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1.
Most of the current analytical methods depend largely on laboratory-based analytical techniques that require expensive and bullky equipment,potentially incur costly testing,and involve lengthy detection processes.With increasing requirements for point-of-care testing(POCT),more attention has been paid to miniaturized analytical devices.Miniaturized electrochemical(MEC)sensors,including different material-based MEC sensors(such as DNA-,paper-,and screen electrode-based),have been in strong demand in analytical science due to their easy operation,portability,high sensitivity,as well as their short analysis time.They have been applied for the detection of trace amounts of target through measuring changes in electrochemical signal,such as current,voltage,potential,or impedance,due to the oxidation/reduction of chemical/biological molecules with the help of electrodes and electrochemical units.MEC sensors present great potential for the detection of targets including small organic molecules,metal ions,and biomolecules.In recent years,MEC sensors have been broadly applied to POCT in various fields,including health care,food safety,and environmental monitoring,owing to the excellent advantages of electrochemical(EC)technologies.This review summarized the state-of-the-art advancements on various types of MEC sensors and their applications in POCT.Furthermore,the future perspectives,opportunities,and challenges in this field are also discussed.  相似文献   

2.
Feng Pan 《结构化学》2020,39(1):7-10
Machine learning is an emerging method to discover new materials with specific characteristics.An unsupervised machine learning research is highlighted to discover new potential lithium ionic conductors by screening and clustering lithium compounds,providing inspirations for the development of solid-state electrolytes and practical batteries.  相似文献   

3.
Designing defect-engineered semiconductor heterojunctions can effectively promote the charge carrier separation.Herein,novel ceria(CeO2) quantum dots(QDs) decorated sulfur-doped carbon nitride nanotubes(SCN NTs) were synthesized via a thermal polycondensation coupled in situ depositionprecipitation method without use of template or surfactant.The structure and morphology studies indicate that ultrafine CeO2 QDs are well distributed inside and outside of SCN NTs offering highly dispersed active sites and a large contact interface between two components.This leads to the promoted formation of rich Ce3+ ion and oxygen vacancies as confirmed by XPS.The photocatalytic performance can be facilely modulated by the content of CeO2 QDs introduced in SCN matrix while bare CeO2 does not show activity of hydrogen production.The optimal catalyst with 10% of CeO2 loading yields a hydrogen evolution rate of 2923.8 μmol h-1 g-1 under visible light,remarkably higher than that of bare SCN and their physical mixtures.Further studies reveal that the abundant surface defects and the created 0 D/1 D junctions play a critical role in improving the separation and transfer of charge carriers,leading to superior solar hydrogen production and good stability.  相似文献   

4.
The demand on low-carbon emission fabrication technologies for energy storage materials is increasing dramatically with the global interest on carbon neutrality.As a promising active material for metal-sulfur batteries,sulfur is of great interest due to its high-energy-density and abundance.However,there is a lack of industry-friendly and low-carbon fabrication strategies for high-performance sulfur-based active particles,which,however,is in critical need by their practical success.Herein,based on a hail-inspired sulfur nano-storm(HSN)technology developed in our lab,we report an energy-saving,solvent-free strategy for producing core-shell sulfur/carbon electrode particles(CNT@AC-S)in minutes.The fabrication of the CNT@AC-S electrode particles only involves low-cost sulfur blocks,commercial carbon nanotubes(CNT)and activated carbon(AC)micro-particles with high specific surface area.Based on the above core-shell CNT@AC-S particles,sulfur cathode with a high sulfur-loading of 9.2 mg cm-2 delivers a stable area capacity of 6.6 mAh cm-2 over 100 cycles.Furthermore,even for sulfur cathode with a super-high sulfur content(72 wt%over the whole electrode),it still delivers a high area capacity of 9 mAh cm-2 over50 cycles in a quasi-lean electrolyte condition.In a nutshell,this study brings a green and industryfriendly fabrication strategy for cost-effective production of rationally designed S-rich electrode particles.  相似文献   

