活性炭表面性质对Pd/C常温氧化CO的影响

采用等体积浸渍法制备了活性炭负载Pd催化剂(Pd/C),通过正交实验研究了活性炭的种类、催化剂的制备条件等对活性炭负载钯催化剂上CO氧化性能的影响,得到了最优的制备条件。并通过N2吸附、程序升温脱附(TPD)、程序升温还原(H2-TPR)和透射电镜(TEM)等对催化剂进行了表征。正交实验极差分析表明制备各因素对催化剂氧化CO活性影响的次序为:还原剂>活性炭>还原剂用量>还原温度>还原溶pH值。催化剂表征结果表明活性炭的比表面积和孔径分布不是决定Pd/C催化剂性能的关键因素,活性炭的种类、表面组成和性质对催化剂的性能有显著的影响。其中椰壳炭(AC1)表面羧基的活性较高,同时具有较强的表面碱性,有利于活性金属Pd在载体表面的分散,并提高了Pd与载体之间的相互作用,从而使催化剂具有较高的CO氧化性能。提高Pd的担载量,可显著提高催化剂稳定性。以乙二醇作为还原剂,在pH=10,还原温度为60℃的条件下所制备的0.5%Pd/AC催化剂,在反应温度20℃时连续反应120 h仍可保持CO的全转化。     

Rh/C催化剂的制备及其催化性能研究

以RhCl3.3H2O为前驱体,活性炭为载体,采用浸渍法制备了Rh/C催化剂,并使用场发射透射电镜对催化剂进行了表征。同时考察了制备条件对Rh/C催化剂在6-羟基-3,4-二氢异喹啉-2-甲酸甲酯-3-甲酸乙酯加氢反应中催化性能的影响。     

烧结烟气脱硫脱硝活性炭的研究进展

活性炭因具有较大的比表面积和孔容,较强的吸附能力,原料成本低,制备方式简单及可重复使用等优点成为目前常用的脱硫脱硝方式之一,在烟气净化领域得到广泛的应用。活性炭的比表面积、表面的孔结构和表面官能团及活性组分对活性炭脱硫脱硝性能有较大影响,适当增加活性炭含氧、氮官能团或表面活性组分有利于活性炭物理吸附和化学吸附能力协同增长。介绍了活性炭脱硫脱硝的原理,综述了脱硫脱硝活性炭的制备和表面改性的研究进展,分析了活性炭原料配比、活性剂种类、改性方式对活性炭脱硫脱硝的影响。明确了优化制备原料及改性方式与活性炭脱硫脱硝反应之间的机制和规律性研究将会成为未来的研究重点。     

镍基钯、铂双组分催化剂催化燃烧的研究

以甲苯蒸气和正己烷蒸气作为催化燃烧气,研制和考察了镍基合金作为载体Pd,Pt双组分燃烧催化剂的对有机废气催化燃烧性能的影响,并对催化剂的表面形貌进行了分析。结果表明,在Pd含量一定的情况下,Pt含量的不同对催化剂的活性有一定的影响,特别是对直链烃的催化燃烧有较大的影响,在此基础上确定了合理的Pd,Pt负载含量。     

DMFC阳极催化剂Pt-Ru/SWCNTs制备工艺和性能研究

采用化学液相还原法在单壁碳钠米管（SWCNTs）载体上制备了20％Pt-10％Ru／SWCNTs甲醇阳极催化剂。研究了H2PtCk—RuCl3浓度、反应温度和SWCNTs纯化对PtRu／SWCNTs催化剂颗粒的影响。以20％Pt／C作阴极催化剂，以氧气作阴极氧化剂，考察了PtRu／SWCNTs阳极催化剂用量、Nation含量和PrrFE含量对单DMFC性能的影响。实验结果表明，H2PtCl6-RuCl3浓度为0．005-0．005g·cm^-1，反应温度为60℃，单壁碳纳米管经纯化后所制备的PtRu／SWCNTs催化剂具有较小的粒径和较大的表面积。PtRu／SWCNTs用量和Nafion与PTFE含量分别为0．6mgPt·cm^-2，7％和为5％时，单电池具有较好的性能。     

