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jakejzhy铜虫 (正式写手)
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Cyanide bridged transition metal polymers are versatile materials with a wide range of properties including reversible gas storage, high magnetic Curie temperature and photoinduced magnetization. 1–5 Traditionally these materials have been synthesized and studied as crystalline bulk phases, of which Prussian Blue is the prototypical example.6 However, recent attention has been drawn to the observation that these materials can be produced in nanocrystalline form.7–11 Nanoparticle synthesis has been driven by the production of new materials with properties such as superparamagnetism and by the desire to tune the existing properties of the polymer via quantum confinement.8,9 Synthesis of soluble nanoparticles of cyanide-bridged polymers has to date focused on crystalline Prussian Blue and its analogs, using a variety of stabilizing strategies.7–11 In this work, the synthesis of soluble nanoparticles is expanded to include cyanogels, a group of amorphous, cyanide bridged, coordination polymers fundamentally different from Prussian Blue. Cyanogels are amorphous polymers formed through the reaction of a chlorometalate ([MCl4]2) and a cyanometalate ([M0(CN)n]2/3 (n ¼ 4, 6)) utilizing a large variety of metals (Pd, Pt, Co, Fe, Ru, Os, Ni, Cr).12 This reaction results in a negatively charged, cyanide linked, transition metal polymer through the substitution of two trans chloride ligands on the chlorometalate by the nitrogen of the cyanometalate complex (Fig. 1).13 The polymer initially forms as small sol particles (cyanosol) that undergo a sol–gel transition to form a bulk gel (cyanogel).14 The sol–gel transition indicates that the cyanosol nanoparticles areunstable with respect to agglomeration. Once agglomeration has occurred the lyophobic particles cannot be redispersed into solution by physical manipulation. Therefore, to isolate stable cyanosol particles, agglomeration must be inhibited by preventing the formation of strong inter-particle interactions.15,16 Previous work on cyanosol isolation has focused on immobilizing the particles using strategies such as spin coating or confinement of the sol particles to the interior pores of silica gel.17,18 The immobilization of the nanoparticles prevents either covalent or van der Waals coagulation by maintaining large inter-particle distances. While effective, these techniques hinder the utilization of particles due to a lack of particle solubility and chemical availability. The aim of this work is to isolate stable, soluble, and chemically available cyanosol nanoparticles without immobilizing the cyanosol on a solid support. |
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2楼2010-01-24 11:32:27
allain
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jakejzhy(金币+150): 1-25 09:34
jakejzhy(金币+150): 1-25 09:34
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献丑了 不正之处 请谅解 氰化物桥联的过渡金属聚合物是具有广泛用途的材料，具有多种性能，包括可逆储气，高的磁居里温度和光致磁化。传统上，这些材料都是以结晶块体作为合成与研究对象，普鲁士蓝是典型的例子。但是，最近这些材料的纳米晶体的合成引起了注意。纳米颗粒的合成是在对具有超顺磁性等新材料的研究和运用量子限域效应来调节聚合物的现有性能的背景下展开的。迄今为止合成可溶性的氰化物桥联的聚合物纳米颗粒集中在用稳定机制制备普鲁士蓝晶体及其类似化合物。在本工作中，可溶性纳米颗粒的合成推广到包括氰化物凝胶，一组不同于普鲁士蓝的非晶，氰化物桥联的配位聚合物。 氰化物凝胶是通过金属氯化物和金属氰化物(Pd, Pt, Co, Fe, Ru, Os, Ni, Cr)之间反应形成的非晶聚合物。这个反应通过金属氰化物基团的氮原子取代金属氯化物的两个反式氯配体形成氰化物为骨架的带负电荷的过渡金属聚合物网络。这个聚合物起初形成小的溶胶粒子，然后通过溶胶-凝胶转变形成凝胶块体。溶胶-凝胶转变表明氰化物溶胶纳米颗粒不稳定，有团聚的倾向。一旦团聚形成，这种疏液性的颗粒很难通过物理方法再次分散。因此，为了形成稳定的溶胶粒子，必须阻止颗粒间的强烈的相互作用防止团聚形成。 以前关于氰化物溶胶颗粒的隔离方面的研究集中在通过诸如旋涂法或者限制溶胶颗粒在硅凝胶的内部气孔里来固定溶胶颗粒。通过固定纳米颗粒，形成了大的颗粒间距，阻止了共价或范德法凝聚。这些方法虽然有效，但是降低了颗粒的利用率，因为颗粒缺乏溶解性和化学活性。本工作的目的是不通过固定氰化物溶胶颗粒在一个固体基体上，而采取其他方法来隔离稳定的，可溶的，具有化学活性的氰化物溶胶粒子。 |
3楼2010-01-24 20:47:43