5.
Transition metal selenides have been widely studied as anode materials of sodium ion batteries(SIBs),however,the investigation of solid-electrolyte-interface(SEI)on these materials,which is critical to the electrochemical performance of SIBs,remains at its infancy.Here in this paper,ZnSe@C nanoparticles were prepared from ZIF-8 and the SEI layers on these electrodes with and without reduced graphene oxide(rGO)layers were examined in details by X-ray photoelectron spectroscopies at varied charged/discharged states.It is observed that fast and complicated electrolyte decomposition reactions on ZnSe@C leads to quite thick SEI film and intercalation of solvated sodium ions through such thick SEI film results in slow ion diffusion kinetics and unstable electrode structure.However,the presence of rGO could efficiently suppress the decomposition of electrolyte,thus thin and stable SEI film was formed.ZnSe@C electrodes wrapped by rGO demonstrates enhanced interfacial charge transfer kinetics and high electrochemical performance,a capacity retention of 96.4%,after 1000 cycles at 5 A/g.This study might offer a simple avenue for the designing high performance anode materials through manipulation of SEI film.  相似文献   

6.
CXN天然沸石的研究2: 吸附性质   总被引:3,自引:0,他引:3  
李军  邱瑾  龙英才 《化学学报》2000,58(8):988-991
采用N~2,NH~3,CO~2,乙烯,丙烯,水,甲醇,乙醇,丙醇等作为吸附剂,研究了由我国CXN天然沸石改性制得的H-STI和Na-STI沸石的吸附性质,H-STI和Na-STI沸石的BET表面积及微孔孔体积约为420m^2/g和0.20m^3/g。根据NH~3和CO~2在H-STI沸石上的吸附等温线计算得到它们的吸附热分别为44.8和26.5kJ/mol。乙烯,丙烯,甲醇,乙醇,丙醇等在Na-STI沸石上的吸附等温线表明该沸石对有机分子的吸附具有链长选择性。在低分压下水相对于甲醇的吸附量表明沸石具有一定的疏水性质。  相似文献   

7.
常温常湿条件下Au/MeO~x催化剂上CO氧化性能   总被引:12,自引:0,他引:12  
王桂英  张文祥  蒋大振  吴通好 《化学学报》2000,58(12):1557-1562
利用共沉淀法制备了Au/MeO~x催化剂(Me=Al,Co,Cr,Cu,Fe,Mn,Ni,Zn)。在常温常湿条件下,考察了不同氧化物负载的金基催化剂的CO氧化性能。结果表明,氧化物种类对催化剂的活性和稳定性均有较大的影响。Cu,Mn,Cr等氧化物负载的金基催化剂的活性较差,而Zn,Fe,Co,Ni,Al等金属氧化物负载的金基催化剂可将CO完全氧化,又具有一定的稳定性,在相同反应条件下,CO完全转化时的稳定性顺序为Au/ZnO>Au/α-Fe~2O~3>Au/Co~3O~4>Au/γ-Al~2O~3≈Au/NiO。还发现水对Au/MnO~x催化剂的活性和稳定性有负作用,而对180℃焙烧制备的Au/ZnO-180催化剂的活性和稳定性均有明显的湿度增强作用。  相似文献   

8.
Cost-effective atomically dispersed Fe-N-P-C complex catalysts are promising to catalyze the oxygen reduction reaction(ORR)and replace Pt catalysts in fuel cells and metal-air batteries.However,it remains a challenge to increase the number of atomically dispersed active sites on these catalysts.Here we report a highly efficient impregnation-pyrolysis method to prepare effective ORR electrocatalysts with large amount of atomically dispersed Fe active sites from biomass.Two types of active catalyst centers were identified,namely atomically dispersed Fe sites and FexP particles.The ORR rate of the atomically dispersed Fe sites is three orders of magnitude higher than it of FexP particles.A linear correlation between the amount of the atomically dispersed Fe and the ORR activity was obtained,revealing the major contribution of the atomically dispersed Fe to the ORR activity.The number of atomically dispersed Fe increases as the Fe loading increased and reaching the maximum at 1.86 wt%Fe,resulting in the maximum ORR rate.Optimized Fe-N-P-C complex catalyst was used as the cathode catalyst in a homemade Zn-air battery and good performance of an energy density of 771 Wh kgZn-1,a power density of 92.9 m W cm-2 at 137 m A cm-2 and an excellent durability were exhibited.  相似文献   

