Zhang Shujie, Li Kejiang, Ma Yan, Bu Yushan, Liang Zeng, Yang Zonghao, Zhang Jianliang
School of Metallurgical and Ecological Engineering, University of Science and Technology Beijing, Beijing 100083, China.
Max-Planck-Institut für Eisenforschung, Max-Planck-Straße 1, 40237 Dusseldorf, Germany.
Nanomaterials (Basel). 2023 Jul 11;13(14):2051. doi: 10.3390/nano13142051.
The hydrogen-based direct reduction of iron ores is a disruptive routine used to mitigate the large amount of CO emissions produced by the steel industry. The reduction of iron oxides by H involves a variety of physicochemical phenomena from macroscopic to atomistic scales. Particularly at the atomistic scale, the underlying mechanisms of the interaction of hydrogen and iron oxides is not yet fully understood. In this study, density functional theory (DFT) was employed to investigate the adsorption behavior of hydrogen atoms and H on different crystal FeO surfaces to gain a fundamental understanding of the associated interfacial adsorption mechanisms. It was found that H molecules tend to be physically adsorbed on the top site of Fe atoms, while Fe atoms on the FeO surface act as active sites to catalyze H dissociation. The dissociated H atoms were found to prefer to be chemically bonded with surface O atoms. These results provide a new insight into the catalytic effect of the studied FeO surfaces, by showing that both Fe (catalytic site) and O (binding site) atoms contribute to the interaction between H and FeO surfaces.
基于氢气的铁矿石直接还原是一种突破性工艺，用于减少钢铁行业产生的大量一氧化碳排放。氢气对氧化铁的还原涉及从宏观到原子尺度的各种物理化学现象。特别是在原子尺度上，氢气与氧化铁相互作用的潜在机制尚未完全理解。在本研究中，采用密度泛函理论（DFT）研究氢原子和氢气在不同晶体FeO表面的吸附行为，以深入了解相关的界面吸附机制。研究发现，氢分子倾向于物理吸附在铁原子的顶部位置，而FeO表面的铁原子作为活性位点催化氢的解离。解离后的氢原子更倾向于与表面氧原子化学键合。这些结果通过表明铁（催化位点）和氧（结合位点）原子都有助于氢气与FeO表面之间的相互作用，为所研究的FeO表面的催化作用提供了新的见解。
