论文标题
量子蒙特卡洛方法建模支持的金属催化：Ni（111）将吸附的emyl转换为氢气
Quantum Monte Carlo method modeling supported metal catalysis: Ni(111) converting adsorbed formyl 'en route' to hydrogen
论文作者
论文摘要
作为化石燃料的干净，可持续替代品的氢生产正在采取速度。即使在即将举行的奥运会上，巴黎CDG机场的容量也已停止，直到可以使用氢供电的飞机为止。 因此，及时处理催化选择性氢生产并优化催化剂结构。超过90％的化学生产都使用固体催化剂。这项工作描述了在Ni（111）中稳定Ni-H链接的Ni（111）化学吸附剂中C-H键的解离。作为此机械步骤的一部分，放出了气态氢。 许多化学反应涉及键合。此过程通常是固体表面上限速反应步骤的关键。 由于Hartree-Fock和DFT方法对破键的描述很差，因此使用了我们嵌入的活性位点方法。这项工作展示了使用非常简单的单层Ni（111）表面模型的量子蒙特卡洛（QMC）方法。
Hydrogen production as a clean, sustainable replacement for fossil fuels is gathering pace. Doubling the capacity of Paris-CDG airport has been halted, even with the upcoming Olympic Games, until hydrogen-powered planes can be used. It is thus timely to work on catalytic selective hydrogen production and optimise catalyst structure. Over 90 % of all chemical manufacture uses a solid catalyst. This work describes the dissociation of a C-H bond in formyl radicals, chemisorbed at Ni(111) that stabilises the ensuing Ni-H linkage. As part of this mechanistic step, gaseous hydrogen is given off. Many chemical reactions involve bond-dissociation. This process is often the key to rate-limiting reaction steps at solid surfaces. Since bond-breaking is poorly described by Hartree-Fock and DFT methods, our embedded active site approach is used. This work demonstrates Quantum Monte Carlo (QMC) methodology using a very simple monolayer Ni(111) surface model.
