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各向异性金纳米粒子的制备及其在催化中的应用 总被引:1,自引:0,他引:1
Peter Priecel Hammed Adekunle Salami Romen Herrera Padilla Ziyi Zhong Jose Antonio Lopez-Sanchez 《催化学报》2016,(10):1619-1650
尽管有关金纳米粒子催化的研究工作很多,但其中大多数都是采用传统的浸渍法将金盐负载到载体上、共沉淀或沉积-沉淀法制得负载的纳米粒子,但这些方法并未吸收最新的纳米技术。最近,金催化剂的研究者开发了在胶态悬浮液中制取金属纳米粒子,然后进行固载,从而使得单金属和双金属催化剂的催化活性和形貌控制取得较大进展。另一方面,最近十年出现了金纳米粒子合成的高级控制技术,得到了许多各向异性的金纳米粒子,且很容易制得新的形貌,可以控制纳米粒子的表面原子配位数和光学特性(可调的等离子体带),这些都与催化密切相关。这些形貌包括纳米棒、纳米星、纳米花、树枝状纳米结构或多面体纳米粒子等。除了高度关注各向异性金纳米粒子的最新开发的制备方法和性质,本综述也清楚地总结了这些纳米粒子独特的催化性能,以及通过提供更高催化性能的金催化剂、控制暴露的活性位,以及热、电和光催化的鲁棒性和可调性,从而给多相催化领域带来令人惊奇的潜在变革。 相似文献
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Ag@AgCl修饰的锐钛矿相TiO2纳米管的制备及其光催化性能 总被引:3,自引:0,他引:3
首先采用水热合成法和双氧水处理制备了具有锐钛矿相的TiO2纳米管,然后通过沉淀和光化学反应将Ag@AgCl纳米粒子负载于其上,从而制得TiO2纳米管负载的表面等离子体光催化剂.结果表明,经Ag@AgCl纳米粒子修饰后,锐钛矿相TiO2纳米管因表面等离子共振效应而对可见光具有明显的响应,光生电子-空穴对更容易分离,因而T... 相似文献
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《催化学报》2016,(10)
尽管有关金纳米粒子催化的研究工作很多,但其中大多数都是采用传统的浸渍法将金盐负载到载体上、共沉淀或沉积-沉淀法制得负载的纳米粒子,但这些方法并未吸收最新的纳米技术.最近,金催化剂的研究者开发了在胶态悬浮液中制取金属纳米粒子,然后进行固载,从而使得单金属和双金属催化剂的催化活性和形貌控制取得较大进展.另一方面,最近十年出现了金纳米粒子合成的高级控制技术,得到了许多各向异性的金纳米粒子,且很容易制得新的形貌,可以控制纳米粒子的表面原子配位数和光学特性(可调的等离子体带),这些都与催化密切相关.这些形貌包括纳米棒、纳米星、纳米花、树枝状纳米结构或多面体纳米粒子等.除了高度关注各向异性金纳米粒子的最新开发的制备方法和性质,本综述也清楚地总结了这些纳米粒子独特的催化性能,以及通过提供更高催化性能的金催化剂、控制暴露的活性位,以及热、电和光催化的鲁棒性和可调性,从而给多相催化领域带来令人惊奇的潜在变革. 相似文献
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通过热解自聚合多巴胺法制备了氮掺杂空心碳微球(N-HCMS), 并采用微波辅助乙二醇还原方法把Pt纳米粒子负载于N-HCMS上制得了Pt/N-HCMS催化剂. 催化剂的表面形貌、晶体结构及其比表面积和孔径分布等分别采用扫描电子显微镜、透射电子显微镜、X射线衍射仪及比表面分析仪等进行表征. 采用循环伏安法和线性扫描伏安法研究了Pt/N-HCMS 催化剂在酸性条件下的电催化氧还原性能. Pt/N-HCMS 催化剂由于Pt纳米粒子的均匀分散、N-HCMS载体的快速电子传递及其独特的微孔和中空结构而具有很高的电催化氧还原活性, 其质量比活性是E-TEK Pt/C 催化剂的近两倍. Pt/N-HCMS 催化剂还具有优良的稳定性. 本工作对于开发高性能的燃料电池阴极催化剂具有重要意义. 相似文献
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负载型贵金属纳米催化剂中的金属纳米粒子易发生团聚或流失,因此提高金属活性组分的分散性和稳定性很重要。我们报道了一种制备高分散钯纳米催化剂的方法,通过浸泡法将氯钯酸前驱体负载到苯并噁嗪聚合物上,再经过惰性气氛一步热解得到纳米炭球担载钯催化剂.催化剂性能通过温和条件下苯甲醇氧化反应进行评价.经过500℃热处理制备的催化剂,从TEM图可以看出Pd纳米粒子均匀分散在载体上,尺寸大小约为3 nm,这是由于载体和钯活性组分的配位作用有利于提高钯纳米粒子的分散性和稳定性.通过调控金属负载量及负载时间,尽可能地实现活性组分分布在载体外表面,制备的催化剂上最高TOF为690 h-1.此催化剂同时具有较好的循环稳定性,失活后的催化剂经过200℃焙烧即可实现再生. 相似文献
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《中国科学:化学》2017,(5)
