-air battery device assembled by the Fe@Fe_(SA)-N-C-900 possesses remarkably stable performance with a small voltage gap without obvious voltage loss after500 h of operation.The facile synthesis strategy for the high-performance composites represents another viable avenue to stable and low-cost electrocatalysts for ORR catalysis.展开更多
An electrochemical method for the simultaneous detection of two different DNA sequences from PAT and FMV 35S gene sequence using CdS and PbS quantum dots (QDs) as labels was described. The QDs were readily functiona...An electrochemical method for the simultaneous detection of two different DNA sequences from PAT and FMV 35S gene sequence using CdS and PbS quantum dots (QDs) as labels was described. The QDs were readily functionalized with oligonucleotides as electrochemical DNA probes and selectively hybridized to the complementary sequences immobilized on the microplate. The QDs anchored on the hybrids were dissolved in the solution by the oxidation of HNO3 and further detected by a sensitive differential pulse anodic stripping voltammetric method (DPASV). The DPASV signals of the oxidation of Cd^2+ and Pb^2+ ions present in the solution were different and reflected the identity of corresponding ssDNA targets sequences.展开更多
An electrochemical sensor for the detection of the natural double-stranded DNA(dsDNA) damage induced by PbSe quantum dots(QDs) under UV irradiation was developed.The biosensing membranes were prepared by successively ...An electrochemical sensor for the detection of the natural double-stranded DNA(dsDNA) damage induced by PbSe quantum dots(QDs) under UV irradiation was developed.The biosensing membranes were prepared by successively assembling 3- mercaptopropionic acid,polycationic poly(diallyldimethyl ammonium) and dsDNA on the surface of the gold electrode.Damage of dsDNA was fulfilled by immersing the sensing membrane electrode in PbSe QDs suspension and illuminating it with an UV lamp. Cyclic voltammetry was utilized to detect dsDNA damage with Co(phen)_3^(3+) as the electroactive probe.The UV irradiation,Pb^(2+) ions liberated from the PbSe QDs under the UV irradiation and the reactive oxygen species(ROS) generated in the presence of the PbSe QDs also under the UV irradiation were the three factors of inducing the dsDNA damage.The synergistic effect of the three factors might dramatically enhance the damage of dsDNA.This electrochemical sensor provided a simple method for detecting DNA damage,and may be used for investigating the DNA damage induced by other QDs.展开更多
基金sponsored by the National Natural Science Foundation of China(51772162,52072197)the China Postdoctoral Science Foundation(2023M732132)+4 种基金Youth Innovation Team Development Program of Shandong Higher Education Institutions(2022KJ155)Outstanding Youth Foundation of Shandong Province,China(ZR2019JQ14)Taishan Scholar Young Talent Program(tsqn201909114)Major Scientific and Technological Innovation Project(2019JZZY020405)Major Basic Research Program of Natural Science Foundation of Shandong Province under Grant(ZR2020ZD09).
文摘Realizing the hydrogen economy by water electrolysis is an attractive approach for hydrogen production,while the efficient and stable bifunctional catalysts under high current densities are the bottleneck that limits the half-cell reactions of water splitting.Here,we propose an approach of hydrothermal and thermal annealing methods for robust MoO_(2)/MoNi_(4)@Ru/RuO_(2) heterogeneous cuboid array electrocatalyst with multiplying surface-active sites by depositing a monolayer amount of Ru.Benefiting from abundant MoO_(2)/MoNi_(4)@Ru/RuO_(2)heterointerfaces,MoO_(2)/MoNi_(4)@Ru/RuO_(2) heterogeneous cuboid array electrocatalysts effectively drive the alkaline water splitting with superior hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)performances.The synthesized MoO_(2)/MoNi_(4)@Ru/RuO_(2) has high HER activity,which realizes the working overpotentials of 48 mV at 50 mA·cm^(-2),further achieving overpotentials of 230 mv for industry-level 1000 mA·cm^(-2) in alkaline water electrolysis.Moreover,it also showed an enhanced OER activity than commercial RuO_(2) with a small overpotential of 280 mV at 200 mA·cm^(-2) in alkaline media.When building an electrolyzer with electrodes of(-)MoO_(2)/MoNi_(4)@Ru/RuO_(2)IIMo02/MoNig@Ru/RuO_(2)(+),a cell voltage of 1.63 V and 1.75 V is just required to support the current density of 200 mA·cm^(-2) and 500 mA-cm^(-2) in alkaline water electrolysis,much lower than that of the electrolyzer of(-)Pt/CIIRuO_(2)(+).This work demonstrates that MoO_(2)/MoNig@Ru/RuO_(2) heterogeneous nanosheet arrays are promising candidates for industrial water electrolysis applications,providing a possibility for the exploration of water electrolysis with a large currentdensity.