Pt-NbOx/C、Pt-ZrO2/C复合氧电极催化剂的制备及性能研究

以NbOx、ZrO2作为助催化剂,采用分步法制备得到Pt-NbOx/C、Pt-ZrO2/C复合催化剂,采用XRD、SEM等手段分析了催化剂的物相及形貌特征。通过循环伏安法、阴极极化曲线等电化学方法对催化剂的电化学性能进行了研究。结果表明,Pt均匀分布在载体表面,颗粒大小均在5 nm以下;NbOx和ZrO2的加入没有改变氧的还原反应机理,与Pt/C、Pt-ZrO2/C催化剂相比,Pt-NbOx/C复合催化剂催化氧电化学还原过程的活性有了明显提高。     

不同孔结构硅藻土载体对钒催化剂催化性能的影响

用3种不同孔结构硅藻土作载体制备钒催化剂,研究了载体孔结构对钒催化剂催化性能的影响,借助XRF、XRD、FT-IR、SEM、MIP等对钒催化剂进行表征,在小型固定床反应器中对催化性能进行评价。结果表明:硅藻土的孔结构对钒催化剂的催化性能有显著影响,负载硅藻土后,钒催化剂孔径增大,催化活性增强。     

Al-Si@Al2O3核壳结构载体的制备及其催化应用

以微米级铝硅（Al-Si）合金粉为原料,采用简单的水热反应,设计开发出一种以鳞片状Al2O3为壳、Al-Si 合金为核的催化剂载体（Al-Si@Al2O3）。通过傅里叶红外分析（FT-IR）、X 射线衍射（XRD）、扫描电镜（SEM）及透射电镜（TEM）等表征分析表明,经过水热反应后,Al-Si 合金表面原位生成片状的AlOOH,内核为未反应的Al-Si合金,500℃煅烧后浸渍载Pd制备出Pd/Al-Si@Al2O3催化剂,活性组分Pd粒子均匀分散在载体表面。以苯乙烯加氢为探针反应考察Al-Si合金原料的粒径、铝含量等因素对所制备催化剂性能的影响,同时还与水浴、碱处理及酸处理所制备的载体和传统载体活性炭、活性氧化铝进行比较。结果表明,在水热条件下,以粒径为5μm、铝含量为88%的Al-Si合金粉为原料制备的Pd/Al-Si@Al2O3具有较优的催化性能,且其催化活性优于活性炭和活性氧化铝载Pd催化剂。     

介孔CeO_2载体织构性质对Au-Pd催化剂性能的影响

以硝酸铈铵为前驱体,分别采用表面活性剂嵌段共聚物F127、十六烷基三甲基溴化铵(CTAB)和十六胺(HDA)合成介孔CeO2(m-CeO2)载体,研究了m-CeO2织构性质对Au-Pd双金属催化剂甲醇部分氧化制氢性能的影响,并运用HRTEM、XRD、TPR、H2-TPD、CO2-TPD和低温N2吸附等手段对Au-Pd双金属催化剂进行了表征。结果表明,HDA为表面活性剂合成的m-CeO2(H4)具有较大的比表面、孔容和孔径。H4负载的Au-Pd催化剂显示出较高的催化活性和氢气选择性。表征结果表明,Au-Pd/H4催化剂中贵金属的分散度较高、形成的Au、Pd活性中心较多,金属与载体的相互作用较强,表面的碱中心较多,产物H2较易脱附。     

有机废气燃烧镍基钯催化剂的研究

以甲苯蒸气和乙二醇二甲醚蒸气作为催化燃烧气,研究了3种不同钯含量镍基合金负载型催化剂对有机废气催化燃烧性能的影响,并用SEM和EDS对催化剂的表面形貌进行了分析。结果表明,钯含量的不同对催化剂的活性有较大影响,确定了合理的钯负载含量。以一定预处理后的镍基合金作为载体,钯催化剂性能优良,并提出了该催化剂较好的制备方法。     