9.
Lithium-sulfur(Li-S)battery is regarded as one of the most promising next-generation energy storage systems due to the ultra-high theoretical energy density of 2600 Wh kg-1.To address the insulation nature of sulfur,nanocarbon composition is essential to afford acceptable cycling capacity but inevitably sacrifices the actual energy density under working conditions.Therefore,rational structural design of the carbon/sulfur composite cathode is of great significance to realize satisfactory electrochemical performances with limited carbon content.Herein,the cathode carbon distribution is rationally regulated to construct high-sulfur-content and high-performance Li-S batteries.Concretely,a double-layer carbon(DLC)cathode is prepared by fabricating a surface carbon layer on the carbon/sulfur composite.The surface carbon layer not only provides more electrochemically active surfaces,but also blocks the polysulfide shuttle.Consequently,the DLC configuration with an increased sulfur content by nearly 10 wt%renders an initial areal capacity of 3.40 mAh cm-2 and capacity retention of 83.8%during 50 cycles,which is about two times than that of the low-sulfur-content cathode.The strategy of carbon distribution regulation affords an effective pathway to construct advanced high-sulfur-content cathodes for practical high-energy-density Li-S batteries.  相似文献   

10.
Carbon dioxide and methane are two main greenhouse gases which are contributed to serious global warming.Fortunately,dry reforming of methane(DRM),a very important reaction developed decades ago,can convert these two major greenhouse gases into value-added syngas or hydrogen.The main problem retarding its industrialization is the seriously coking formation upon the nickel-based catalysts.Herein,a series of confined indium-nickel(In-Ni)intermetallic alloy nanocatalysts(InxNi@SiO2)have been prepared and displayed superior coking resistance for DRM reaction.The sample containing 0.5 wt.%of In loading(In0.5Ni@SiO2)shows the best balance of carbon deposition resistance and DRM reactivity even after 430 h long term stability test.The boosted carbon resistance can be ascribed to the confinement of core–shell structure and to the transfer of electrons from Indium to Nickel in In-Ni intermetallic alloys due to the smaller electronegativity of In.Both the silica shell and the increase of electron cloud density on metallic Ni can weaken the ability of Ni to activate C–H bond and decrease the deep cracking process of methane.The reaction over the confined InNi intermetallic alloy nanocatalyst was conformed to the Langmuir-Hinshelwood(L-H)mechanism revealed by in situ diffuse reflectance infrared Fourier transform spectroscopy(in-situ DRIFTS).This work provides a guidance to design high performance coking resistance catalysts for methane dry reforming to efficiently utilize these two main greenhouse gases.  相似文献   

11.
Platinum (Pt) is recognized as an excellent cocatalyst which not only suppresses the charge carrier recombination of the photocatalyst but also reduces the overpotential for photocatalytic H2 generation. Albeit of its good performance, the high cost and low abundance restricted the utilization of Pt in large-scale photocatalytic H2 generation. Pt based transition metal alloys are demonstrated to reveal enhanced activities towards various catalytic reactions, suggesting the possibility to substitute Pt as the cocatalyst. In the present work, Pt was partially substituted with Co, Ni, and Fe and Pt-M (M = Co, Ni, and Fe)/g-C3N4 composites were constructed through co-reduction of H2PtCl6 and transition metal salts by the reductant of ethylene glycol. The crystal structure and valence states were measured by X-ray diffractometer (XRD) and X-ray photoelectron spectrometer (XPS), respectively. The higher degree of XRD peaks and larger binding energies for Pt 4f5/2 and Pt 4f7/2 after incorporating Co2+ ions indicated that Co was successfully introduced into the lattice of Pt and Pt-Co bimetallic alloys was attained through the solvothermal treatment. The morphology was subsequently observed by transmission electron microscope (TEM), which showed a good dispersion of Pt-Co nanoparticles on the surface of g-C3N4. Meanwhile, the shrinkage of lattice fringe after introducing cobalt salt further confirmed the presence of Pt-Co bimetallic alloys. The UV-Vis absorption spectra of g-C3N4 and Pt, Pt-Co deposited g-C3N4 were subsequently performed. It was found that the absorption edges were all consistent for all three samples as anticipated, implying that the band gap energy was maintained after hybridizing with Pt or Pt-Co alloys. Furthermore, the photocatalytic H2 generation was carried out over the as-prepared composites with triethanolamine (TEOA) as sacrificial reagent. Under visible-light illumination, the1% (w) Pt2.5M/g-C3N4 (M = Co, Fe, Ni) composites all exhibited higher or comparable activity towards photocatalytic H2 generation when compared to 1% (w) Pt loaded counterpart. In addition, the atomic ratios of Pt/Co and the loading amount of Pt-Co cocatalyst were modified to optimize the photocatalytic performance, among which, 1% (w) Pt2.5Co/g-C3N4 composite revealed the highest activity with a 1.6-time enhancement. Electrochemical impedance spectra (EIS) and photoluminescence (PL) spectra indicated that the enhancement might be attributed to improved charge transfer from g-C3N4 to Pt2.5Co cocatalyst and inhibited charge carrier recombination in the presence of Pt2.5Co cocatalyst. Therefore, the present study demonstrates the great potential to partially replace Pt with low-cost and abundant transition metals and to fabricate Pt based bimetallic alloys as promising cocatalysts for highly efficient photocatalytic H2 generation.  相似文献   