文摘Urea and oxalic acid are critical component in various chemical manufacturing industries.However,achieving simultaneous generation of urea and oxalic acid in a continuous-flow electrolyzer is a challenge.Herein,we report a continuous-flow electrolyzer equipped with 9-square centime-ter-effective area gas diffusion electrodes(GDE)which can simultaneously catalyze the glycerol oxidation reaction in the anode region and the reduction reaction of CO_(2) and nitrate in the cathode region,producing oxalic acid and urea at both the anode and cathode,respectively.The current density at low cell voltage(0.9 V)remained above 18.7 mA cm^(-2) for 10 consecutive electrolysis cycles(120 h in total),and the Faraday efficiency of oxalic acid(67.1%) and urea(70.9%)did not decay.Experimental and theoretical studies show that in terms of the formation of C-N bond at the cathode,Pd-sites can provide protons for the hydrogenation process of CO_(2) and NO_(3)^(-),Cu-sites can promote the generation of *COOH and Bi-sites can stabilize *COOH.In addition,in terms of glycerol oxidation,the introduction of Cu and Bi into Pd metallene promotes the oxidation of hydroxyl groups and the cleavage of C-C bond in glycerol molecules,respectively.
文摘The electrolysis of water powered by renewable energy sources offers a promising method of"green hydrogen"production,which is considered to be at the heart of future carbon-neutral energy systems.In the past decades,researchers have reported a number of hydrogen evolution reaction(HER)electrocatalysts with activity comparable to that of commercial Pt/C,but most of them are tested within a small current density range,typically no more than 500 mA cm^(-2).To realize the industrial application of hydrogen production from water electrolysis,it is essential to develop high-efficiency HER electrocatalysts at high current density(HCD≥500 mA cm^(-2)).Nevertheless,it remains challenging and significant to rational design HCD electrocatalysts for HER.In this paper,the design strategy of HCD electrocatalysts is discussed,and some HCD electrocatalysts for HER are reviewed in seven categories(alloy,metal oxide,metal hydroxide,metal sulfide/selenide,metal nitride,metal phosphide and other derived electrocatalysts).At the end of this article,we also pro-pose some viewpoints and prospects for the future development and research directions of HCD electrocatalysts for HER.
文摘BiOBr/ZnO composite photocatalysts were prepared by a simple hydrothermal method. The as-prepared samples were characterized by X-ray diffraction(XRD), scanning electron microscopy(SEM), transmission electron microscopy(TEM), high-resolution transmission electron microscopy(HRTEM), UV–Vis diffusion reflectance spectroscopy(DRS) and photoluminescence(PL) spectroscopy, respectively. The photocatalytic activities were evaluated by the degradation of methyl blue(MB) under the simulated sunlight irradiation. Among all the samples, the BiOBr/ZnO composite with a mole ratio of 3:1(Bi:Zn) exhibited the best photocatalytic activity. The improvement of photocatalytic activity was mainly attributed to the low recombination ratio of photo-induced electron-hole pairs. The possible photocatalytic mechanism was discussed on the basis of the band structures of BiOBr and ZnO.