Support interaction of Pt/CeO_2 and Pt/SiC catalysts prepared by nano platinum colloid deposition for CO oxidation

The interaction between Pt and its various supports can regulate the intrinsic electronic structure of Pt particles and their catalytic performance.Herein,Pt/CeO_2 and Pt/SiC catalysts were successfully prepared via a facile Pt colloidal particle deposition method,and their catalytic performance in CO oxidation was investigated.XRD,TEM,XPS and H_2-TPR were used to identify the states of Pt particles on the support surface,as well as their effect on the performance of the catalysts.Formation of the Pt-O-Ce interaction is one of the factors controlling catalyst activity.Under the oxidative treatment at low temperature,the Pt-O-Ce interaction plays an important role in improving the catalytic activity.After calcining at high temperature,enhanced Pt-O-Ce interaction results in the absence of metallic Pt~0 on the support surface,as evidenced by the appearance of Pt~(2+) species.It is consistent with the XPS data of Pt/CeO_2,and is the main reason behind the deactivation of the catalyst.By contrast,either no interaction is formed between Pt and SiC or Pt nanoparticles remain in the metallic Pt~0 state on the SiC surface even after aging at 800℃in an oxidizing atmosphere.Thus,the Pt/SiC shows better thermal stability than Pt/CeO_2.The interaction between Pt and the active support may be concluded to be essential for CO oxidation at low temperature,but strong interactions may induce serious deactivation of catalytic activity.     

NiO催化臭氧氧化降解水中双酚A的研究

采用均匀沉淀法制备NiO催化剂催化臭氧氧化降解水中双酚A,并利用XRD、SEM、BET及孔径分析等表征手段对催化剂结构和性质进行表征.研究不同pH、臭氧流量、催化剂投加量、反应时间等因素对双酚A降解效果的影响.结果表明,制备的NiO催化剂成絮状结构,催化剂表面蓬松且粗糙,催化剂比表面积较大,且成介孔结构,在催化反应中可提供较多的反应活性位点.在初始pH值为6,臭氧流量为10 mg/min,催化剂投加量为1.0 g/L,反应时间为75 min条件下,双酚A初始浓度为100 mg/L时其降解率达95.3 %.叔丁醇抑制实验表明,NiO催化臭氧氧化降解水中双酚A主要为催化剂催化O₃分解产生·OH间接氧化.      

Effect of active oxygen on the performance of Pt/CeO2 catalysts for CO oxidation

This study was focused on the influence of active oxygen on the performance of Pt/CeO_2 catalysts for CO oxidation. A series of CeO_2 supports with different contents of active oxygen were obtained by adding surfactant at different synthesis steps. 0.25 wt% Pt was loaded on these CeO_2 supports by incipientwetness impregnation methods. The catalysts were characterized by N2 adsorption, X-ray diffraction(XRD), high-resolution transmission electron microscopy(HRTEM), H_2 temperature-programmed reduction(H_2-TPR), dynamic oxygen storage capacity(DOSC) and in-situ DRIFTS technologies. For S-f supports, the surfactant was added into the solution before spray-drying in the synthesis process, which facilitates more active oxygen formation on the surface of CeO_2. After loading Pt, the more active oxygen on CeO_2 contributes to dispersing Pt species and enhancing the CO oxidation activity. As for the aged samples,Pt-R-h shows the highest activity above 190 ℃ because of the presence of more partly oxidized Pt~(δ+) species. Thus the activity is also influenced by the states of Pt and the Pt~(δ+) species may contribute to the high activity at elevated temperature.     

