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Efficient metal borate catalysts for oxidative dehydrogenation of propane

机译：有效的金属酿酒催化剂，用于丙烷的氧化脱氢作用

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摘要

Boron-based catalysts have attracted attention in recent years, due to their high selectivity for light olefins in the catalytic oxidative dehydrogenation of propane (ODHP). But they still face drawbacks such as low activity at mild reaction temperature and more or less boron leaching from the catalyst surface during the reaction. Hence, it is necessary to exploit more efficient boron-based catalysts with higher stability. In this study, metal borate catalysts (CoB4O7 and Ni3B2O6) were prepared by a co-precipitation method and evaluated for the ODHP. Reaction tests showed that both metal borates could catalyze propane dehydrogenation efficiently at 450–540 °C with high selectivity and stability. In particular, the CoB4O7 catalyst, after activation at 490 °C for 70 h, exhibited rather high stability with propane conversion of 17.6% and an appreciable selectivity for light olefins of 91.4% during the subsequent reaction run. The structural stability and active sites of the metal borate catalysts were investigated by SEM, TEM, XRD, FTIR, ICP-MS and XPS. The results showed that the morphology and crystal structure of the catalysts as well as the composition of bulk and surface elements changed little after reaction, showing excellent structural stability. Besides, the M–B–O (M = Co, Ni) and B–OH species on the catalysts surface were considered to be the active sites, which gradually increased and reached an abundant content without boron leaching during the induction period of the catalysts, affording the high catalytic activity and selectivity for light olefins.
机译：近年来，基于硼的催化剂吸引了人们对光烯烃在丙烷（ODHP）催化氧化脱氢作用中的高选择性。但是它们仍然面临缺点，例如在轻度反应温度下的活性低以及在反应过程中从催化剂表面浸出或多或少。因此，有必要利用具有更高稳定性的更有效的基于硼的催化剂。在这项研究中，通过共沉淀法制备了金属硼酸盐催化剂（COB4O7和NI3B2O6），并对ODHP进行了评估。反应测试表明，两种金属硼酸盐均可以高选择性和稳定性在450–540°C时有效地催化丙烷脱氢。特别是，在490°C激活70小时后，COB4O7催化剂表现出相当高的稳定性，丙烷转化率为17.6％，在随后的反应过程中对91.4％的光烯烃的选择性明显。通过SEM，TEM，XRD，FTIR，ICP-MS和XPS研究了金属硼酸酯催化剂的结构稳定性和活性位点。结果表明，催化剂的形态和晶体结构以及反应后的大量和表面元素的组成几乎没有变化，显示出极好的结构稳定性。此外，催化剂表面上的MB – O（M = CO，Ni）和B – OH物种被认为是活性位点，在催化剂诱导期间，它们逐渐增加并达到丰富的含量而无需硼浸出的含量，为光烯烃提供高催化活性和选择性。

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