基金the National Natural Science Foundation of China(Nos.20405008,20635020)
文摘Direct electrochemical reduction ofp-nitrophenol (PNP) was investigated on a room temperature ionic liquid N-butylpyridinium hexafluorophosphate (BPPF6) modified carbon paste electrode (CILE). The cathodic peak potential was positively shifted and the peak currents were increased compared to that obtained on traditional carbon paste electrode (CPE). The results indicated that the presence of ionic liquid BPPF6 on the electrode surface showed excellent catalytic ability to the electrochemical reduction of PNP. The electrochemical behaviors of PNP on the CILE were investigated by cyclic voltammetry and the conditions such as the scan rate, the buffer pH, the substrate concentration were optimized. The electrochemical parameters were further calculated with the results of the electron transfer number (n), the charge-transfer coefficient (α) and the surface concentration (Гr) as 1.76, 0.37 and 2.47 × 10^-9 mol/cm^2, respectively, for the selected reductive peak. The results indicated that PNP showed an irreversible adsorption-controlled electrode process on the CILE.
文摘Among the sustainable energy sources,hydrogen is the one most promising for alleviating the pollution issues related to the usage of conventional fuels,as it can be produced in an efficient and eco-friendly way via electrocatalytic water splitting.The hydrogen evolution reaction(HER,a half-reaction of water splitting)plays a pivotal role in decreasing the price and increasing the catalytic efficiency of hydrogen production and is efficiently promoted by metal phosphides in different electrolytes.Herein,we summarize the recent advances in the development of metal phosphides as HER electrocatalysts,focus on their synthesis(post-treatment,in situ generation,and electrodeposition methods)and the enhancement of their electrocatalytic activity(via elemental doping,interface and vacancy engineering,construction of specific supports and nanostructures,and the design of bior polymetallic phosphides),and highlight the crucial issues and challenges of future development.
基金This work was supported by the National Natural Science Foundation of China(52072197,21971132)Outstanding Youth Foundation of Shandong Province,China(ZR2019JQ14)+1 种基金Major Scientific and Technological Innovation Project(2019JZZY020405)Major Basic Research Program of Natural Science Foundation of Shandong Province under Grant(ZR2020ZD09).
文摘The hydrogen energy generated by the electrocatalytic water splitting reaction has been established as a renewable and clean energy carrier with ultra-high energy density,which can well make up for shortcomings of conventional renewable energy sources,such as geographical limitations,climatic depen-dence,and energy wastage.Notably,the introduction of electrocatalysts can enhance the efficiency of the water splitting process to generate hydrogen.Particularly,the heterostructure electrocatalysts constructed by coupling mul-tiple components(or phases)have emerged as the most promising option for water splitting due to the well-known electronic and synergistic effects.The existing reviews on interface engineering for electrocatalyst design mostly focus on the relationship between the heterostructures and specific electrocatalytic reactions.However,a comprehensive overview of the integra-tion of model building,directional synthesis,and electrocatalytic mechanism has been rarely reported.To this end,in this review,the development of heterostructure catalysts is systematically introduced from the perspective of interface classification,interface growth and synthesis,and regulation of electrocatalytic performance based on the interfacial microenvironment(bonding,electronic configuration,lattice strain,etc.),thereby offering useful insights on the design and construction of interfacial models.Besides,com-bined with the current development and applications of interface engineering strategies,the challenges of future heterostructure catalysts are discussed and relevant solutions are proposed.Overall,this review can serve as a useful theo-retical reference for the integration of interfacial model building,directional synthesis,and electrocatalytic mechanism,which can further promote the development of hydrogen production technologies with low energy consump-tion and high yield.
