Y-Mn-O负载的Ni基催化剂用于乙酸自热重整产氢

为了有效地从生物质衍生的乙酸中获得高氢气产率,通过水热法合成了一系列的NiMnY催化剂并用于乙酸自热重整(ATR)过程中,并采用X射线衍射(XRD)、N2吸附-脱附测试、H2程序升温还原(H2-TPR)探究催化剂中的内在联系.在Ni0.39Mn0.61YO3.11±δ催化剂中,经焙烧后形成了类钙钛矿型(Ni,Mn)YO...     

La_(0.5)Pr_(0.5)Ni_(0.7)Co_(0.3)O_3在乙醇水蒸气重整中催化性能研究

用共沉淀法制备了La_(0.5)Pr_(0.5)Ni_(0.7)Co_(0.3)O_3钙钛矿氧化物催化剂,用XRD、SEM、TPR、TG等对La_(0.5)Pr_(0.5)Ni_(0.7)Co_(0.3)O_3钙钛矿氧化物的晶相结构、还原性能及反应50 h后的La_(0.5)Pr_(0.5)Ni_(0.7)Co_(0.3)O_3钙钛矿氧化物表面积碳情况进行了分析,同时用微反色谱装置在不同的反应温度条件下的La_(0.5)Pr_(0.5)Ni_(0.7)Co_(0.3)O_3钙钛矿氧化物的初活性、氢气平均选择性和积碳性能进行了探讨。结果表明,La_(0.5)Pr_(0.5)Ni_(0.7)Co_(0.3)O_3钙钛矿氧化物在乙醇水蒸气重整反应中具有较好的低温初活性和氢气的选择性,乙醇的平均转化率和氢气的选择性随着反应温度的升高而增大。当温度大于550℃时,转化率增幅不大,氢气的平均选择性在600℃时有所下降。反应温度升高催化剂的积碳量有所增多,积碳主要是不定型碳。     

磁铅石型复合氧化物LaNi_xCo_(1-x)Al_(11)O_(19+δ)催化剂上CH_4和CO_2重整反应的研究

考察了磁铅石型复合氧化物LaNi_(0.5)M_(0.5)Al_(11)O_(19 + δ) (M = Co, Fe, Mn, Cu)和LaNi_xCo_(1-x)Al_(11)O_(19+δ)催化剂在CH_4与CO_2重整制合成 气反应中的催化活性，并应用XRD，TPR，UV-DRS技术着重表征LaNi_xCo_(1-x)Al_ (11)O_(19+δ)催化剂的结构和性能。研究结果表明该系列催化剂具有相同的晶体 结构和相似的还原稳定性。对不同过渡金属取代的催化剂来说，以LaNi_(0.5)Co_ (0.5)Al_(11)O_(19+δ)催化剂具有最好的反应活性。而对于LaNi_xCo_(1-x)Al_ (11)O_(19+δ)系列催化剂，当x ≤ 0.375时，随x值的增大，催化活性明显提高， 但在0.375 ≤ x ≤ 1.0范围内，催化活性几乎保持不变。由此得到结论，对于此 反应来说，控制Ni量在0.375 ≤ x ≤ 0.50范围内比较合适。     

焙烧温度对甲醇水蒸气重整制氢Ce/Cu/Zn-Al水滑石衍生催化剂的影响

采用原位合成法在γ-Al_2O_3载体表面上合成了Zn-Al水滑石,再采用顺序浸渍法制备了一系列Ce/Cu/Zn-Al催化剂,并采用XRD、BET、H_2-TPR和XPS等手段对催化剂进行了表征,考察了焙烧温度对Ce/Cu/Zn-Al催化剂表面结构及其催化甲醇水蒸气重整制氢性能的影响。结果表明,焙烧温度主要影响了催化剂的Cu比表面积、表面氧空穴含量和Cu-Ce间相互作用。当焙烧温度为500℃时,催化剂Cu的比表面积较大,表面氧空穴含量较多,Cu-Ce间相互作用较强,因此,催化甲醇水蒸气重整制氢活性较好。当焙烧温度升高到700℃时,Cu物种主要以稳定的CuAl_2O_4尖晶石形式存在,不利于甲醇水蒸气重整制氢反应的进行,因此,催化活性较差。     

