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1.
以硝酸钴(Co(NO3)2·6H2O)为钴源,考察了不同沉淀剂(6 mol/L氨水、1 mol/L NaOH溶液、饱和碳酸铵溶液)对Co3O4吸附2,4-二氯苯酚(2,4-DCP)性能的影响。考察了焙烧温度、pH值、沉淀剂种类、吸附剂用量、2,4-DCP初始质量浓度对Co3O4吸附性能的影响,并进行了离子干扰实验。结果表明,焙烧温度为300℃、pH=9.0、沉淀剂为1 mol/L NaOH时,Co3O4对20 mg/L 2,4-DCP吸附性能最佳。Co3O4对2, 4-DCP的动力学吸附过程符合准二级动力学方程,等温吸附方程符合Langmuir方程,吸附过程以单分子层化学吸附为主。  相似文献   

2.
采用熔融-淬冷法制备了不同(Al2O3+P2O5)含量的碱铝硅酸盐玻璃,通过拉曼光谱、X射线衍射光谱、扫描电镜研究了其结构特征和析晶性能。发现随着(Al2O3+P2O5)含量减少,玻璃中Na2O含量增加,玻璃化转变温度从685 ℃降低到622 ℃,当减少至摩尔分数为22%时,出现析晶峰且起始析晶温度降低。拉曼光谱表明Q4P对应的拉曼峰强度变低且逐渐向低波数方向移动,说明Na2O作为网络修饰体使硅酸盐玻璃结构逐步解聚,玻璃的析晶能力逐渐增强。结果表明:当(Al2O3+P2O5)摩尔分数为22%时热处理后的样品存在晶型转变,700 ℃热处理时以NaAlSiO4霞石晶体为主,900 ℃时转变为以Na6.8Al6.3Si9.7O32霞石晶体为主。当(Al2O3+P2O5)的摩尔分数为21%和20%时,热处理后的样品能稳定析出Na3PO4和Na6.8Al6.3Si9.7O32晶体。热处理后的样品析出了耐酸侵蚀性较差的富磷相和Na3PO4晶体,导致化学稳定性变差。  相似文献   

3.
Dispersing La2O3 on δ- or γ-Al2O3 significantly enhances the rate of NO reduction by CH4 in 1% O2, compared to unsupported La2O3. Typically, no bend-over in activity occurs between 500° and 700°C, and the rate at 700°C is 60% higher than that with a Co/ZSM-5 catalyst. The final activity was dependent upon the La2O3 precursor used, the pretreatment, and the La2O3 loading. The most active family of catalysts consisted of La2O3 on γ-Al2O3 prepared with lanthanum acetate and calcined at 750°C for 10 h. A maximum in rate (mol/s/g) and specific activity (mol/s/m2) occurred between the addition of one and two theoretical monolayers of La2O3 on the γ-Al2O3 surface. The best catalyst, 40% La2O3/γ-Al2O3, had a turnover frequency at 700°C of 0.05 s−1, based on NO chemisorption at 25°C, which was 15 times higher than that for Co/ZSM-5. These La2O3/Al2O3 catalysts exhibited stable activity under high conversion conditions as well as high CH4 selectivity (CH4 + NO vs. CH4 + O2). The addition of Sr to a 20% La2O3/γ-Al2O3 sample increased activity, and a maximum rate enhancement of 45% was obtained at a SrO loading of 5%. In contrast, addition of SO=4 to the latter Sr-promoted La2O3/Al2O3 catalyst decreased activity although sulfate increased the activity of Sr-promoted La2O3. Dispersing La2O3 on SiO2 produced catalysts with extremely low specific activities, and rates were even lower than with pure La2O3. This is presumably due to water sensitivity and silicate formation. The La2O3/Al2O3 catalysts are anticipated to show sufficient hydrothermal stability to allow their use in certain high-temperature applications.  相似文献   