本文通过采用脉冲电沉积技术在氮化物纳米粒子表面沉积原子层厚度的铂,成功地制得了以碳纳米管负载氮化物纳米粒子为核的新型核壳结构催化剂TiN@Pt/NCNTs,并考察了催化剂对于甲酸氧化的催化活性和稳定性.在相同铂负载量情况下,TiN@Pt/NCNTs催化剂的甲酸氧化质量活性可达商业Pt/C催化剂的3.3倍,并表现出良好的抗CO中毒能力和电化学稳定性.研究发现,在TiN中添加少量Cu制得的TiCuN@Pt/NCNTs比TiN@Pt/NCNTs表现出更高的催化活性,其Pt的质量活性可达商品Pt/C催化剂的4.5倍.扫描透射电镜(STEM)及能谱图谱(EDS mapping)清楚地揭示了催化剂的核壳结构.独特的核壳结构使得Pt原子得到了良好的分散是催化剂表现出良好活性的重要原因,同时Cu元素在氮化钛中的掺杂可使得Pt的d电子能级进一步降低,使得催化剂的活性得到了进一步的提升. 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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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
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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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A general synthesis of previously unknown semicarbazone-based α-amidoalkylating reagents, 4-(tosylmethyl)semicarbazones, has been developed. The synthesis involved three-component condensation of semicarbazones of aliphatic or aromatic aldehydes with the same or other aldehydes and p-toluenesulfinic acid. The scope and limitations of this reaction were investigated. The compounds obtained were demonstrated to be an efficient α-(4-semicarbazono)alkylating agents. They were reacted with H- (sodium borohydride), O- (sodium methylate), S- (sodium phenylthiolate), N- (pyrrolidine, sodium succinimide), P- (trialkyl phosphites), and C-nucleophiles (sodium diethyl malonate) to give the corresponding products of the tosyl group substitution, 4-substituted semicarbazones, including analogues of nitrofurazone. Among the prepared compounds tested in vitro for antibacterial and antifungal activity, three nitrofuryl-containing semicarbazones exhibited high biological activities with minimum inhibitory concentration (MIC) values of 8–32 μg/mL. 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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A small library of new chiral bidentate hydroxyalkyl-imidazolium salts 1 is conveniently synthesized on multi-gram scale from inexpensive and commercially available chiral pool amino acids. The corresponding carbenes, generated by deprotonation of imidazolium salts 1, in combination with palladium(II) chloride were tested in the Mizoroki–Heck coupling reaction. The most significant results in terms of yields and reactivities were achieved with low catalyst loading. The catalytic activities of these imidazolium salts were also investigated in the asymmetric addition of diethylzinc to benzaldehyde. The use of MgO nanoparticles as an additive in conjunction with these ligands played a crucial role in increasing the efficiency of these reactions. 相似文献