Ce的浸渍顺序对Cu/Zn-Al水滑石衍生催化剂用于甲醇水蒸气重整制氢性能的影响

采用原位合成法在γ-Al_2O_3载体上合成了锌铝水滑石,再经浸渍法制备了Cu/Zn-Al、Ce/Cu/Zn-Al、Cu/Ce/Zn-Al和Cu-Ce/Zn-Al催化材料,使用XRD、XRF、SEM、氮吸附,XPS、H_2-TPR和N_2O滴定等手段对其进行了表征,探讨了Ce的浸渍顺序对Cu/Zn-Al水滑石衍生材料甲醇水蒸气重整制氢反应催化性能的影响。结果表明,Ce的浸渍顺序主要影响催化剂的还原性质,进而影响了其催化性能。其中,Ce/Cu/Zn-Al催化剂的催化性能最佳,在250℃、水醇物质的量比为1.2、甲醇气体空速为800 h~(-1)的条件下,甲醇转化率达到100%;与Cu/Zn-Al催化剂相比,甲醇转化率提高了近40%。     

铁取代六铝酸盐的制备及其对甲烷燃烧的催化性能

 采用共沉淀-水热处理法制备了铁取代六铝酸盐(BaFexAl12-xO19-δ,x≤3)催化剂,并用XRD,SEM,UV-Vis和BET等技术对催化剂进行了表征. 结果表明,经1000 ℃焙烧后催化剂开始出现少量六铝酸盐相,1100 ℃焙烧后六铝酸盐相为主要的晶相,当x＞3时催化剂中的杂质相不可忽略. Fe取代六铝酸盐中的Fe主要为Oh配位. 在x≤3范围内,随着Fe取代量的增加,催化剂对甲烷燃烧的催化活性逐渐升高,其中BaFe3Al9O19-δ的起燃温度最低(515 ℃); 继续增加Fe含量,催化剂的高温活性反而下降. 向Fe单取代六铝酸盐晶格中引入La制得的Ba0.5La0.5FeAl11O19-δ催化剂,其起燃活性与BaFeAl11O19-δ的基本相同,但高温活性有较大提高. 反应气组成对催化剂的活性有显著影响,提高O2分压可以降低催化剂的起燃温度,但对高温活性的影响不大. BaFe2Al10O19-δ催化剂在800 ℃下运行100 h没有发生失活现象.     

铈镧比对Ce_xNi_(0.5)La_(0.5-x)O系催化剂甘油氧化蒸汽重整制氢性能的影响（英文）

利用共沉淀法制备了CeO_2和La_2O_3复合载体的Ce_xNi_(0.5)La_(0.5-x)O(CeNiLaO)系催化剂,在固定床反应器中考察其甘油氧化蒸汽重整制氢(OSRG)性能,并采用X射线衍射(XRD)、程序升温还原(H_2-TPR)、激光拉曼光谱(Raman)、扫描电子显微镜(SEM)、透射电子显微镜(TEM)和X射线光电子能谱(XPS)等手段对催化剂进行表征分析。结果表明:La_2O_3能够有效地分散Ni颗粒,减弱Ni颗粒在反应过程中的烧结,CeO_2提供的晶格氧能够消除催化剂表面的积碳,同时La会部分进入Ce的晶格取代部分Ce~(4+)造成晶格畸变,提高表面的氧空穴数。La_2O_3和CeO_2的共同作用有利于减弱Ni因为烧结和积碳引起的失活。在不同Ce/La摩尔比的催化剂中,Ce_(0.4)Ni_(0.5)La_(0.1)O表现出最好的催化活性,并且该催化剂在长达210 h的稳定性测试中,甘油的转化率都在95%以上,气相产物中的氢气浓度达50%。     

低温下Pt/Al_2O_3和Pd/Al_2O_3光辅助乙二醇水相重整制氢研究

采用浸渍还原法制备了氧化铝负载的Pt和Pd纳米颗粒催化剂,用于光辅助乙二醇水相重整制氢反应。结果表明,光照能够有效降低乙二醇水相重整制氢的活化能,Pt/Al_2O_3比Pd/Al_2O_3具有更高的H_2转换频率(TOF)和更低的CO选择性。采用XRD、TEM、UV-vis等技术对催化剂的结构和形貌进行了表征,原位漫反射红外光谱(DRIFTS)表明,光照能促进乙二醇分子O-H键的断裂。理论计算表明,Pt/Al_2O_3催化乙二醇重整制氢反应产物中较低的CO选择性主要归因于CO在Pt表面较小的反应能垒,能够较快与H_2O解离的O反应生成CO_2。     

Co-Ni／SiO2催化剂催化乙酸重整制氢反应研究

用浸渍法制备了一系列Co-Ni/SiO2催化剂,利用固定床反应器对催化剂在乙酸重整制氢反应中的催化性能进行了测试,详细研究了Co-Ni配比、活性组分负载量,反应温度,空速及水碳比对催化剂活性的影响.实验结果表明,该催化剂能高效催化乙酸重整反应.当Co和Ni摩尔比例为0.5∶1,活性组分质量百分含量为15%时催化剂呈现最好的催化活性,在水碳摩尔比为7.5∶1,温度大于500℃时可使乙酸完全转化,并且氢和二氧化碳选择性均达95%以上.     

