水热法催化氧化哈密风化煤制备腐植酸的工艺研究

采用Fe2O3-V2O5二元固体酸催化剂,对哈密风化煤通过水热法催化氧化工艺制备腐植酸。通过正交实验对催化氧化工艺条件进行了优化,并且采用X射线衍射(XRD)、扫描电子显微镜(SEM)、透射电子显微镜(TEM)、热重分析(TGA)研究了Fe2O3-V2O5二元固体酸催化剂的微观结构及形貌。结果表明:在酸煤比2∶l(m L/g),反应温度100℃,反应时间0.5 h,催化剂Fe2O3-V2O5用量为2%时腐植酸产率可达73.6%,比碱溶酸析工艺处理的风化煤中腐植酸产率提高了9.6%,表明水热法催化氧化工艺能明显提高腐植酸的产率。微观结构分析表明,Fe2O3-V2O5二元固体酸催化剂结晶性较好,同时具有良好的分散性和热稳定性。     

Ag-Fe_2O_3-V_2O_5/TiO_2催化剂制备及其甲基吡啶催化氧化脱甲基性能

针对甲基吡啶氧化脱甲基反应,以TiO_2为载体经浸渍法制备Ag-Fe_2O_3-V_2O_5/TiO_2催化剂,结合结构表征和催化剂性能评价,考察制备条件对其催化甲基吡啶氧化脱甲基性能的影响。结果表明,通过Fe_2O_3改性可以提高Ag-V_2O_5/TiO_2催化剂对3-甲基吡啶氧化脱甲基化反应的催化性能,其作用主要是抑制V_2O_5团聚,促进V物种的分散。同时,锐钛矿相TiO_2载体表面B酸中心有利于催化3-甲基吡啶脱甲基,提高产物吡啶选择性。经实验优化,Ag-Fe_2O_3-V_2O_5/TiO_2催化剂适宜制备条件为:焙烧温度450℃、焙烧时间4 h、V_2O_5和Ag的负载质量分数分别为15%和1.5%、Fe与V物质的量比1∶2。在优化条件下,吡啶收率与选择性最高可达到62.97%和78.75%。     

新型催化剂催化氧化风化煤制备腐植酸

采用溶胶-凝胶法制备了Fe_2O_3/TiO_2和FePc(NO_2)_4/TiO_2复合粒子催化剂,通过金相显微镜、XRD等对形貌和晶相结构进行表征,研究催化剂在风化煤氧解制备腐植酸中的催化性能。结果表明,两种催化剂都是无均一形貌的片状结构,负载催化剂的二氧化钛为锐钛矿相。TiO_2负载Fe_2O_3和TiO_2负载FePc(NO_2)_4催化剂明显提高了氧化剂的反应活性,使得总腐植酸的产率分别提高了19.0%和31.3%,游离腐植酸的产率分别提高了7.0%和14.4%。     

新型催化剂催化氧化风化煤制备腐植酸

采用溶胶-凝胶法制备了Fe_2O_3/TiO_2和FePc(NO_2)_4/TiO_2复合粒子催化剂,通过金相显微镜、XRD等对形貌和晶相结构进行表征,研究催化剂在风化煤氧解制备腐植酸中的催化性能。结果表明,两种催化剂都是无均一形貌的片状结构,负载催化剂的二氧化钛为锐钛矿相。TiO_2负载Fe_2O_3和TiO_2负载FePc(NO_2)_4催化剂明显提高了氧化剂的反应活性,使得总腐植酸的产率分别提高了19.0%和31.3%,游离腐植酸的产率分别提高了7.0%和14.4%。     

磁性固体酸SO_4~(2-)/ZrO_2/Cr_2O_3/Fe_3O_4催化纤维素液化反应的研究

采用化学共沉淀法合成了磁性固体酸催化剂SO_4^(2-)/Zr O_2/Cr_2O_3/Fe_3O_4,用于催化水体系中纤维素的液化反应,探讨了反应温度、时间以及催化剂用量对纤维素液化反应的影响。研究表明,在240℃下反应8 h,纤维素的转化率达到99%以上,油产率为16.6%,水溶性物质产率达到35.9%。GC-MS分析表明,油相产物的主要成分为醛、酮以及羧酸类物质。     

磁性固体酸SO_4~(2-)/ZrO_2/Cr_2O_3/Fe_3O_4催化纤维素液化反应的研究

采用化学共沉淀法合成了磁性固体酸催化剂SO_4~(2-)/Zr O_2/Cr_2O_3/Fe_3O_4,用于催化水体系中纤维素的液化反应,探讨了反应温度、时间以及催化剂用量对纤维素液化反应的影响。研究表明,在240℃下反应8 h,纤维素的转化率达到99%以上,油产率为16.6%,水溶性物质产率达到35.9%。GC-MS分析表明,油相产物的主要成分为醛、酮以及羧酸类物质。     