12.
Pt0被认为是NO氧化的活性物种,而催化剂的制备方法对活性物种的含量起着决定性作用。本文采用非惰性气氛保护的改性醇还原-浸渍法(MARI)合成了高分散高Pt0含量的1% (w, 质量分数) Pt/SiO2-Al2O3催化剂(MA-Pt/SA)。X射线粉末衍射(XRD)、CO-漫反射傅里叶变换红外吸收光谱(CO-DRIFTS)和透射电镜(TEM)表征证实在550 ℃焙烧3 h后催化剂的Pt颗粒仅有3.8 nm。同时,X射线光电子能谱(XPS)和H2-程序升温还原(H2-TPR)结果表明催化剂具有高Pt0含量(60.3%)。模拟柴油车尾气气氛进行活性测试,并与传统浸渍法制备的1% (w) Pt/SiO2-Al2O3催化剂(C-Pt/SA)对比,结果显示MA-Pt/SA具有优异的催化氧化性能,其NO最大转化率高达74%,比C-Pt/SA的NO转化率高了23%。经670 ℃高温老化15 h后,老化的MA-Pt/SA的NO转化率仍然高达69%。此外NO + O2共吸附原位漫反射傅里叶变换红外吸收光谱(in situ DRIFTS of NO + O2 co-adsorption)表明高的Pt分散度和高Pt0含量能够促进中间物种桥式硝酸盐的生成及分解,进而导致了优异的NO氧化活性。最后,利用同样方法将Pt的负载量降低至0.5% (w)制备催化剂,NO转化率仍达64%。这种制备方法能够获得低贵金属高性能的Pt基催化剂。  相似文献   

13.
从Pd纳米粒子出发制备了具有核壳结构的新型纳米Pd@SiO2/Ce0.4Zr0.6O2三效催化剂及作为参比的Pd/Ce0.4Zr0.6O2催化剂, 采用X射线衍射、 透射电子显微镜、 氢气程序升温还原和氮气低温吸附-脱附等技术对催化剂的物化性质进行了表征, 研究了Pd@SiO2/Ce0.4Zr0.6O2和Pd/Ce0.4Zr0.6O2催化剂的三效反应催化活性和热稳定性. 结果表明, SiO2壳层可以抑制Pd粒子的团聚, 同时还能抑制Pd物种的再分散, 减少Pd的流失. 具有核壳结构的纳米Pd@SiO2/Ce0.4Zr0.6O2催化剂具有更好的三效催化活性和更高的热稳定性.  相似文献   

14.
The hetro-structured oxide thin films from metal fluorocomplex solution have been prepared by the liquid phase deposition (LPD) method. The Pt/Nb2O5 and Au/Nb2O5 composite films can be prepared from a mixed solution of niobium source, H3BO3, Pt(NH3)4Cl2 and HAuCl4 aqueous solutions under the ambient temperature and atmosphere. In the case of Au/SiO2 composite film, (NH4)2SiF6 solution is used as a mother solution. The Pt and Au ionic species are deposited in Nb2O5 and SiO2 matrices. They are reduced to their metallic state after treatment above 200 °C. The size of dispersed particles can be controlled by heat treatment temperature. It is also clear that, gold nanoparticles are also found to interact with SiO2, although the interaction is smaller than that with Nb2O5 showing the size of Au nanoparticles remain smaller in Nb2O5 that in SiO2.  相似文献   

