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Chromium(III) supported on aluminum-nitride-surfaced alumina: characteristics and dehydrogenation activity

机译:氮化铝表面氧化铝上负载的铬(III):特性和脱氢活性

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Chromium catalysts were prepared by the saturating chemisorption of chromium(III) acetylacetonate (Cr(acac)_3) at 200 deg C on alumina and on alumina that had been surfaced with aluminum nitride. According to elemental analysis, inrfared spectroscopy, and electron spin resonance spectroscopy, chemisorption occurred through liand exchange reaction of Cr(acac)_3 with surface Oh and NH_x groups and dissociation of Cr(acac)_3 or hacac on coordinatively unsaturated sites on the surface. Steric hindrance imposed by the acac ligands defined saturation of the surface with adsorbed species; the same chromium loading (0.64 +- 0.06 atoms per nm~2) was obtained on all supports. After removal of the ligands with oxygen, water, or ammonia, the samples were active in isobutane dehydrogenation. For chromium sites with high activity, nearby oxygen ions were needed. The activity of a Cr~(3+) ion was mainly determined by its environment and not by whether it had been formed through reduction.
机译:铬催化剂是通过在200°C下在氧化铝和表面氮化铝上饱和化学吸附乙酰丙酮铬(III)(Cr(acac)_3)来制备的。根据元素分析,红外光谱和电子自旋共振光谱,化学吸附是通过Cr(acac)_3与表面Oh和NH_x基团的配体交换反应以及Cr(acac)_3或hacac在表面配位不饱和位点上的离解而发生的。 acac配体施加的立体位阻定义了吸附物质在表面的饱和度;在所有载体上获得相同的铬负载量(0.64±0.06原子/ nm〜2)。用氧,水或氨除去配体后,样品在异丁烷脱氢中具有活性。对于具有高活性的铬位点,需要附近的氧离子。 Cr〜(3+)离子的活性主要取决于其环境,而不取决于是否通过还原形成。

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