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Highly dispersed CoOx in layered double oxides for oxidative dehydrogenation of propane: guest–host interactions

机译：层状双氧化物中高度分散的CoO x 用于丙烷的氧化脱氢：客体间相互作用

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摘要

Co–Al layered-double-oxides (LDOs) derived from inorganic anion (nitrate, carbonate, sulfate and phosphate) pillared Co–Al layered-double-hydroxides (LDHs) were synthesized. These LDO samples exhibited impressive catalytic performances in oxidative dehydrogenation of propane (ODHP) at low temperatures. Characterization techniques such as XRD, TEM, H2-TPR and O2-TPD were used to measure the physicochemical properties of the samples. The results showed that the LDO samples consisted of homogeneously mixed cobalt spinel oxides (Co2AlOx) containing both Co(III) and Co(II). Co(III) instead of Co(II) was linked with the active sites for ODHP at low temperatures. The sulfate and phosphate anions were preserved in the corresponding LDO samples, unlike the nitrate and carbonate pillars. Sulfate (phosphate) around the cobalt decreased the size of the spinel oxide particles more relative to nitrate and carbonate, and so the dispersion of CoOx in the LDO and the selectivity to propylene in ODHP over these catalysts were improved. Both surface adsorbed oxygen species and surface lattice oxygen species were significantly found over the phosphate-pillared LDO, but only lattice oxygen species were available over the sulfate-pillared LDO. Different mechanisms of propane activation were exhibited over these LDO samples for ODHP.
机译：合成了源自无机阴离子（硝酸根，碳酸根，硫酸根和磷酸根）的Co-Al层状双氢氧化物（LDHs）。这些LDO样品在低温下丙烷的氧化脱氢（ODHP）中表现出令人印象深刻的催化性能。使用XRD，TEM，H 2 -TPR和O 2 -smallTPD等表征技术来测量样品的理化特性。结果表明，LDO样品由均匀混合的钴尖晶石氧化物（Co 2 AlO x ）同时包含Co（ III ）和Co（ II ）。 Co（ III ）代替Co（ II ）在低温下与ODHP的活性位点相连。与硝酸根和碳酸根不同，硫酸根和磷酸根阴离子保留在相应的LDO样品中。相对于硝酸盐和碳酸盐，钴周围的硫酸盐（磷酸盐）减小了尖晶石氧化物颗粒的尺寸，因此CoO x 的分散在这些催化剂上，LDO中的烯烃的选择性提高，并且ODHP中对丙烯的选择性得到改善。在磷酸盐接枝的LDO上均明显发现了表面吸附的氧和表面晶格氧，但在硫酸盐接枝的LDO上仅存在晶格氧。在这些用于ODHP的LDO样品上，丙烷活化的机理不同。

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