Oxidative dehydrogenation of propane over transition metal sulfides using sulfur as an alternative oxidant,Catalysis Science & Technology

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Oxidative dehydrogenation of propane over transition metal sulfides using sulfur as an alternative oxidant
Catalysis Science & Technology ( IF 4.4 ) Pub Date : 2020-08-31 , DOI: 10.1039/d0cy01039a
Allison M. Arinaga _{1,

2,

3,

4} , Shanfu Liu _{1,

2,

3,

4} , Tobin J. Marks _{1,

2,

3,

4}

Affiliation

The use of alternative oxidants for the oxidative dehydrogenation of propane (ODHP) is a promising strategy to suppress the facile overoxidation to CO_x that occurs with O₂. Gaseous disulfur (S₂) represents a thermodynamically “softer” oxidant that has been underexplored and yet offers a potential route to more selective propylene formation. Here we describe a system for sulfur-ODHP (SODHP). We demonstrate that various metal sulfide catalysts generate unique reaction product distributions, and that propylene selectivities as high as 86% can be achieved at 450–550 °C. For a group of 6 metal sulfide catalysts, apparent activation energies for propylene formation range from 72–134 kJ mol⁻¹ and parallel the corresponding catalyst XPS sulfur binding energies, indicating that M–S bond strength plays a key role in SODHP activity. Kinetic data over a sulfided ZrO₂ catalyst indicate a rate law which is first-order in propane and zero-order in sulfur, suggesting that SODHP may occur via a mechanism analogous to the Mars van Krevelen cycle of traditional ODHP. The present results should motivate further studies of SODHP as a route to the selective and efficient oxidative production of propylene.

中文翻译：

使用硫作为替代氧化剂，在过渡金属硫化物上进行丙烷的氧化脱氢

使用替代氧化剂对丙烷进行氧化脱氢（ODHP）是一种有前景的策略，可以抑制O ₂引起的容易发生的CO _x过氧化。气态二硫（S ₂）代表一种热力学上“较软”的氧化剂，该氧化剂尚未被充分开发，但为进一步形成丙烯提供了可能的途径。在这里，我们描述了硫-ODHP（SODHP）的系统。我们证明了各种金属硫化物催化剂都能产生独特的反应产物分布，并且在450–550°C下可以实现高达86％的丙烯选择性。对于一组六种金属硫化物催化剂，丙烯形成的表观活化能范围为72–134 kJ mol ^-1并与相应的催化剂XPS硫结合能平行，这表明M–S键强度在SODHP活性中起关键作用。硫化ZrO ₂催化剂的动力学数据表明速率速率规律在丙烷中为一级，在硫中为零级，这表明SODHP可能通过类似于传统ODHP的Mars van Krevelen循环的机理发生。目前的结果应激发进一步研究SODHP，作为选择性和有效氧化丙烯的途径。

更新日期：2020-10-19

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