Formation, electronic, gas sensing and catalytic characteristics of graphene-like materials: A first-principles study
Formation, electronic, gas sensing and catalytic characteristics of graphene-like materials: A first-principles study
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类石墨烯材料的形成、电子、气体传感和催化特性：第一性原理研究
DOI：
10.1016/j.apsusc.2020.147178
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发表时间：
2020-11
影响因子：
6.7
通讯作者：
Xianqi Dai
中科院分区：
文献类型：
--
作者：
Yanan Tang;Weiguang Chen;Zhiwen Wang;Gao Zhao;Yingqi Cui;Zhaohan Li;Yi Li;Zhen Feng;Xianqi Dai
采用第一性原理计算方法，研究了单原子Fe在不同纳米多孔碳材料（石墨烯-Fe和γ-石墨烯-Fe）上的形成几何、电子性质、气敏性和反应活性.首先，亚石墨烯基结构比γ-石墨烯片更稳定。不同的应变（从-10%到+10%）可以调节石墨烯片的金属和半导体性质。与γ-石墨烯-Fe相比，单一或两种反应气体在石墨烯-Fe片上的吸附能更大。同时，这些吸附物种可以改变石墨烯-Fe的电子结构和磁性。其次，进一步分析了不同气体反应物在γ-石墨炔-Fe和石墨烯-Fe两种薄片上共吸附时NO和CO的催化氧化构型，根据Langmuir-Hinshelwood（LH）机理，CO和O2在石墨烯-Fe上的共吸附比相同机理的NO氧化具有更低的反应势垒。此外，吸附的2NO分子能够通过Eley − Rideal（ER）机理（<0. 6 eV）促进2CO的氧化反应（2NO +2CO → 2CO2 + N2），这为探索新型纳米多孔类石墨烯催化剂用于有毒气体的脱除提供了理论参考。
The formation geometry, electronic property, gas sensing and reactive activity of single-atom Fe anchored on different nanoporous carbon materials (graphenylene-Fe and γ-graphyne-Fe) are comparably analyzed by using first-principles calculations. Firstly, the graphenylene structure is more stable than that of γ-graphyne sheet. The varied strains (from −10% to +10%) can regulate the metal and semiconducting properties of graphenylene sheet. Compared with the γ-graphyne-Fe, the single or two reactive gases have larger adsorption energies on graphenylene-Fe sheet. Meanwhile, the electronic structures and magnetic properties of graphenylene-Fe can be modified by these adsorbed species. Secondly, the coadsorbed configurations of different gas reactants on two kinds of γ-graphyne-Fe and graphenylene-Fe sheets are further analyzed for the catalytic oxidation of NO and CO. By the Langmuir–Hinshelwood (LH) mechanism, the coadsorption of CO and O2on graphenylene-Fe has lower reaction barriers than the same mechanism for NO oxidation. Furthermore, the adsorbed 2NO molecules can promote the oxidation reactions of 2CO (2NO + 2CO → 2CO2+ N2) through Eley − Rideal (ER) mechanism (<0.6 eV), which provides a theoretical reference on exploring new nanoporous graphene-like catalyst for toxic gases removal.
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