A DFT study of arsine adsorption on palladium doped graphene: Effects of palladium cluster size
A DFT study of arsine adsorption on palladium doped graphene: Effects of palladium cluster size
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DOI：
10.1016/j.apsusc.2016.01.139
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发表时间：
2016-03
影响因子：
6.7
通讯作者：
Manaschai Kunaseth;Tanabat Mudchimo;S. Namuangruk;N. Kungwan;V. Promarak;Siriporn Jungsuttiwong
中科院分区：
文献类型：
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作者：
Manaschai Kunaseth;Tanabat Mudchimo;S. Namuangruk;N. Kungwan;V. Promarak;Siriporn Jungsuttiwong
在这项研究中，我们利用密度泛函理论计算研究了钯（Pd）掺杂单空位缺陷石墨烯（SDG）表面的尺寸对ash3及其脱氢产物在Pd上吸附的影响。在这里，Pd簇结合研究表明，pd6纳米簇与SDG表面的结合最强，而AsHx（x= 0-3）在最稳定的Pd掺杂SDG上的吸附表明，脱氢的arsine化合物比原始的ash3分子在表面的吸附更强。电荷分析表明，吸附后Pd向脱氢arsine分子的大量电荷迁移可能构成对脱氢arsine的强吸附。此外，对掺杂Pd的SDG吸附剂上ash3脱氢热力学途径的研究表明，在SDG吸附剂上掺杂Pd簇比单掺杂Pd原子的SDG更有利于ash3的分解。因此，我们的研究表明，掺杂SDG的pd6簇更有利于作为去除ash3的吸附材料。
In this study, we have investigated the size effects of palladium (Pd) doped single-vacancy defective graphene (SDG) surface to the adsorption of AsH3and its dehydrogenated products on Pd using density functional theory calculations. Here, Pd cluster binding study revealed that Pd6nanocluster bound strongest to the SDG surface, while adsorption of AsHx(x= 0–3) on the most stable Pdndoped SDG showed that dehydrogenated arsine compounds adsorbed onto the surface stronger than the pristine AsH3molecule. Charge analysis revealed that considerable amount of charge migration from Pd to dehydrogenated arsine molecules after adsorption may constitute strong adsorption for dehydrogenated arsine. In addition, study of thermodynamic pathways of AsH3dehydrogenation on Pdndoped SDG adsorbents indicated that Pd cluster doping on SDG adsorbent tends to be thermodynamically favorable for AsH3decomposition than the single-Pd atom doped SDG. Hence, our study has indicated that Pd6clusters doped SDG is more advantageous as adsorbent material for AsH3removal.