4.
The utilization of CO2 as rawmaterial for chemical synthesis has the potential for substantial economic and green benefits. Thermal decomposition of hexamethylene-1,6-dicarbamate (HDC) is a promising approach for indirect utilization of CO2 to produce hexamethylene-1,6-diisocyanate (HDI). In this work, a green route was developed for the synthesis of HDI by thermal decomposition of HDC over Co3O4/ZSM-5 catalyst, using chlorobenzene as lowboiling point solvent. Different metal oxide supported catalysts were prepared by incipientwetness impregnation (IWI), PEG-additive (PEG) and deposition precipitation with ammonia evaporation (DP) methods. Their catalytic performances for the thermal decomposition of HDC were tested. The catalyst screening results showed that Co3O4/ZSM-525 catalysts prepared by different methods showed different performances in the order of Co3O4/ZSM-525(PEG) N Co3O4/ZSM-525(IWI) N Co3O4/ZSM-525(DP). The physicochemical properties of Co3O4/ZSM- 525 catalyst were characterized by XRD, FTIR, N2 adsorption-desorption measurements, NH3-TPD and XPS. The superior catalytic performance of Co3O4/ZSM-525(PEG) catalyst was attributed to its relative surface content of Co3+, surface lattice oxygen content and total acidity. Under the optimized reaction conditions: 6.5% HDC concentration in chlorobenzene, 1 wt% Co3O4/ZSM-525(PEG) catalyst, 250 °C temperature, 2.5 h time, 800 ml·min?1 nitrogen flow rate and 1.0 MPa pressure, the HDC conversion and HDI yield could reach 100% and 92.8% respectively. The Co3O4/ZSM-525(PEG) catalyst could be facilely separated from the reaction mixture, and reused without degradation in catalytic performance. Furthermore, a possible reaction mechanism was proposed based on the physicochemical properties of the Co3O4/ZSM-525 catalysts.  相似文献   

5.
Fe3O4 magnetic nanoparticles (MNPs) were synthesised, characterised, and used as a peroxidase mimetic to ac-celerate levofloxacin sono-degradation in an ultrasound (US)/H2O2 system. The Fe3O4 MNPs were in nanometre scale with an average diameter of approximately 12 to 18 nm. The introduction of Fe3O4 MNPs increased levofloxacin sono-degradation in the US/H2O2 system. Experimental parameters, such as Fe3O4 MNP dose, initial solution pH, and H2O2 concentration, were investigated by a one-factor-at-a-time approach. The results showed that Fe3O4 MNPs enhanced levofloxacin removal in the pH range from 4.0 to 9.0. Levofloxacin removal ratio in-creased with Fe3O4 MNP dose up to 1.0 g·L?1 and with H2O2 concentration until reaching the maximum. More-over, three main intermediate compounds were identified by HPLC with electrospray ionisation tandem mass spectrometry, and a possible degradation pathway was proposed. This study suggests that combination of H2O2, Fe3O4 MNPs and US is a good way to improve the degradation efficiency of antibiotics.  相似文献   

6.
Mesoporous transition metal oxide catalysts are well-used in the elimination of volatile organic compounds. In this study, we developed an efficient method for the preparation of mesoporous-Mn3O4 (m-Mn3O4) without the use of templates or surfactants. In this method, KCl protects oxygen defects on the surface of fresh Mn3O4 crystallites. m-Mn3O4 shows higher ameliorative catalytic activity than bulk-Mn3O4 (b-Mn3O4) and calcined-Mn3O4 (c-Mn3O4), achieving toluene catalytic oxidation of T10 and T90 (the temperature at a conversion rate of about 10% and 90%) at 191 ℃ and 230 ℃, respectively (WHSV = 40,000 ml·g-1·h-1). Based on various characterizations, the prepared m-Mn3O4 has large specific surface area and abundant oxygen defects, and thus can provide more surface active sites, which give it superior toluene combustion activity.  相似文献   