微波水热改性制备S_2O_8~(2-)/Fe_2O_3-SiO_2固体酸及催化性能

对共沉淀法得到的Fe2O3-SiO2混合氧化物前驱物进行微波水热改性处理,经浸渍(NH4)2S2O8后再焙烧得S2O82-/Fe2O3-SiO2固体酸催化剂。用XRD、TEM、N2气吸附/脱附及化学分析方法对其进行了表征,用乙酸/丁醇酯化催化反应评估固体酸的催化性能,并与通常条件下制得的催化剂进行了比较。结果显示,引入SiO2会延迟Fe2O3晶体的形成与长大;对前驱物用250W的微波水热改性处理1.5h,制得的固体酸具有适中的比表面积、均匀的孔径分布,含硫量为6.02%,比表面积为37.1m2/g。该固体酸对乙酸丁醇酯化反应有很高的催化活性,催化酯化反应3h,乙酸的转化率高达97.7%。     

Sol–gel synthesis of nanocrystalline Zn1−xNixFe2O4 ceramics and its structural,magnetic and dielectric properties

Zn_1?xNi_xFe₂O₄ (0.0 ≤ x ≤ 1.0) nanoparticles are prepared by sol–gel method using urea as a neutralizing agent. The evaluation of XRD patterns and TEM images indicated fine particle nature. The average crystallite size increased from 10 to 24 nm, whereas lattice parameters and density decreased with increasing Ni content (x). Infrared spectra showed characteristic features of spinel structure along with a strong influence of compositional variation. Magnetic measurements reveal a maximum saturation magnetization for Zn_0.5Ni_0.5Fe₂O₄ (x = 0.5); however, reduced value of magnetization is attributed to the canted spin structure and weakening of Fe³⁺(A)–Fe³⁺(B) interactions at the surface of the nanoparticles. Impedance analysis for different electro-active regions are carried out at room temperature with Ni substitution. The existence of different relaxations associated with grain, grain boundaries and electrode effects are discussed with composition. It is suggested that x = 0.5 is an optimal composition in Zn_1?xNi_xFe₂O₄ system with moderate magnetization, colossal resistivity and high value of dielectric constant at low frequency for their possible usage in field sensor applications.     

Nanocrystalline Ni0.6Zn0.4Fe2O4: A novel semiconducting material for ethanol detection

The structure and crystal phase of the nanocrystalline powders of Ni_1−xZn_xFe₂O₄ (0 ≤ x ≤ 0.5) mixed ferrite, synthesized by ethylene glycol mediated citrate sol-gel method, were characterized by X-ray diffraction and microstructure by transmission electron microscopy. Further studies by Fourier transform infrared spectroscopy were also conducted. Moreover, DC electrical properties of the prepared nanoparticles were studied by DC conductivity measurements. The response of prepared Ni_1−xZn_xFe₂O₄ mixed ferrites to different reducing gases (ethanol, hydrogen sulfide, ammonia, hydrogen and liquefied petroleum gas) was investigated. In particular, Ni_0.6Zn_0.4Fe₂O₄ composition exhibited high response to 100 ppm ethanol gas at 300 °C. Incorporation of palladium further improved the response, selectivity and response time of Ni_0.6Zn_0.4Fe₂O₄ to ethanol gas with the blue shift in the operating temperature by 25 °C.     