基金supported by the National Major Research Project(2016YFB0101208)the National Natural Science Foundation of China(21576257)+1 种基金the Natural Science Foundation-Liaoning United Fund(U1508202)the Strategic Priority Research Program of the Chinese Academy of Sciences(XDB06050303)~~
文摘To accelerate the kinetics of the oxygen reduction reaction(ORR)in proton exchange membrane fuel cells,ultrafine Pt nanoparticles modified with trace amounts of cobalt were fabricated and decorated on carbon black through a strategy involving modified glycol reduction and chemical etching.The obtained Pt36Co/C catalyst exhibits a much larger electrochemical surface area(ECSA)and an improved ORR electrocatalytic activity compared to commercial Pt/C.Moreover,an electrode prepared with Pt36Co/C was further evaluated under H2-air single cell test conditions,and exhibited a maximum specific power density of 10.27 W mgPt^-1,which is 1.61 times higher than that of a conventional Pt/C electrode and also competitive with most state-of-the-art Pt-based architectures.In addition,the changes in ECSA,power density,and reacting resistance during the accelerated degradation process further demonstrate the enhanced durability of the Pt36Co/C electrode.The superior performance observed in this work can be attributed to the synergy between the ultrasmall size and homogeneous distribution of catalyst nanoparticles,bimetallic ligand and electronic effects,and the dissolution of unstable Co with the rearrangement of surface structure brought about by acid etching.Furthermore,the accessible raw materials and simplified operating procedures involved in the fabrication process would result in great cost-effectiveness for practical applications of PEMFCs.
基金supported by the National Natural Science Foundation of China under Grant No.52072196,52002199,52002200,52102106Major Basic Research Program of Natural Science Foundation of Shandong Province under Grant No.ZR2020ZD09+2 种基金the Natural Science Foundation of Shandong Province under Grant No.ZR2019BEM042,ZR2020QE063the Innovation and Technology Program of Shandong Province under Grant No.2020KJA004the Taishan Scholars Program of Shandong Province under No.ts201511034
文摘Three-dimensional(3D)ordered porous carbon is generally believed to be a promising electromagnetic wave(EMW)absorbing material.However,most research works targeted performance improvement of 3D ordered porous carbon,and the specific attenuation mechanism is still ambiguous.Therefore,in this work,a novel ultra-light egg-derived porous carbon foam(EDCF)structure has been successfully constructed by a simple carbonization combined with the silica microsphere template-etching process.Based on an equivalent substitute strategy,the influence of pore volume and specific surface area on the electromagnetic parameters and EMW absorption properties of the EDCF products was confirmed respectively by adjusting the addition content and diameter of silica microspheres.As a primary attenuation mode,the dielectric loss originates from the comprehensive effect of conduction loss and polarization loss in S-band and C band,and the value is dominated by polarization loss in X band and Ku band,which is obviously greater than that of conduction loss.Furthermore,in all samples,the largest effective absorption bandwidth of EDCF-3 is 7.12 GHz under the thickness of 2.13 mm with the filling content of approximately 5 wt%,covering the whole Ku band.Meanwhile,the EDCF-7 sample with optimized pore volume and specific surface area achieves minimum reflection loss(RL_(min))of−58.08 dB at 16.86 GHz while the thickness is 1.27 mm.The outstanding research results not only provide a novel insight into enhancement of EMW absorption properties but also clarify the dominant dissipation mechanism for the porous carbon-based absorber from the perspective of objective experiments.
基金support from the National Natural Science Foundation of China(G.Nos.52173055,21961132024,and 51925302)the Ministry of Science and Technology of China(G.No.2021YFE0105100)+3 种基金the Textile Vision Basic Research Program(No.J202201)the International Cooperation Fund of Science and Technology Commission of Shanghai Municipality(G.No.21130750100)the Fundamental Research Funds for the Central Universitiesthe DHU Distinguished Young Professor Program(G.No.LZA2020001)。
文摘The seawater desalination based on solardriven interfacial evaporation has emerged as a promising technique to alleviate the global crisis on freshwater shortage.However,achieving high desalination performance on actual,oil-contaminated seawater remains a critical challenge,because the transport channels and evaporation interfaces of the current solar evaporators are easily blocked by the oil slicks,resulting in undermined evaporation rate and conversion efficiency.Herein,we propose a facile strategy for fabricating a modularized solar evaporator based on flexible MXene aerogels with arbitrarily tunable,highly ordered cellular/lamellar pore structures for high-efficiency oil interception and desalination.The core design is the creation of 1D fibrous MXenes with sufficiently large aspect ratios,whose superior flexibility and plentiful link forms lay the basis for controllable 3D assembly into more complicated pore structures.The cellular pore structure is responsible for effective contaminants rejection due to the multi-sieving effect achieved by the omnipresent,isotropic wall apertures together with underwater superhydrophobicity,while the lamellar pore structure is favorable for rapid evaporation due to the presence of continuous,large-area evaporation channels.The modularized solar evaporator delivers the best evaporation rate(1.48 kg m-2h-1)and conversion efficiency(92.08%)among all MXene-based desalination materials on oil-contaminated seawater.