7.
Novel magnetic nanoparticles (MNPs), Fe3O4@SiO2 and Fe3O4@SiO2@PEG-(COOH)2, were prepared by loading different amounts of SiO2 or/and PEG-(COOH)2 onto Fe3O4 nanoparticles, and their feasibility to be used as forward osmosis (FO) draw solutes was investigated. The characterization of the materials showed that, compared to normal Fe3O4 nanoparticles, the modified MNPs exhibited enhanced dispersity and high osmotic pressure in aqueous solution. The FO experiment indicated that the synthesized draw solutes could obtain a water flux as high as 10 L·m-2·h-1 with an aquaporin FO membrane. The optimal concentration of the added tetraethyl orthosilicate was 30% during the synthesis. The novel MNPs could be easily recovered from draw solutions by magnetic field, and the recovery rate of Fe3O4@SiO2 and Fe3O4@SiO2@PEG-(COOH)2 was 83.95% and 63.37%, respectively. Moreover, after 5 recycles of reuse, the water flux of Fe3O4@SiO2 and Fe3O4@SiO2@PEG-(COOH)2 as draw solutes still remained 64.36% and 85.26%, respectively. The experimental results demonstrated that the synthesized core–shell magnetic nanoparticles are promising draw solutes, and the Fe3O4@SiO2@PEG-(COOH)2 was more suitable to be used as draw solute in FO process.  相似文献   

8.
Four spinel-type catalysts AB2O4 (CoCr2O4, MnCr2O4, MgFe2O4 and CoFe2O4) were prepared and characterized by XRD, BET, TEM and FESEM techniques. The activity of these catalysts towards the combustion of methane was evaluated in a temperature-programmed combustion (TPC) apparatus. Spinel-type-oxides containing Cr at the B site were found to provide the best results. The half-conversion temperature of methane over the CoCr2O4 catalyst was 376 °C with a W/F = 0.12 g s/cm−3. On the basis of temperature-programmed oxygen desorption (TPD) analysis as well as of catalytic combustion runs, the prevalent activity of the CoCr2O4 catalyst could be explained by its higher capability to deliver suprafacial, weakly chemisorbed oxygen species. This catalyst, promoted by the presence of 1 wt% of palladium deposited by wet impregnation, was lined on cordierite monoliths and then tested in a lab-scale test rig. The combination of Pd and CoCr2O4 catalysts enables half methane conversion at 330 °C (GHSV = 10,000 h−1), a performance similar to that of conventional 4 wt% Pd-γ-Al2O3 catalysts but enabled with just a four-fold lower amount of noble metal.  相似文献   

9.
以Er2O3-Mg2Si-Yb2O3为三元复合烧结助剂,制备了力学性能优异的高导热氮化硅陶瓷,研究了Er2O3-Mg2Si-Yb2O3体系对氮化硅陶瓷致密化、微观结构、力学性能、热导率的影响。研究表明,当添加5%(质量分数,下同)Er2O3+2%Mg2Si+4%Yb2O3烧结助剂时,烧结助剂对氮化硅陶瓷致密度与晶界相含量的平衡效果最佳,此时氮化硅陶瓷具有最佳性能:抗弯强度为765 MPa,断裂韧性为7.2 MPa·m1/2,热导率为67 W/(m·K)。在烧结过程中,只添加5%Er2O3+2%Mg2Si的烧结助剂产生的液相量少且黏度高,不能使氮化硅陶瓷完成致密化;此外,当添加的Yb2O3含量超过4%时,烧结助剂产生大量的晶界相,降低了氮化硅陶瓷的性能。  相似文献   