Ultrasonic-assisted synthesis of PMMA/Ni0.5Zn0.5Fe2O4 nanocomposite in mixed surfactant system

PMMA/Ni_0.5Zn_0.5Fe₂O₄ nanocomposite with superparamagnetic behavior was synthesized by in situ emulsion polymerization of methylmethacrylate (MMA) monomer in the presence of Ni_0.5Zn_0.5Fe₂O₄ colloidal suspension assisted by ultrasonic irradiation. The obtained samples were characterized by X-ray diffraction (XRD), Fourier transform infrared spectra (FT-IR), transmission electron microscopy (TEM) and vibrating sample magnetometer (VSM). XRD and FT-IR spectra confirmed the formation of PMMA/Ni_0.5Zn_0.5Fe₂O₄ nanocomposite. TEM images showed that Ni_0.5Zn_0.5Fe₂O₄ nanoparticles with the particle sizes of about 12 nm were well dispersed in the polymer matrix. The nanocomposite at room temperature exhibited superparamagnetic behavior under applied magnetic field. The formation mechanism of PMMA/Ni_0.5Zn_0.5Fe₂O₄ nanocomposite was proposed as well.     

Influence of solid-phase ferritization method on phase composition of lithium-zinc ferrites with various concentration of zinc

Methods of X-ray phase analysis (XRPA) and differential thermogravimetry in a magnetic field (DTG(M)) are used to investigate the phase composition of Li_0.5(1?x)Fe_2.5?0.5x Zn _x O₄ (x _Zn?=?0.2, 0.4, and 0.6) ferrite spinels synthesized at a temperature of 700?°C during 120?min by thermal annealing of a reagent mixture in a furnace and heating of the mixture using high-power beam of accelerated electrons with energy of 2.4?MeV. Thermal ferritization of all compositions leads to the formation of phases whose composition is close to simple monoferrites. Lithium?Czinc ferrite phases are formed during annealing under electron irradiation. It is concluded that the rate of controllable diffusion interaction of monoferrite phases significantly increases under conditions of high-power electron irradiation.     

单分散NixZn1-xFe2O4纳米颗粒的制备及其磁热效应

以乙酰丙酮金属盐为前驱体,三乙二醇为溶剂,采用多元醇法制备了镍锌不同配比的Ni_xZn_(1-x)Fe_2O_4(x=0,0.3,0.5,0.7和1.0)铁氧体,并通过X射线衍射仪(XRD),透射电子显微镜(TEM)和振动样品磁强计(VSM)等对样品的结构、形貌、磁性能和磁热性能进行了表征。结果表明:Ni_xZn_(1-x)Fe_2O_4铁氧体分散性较好,尺寸均一,形状近似球形,平均粒径为4~5 nm。Ni_xZn_(1-x)Fe_2O_4纳米颗粒在室温下表现出亚铁磁性,饱和磁化强度随着镍含量的增加先增大后减小,当x=0.5时达到最大值29.38 emu·g~(-1)。在382k Hz交变磁场作用下,Ni_(0.5)Zn_(0.5)Fe_2O_4铁氧体温度可升温至313 K,表现出较好的磁热性能。     

Mechanism of NiZn ferrite formation

The regularities in the change of character of the ferrite formation process as a function of Ni_1?xZn_xFe₂O₄ solid solution and of the degree of zinc oxide saturation of the Ni_1?xZn_xO solid solution (x = 0.14; 0.29; 0.43) are established in the temperature range 1220–1305°C. It is shown that in the reaction zone of interacting NiO, (Ni, ZnO), or ZnO with Fe₂O₃ the ferrite phase crystallizes only on iron oxide. The distribution of the Fe, Ni, and Zn concentrations over the reaction layer thickness using electron probe and X-ray spectrum analysis is obtained. The interdiffusion coefficients over the investigated temperature range calculated in the (Ni, Zn, Fe)O and ferrite phases change from (0.8 – 7.0) × 10^?9 to (1.0 – 12.0) × 10^?10 cm²/sec, respectively. The interaction of (Ni, Zn)O with Fe₂O₃ takes place by the mechanism of interaction of interdiffusion of Fe³⁺, Fe²⁺ and Ni²⁺, Zn²⁺ along with a current of Zn²⁺ ions and electrons or oxygen ions directed to the $\text{ferrite}\text{Fe}{}_2\text{O}{}_3$ interface.     