纳米Fe_3O_4-PO_4~(3-)/ZrO_2催化制备文冠果生物柴油

采用共沉淀法制备纳米Fe_3O_4-PO■/ZrO_2固体酸催化剂,利用X-射线衍射(XRD)、N_(2 )吸脱附、红外光谱(FTIR)和热重分析(TG)对催化剂的结构进行表征,探讨了纳米Fe_3O_4加入量、焙烧温度和时间对固体酸催化剂性能的影响。考察了纳米Fe_3O_4负载量、醇油摩尔比、反应温度和反应时间对制备文冠果生物柴油的影响。结果表明,当Zr(OH)_4与纳米Fe_3O_4摩尔比为3∶1,焙烧温度为750℃,焙烧时间为3 h时,纳米Fe_3O_4-PO■/ZrO_2固体酸催化剂的催化性能最佳,生物柴油酯化率达85.4%。当催化剂的用量为油重的1%,醇油摩尔比为9∶1,反应温度为80℃和反应时间为4 h时,文冠果生物柴油的转化率可达到92.8%。     

铁系固体超强酸Fe_2O_3/S_2O_8~(2-)的制备及丁酸异戊酯的合成

Fe_2O_3/S_2O_8~(2-)超强酸是直接由Fe_2O_3制备而成。本文研究了焙烧温度对催化活性的影响,探索了催化酯化反应的最佳条件。实验结果表明:Fe_2O_3/S_2O_8~(2-)超强酸催化剂是一种性能良好的酯化催化剂,制备简单,能够循环使用,无三废污染,催化效率高,对丁酸异戊酯酯化产率可高达96.02％。     

水体中常见离子对Fe_3O_4/H_2O_2降解孔雀石绿的影响

磁性纳米Fe_3O_4作为类Fenton催化剂,能够有效催化H_2O_2降解孔雀石绿(MG)废水。而实际染料废水中常含有多种无机离子和有机物,选取五种典型离子(SO42-、Cl-、Ca~(2+)、Mg~(2+)和腐植酸),探讨不同浓度离子对Fe_3O_4/H_2O_2降解MG的影响,并对反应前后Fe_3O_4的晶体结构进行分析。结果表明:腐植酸对Fe_3O_4/H_2O_2降解MG具有促进作用;Cl-和SO42-在不同程度上抑制了该催化降解反应;Ca~(2+)和Mg~(2+)对MG的降解没有明显影响;Fe_3O_4的晶体结构没有因为上述典型离子的加入而发生改变。     

Fe_2O_3/γ-Al_2O_3/H_2O_2/O_3对制药二级生化出水的深度处理研究

采用浸渍法将Fe_2O_3负载在γ-Al_2O_3表面,制备高活性催化剂。采用Fe_2O_3/γ-Al_2O_3/H_2O_2/O_3催化氧化深度处理制药二级生化出水,考察催化剂投加量、pH值、双氧水投加量、臭氧流量等对废水中COD去除率的影响。结果显示,在催化剂投加量3 g/L,废水pH为9,双氧水投加量1 mg/L,臭氧流量1.0 L/min条件下,COD去除率达到85.96%。催化剂循环使用10次后,COD去除率仍然可达到83%以上,证明催化剂稳定性良好。     

钕-铝系稀土色料的研制

通过钕-铝系列色料合成实验,分析不同配比及不同矿化剂等对色料呈色效果的影响,确定最佳工艺方法。对实验结果进行XRD及色度分析,确定其主晶相为钕酸铝,试样的明度均在70以上,色彩鲜艳亮丽。     

Phase equilibrium in binary La2O3-Dy2O3 and ternary CeO2-La2O3-Dy2O3 systems

Cerium oxide doped with oxides of rare earth elements is a multifunctional material, a wide range of uses which is associated with its unique physicochemical properties. Phase diagrams of multicomponent systems are the physicochemical basis for the creation of new materials with improved characteristics.In this work, phase equilibria in ternary CeO₂–La₂O₃–Dy₂O₃ and binary La₂O₃–Dy₂O₃ systems in the whole concentration range were studied. No new phases have been identified in these systems. An isothermal section of the phase diagram of the CeO₂–La₂O₃–Dy₂O₃ system at a temperature of 1500 °С is constructed. No new phases have been detected in the system. It was found that in the studied ternary system solid solutions are formed on the basis of (F) modification of CeO₂ with structure of fluorite type, monoclinic (B), cubic (C) and hexagonal (A) modifications of Ln₂O₃.In the La₂O₃–Dy₂O₃ binary system (1500–1100 °С) three types of solid solutions are formed: based on hexagonal modification A-La₂O₃, monoclinic modification B-Dy₂O₃ and cubic modification C-Dy₂O₃ separated by two-phase fields (A+B) and (B+C), respectively. The boundaries of the regions of homogeneity of solid solutions based on A-La₂O₃ are determined by compositions containing 35–40, 20–25, 15–20 mol% Dy₂O₃ at 1500, 1250, 1100 °C, respectively. From the obtained data it follows that the solubility of Dy₂O₃ in the hexagonal modification of lanthanum oxide is 39 mol% at 1500 °C, 23 mol. % at 1250 °C and 16 mol% at 1100 °C. The limits of existence of solid solutions based on monoclinic B-modification are determined by compositions containing 30–35, 65–60 (1250 °С), 35–40, 55–60 (1100 °С) 40–45, 70–75 (1500 °C) mol% Dy₂O₃.In the studied system, with a decrease in temperature from 1500° to 1100°C, there is a decrease in the solubility of La₂O₃ in the crystal lattice of cubic solid solutions of C-type from 16 to 10 mol%.     