10.
Nb2O5 loaded on the supports and mixed with oxides was studied to investigate the activity and acidity for Friedel-Crafts benzylation of anisole. From the study on the loaded catalysts, a preliminary conclusion for the selection of metal oxide was obtained; namely, such an acidic oxide as silica was suitable for the support of Nb2O5. Then, MoO3 and WO3 were mixed with Nb2O5, and prominent high catalytic activity and acidities were observed. Both oxides of Nb2O5-MoO3 and Nb2O5-WO3 showed almost similar behavior with respect to characterization and catalytic activity. Surface area increased, X-ray diffraction (XRD) and Raman bands were lost, acid sites, both Brønsted and Lewis characters generated, and surface acid site density was as high as 2–4 nm−2. The acid sites were generated on the amorphous metal oxides consisting of Nb and Mo or W oxides, different in nature from those of Nb2O5 calcined and un-calcined, and active for Friedel-Crafts benzylation.  相似文献   

11.
以Bi(NO3)3·5H2O、Co(CH3COO)2·4H2O为原料,采用化学沉淀-水热法制备了Co3O4-Bi2O2CO3异质结构复合半导体光催化剂,并通过X射线衍射仪(XRD)、扫描电镜(SEM)、X射线光电子能谱(XPS)、紫外可见漫反射光谱(DRS)、荧光光谱(PL)等手段对所合成的复合型催化剂进行了理化性能表征。研究结果表明:引入Co3O4没有改变Bi2O2CO3物相结构,但促进了Bi2O2CO3 对可见光的吸收能力,提高了Bi2O2CO3表面吸附氧物种的数量,抑制了光生载流子复合。复合光催化剂对罗丹明B(RhB)的光催化脱色实验显示引入Co3O4能够明显提高Bi2O2CO3催化剂的光催化脱色能力。尤其是Co3O4引入量为0.6%的Co3O4-Bi2O2CO3样品对罗丹明B染料的光催化脱色率可达到97%(模拟日光照射30min)。本文为复合型光催化剂制备提供了简单易行的技术路线,制备的新型半导体复合光催化剂Co3O4-Bi2O2CO3在环境净化方面表现出了较好的应用前景。  相似文献   

12.
以Co(NO_3)_2·6H_2O和CO(NH_2)_2为原料,十六烷基三甲基溴化铵为活性剂,采用水热-热分解法在不同加热时间(2 h、3 h、4 h、5 h)条件下制备纯相尖晶石结构的Co_3O_4颗粒。利用X射线衍射和电子扫描电镜研究Co_3O_4颗粒的结构和形貌,并以甲基橙为模拟废水,研究加热时间对Co_3O_4颗粒光催化性能的影响。结果表明,加热时间对Co_3O_4颗粒形貌影响很大,并直接影响其光催化性能。加热时间5 h制备的Co_3O_4结构疏松多孔,光催化性能最好,光照20 min,甲基橙降解率达95%。  相似文献   

13.
The solvothermal reaction of mixtures of aluminum isopropoxide (AIP) and gallium acetylacetonate (Ga(acac)3) directly yielded the mixed oxides of γ-Ga2O3-Al2O3. In the solvothermal synthesis, the crystal structure of mixed oxides was controlled by the initial formation of γ-Ga2O3 nuclei. The mixed oxides prepared in diethylenetriamine have extremely high activities for selective catalytic reduction (SCR) of NO with methane as a reducing agent. With increasing crystallite size of the spinel structure, the catalytic activity increased. The ratio of the amount of methane consumed by combustion to total methane conversion was proportional to the density of acid sites on the surface of the mixed oxides. The mixed oxide catalysts prepared in diethylenetriamine had lower densities of acid sites and showed a higher methane-efficiency for CH4-SCR than those prepared in other solvents. These catalysts maintained their high activity even when the reaction was carried out under the severe conditions (i.e., high space velocity and low NO concentration).  相似文献   