Effect of cerium oxide prepared under different hydrothermal time on electrocatalytic performance of Pt-based anode catalysts

In this paper,CeO_2 with a pore size of 2-4 nm was synthesized by hydrothermal method.The CeO_2 modified graphene-supported Pt catalyst was prepared by the microwave-assisted ethylene glycol reduction chloroplatinic acid method,and the effect of the addition of CeO_2 prepared by different hydrothermal reaction time on the catalytic performance of Pt-based catalysts was investigated.The microstructures of CeO_2 and catalysts were characterized by X-ray diffraction(XRD),X-ray photoelectron spectroscopy(XPS),specific surface area and pore size analyzer(BET),scanning electron microscopy(SEM) and electron spectroscopy(EDAX),transmission electron microscopy(TEM),and the catalysts electrochemical performance was tested by electrochemical workstation.The results show that the catalytic performance of the four catalysts with CeO_2 is better than that of the catalyst without CeO_2.Adding CeO_2 with a specific surface area of 120.15 m~2/g prepared by hydrothermal reaction time of 39 h to Pt/C synthesis catalyst,its electrocatalytic performance,stability and resistance to poisoning are the best.The electrochemical active surface area is 102.83 m~2/g,the peak current density of ethanol oxidation is 757.17 A/g and steady-state current density of 1100 s is 108.17 A/g which shows the lowest activation energy for ethanol oxidation reaction.When the cyclic voltammogram is scanned for 500 cycles,the oxidation peak current density retention rate is 87.74%.     

Mechanism of CeO_2 synthesized by thermal decomposition of Ce-MOF and its performance of benzene catalytic combustion

In this paper,the formation mechanism of mesoporous CeO_2 synthesized by thermal decomposition of Ce-MOF and its performance of benzene catalytic combustion,as well as the structure-activity relationship between them were studied in depth.The self-assembly process and physicochemical properties of CeO_2 were characterized by thermogravimetry analysis,powder X-ray diffraction,N_2 adsorption/desorption,high-resolution transmission electron microscopy and X-ray photoelectron spectroscopy techniques.Characterization results show that Ce-MOF is completely decomposed into pure mesoporous CeO_2 when the decomposition temperature is higher than 400℃.At this threshold temperature,CeO_2(400) has the largest specific surface area and pore volume of 114 m~2/g and 0.152 cm3/g,respectively.CeO_2(400) exhibits very high catalytic activity for benzene combustion,which can completely catalyze the degradation of benzene at 260℃.Meanwhile,the mesoporous CeO_2(400) supported Pt nanocrystalline catalysts were prepared by high temperature solution-phase reduction method.Pt/CeO_2(400)can completely degrade benzene at about 200℃ and represents high durability and good waterresistance for benzene combustion during 100 h of continuous reaction.     

Preparation of Au/CeO2 catalyst and its catalytic performance for HCHO oxidation

Aqueous precipitation and deposition-precipitation method were used to prepare CeO2 supports and Au/CeO2 catalysts, respectively. The effect of preparation condition of support on the catalyst activity was investigated. The catalytic combustion of HCHO was considered as the probe reaction for comparing the catalyst activity. The BET, X-ray diffraction, X-ray photoelectron spectroscopy （XPS）, and reduction （TPR） were carried out to analyze the influence factor on the catalysts activity. The results showed that the addition of dispersant and use of microwave in the support preparation procedure could be beneficial for enhancing the interaction of supports and gold species and thus improved the catalytic activity. The total conversion temperature for HCHO was 146 ℃ over AC400. With the modification during supports preparation process, the catalytic activity increased with total conversion temperature decreasing to 98 ℃. The results of XPS indicated that Au^0 and Au^＋1 species coexisted in these catalysts and the activity of catalyst correlated with Au^＋1/Au^0 ratio. Temperature-programmed reduction results demonstrated that the reduction peak appeared between 100-170 ℃ with the inducing of gold. The dependence of activity on the reduction peak temperature implied that ionic gold was catalytic activity component for HCHO oxidation.     