基金This work was supported by the National Natural Science Foundation of China(Nos.51772162,22001143,and 52072197)Youth Innovation and Technology Foundation of Shandong Higher Education Institutions,China(No.2019KJC004)+4 种基金Outstanding Youth Foundation of Shandong Province,China(No.ZR2019JQ14)Taishan Scholar Young Talent Program,China(Nos.tsqn201909114 and tsqn201909123)Natural Science Foundation of Shandong Province,China(No.ZR2020YQ34)Major Scientific and Technological Innovation Project,China(No.2019JZZY020405)Major Basic Research Program of Natural Science Foundation of Shandong Province,China(No.ZR2020ZD09).
文摘Coordination engineering can enhance the activity and stability of the catalyst in heterogeneous catalysis.However,the axial coordination engineering between different groups on the carbon carrier and molecular catalysts in the electrocatalytic carbon dioxide reduction reaction(CO_(2)RR)has been studied rarely.Through coordination engineering strategy,a series of amino(NH_(2)),hydroxyl(OH),and carboxyl(COOH)groups functionalized carbon nanotubes(CNT)immobilized cobalt phthalocyanine(CoPc)catalysts are designed.Compared with no groups,OH groups and COOH groups,NH_(2)groups can effectively change the coordination environment of the central metal Co,thereby significantly increasing the turnover frequency(TOF)(31.4 s^(-1)at-0.6 V vs.RHE,CoPc/NH_(2)-CNT>CoPc/OH-CNT>CoPc/COOH-CN>CoPc/CNT).In the flow cell,the CoPc/NH_(2)-CNT catalyst has high carbon monoxide(CO)selectivity at high current density(~100%at-225 mA·cm^(-2),~96%at-351 mA·cm^(-2)).Importantly,the CoPc/NH_(2)-CNT catalyst can operate stably for 100 h at 225 mA·cm^(-2).Theoretical calculations reveal that CoPc/NH_(2)-CNT catalyst is beneficial to the formation of^(*)COOH and desorption of^(*)CO,thus promoting CO_(2)RR.This work provides an excellent platform for understanding the effect of coordination engineering on electrocatalytic performance and promotes a way to explore efficient and stable catalysts in other applications.
基金supported jointly by the National Natural Science Foundation of China (20977055)the State Key Laboratory Foundation of Geological Processes and Mineral Resources, China University of Geosciences (GPMR201102)
文摘The purpose of this study is to comparatively investigate the plant uptake, accumulation and translocation behaviors of polycyclic aromatic hydrocarbons (PAHs) as priority pollutants in soil contaminated with oily sludge. The influence of different oily sludge application doses on the uptake of contaminants was studied together with the profile of individual PAH in roots, straws and leaves of winter wheat. Pot experiments were conducted using oily sludge application doses of 0, 5, 10, 15 and 20 percent, respectively. The total PAHs contents of control soil and oily sludge were 16.96 and 3504.66 μg/g, respectively. Analysis for the contents of the 16 PAHs was carried out with a HPLC-UV using plant tissue samples obtained at the 265th day of growth. The total PAHs contents in treated winter wheat were 9.02-334.81 ng/g for roots, 8.45-336.52 ng/g for straws and 10.70-406.32 ng/g for leaves. In addition to 5% of oily sludge dose, the total PAHs content in leaves was always highest under other doses of oily sludge application. With respect to individual PAH, the content did not show a significant plant tissue related trend. However, both the total content and individual content of PAHs in treated winter wheat tissues did increase with increasing oily sludge application dose. Another analysis for the control soil indicates that the degradation rate of PAHs was significantly enhanced by winter wheat after 265 days of growth based on the residual concentrations of PAHs in planted and unplanted soils.