14.
以FeSO4·7H2O[Fe(NO3)3·9H2O]为铁源,采用新型微波热解法制备γ-Fe2O3[a-Fe2O3]催化剂样品,通过XRD、N2等温吸附-脱附、压汞法等实验手段对催化剂样品晶相、微观孔结构等进行表征;考察两种催化剂样品的NH3-SCR脱硝性能,通过归一化处理得到两种催化剂在不同温度下的本征脱硝反应速率,同时对比研究了γ-Fe2O3与钒系催化剂的脱硝活性;研究氨氮比、氧浓度等运行参数对γ-Fe2O3催化剂NH3-SCR脱硝性能的影响规律,并对其抗硫抗水性能进行考察.结果表明:采用新型微波热解法可得到纯度较高的γ-Fe2O3催化剂,其介孔分布合理且大孔数量丰富;同时γ-Fe2O3催化剂表现出优于a-Fe2O3催化剂的脱硝性能,400℃时最大NOx转化率达到96%,300、325、350℃下单位面积脱硝速率达到a-Fe2O3催化剂的3倍左右;γ-Fe2O3催化剂具备优良的抗硫抗水性能,其最佳氨氮比为1、最佳氧体积分数为3.5%.  相似文献   

15.
采用3种不同添加方式制备La2O3改性的Al2O3材料La-Al2O3。La-Al2O3分别经500 ℃、1 000 ℃和1 200 ℃焙烧,采用物理吸附、X射线衍射和荧光光谱等对高温处理的La-Al2O3进行比表面积和结构表征。结果表明,La2O3的添加能有效抑制Al2O3在高温条件下向热力学稳定态α-Al2O3转变,同时提高高温处理后La-Al2O3比表面积,使Al2O3热稳定性得到明显提高。在3种La2O3添加方式中,La(NO3)3浸渍法效果最为显著,制得的La-Al2O3(N)材料经1 200 ℃焙烧4 h的比表面积为30 m2·g-1,是未经改性的Al2O3样品经同等温度焙烧比表面积的2.2倍。  相似文献   

16.
王子帅  王耀强  肖刚  苏海佳 《化工学报》2019,70(10):4062-4071
通过溶胶-凝胶法、水热法和煅烧法,成功制备出具有光催化活性的Fe3O4@TiO2磁性纳米复合材料,将超顺磁性的Fe3O4与TiO2复合,实现材料的快速回收与可见光响应能力的结合。进一步将Fe3O4@TiO2磁性纳米复合材料应用于Cr(Ⅵ)的去除,实验结果表明,在可见光照射下Fe3O4@TiO2对Cr(Ⅵ)的去除能力是P25的1.96倍。并深入探究了Fe3O4@TiO2中TiO2含量、Cr(Ⅵ)溶液的pH以及空穴去除剂对Fe3O4@TiO2可见光下光催化还原Cr(Ⅵ)能力的影响,实验表明当Fe3O4@TiO2中TiO2含量为1.0 g/g,添加甲酸作为空穴去除剂并且溶液pH=2时Fe3O4@TiO2对Cr(Ⅵ)的去除能力最佳,此条件下Cr(Ⅵ)的去除率达到99.85%,重复使用4次,催化能力依然保持较高水平。此外,Fe3O4@TiO2对5~500 mg/L浓度范围内的Cr(Ⅵ)都具有良好的去除能力。Fe3O4@TiO2磁性纳米复合材料对Cr(Ⅵ)具备优异的去除能力,具有良好的应用前景。  相似文献   

17.
The role of ozone was studied for two different configurations combining non-thermal plasma (NTP) and heterogeneous catalysis, namely the use of a gas phase plasma with subsequent exposure of the effluent to a catalyst in a packed-bed reactor (post-plasma treatment) and the placement of the catalyst directly in the discharge zone (in-plasma catalysis). Non-porous and porous alumina and silica were deployed as model catalysts. The oxidation of immobilised hydrocarbons, toluene as a volatile organic compound and CO as an inorganic pollutant were studied in both operational modes.