15.
以制得的纳米Fe3O4颗粒作为载体,用还原法将还原出的Au与Pt分别负载到Fe3O4颗粒表面,制得纳米Pt/Au/Fe3O4复合材料。对Pt/Au/Fe3O4进行紫外可见光吸收光谱、透射电子显微镜、X射线衍射及光电子能谱等物理表征,结果表明,Au与Pt均匀地沉积到了Fe3O4纳米颗粒表面。对纳米Pt/Au/Fe3O4复合材料进行循环伏安扫描,当H2PtCl6的加入量达到8 mL时,Pt/Au/Fe3O4催化性能最佳;正扫电流峰ip与扫描速率的平方根v1/2线性相关,Pt/Au/Fe3O4催化氧化甲醇的过程受扩散控制;对催化剂进行201次循环伏安扫描,催化剂仍然能保持较好的催化性能且稳定性良好。因此,所合成催化剂Pt/Au/Fe3O4是一种具有良好化学稳定性的阳极催化剂材料。  相似文献   

16.
选取化学惰性的β-SiC为载体, 通过共浸渍法制备了Co-Pt/SiC催化剂; 利用球差校正的电子显微镜(AC-STEM), 结合氢气程序升温还原(H2-TPR)、 CO化学吸附以及准原位X射线吸收光谱(XAS)等手段, 研究了Co-Pt/SiC催化剂中贵金属Pt对于钴基费托反应的促进作用. 结果表明, Pt助剂从提高分散度和还原度两个方面增加了Co0活性相的数量, 从而提升了催化剂的费托反应活性. 通过AC-STEM表征了Pt在催化剂上的微观结构状态, 发现Pt助剂主要以单原子或团簇的形式分散在金属Co上. 这种分散形式的Pt对钴基催化剂的促进作用可能遵循氢气解离和氢溢流机理: 分布在Co上的Pt显著提高了催化剂解离氢气的能力, 这有利于促进钴物种的还原, 提高还原度, 同时也有利于促进费托反应过程中H2的活化以及CO的氢助解离, 提高了催化剂的反应活性, 以及饱和烷烃的选择性.  相似文献   

17.
Bimetallic nanoparticles(AmBn)usually exhibit rich catalytic chemistry and have drawn tremendous attention in heterogeneous catalysis.However,challenged by the huge configuration space,the understanding toward their composition and distribution of A/B element is known little at the atomic level,which hinders the rational synthesis.Herein,we develop an on-the-fly training strategy combing the machine learning model(SchNet)with the genetic algorithm(GA)search technique,which achieve the fast and accurate energy prediction of complex bimetallic clusters at the DFT level.Taking the 38-atom PtmAu38-mnanoparticle as example,the element distribution identification problem and the stability trend as a function of Pt/Au composition is quantitatively re solved.Specifically,results show that on the Pt-rich cluster Au atoms prefer to occupy the low-coordinated surface corner sites and form patch-like surface segregation patte rns,while for the Au-rich ones Pt atoms tend to site in the co re region and form the co re-shell(Pt@Au)configuration.The thermodynamically most stable PtmAu38-mcluster is Pt6 Au32,with all the core-region sites occupied by Pt,rationalized by the stronger Pt-Pt bond in comparison with Pt-Au and Au-Au bonds.This work exemplifies the potent application of rapid global sea rch enabled by machine learning in exploring the high-dimensional configuration space of bimetallic nanocatalysts.  相似文献   

