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1.
以草酸铌、草酸钾和氟化钾为原料,采用改进的固相法在较低温度(600℃)下合成了层状K2NbO3F;测定了其对甲基橙光催化降解的催化作用,并基于紫外-可见漫反射光谱分析和X射线衍射分析初步探讨了甲基橙在自然光照条件下的光催化反应过程及降解机理.结果表明,合成的K2NbO3F与微量H2O2作用后,在自然光照条件下几乎可以使甲基橙染料完全降解;当反应温度为45℃,催化剂投加量为1g/L,H2O2用量为0.33%(体积分数)时,2h内可将初始浓度为15mg/L的甲基橙溶液几乎完全降解.就甲基橙的光催化降解机理而言,·OH自由基在其降解过程中起重要作用. 相似文献
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基于微波水热法和微乳液法合成SnO2/TiO2纳米管复合光催化剂.通过X射线衍射(XRD)、配有能量色散X射线光谱仪(EDX)的透射电镜(TEM)和电化学手段对光催化剂进行表征.以甲苯为模型污染物,考察光催化剂在紫外光(UV)和真空远紫外光(VUV)下的性能及失活再生.结果表明,SnO2/TiO2纳米管复合光催化剂形成三元异质结(锐钛矿相TiO2(A-TiO2)/金红石相TiO2(R-TiO2)、A-TiO2/SnO2和R-TiO2/SnO2异质结),促使光生电子-空穴对的有效分离,提高光催化活性.SnO2/TiO2表现出最佳的光催化性能,UV和VUV条件下的甲苯降解率均达100%,CO2生成速率(k2)均为P25的3倍左右.但由于UV光照矿化能力不足,中间产物易在催化剂表面累积.随着UV光照时间的增加,SnO2/TiO2逐渐失活,20 h后k2由138.5 mg·m-3·h-1下降到76.1 mg·m-3·h-1.利用VUV再生失活的SnO2/TiO2,过程中产生的·OH、O2-·、O(1D)、O(3P)、O3等活性物质可氧化吸附于催化剂活性位的难降解中间产物,使催化剂得以再生,12 h后k2恢复到143.6 mg·m-3·h-1.UV和VUV的协同效应使UV降解耦合VUV再生成为一种可持续的光催化降解污染物模式. 相似文献
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在TiO2悬浮体系下,采用对甲基苯磺酸模拟废水进行半导体光催化氧化降解静态试验;利用正交试验研究了光催化氧化降解的主要影响因素(pH值、催化剂用量、光照强度、光照时间).结果表明:在一定条件下,催化剂投加量、溶液pH、照射光强度及光照时间均存在一个最佳值;依据其影响对甲基苯磺酸废水光催化降解反应的大小,各因素排列顺序为:光照时间(光照强度(初始pH(催化剂用量.在试验最佳条件下(pH=3,催化剂用量80 mg.L-1,光照强度500 W,光照时间120 min),对甲基苯磺酸能够完全降解. 相似文献
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孔道结构H3PW12O40/TiO2的制备及其可见光光催化降解水溶性染料的性能 总被引:3,自引:0,他引:3
采用溶胶-凝胶方法制备了孔道结构复合材料H3PW12O40/TiO2,采用ICP-AES,UV/DRS,31P MAS NMR,TEM和N2吸附等技术对其组成和结构进行了表征. 结果表明,催化剂中活性组分H3PW12O40的基本骨架结构未发生改变,H3PW12O40的担载量为22.29%,催化剂平均粒径为40 nm,具有双孔结构,其平均微孔和介孔孔径分别为0.61和3.06 nm. 考察了催化剂可见光光催化降解6种水溶性染料的性能. 结果表明,6种染料均可不同程度地被降解和矿化. 通过对染料中性红的光催化降解实验,比较了H3PW12O40/TiO2,Degussa P-25和锐钛矿结构TiO2的可见光光催化活性,其中,H3PW12O40/TiO2活性最高,且催化剂最易分离,可循环使用. 相似文献
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Eu2Sn2O7的水热合成及其光催化活性的研究 总被引:3,自引:3,他引:0
采用水热法制备了Eu2Sn2O7纳米颗粒, 并用TEM、 XRD、 IR、 Raman等技术对其进行了表征. 结果表明: Eu2Sn2O7纳米颗粒的粒径约为75nm左右, 且尺寸分布均匀. 以紫外光为光源, 甲基橙为目标降解物, 研究了该纳米催化剂的光催化活性, 结果显示其具有较高的催化效率. 另外, 对甲基橙催化降解后的产物进行了UV-Vis、 IR、 Fluorescence表征分析, 并初步探索了甲基橙分子在该实验条件下的光催化降解机理. 相似文献
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LaBO3(B=Fe,Co)中氧的迁移与光催化反应活性 总被引:10,自引:0,他引:10
以柠檬酸法合成的钙钛矿型复合氧化物LaBO3(B=Fe,Co)为催化剂,对水溶性染料进行光催化降解,实验结果表明,其光催化活性与钙钛矿型结构中氧空位沿BO6八面体棱边以曲线而非直线的迁移机制有关.在光催化氧化过程中,光生电子首先被表面氧空位束缚,再与表面的吸附氧反应生成超氧基(O2-·)而加速对染料分子的降解.钙钛矿型复合氧化物中的氧空位是由氧的迁移产生的,它可以作为电子的陷阱而捕俘电子,并作为氧的吸附中心而提高催化剂表面的吸附氧量. 相似文献
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新型仿生光催化剂的合成及在孔雀绿光催化降解中的作用 总被引:8,自引:0,他引:8
通过付-克反应用磺酸铁酞菁(FePcS)修饰中孔分子筛HMS,首次得到了一种新型光反应催化剂(简称为HMS-FePcS),并用XRD,TG,FT-IR, SEM/TEM,元素分析及固体紫外漫反射光谱等手段对催化剂进行了表征. 实验结果表明,催化剂能高效地催化H2O2氧化降解孔雀绿染料,光照下,在500 ml浓度为0.1 mmol/L的孔雀绿溶液中加入0.3 ml 30%的H2O2和20 mg HMS-FePcS催化剂,于50 ℃下反应 1200 min,脱色率接近100%,总有机碳的去除率达到73%. 对孔雀绿光催化降解的机理进行了初步探讨. 相似文献
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《化学研究与应用》2015,(11)
