Cyclohexane dehydrogenation catalyst design based on spin polarization effects
Cyclohexane dehydrogenation catalyst design based on spin polarization effects
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基于自旋极化效应的环己烷脱氢催化剂设计
DOI：
10.1088/0953-8984/16/48/035
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发表时间：
2004
期刊：
影响因子：
--
通讯作者：
H. Kasai
中科院分区：
文献类型：
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作者：
M. Tsuda;W. Diño;Susumu Watanabe;H. Nakanishi;H. Kasai
我们通过基于密度泛函理论 (DFT) 进行总能量计算，研究并讨论了使用 Ni 原子作为测试催化剂的环己烷 (C6H12) 脱氢的自旋极化效应。我们将结果与众所周知的催化剂 Pt 的结果进行比较。我们考虑环己烷接近过渡金属 M（M：Ni 和 Pt）的过程，并根据计算的单线态环己烷/M 和三线态环己烷/Ni 体系的势能面 (PES) 确定反应路径。与单线态环己烷/Ni 不同，三线态环己烷/Ni 从 H-Ni 体系中分离环己基中间体 (C6H11) 不需要能量。我们的结果表明，自旋极化Ni的催化反应活性变得接近Pt，而Pt被认为是迄今为止最好的环己烷脱氢催化剂。
We investigate and discuss spin polarization effects on cyclohexane (C6H12) dehydrogenation using a Ni atom as a test catalyst, by performing total energy calculations based on the density functional theory (DFT). We compare the results with those of the well known catalyst Pt. We consider the process where cyclohexane approaches a transition metal M (M: Ni and Pt), and determine the reaction paths from the calculated potential energy surfaces (PESs) for singlet cyclohexane/M and triplet cyclohexane/Ni systems. Unlike the singlet cyclohexane/Ni, no energy is required to separate cyclohexyl intermediate (C6H11) from the H–Ni system for the triplet cyclohexane/Ni. Our results suggest that the catalytic reactivity of spin-polarized Ni becomes close to that of Pt, which is considered to be, up to now, the best catalyst for cyclohexane dehydrogenation.