While conversion and selectivity of hydrocarbon oxidation in the case of catalytic post-plasma treatment can be fully explained by the catalytic decomposition of O3 on γ-Al2O3, the conversion processes for in-plasma catalysis are more complex and significant oxidation was also measured for the other three materials (-Al2O3, quartz and silica gel). It became obvious that additional synergetic effects can be utilised in the case of in-plasma catalysis due to short-lived species formed in the NTP.

The capability of porous alumina for ozone decomposition was found to be correlated with its activity for oxidation of carbon-containing agents. It could be clearly shown that the reaction product CO2 poisons the catalytic sites at the γ-Al2O3 surface. The catalytic activity for O3 decomposition can be partially re-established by NTP treatment. However, for practical purposes the additional reaction pathways provided by in-plasma catalytic processes are essential for satisfactory conversion and selectivity.  相似文献   


18.
Four series of cobalt-based catalysts, such as bare Co3O4 and CoO, CoOx–CeO2 mixed oxides, CoOx supported over alumina and alumina–baria and CoMgAl and CoNiAl hydrotalcites have been synthesized and investigated for the oxidative degradation of phenol in the presence of ozone. Characterizations were obtained by several techniques in order to investigate the nature of cobalt species and their morphological properties, depending on the system. Analyses by XRD, BET, TPR, UV–visible diffuse reflectance spectroscopy and TG/DT were performed.

The CoNiAl hydrotalcite exhibits, after 4 h of reaction, the highest phenol ozonation activity followed by Co(3 wt%)/Al2O3–BaO and CoMgAl. The samples Co(1 wt%)/Al2O3–BaO and Co(1 and 3 wt%)/Al2O3 show a comparable medium activity, while the oxidation properties of bare oxides Co3O4, CoO and CoOx–CeO2 are really low. Leaching of cobalt ions in the water solution was detected during the reaction, the amount varied depending on the nature of catalysts. A massive release was observed for the CoMgAl and CoNiAl hydrotalcites, while cobalt catalysts over alumina and alumina–baria look much more stable. The recycle of CoOx/Al2O3 and CoOx/Al2O3–BaO was studied by performing three consecutive cycles in the phenol oxidation. Because of the potential interest of the cobalt-supported catalysts in the ozonation process, the oxidative degradation of naphtol blue black was also investigated.

On the basis of TPR and UV–visible results it appears that highly dispersed Co2+ ions especially present over Co(3 wt%)/Al2O3–BaO are the main active sites for phenol and naphtol blue black oxidative degradation by ozone.  相似文献   


19.
Deposition of γ-Al2O3 washcoats onto Aluminium and FeCrAlloy® supports in the form of slabs and onto -Al2O3 tubes was performed according to a two-step procedure involving: (a) deposition of a bohemite primer, (b) deposition of the γ-Al2O3 layer, both by dip coating into powder dispersions in HNO3 aqueous solutions. We present herein data concerning the effects of the major preparation variables (HNO3 and H2O concentrations in the dispersion, withdrawal velocity, drying temperature, number of dipping cycles, calcination temperature) on the deposited coating load and on the adherence of the washcoat. Based on a rheological characterisation of the γ-Al2O3 dispersions, we propose also a correlation between their apparent viscosity and the washcoat load. Finally, we briefly illustrate the activity in catalytic combustion reactions of structured Pd-based catalysts prepared according to the investigated washcoating methods.  相似文献   

20.
考察过渡金属Ni对Pd/Al_2O_3催化剂甲烷催化燃烧活性的影响以及过渡金属负载量及循环条件对甲烷降解性能的影响,采用扫描电镜、N_2吸附-脱附以及H_2程序升温还原技术对催化剂进行表征。结果表明,过渡金属Ni的添加对催化剂在(375~475)℃下的甲烷催化燃烧活性产生影响。催化剂经多次重复使用后,催化燃烧活性提高。分析原因为经过渡金属Ni改性后,可与载体形成NiAl_2O_4尖晶石,促进活性组分形成较小晶粒,并改善活性组分分散度,提高催化剂催化活性。  相似文献   

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