文摘In this study,Ni_(2)P-Cd_(0.9)Zn_(0.1)S(NPCZS)composites were synthesized by coupling tetrapod bundle Cd_(0.9)Zn_(0.1)S(CZS)and coralline-like Ni_(2)P(NP)via a simple calcination method.CZS shows outstanding activity in photocatalytic hydrogen evolution(1.31 mmol h^(‒1)),owing to its unique morphology and heterophase homojunctions(ZB/WZ),which accelerate the separation and transfer of photogenerated charges.After coupling with NP,the photoactivity of NPCZS was enhanced,and the maximum hydrogen evolution rate of 1.88 mmol h^(‒1)was reached at a NP content of 12 wt%,which was 1.43 times higher than that of pure CZS.The experimental results of the photocatalytic activity,viz.photoluminescence spectra,surface photovoltage spectra,and electrochemical test showed that the enhanced photoactivity of NPCZS should be attributed to the synergistic effects of the novel tetrapod-bundle morphology,heterophase homojunctions,and decoration of the NP co-catalyst.Moreover,the as-prepared NPCZS composites exhibited excellent photostability and recyclability.Herein,we propose a possible mechanism for the enhanced photocatalytic activity.
基金supported by the National Natural Science Foundation of China (21476120)the Shandong Province Prioritized Development Plan (2017GGX40107)the Taishan Scholar Project of Shandong Province in China (ts201511033)
文摘The Br?nsted-acidic polyether ionic liquids(ILs)with different polymerization degrees(n value)were prepared via the reaction of tetramethylguanidine and epoxy ethane,followed by successive reactions with 1,3-propane sultone and trifluoromethanesulfonic acid(TfOH).The prepared ILs were characterized by infrared spectroscopy and 1H nuclear magnetic resonance spectroscopy,and their thermal stability was determined by thermal gravimetry.The synthesized polyether ILs coupled with TfOH were used to catalyze the alkylation reaction of isobutane and isobutene for the preparation of alkylate gasoline.The polyether ILs could improve the substrate dissolution and promote the separation of the catalyst from the products.The ideal IL(n=94)was determined.The optimized alkylation reaction conditions covered:a VTfOH/VIL ratio of 0.35,a reaction temperature of 40℃,a reaction time of 50 min,and a stirring speed of 800 r/min.The conversion of isobutene was 92.4%and the selectivity for the C8-product was 81.6%.Under optimal conditions,the catalyst life was determined and TfOH showed improved cyclic performance in the polyether ILs.After 8 operating cycles,the catalytic activity of the catalyst showed negligible decline.
基金the NSFC(Grant Nos.21875285 and 21805155)Taishan Scholars Program(ts201511019)+1 种基金Key Research and Development Projects of Shandong Province(2019JZZY010331)the Fundamental Research Funds for the Central Universities(19CX05001A).
文摘Constructing heterojunction is a promising way to improve the charge transfer efficiency and can thus promote the electrochemical properties.Herein,a facile and effective epitaxial-like growth strategy is applied to NiSe2 nano-octahe-dra to fabricate the NiSe2-(100)/Ni(OH)2-(110)heterojunction.The heterojunction composite and Ni(OH)2(performing high electrochemical activity)is ideal high-rate battery-type supercapacitor electrode.The NiSe2/Ni(OH)2 electrode exhibits a high specific capacity of 909 C g^-1 at 1 A g^-1 and 597 C g^-1 at 20 A g^-1.The assembled asymmetric supercapacitor composed of the NiSe2/Ni(OH)2 cathode and p-phenylenediamine-functional reduced graphene oxide anode achieves an ultrahigh specific capacity of 303 C g^-1 at 1 A g^-1 and a superior energy density of 76.1 Wh kg^-1 at 906 W kg^-1,as well as an outstanding cycling stability of 82%retention for 8000 cycles at 10 A g^-1.To the best of our knowledge,this is the first example of NiSe2/Ni(OH)2 heterojunction exhibiting such remarkable supercapacitor performance.This work not only provides a promising candidate for next-generation energy storage device but also offers a possible universal strategy to fabricate metal selenides/metal hydroxides heterojunctions.