Enzyme mimics of spinel-type CoxNi1−xFe2O4 magnetic nanomaterial for eletroctrocatalytic oxidation of hydrogen peroxide

A series of spinel-type Co_xNi_1−xFe₂O₄ (x = 0, 0.2, 0.4, 0.5, 0.6, 0.8, 1.0) magnetic nanomaterials were solvothermally synthesized as enzyme mimics for the eletroctrocatalytic oxidation of H₂O₂. X-ray diffraction and scanning electron microscope were employed to characterize the composition, structure and morphology of the material. The electrochemical properties of spinel-type Co_xNi_1−xFe₂O₄ with different (Co/Ni) molar ratio toward H₂O₂ oxidation were investigated, and the results demonstrated that Co_0.5Ni_0.5Fe₂O₄ modified carbon paste electrode (Co_0.5Ni_0.5Fe₂O₄/CPE) possessed the best electrocatalytic activity for H₂O₂ oxidation. Under optimum conditions, the calibration curve for H₂O₂ determination on Co_0.5Ni_0.5Fe₂O₄/CPE was linear in a wide range of 1.0 × 10⁻⁸–1.0 × 10⁻³ M with low detection limit of 3.0 × 10⁻⁹ M (S/N = 3). The proposed Co_0.5Ni_0.5Fe₂O₄/CPE was also applied to the determination of H₂O₂ in commercial toothpastes with satisfactory results, indicating that Co_xNi_1−xFe₂O₄ is a promising hydrogen peroxidase mimics for the detection of H₂O₂.     

A highly coercive carbon nanotube coated with Ni0.5Zn0.5Fe2O4 nanocrystals synthesized by chemical precipitation-hydrothermal process

Novel magnetic composites (Ni_0.5Zn_0.5Fe₂O₄-MWCNTs) of multi-walled carbon nanotubes (MWCNTs) coated with Ni_0.5Zn_0.5Fe₂O₄ nanocrystals were synthesized by chemical precipitation-hydrothermal process. The composites were characterized by X-ray powder diffractometer (XRD), X-ray photoelectron spectrometer (XPS), Fourier transform infrared spectroscopy (FTIR), Mössbauer spectroscopy (MS), transmission electron microscopy (TEM), and selected area electron diffraction (SAED), etc. A temperature of about 200 °C was identified to be an appropriate hydrothermal condition to obtain Ni_0.5Zn_0.5Fe₂O₄-MWCNTs, being lower than the synthesis temperature of a single-phase Ni_0.5Zn_0.5Fe₂O₄ nanocrystals. The sizes of Ni_0.5Zn_0.5Fe₂O₄ in the composites were smaller than those of Ni_0.5Zn_0.5Fe₂O₄ nanocrystals in single phase. The composites exhibited more superparamagnetic than Ni_0.5Zn_0.5Fe₂O₄ nanocrystals in their relaxation behaviors. The magnetic properties measured by a vibrating sample magnetometer showed that the composites had a high coercive field of 386.0 Oe at room temperature, higher than those of MWCNT and Ni_0.5Zn_0.5Fe₂O₄ nanocrystals.     

One-dimensional NiCuZn ferrite nanostructures: Fabrication, structure, and magnetic properties

Ni_0.5−xCu_xZn_0.5Fe₂O₄ (0.0≤x≤0.5) ferrite nanofibers with diameters of 80-160 nm have been prepared by electrospinning and subsequent heat treatment. Both the average grain size and lattice parameter are found to increase with the addition of copper. Fourier transform infrared spectra indicate that the portion of Fe³⁺ ions at the tetrahedral sites move to the octahedral sites as some of the substituted Cu²⁺ ions get into the tetrahedral sites. Vibrating sample magnetometer measurements show that the coercivity of these ferrite nanofibers decreases with increasing Cu concentration, whereas the specific saturation magnetization initially increases, reaches a maximum value at x=0.2 and then decreases with the Cu content further increase. Notable differences in magnetic properties at room temperature (298 K) and 77 K for the Ni_0.3Cu_0.2Zn_0.5Fe₂O₄ nanofibers and corresponding powders are observed and mainly arise from the grain size and morphological variations between these two materials.     

Analysis of the phase composition and homogeneity of ferrite lithium-substituted powders by the thermomagnetometry method

In the present work, the possibilities of application of the thermomagnetometry TG(M)/DTG(M) method for estimation of the phase homogeneity of end products of synthesis at different stages of ferritizing annealing are considered on the example of solid-state synthesis of Li_0.5(1?x)Fe_2.5?0.5xZn_xO₄ and Li_0.5(1 + x)Fe_2.5?1.5xTi_xO₄ (x = 0.1, 0.2, 0.3, 0.4, 0.5, and 0.6) lithium-substituted ferrospinels. Results of thermomagnetometric analysis are compared with XRD data. It is shown that the resolution of the TG(M)/DTG(M) method on two orders exceeds capabilities of the traditional XRD method. Considerable influence of both intermediate grinding and mixing of samples and concentration of an inducted impurity on the homogeneity of the synthesized powders is confirmed.