Edge-hydroxylated Boron Nitride for Oxidative Dehydrogenation of Propane to Propylene
Edge-hydroxylated Boron Nitride for Oxidative Dehydrogenation of Propane to Propylene
复制标题
边缘羟基氮化硼用于丙烷氧化脱氢制丙烯
DOI：
10.1002/cctc.201700004
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发表时间：
2017-05-23
期刊：
影响因子：
4.5
通讯作者：
Lu, An-Hui
中科院分区：
文献类型：
--
作者：
Shi, Lei;Wang, Dongqi;Lu, An-Hui
丙烷氧化脱氢制烯烃是工业化直接脱氢的一种有前途的替代路线，但由于过氧化反应产生大量不期望的CO2，因此遇到烯烃选择性控制的困难。在这里，我们报道了边缘羟基化的氮化硼，一种无金属催化剂，其有效地催化丙烷脱氢为丙烯，在给定的丙烷转化率为20.6%的情况下具有上级选择性（80.2%），但仅具有可忽略的CO2形成（0.5%）。通过300小时的试验操作证明了显著的稳定性，具有稳定的转化率和产物选择性。活性BNO中心点的网站，动态生成的B-OH基团的分子氧，通过选择性地打破C-H键，但同时关闭的丙烯过氧化向CO2的途径引发丙烷脱氢。
Oxidative dehydrogenation of propane to olefins is a promising alternative route to industrialized direct dehydrogenation, but encounters the difficulty in selectivity control for olefins because of the overoxidation reactions that produce a substantial amount of undesired CO2. Here we report edge-hydroxylated boron nitride, a metal-free catalyst, that efficiently catalyzed dehydrogenation of propane to propylene with superior selectivity (80.2 %) but with only negligible CO2 formation (0.5%) at a given propane conversion of 20.6 %. Remarkable stability was evidenced by the operation of a 300 h test with steady conversion and product selectivity. The active BNO center dot site, generated dynamically through hydrogen abstraction of B-OH groups by molecular oxygen, triggered propane dehydrogenation by selectively breaking the C-H bond but simultaneously shut off the pathway of propylene overoxidation towards CO2.