基金the financial supports from the Shandong Provincial Natural Science Foundation(Grant No.ZR201910220216)the Key Research and Development Plan of Shandong Province(2019GGX104034)+1 种基金the Foundation of State Key Laboratory of High-efficiency Utilization of Coal,and Green Chemical Engineering(Grant No.2020-KF-18)the Taishan Scholar Program of Shandong Province(No.ts201712045)。
文摘A 2 D-2 D titanium dioxide nanosheet-reduced graphene oxide(TNS-r GO)composite with better electronic conductivity and hydrophilicity was prepared by the hydrothermal method.The as-obtained TNS-r GO composite was further functionalized with 3-aminopropyltriethoxysilane(APTES)to provide a large amount of-NH2 groups on the surface for anchoring ultrafine Pd Ag alloy nanoparticles with an average particle size of 1.69 nm by a facile wet reduction approach.Benefiting from the combined effects of well-dispersed Pd Ag alloy nanoparticles,facilitated electron transfer from TNS-r GO to Pd,and increased electron density of active sites,the Pd8 Ag_(1)/NH_(2)-TNS-r GO catalyst exhibited excellent activity towards dehydrogenation of formic acid without adding any additives at 298 K,corresponding to an initial turn over frequency as high as 1090 h-1,which is much higher than that of most other state-of-theart catalysts.
基金funding support from the National Natural Science Foundation of China(2200206852272222,and 52072197)+12 种基金the Taishan Scholar Young Talent Program(tsqn201909114)the Youth Innovation and Technology Foundation of Shandong Higher Education Institutions,China(2019KJC004)the Outstanding Youth Foundation of Shandong Province,China(ZR2019JQ14)the Major Basic Research Program of Natural Science Foundation of Shandong Province under Grant No.ZR2020ZD09Youth Innovation Team Development Program of Shandong Higher Education Institutions(2022KJ155)the Major Scientific and Technological Innovation Project(2019JZZY020405)the Shandong Province“Double-Hundred Talent Plan”(WST2020003)Project funded by the China Postdoctoral Science Foundation(2021M691700)the Natural Science Foundation of Shandong Province of China(ZR2019BB002ZR2018BB031)the Postdoctoral Innovation Project of Shandong Province(SDCXZG-202203021)the Scientific and Technological Innovation Promotion Project for Small-medium Enterprises of Shandong Province(2022TSGC1257)the Major Research Program of Jining City(2020ZDZP024)。
文摘Constructing highly-efficient electrocatalysts toward hydrogen evolution reaction(HER)/oxygen evolution reaction(OER)/oxygen reduction reaction(ORR)with excellent stability is quite important for the development of renewable energy-related applications.Herein,Co-Ru based compounds supported on nitrogen doped two-dimensional(2D)carbon nanosheets(NCN)are developed via one step pyrolysis procedure(Co-Ru/NCN)for HER/ORR and following low-temperature oxidation process(Co-Ru@RuO_(x)/NCN)for OER.The specific 2D morphology guarantees abundant active sites exposure.Furthermore,the synergistic effects arising from the interaction between Co and Ru are crucial in enhancing the catalytic performance.Thus,the resulting Co-Ru/NCN shows remarkable electrocatalytic performance for HER(70 mV at 10 mA cm^(-2))in 1 M KOH and ORR(half-wave potential E_(1/2)=0.81 V)in 0.1 M KOH.Especially,the Co-Ru@RuO_(x)/NCN obtained by oxidation exhibits splendid OER performance in both acid(230 mV at 10 mA cm^(-2))and alkaline media(270 mV at 10 mA cm^(-2))coupled with excellent stability.Consequently,the fabricated two-electrode water-splitting device exhibits excellent performance in both acidic and alkaline environments.This research provides a promising avenue for the advancement of multifunctional nanomaterials.
