Engineering Specific Mo–O Bond Stretching to Activate Lattice Oxygen in V-Doped Bi2MoO6 for Enhanced Oxidative Dehydrogenation of 1-Butene,Industrial & Engineering Chemistry Research

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Engineering Specific Mo–O Bond Stretching to Activate Lattice Oxygen in V-Doped Bi2MoO6 for Enhanced Oxidative Dehydrogenation of 1-Butene
Industrial & Engineering Chemistry Research ( IF 3.8 ) Pub Date : 2022-12-29 , DOI: 10.1021/acs.iecr.2c03848
Qinyang Zhao ₁ , Xinglin Hou ₁ , Jinling Wang ₁ , Dang-guo Cheng _{1,

2} , Fengqiu Chen _{1,

2} , Xiaoli Zhan _{1,

2}

Affiliation

Structural distortion has been demonstrated to regulate lattice oxygen activity, but its precise regulation has always been a thorny problem, especially for the oxidative dehydrogenation of hydrocarbons. Herein, by synthesizing a series of V-doped Bi₂MoO₆ catalysts, mechanistic insight into the effect of structural distortion on the catalytic activity of oxidative dehydrogenation of 1-butene was provided. Comprehensive characterizations and kinetics tests revealed that the V-doped Bi₂MoO₆-induced active lattice oxygen initiates 1-butene activation by abstracting the C–H bond, which is a rate-determining step. Combined with density functional theory results, an overwhelming effect of the bond length between Mo and apical oxygen atom in the MoO₆ octahedron on lattice oxygen activation and butadiene formation pathway was proposed. The stretching Mo–O_apical bond elicited by V doping enhances the abstraction of hydrogen and accelerates the redox cycle. The sample with a 5% V content possesses the maximum Mo–O_apical bond length, enabling superior catalytic performance at an 87.6% 1,3-butadiene yield.

中文翻译：

工程特定的 Mo-O 键拉伸以激活 V 掺杂 Bi2MoO6 中的晶格氧以增强 1-丁烯的氧化脱氢

结构扭曲已被证明可以调节晶格氧活性，但其精确调节一直是一个棘手的问题，特别是对于碳氢化合物的氧化脱氢。在此，通过合成一系列 V 掺杂的 Bi ₂ MoO ₆催化剂，提供了结构变形对 1- 丁烯氧化脱氢催化活性影响的机理见解。综合表征和动力学测试表明，V 掺杂的 Bi ₂ MoO ₆-诱导的活性晶格氧通过提取 C-H 键启动 1-丁烯活化，这是一个决速步骤。结合密度泛函理论结果，提出了MoO ₆八面体中Mo与顶端氧原子之间的键长对晶格氧活化和丁二烯形成途径的压倒性影响。由 V 掺杂引起的拉伸 Mo-O_顶端键增强了氢的提取并加速了氧化还原循环。V 含量为 5% 的样品具有最大的 Mo-O_顶端键长，能够以 87.6% 的 1,3-丁二烯产率实现优异的催化性能。

更新日期：2022-12-29

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