以过硫酸铵为氧化剂,制备了复合光催化材料α-Si W11Ti/PANI/Ti O2。用UV-Vis、IR、XRD和SEM-EDS等测试手段对其结构及形貌等进行了表征。IR结果表明,复合后聚苯胺的IR振动峰发生红移。N2吸附-脱附显示产物为介孔材料,具有双孔结构,平均孔径约为20.07nm和26.69nm。以刚果红染料废水(15 mg/L)为探针反应,评价了其光催化性能,与一元催化剂Ti O2和二元催化剂/PAIN/Ti O2比较,三元催化剂Si W11Ti/PANI/Ti O2表现出更高的光催化降解性能,经30W紫外灯照射150min后,其降解率为92.44%。 相似文献
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用溶胶-凝胶法以磷钼酸(MPA)的镍盐溶液水解钛酸四丁酯制备了NiPMo/TiO2催化剂.使用ICP、 XRD、 TG-DTA、 IR、 TPD-MS和微反应技术研究了催化剂的化学组成、热稳定性、化学吸附性质和催化反应性能.杂多钼酸盐与TiO2通过O2-在TiO2表面发生了键合.在623 K下,杂多阴离子仍保持原有的Keggin结构.CO2在Lewis酸位Ni(Ⅱ)和Lewis碱位Ni-O-Mo的桥氧协同作用下生成CO2卧式吸附态Ni(Ⅱ)←O-(CO)←(O--Ni).丙烯有多种吸附态在催化剂上吸附.在563 K、 1 MPa和空速1500 h-1的反应条件下,丙烯的摩尔转化率为3.2%,产物MAA选择性为95%. 相似文献
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Toward new camptothecins. Part 6: Synthesis of crucial ketones and their use in Friedländer reaction
Laurent Gavara Thomas Boisse Jean-Pierre Hénichart Adam Daïch Philippe Gautret 《Tetrahedron》2010,66(38):7544-5571
In the context of the preparation of camptothecin and luotonin A analogs, the synthesis of some key keto-precursors and their use in Friedländer condensation are described. This paper also focuses on the stability of these keto intermediates and emphasizes the major differences between indolizinones and pyrroloquinazolinones series. Noteworthy is also the report of some original structures isolated as by-products of some experiments. 相似文献
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The Langevin paramagnetic theory can’t describe the relation between magnetization of ferrofluids and applied magnetic field. The structuralization of ferrofluids, which is considered the main influence factor of the magnetization, is regarded. The part of magnetization works is deposited when the structure is forming. This action influences the magnetization of ferrofluids directly or indirectly. On the base of the “compressing” model, the Langevin function that usually describes the magnetization of ferrofluid is modified, and a well-fitted curve is obtained. An equation of the relation between the equivalent volume fraction after being “compressed” and the intensity of magnetic field is discovered, which approximately describes the process of magnetization. The relation between the approximate initial susceptibility and the volume fraction can be obtained from modified formula. 相似文献
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Rebecca J. Burton Mandy L. CrowtherNeal J. Fazakerley Shaun M. FilleryBarry M. Hayter Jason G. KettleCaroline A. McMillan Paula PerkinsPeter Robins Peter M. SmithEmma J. Williams Gail L. Wrigley 《Tetrahedron letters》2013
The highly regioselective Buchwald–Hartwig amination at C-2 of the cheap and readily accessible reagent, 2,4-dichloropyridine with a range of anilines and heterocyclic amines is described. This new methodology is robust and provides a facile access to 4-chloro-N-phenylpyridin-2-amines on 0.25 mol scale. These intermediates undergo a further Buchwald–Hartwig amination at higher temperature to enable rapid exploration of the chemical space at C-4 and to provide a library of 2,4-bisaminopyridines. 相似文献