基金supported financially by the National Natural Science Foundation of China,China(Grant No.51702180,51772162)the Taishan Scholar Advantage and Characteristic Discipline Team of Eco Chemical Process and Technologythe Scientific and Technical Development Project of Qingdao,China(Grant No.18-2-2-52-jch)。
文摘Non-noble-metal-based electrocatalysts with superior oxygen reduction reaction(ORR)activity to platinum(Pt)are highly desirable but their fabrications are challenging and thus impeding their applications in metal-air batteries and fuel cells.Here,we report a facile molten salt assisted two-step pyrolysis strategy to construct carbon nanosheets matrix with uniformly dispersed Fe_(3) N/Fe nanoparticles and abundant nitrogen-coordinated Fe single atom moieties(Fe@Fe_(SA)-N-C).Thermal exfoliation and etching effect of molten salt contribute to the formation of carbon nanosheets with high porosity,large surface area and abundant uniformly immobilized active sites.Aberration-corrected high-angle annular dark-field scanning transmission electron microscopy(HAADF-STEM)image,X-ray absorption fine spectroscopy,and X-ray photoelectron spectroscopy indicate the generation of Fe(mainly Fe_(3) N/Fe)and Fe_(SA)-N-C moieties,which account for the catalytic activity for ORR.Further study on modulating the crystal structure and composition of Fe_(3) N/Fe nanoparticles reveals that proper chemical environment of Fe in Fe_(3) N/Fe notably optimizes the ORR activity.Consequently,the presence of abundant Fe_(SA)-N-C moieties,and potential synergies of Fe_(3) N/Fe nanoparticles and carbon shells,markedly promote the reaction kinetics.The as-developed Fe@Fe_(SA)-N-C-900 electrocatalyst displays superior ORR performance with a half-wave potential(E_(1/2))of 0.83 V versus reversible hydrogen electrode(RHE)and a diffusion limited current density of 5.6 mA cm^(-2).In addition,a rechargeable Zn-air battery device assembled by the Fe@Fe_(SA)-N-C-900 possesses remarkably stable performance with a small voltage gap without obvious voltage loss after500 h of operation.The facile synthesis strategy for the high-performance composites represents another viable avenue to stable and low-cost electrocatalysts for ORR catalysis.
基金the National Natural Science Foundation of China(Nos.20405008,20635020).
文摘An electrochemical method for the simultaneous detection of two different DNA sequences from PAT and FMV 35S gene sequence using CdS and PbS quantum dots (QDs) as labels was described. The QDs were readily functionalized with oligonucleotides as electrochemical DNA probes and selectively hybridized to the complementary sequences immobilized on the microplate. The QDs anchored on the hybrids were dissolved in the solution by the oxidation of HNO3 and further detected by a sensitive differential pulse anodic stripping voltammetric method (DPASV). The DPASV signals of the oxidation of Cd^2+ and Pb^2+ ions present in the solution were different and reflected the identity of corresponding ssDNA targets sequences.
基金supported by the National Natural Science Foundation of China(No.20635020,No.20805025,No. 20975057)the Doctoral Foundation of the Ministry of Education of China(No.20060426001)+1 种基金the Foundation of Qingdao City(No.09-1-3-25-jch)the Doctoral Fund of QUST(No.0022278)
文摘An electrochemical sensor for the detection of the natural double-stranded DNA(dsDNA) damage induced by PbSe quantum dots(QDs) under UV irradiation was developed.The biosensing membranes were prepared by successively assembling 3- mercaptopropionic acid,polycationic poly(diallyldimethyl ammonium) and dsDNA on the surface of the gold electrode.Damage of dsDNA was fulfilled by immersing the sensing membrane electrode in PbSe QDs suspension and illuminating it with an UV lamp. Cyclic voltammetry was utilized to detect dsDNA damage with Co(phen)_3^(3+) as the electroactive probe.The UV irradiation,Pb^(2+) ions liberated from the PbSe QDs under the UV irradiation and the reactive oxygen species(ROS) generated in the presence of the PbSe QDs also under the UV irradiation were the three factors of inducing the dsDNA damage.The synergistic effect of the three factors might dramatically enhance the damage of dsDNA.This electrochemical sensor provided a simple method for detecting DNA damage,and may be used for investigating the DNA damage induced by other QDs.