Polycrystalline In2O3 and In2O3/Y2O3 photoanodes

Single crystal In₂O₃ shows promise as a photoanode for the decomposition of water. Because of various difficulties in the preparation of the single crystal material, two simple techniques were developed for the preparation of polycrystalline In₂O₃ anodes. One method involves the thermal decomposition of the nitrate while the other utilizes the chemical vapour deposition technique. Voltammograms and photoresponse spectra of these anodes are compared to the single crystal material. Among other observations, it is noted that the quantum efficiencies of the thermally decomposed films are comparable to the single crystal material. It is also shown that the on-set potential can be shifted to more negative values by forming the mixed oxide In₂O₃/Y₂O₃.     

Fe2+/H2O2体系O2生成路径

掌握Fe²⁺/H₂O₂体系O₂的生成路径,可为避免H₂O₂无效分解,开发经济高效的Fe²⁺/H₂O₂体系利用技术指明方向。采用添加自由基捕获剂的方法,探究Fe²⁺/H₂O₂体系内各种自由基对O₂生成速率的影响,进而确定O₂的生成路径。结果表明:Fe²⁺/H₂O₂体系内不会产生大量O₂^-·,O₂^-·不是生成O₂的主要反应物质;O₂^-·被全部捕获后,体系中仍产生大量O₂^-·,但此时无O₂生成,证明生成O₂的反应由·OH和HO₂·两种自由基直接参与。分析认为反应·OH+HO₂·-H₂O+O₂是体系内O₂生成的主要路径。控制Fe²⁺/H₂O₂体系定向生成·OH,抑制HO₂·的产生,是提高Fe²⁺/H₂O₂体系中H₂O₂利用率的有效手段。     

Na2O-Al2O3-Fe2O3系烧结过程中铝、铁的反应行为

以Al2O3, Fe2O3和Na2CO3为原料,对Na2O-Al2O3-Fe2O3系烧结过程中的反应行为进行了详细研究. 基于溶出率与时间、温度的关系,证明Na2O×Al2O3和Na2O×Fe2O3的生成反应动力学都服从Zhuralev-Lesokin-Tempelman模型,表观活化能分别为186.59和80.92 kJ/mol,表明Na2O×Fe2O3比Na2O×Al2O3在动力学上更易形成;Al2O3易与Na2O×Fe2O3反应形成Na2O×Al2O3和Fe2O3,在1273 K烧结30 min,所得熟料Al2O3溶出率达98.51%;Fe2O3对Na2O×Al2O3的形成有双重作用,在1273 K下可加速Na2O×Al2O3的形成,超过1323 K,促使Na2O×Al2O3分解成Na2O和b-Al2O3,且随着温度升高或时间延长,分解程度增高,从而导致熟料中Al2O3溶出率显著降低.     

H2O2 / O3, H2O2 / UV And H2O2 / Fe2+ Processes For The Oxidation Of Hazardous Wastes

Activated hydrogen peroxide produces very reactive OH-radicals which destroy hazardous contaminants in water. The principles and different methods of activation are described. Results from laboratory studies show the numerous applications of this new technology. A successful scaleup of laboratory tests to an industrial level is discussed. Finally, a cost estimate for treating different types of water with hydrogen peroxide is presented.     

Propylene metathesis over Re2O7/Al2O3-B2O3 catalysts

A series of alumina aluminum borate (AAB) with various Al/B molar ratios were prepared by the coprecipitation method. The supported rhenium oxide catalysts with various contents of Re₂O₇ were also prepared by the impregnation method with perrhenic acid. The catalytic activity and stability of Re₂O₇/AAB catalysts for the reaction of propylene metathesis were tested in a fixed-bed microreactor. It was found that Re₂O₇/AAB is more active, stable and regenerable than Re₂O₇/Al₂O₃ for propylene metathesis. The optimum Al/B molar ratio was found to be in the range of 4–10.