离子交换树脂对Pt/C催化剂耐久性的影响

离子交换树脂（Ionomer）是质子交换膜燃料电池催化层的重要组成部分,它在催化层中的主要作用是作为质子传导相传导质子。本文采用旋转圆盘电极法（RDE）,在模拟燃料电池真实的运行环境（模式一）和模拟燃料电池启停环境（模式二）两种模式下,研究了Ionomer对铂碳催化剂电压循环耐久性的影响。通过相同位置透射电镜分析法（IL-TEM）,分析了铂碳催化剂经历模式二耐久性测试后的结构变化。研究发现Ionomer的存在可以提高铂碳催化剂的耐久性。在模式一的测试中:添加Ionomer后,其氧还原半波电位下降值?E从23 mV下降至11 mV;没有发生碳的腐蚀,Pt颗粒的长大是催化剂性能下降的主要原因;Ionomer的存在延缓了Pt电化学比表面积（ECSA）的降低从而有利于保持Pt的活性。在模式二的测试中:添加Ionomer后,其氧还原半波电位下降值?E从25 mV下降至5 mV,除了铂颗粒长大外还发生了载体碳的腐蚀;Ionomer的存在同样可以保持Pt的活性;IL-TEM分析可以看到明显的铂颗粒长大和碳腐蚀,碳载体的腐蚀造成铂的严重流失和团聚。含Nafion的催化剂中铂颗粒平均粒径从2.7 nm增加到了3.76 nm,不含Nafion的催化剂中的铂颗粒平均粒径从2.44 nm增加到了4.19 nm。      

Catalytic Incineration of Acrylonitrile with Platinum Supported on Al2O3

The catalytic decomposition of acrylonitrile with catalysts was investigated in a bench scale fixed bed reactor in this study. Two catalysts, including Pt/γ-Al2O3 and Cr2O3/α-Al2O3, were tested to study their catalytic activity in the complete oxidation of acrylonitrile. The results show that the Pt/γ-Al2O3 catalyst has better performance. The operating parameters such as operating temperature, acrylonitrile concentration, space velocity, and oxygen concentration were conducted in a series of experiments on the Pt/γ-Al2O3 catalyst. The results indicate that decomposition efficiency increases with temperature and oxygen concentration and decreases with the increases of space velocity and acrylonitrile concentration. With a regression model, the operating temperature is the most effective parameter on the decomposition of acrylonitrile. Carbon dioxide is the dominant product and carbon monoxide is an insignificant product of the decomposition of acrylonitrile. Material balance on carbon is good for the experiments. According to the BET and elemental analyzer analysis, major factors that cause the deactivation effect may result from nitrogen poisoning and carbon masking on the catalyst surface, especially at lower temperatures.     

Construction of bimetallic Pt-Pd/CeO2-ZrO2-La2O3 catalysts with different Pt/Pd ratios and its structure-activity correlations for three-way catalytic performance

A series of Pt-Pd bimetallic catalysts supported on CeO₂-ZrO₂-La₂O₃ mixed oxides were synthesized through the conventional impregnation method.Three-way catalytic performance evaluations along with detailed physio-chemical characterizations were carried out to establish possible structure-activity correlations.Results show that on the one hand,different Pt/Pd ratios can strongly affect the TWC behaviors of Pt-Pd/CZL catalysts by modulating the synergis...     

Oxidation of Toluene in Waste Gas Streams Using Mesoporous Ti-Hexagonal Mesoporous Silica

Various mesoporous catalysts with titanium loadings between 0.5 and 4 Ti wt.?% and surface areas between 600 and 1,600 m2/g were synthesized using the molecular designed dispersion technique. These catalysts were tested using toluene oxidation in a fixed bed reactor at temperatures between 300 and 550°C. The reaction products were found to be CO2 and CO with selectivity towards CO2 above 80% for all catalysts. The catalytic activity of the catalysts increases with titanium loading. The total conversion at 550°C was not affected by the textural porosity, but increased textural porosity did significantly reduce the ignition temperature by up to 50°C. The Thiele modulus was calculated to be much less than one for all these materials indicating that the reaction rate is not diffusion limited.