18.
Aseries of Ni catalysts supported on alumina with different Ce contents(1.0%-6.0%, mass fraction) was prepared by the impregnation method and used for dry reforming of methane(DRM) at a relatively low temperature of 650 oC. The promotion effect of Ce with different loading amounts on the physicochemical properties of the catalysts was systematically characterized by transmission electron microscopy(TEM), X-ray diffraction(XRD), N2 adsorption-desorption, thermo elemental IRIS Intrepid inductively coupled plasma atomic emission spectrometer (ICP-AES), UV-visible diffuse reflectance spectroscopy(UV-Vis DRS), Fourier transformation infrared(FTIR) spectra, H2-temperature programmed reduction(H2-TPR) analysis, H2-temperature programmed desorption(H2-TPD), and the X-ray photoelectron spectroscopy(XPS) techniques. The results indicate that all the catalysts mainly exist in the NiAl2O4 phase after being calcined at 750 oC with small Ni particle sizes due to the strong metal-support interaction derived from the reduction of the NiAl2O4 phase. The Ce-promoted catalysts show better catalytic performance as well as the resistance against sintering of Ni particles and deposition of carbon compared to the Ni/Al2O3 catalyst. The Ni-6Ce/Al2O3 exhibits the best catalytic stability and coke resistance among the four catalysts studied, which is due to its small Ni nanoparticles sizes, excellent reducibility as well as high amount of active oxygen species. In a 400 h stability test for DRM reaction at 650 oC, Ni-6Ce/Al2O3 exhibits less coke deposition and small growth of Ni nanoparticles. This work provides a simple way to preparing the Ni-Ce/Al2O3 catalyst with enhanced catalytic performance in DRM. The Ni-6Ce/Al2O3 catalyst has great potential for industrial application due to its anti-sintering ability and resistance to carbon deposition.  相似文献   

19.
Pd-Pt双金属基甲烷氧化催化剂的催化活性、抗水热老化性和耐硫性在一个通有模拟稀燃天然气汽车尾气成分的固定床反应器中进行检测.研究发现Zr掺杂的Pd-Pt/Al2O3 (Pd-Pt/ZrxAl(1-x)O(3+x)/2)提高了催化的催化活性、抗水热老化性和耐硫性.以共沉淀法制备Zr : Al的摩尔比分别为0 : 1、0.25 : 0.75、0.5 : 0.5、0.75 :0.25和1 : 0的材料为载体材料.双金属催化剂的活性组分分别为1.5% (w,质量分数)的Pd和0.3% (w)的Pt,活性组分Pd、Pt通过共浸渍的方法浸渍到以上载体材料上制备得到一系列整体式催化剂.分别采用低温N2吸脱附、X射线衍射(XRD)、H2程序升温还原(H2-TPR)、O2程序升温氧化(O2-TPD)及X射线光电子能谱对制备的催化剂进行表征.结果显示Zr的加入使催化剂的载体材料结晶度提高,活性组分的分散度也得到了相应的提高.同时二价Pd物种与周围电子密度分别增加.相比于Pd-Pt/Al2O3和Pd-Pt/ZrO2催化剂,在不同条件预处理后, Zr的添加对催化剂的性能有明显的提高,其中催化剂Pd-Pt/Zr0.5Al0.5O1.75展现了最好的催化活性、抗水热老化性以及耐硫性.  相似文献   

20.
袁洋  王佳新  曹玉华 《电化学》2019,25(6):757-763
采用表面印迹技术,以磁性二氧化硅纳米粒子(Fe3O4@SiO2 NPs)作为载体、血红蛋白(Hb)为模板分子、正硅酸乙酯(TEOS)为印迹聚合物单体,制备了Hb印迹Fe3O4@SiO2的磁性印迹纳米粒子(MMIPs NPs). MMIPs NPs具有磁性内核和血红蛋白印迹壳层的核壳结构,可以富集并固定Hb. 使用壳聚糖将MMIPs NPs固定于磁性电极表面,构建血红蛋白类酶生物传感器,研究了Hb对过氧化氢(H2O2)的催化活性. MMIPS NPS相比于磁性非印迹纳米粒子(MNIPS NPS),催化电流增加了14.3%. 采用磁性电极,MMIPS NPS、Hb和O2的顺磁性使得该类酶生物传感器对H2O2的催化电流增加了60.0%. 血红蛋白类酶生物传感器电流响应与H2O2浓度在25 ~ 200 μmol·L-1间呈线性关系,检出限为3 μmol·L-1(S/N=3),表明该类酶传感器对H2O2具有良好的催化性能.  相似文献   

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