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NiAl and CoAl materials derived from takovite-like LDHs and related structures as efficient chemoselective hydrogenation catalysts

机译:源自takovite样的LDH和相关结构作为有效的化学选择性氢化催化剂的NIAL和煤炭材料

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摘要

The catalytic performance of metallic catalysts derived from layered double hydroxide (LDH) precursors with nickel or cobalt incorporated in the brucite-like layers besides aluminium (i.e., NiAl takovite and related CoAl) was investigated for the first time in the chemoselective hydrogenation of cinnamaldehyde. The precursors in the as-synthesized and calcined forms were thoroughly analysed by ICP, XRD, nitrogen physisorption, DR UV-vis spectroscopy, TPR and in situ XRD after temperature-programmed reduction. According to the XRD results, both as-synthesized samples contained purely LDH phases with degrees of crystallization depending on the nature of incorporated metal cations (i.e., the CoAl sample presents larger crystallites than the NiAl takovite-like sample). For the calcined NiAl and CoAl samples, well-crystallized oxide phases of NiO and CO3O4, respectively, besides amorphous alumina and corresponding spinels were evidenced by XRD. The TPR and in situ XRD results for the calcined samples indicated strong metal-alumina interactions, which resulted in depressed sintering of evolved metal nanoparticles in the high-temperature range of 600-800 °C, in well agreement with TEM analysis. Materials derived from the studied LDH systems are found to be efficient catalysts for the hydrogenation of cinnamaldehyde, showing enhanced control over the activity or selectivity, depending on the nature of active metals and the thermal regime of the catalyst activation.
机译:从铝制层(即Nial Takovite和相关煤炭)除铝制层中均与镍或钴掺入的层状双氢氧化物(LDH)前体衍生的金属催化剂的催化性能,这是第一次在cinnamaldeyde的化学氢化中。通过ICP,XRD,氮物理吸附,DR UV-VIS光谱,TPR和原位XRD彻底分析了合成和钙化形式中的前体。根据XRD的结果,这两个实质性样品均包含纯粹的LDH相,其结晶度程度取决于掺入金属阳离子的性质(即煤样品比Nial Takovite样品更大的结晶石)。对于钙化的NIAL和煤样品,除非无定形氧化铝和相应的尖晶石,XRD还证明了NiO和CO3O4的良好结晶氧化物相。钙化样品的TPR和原位XRD结果表明,在600-800°C的高温范围内,进化金属纳米颗粒的烧结降低,与TEM分析一致。发现源自研究的LDH系统的材料是肉桂醛氢化的有效催化剂,根据活性金属的性质和催化剂激活的热状态显示出对活性或选择性的增强的控制。

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