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KMnO4-mediated oxidative CN bond cleavage of tertiary amines producing secondary amine was introduced, which was trapped by electrophiles (acyl chloride and sulfonyl chloride) to form amides and sulfonamides. The reaction could take place at mild condition, tolerating a wide range of function groups and affording products in moderate to excellent yields. 相似文献
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N. A. Nedolya 《Chemistry of Heterocyclic Compounds》2008,44(10):1165-1219
The review contains a concise historical account and information on the most significant researches undertaken by the staff
at the A. E. Favorsky Irkutsk Institute of Chemistry, Siberian Branch of the Russian Academy of Sciences on the Chemistry
of Heterocyclic Compounds.
Dedicated to Academician of the Russian Academy of Sciences B. A. Trofimov on his 70th jubilee.
Translated from Khimiya Geterotsiklicheskikh Soedinenii, No. 10, pp. 1443–1502, October, 2008. 相似文献
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Regiospecific and direct imidation of the methyl C(sp3)–H bond of thioanisoles is realized under mild and metal-free conditions with N-fluorobis(benzenesulfonyl)imide as an oxidant and nitrogen source. Proposed mechanism suggests that thionium ion intermediates and a Pummerer-type reaction are involved. The imidation has advantages such as high step-economy, excellent functionality tolerance, and regiospecificity, giving structurally diverse imidation products. 相似文献
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《Tetrahedron》2014,70(21):3377-3384
The Rh(II)-catalyzed reaction of 2-carbonyl-substituted 2H-azirines with ethyl 2-cyano-2-diazoacetate or 2-diazo-3,3,3-trifluoropropionate provides an easy access to 2H-1,3-oxazines and 1H-pyrrol-3(2H)-ones. These compounds can be selectively prepared from the same starting material using temperature as the only varied parameter. The 2-azabuta-1,3-diene intermediate, a common precursor for both heterocyclic products, isomerizes into 2H-1,3-oxazine under kinetic control, while 1H-pyrrol-3(2H)-one is the sole product of the reaction at elevated temperatures. According to DFT-calculations a one-atom oxazine ring contraction involving ring-opening to a 2-azabuta-1,3-diene intermediate, followed by a 1,5- and 1,2-prototropic shift leads to the consecutive formation of imidoylketene and azomethine ylide, which then further undergo cyclization to the pyrrole derivative. 相似文献
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Different approaches for the synthesis of 1-benzyloxypyrazin-2(1H)-one derivatives from simple amino acids have been investigated. A library of 33 precursors for the preparation of N-hydroxy pyrazinones was obtained in moderate to good yields. 相似文献