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首页> 外文期刊>Journal of Materials Chemistry, A. Materials for energy and sustainability >The tunable effect of nitrogen and boron dopants on a single walled carbon nanotube support on the catalytic properties of a single gold atom catalyst: a first principles study of CO oxidation
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The tunable effect of nitrogen and boron dopants on a single walled carbon nanotube support on the catalytic properties of a single gold atom catalyst: a first principles study of CO oxidation

机译：氮和硼掺杂剂对单壁碳纳米管催化性能的可调效应对单金原子催化剂的催化性质：CO氧化的第一个原理研究

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摘要

The mechanism of CO oxidation by O-2 on a single Au atom supported on pristine and nitrogen or boron doped (5,5) and (8,0) single-walled carbon nanotubes (SWCNTs) has been systematically investigated theoretically using density functional theory. Fundamental aspects such as the optimized geometry, adsorption energy and charge transfer are elucidated to analyze the adsorption properties of CO and O-2. The results reveal that boron and nitrogen doped SWCNTs can enhance the binding strength and catalytic activity of Au catalysts compared with the pristine SWCNTs. Moreover, the boron and nitrogen doping donate or withdraw charges to and from the Au atom. The excess positive or negative charges on Au can significantly modify its interactions with CO and O-2 molecules. We have found that O-2 binds stronger than CO on Au/B-SWCNTs, but weaker than CO on Au/SWCNTs and Au/N-SWCNTs. The adsorption preference of CO and O-2 molecules on the doped SWCNTs gives a distinct coadsorption pattern of the reactants which is closely related to the dopant configurations. Furthermore, the calculations reveal that the reactions proceed via either the bi-molecular Langmuir-Hinshelwood (BLH) mechanism or the bi-molecular Eley-Rideal (BER) mechanism with a relatively low energy barrier of 0.22 and 0.28 eV. The peroxide-like (OOCO) complex is a key intermediate in the reaction pathway in both BER and BLH mechanisms. There are two different pathways from OOCO to the final product CO2: a two-step pathway, where two CO2 molecules are formed independently, and a self-promotion pathway, where the oxidation of the first CO molecule is promoted by the second CO molecule with a much lower barrier. Besides the traditional BLH and BER mechanisms, a tri-molecular Eley-Rideal (TER) mechanism is also observed, which is almost a barrierless process on Au/B-SWCNTs. In the tri-molecule mechanism, the oxygen molecule is activated by the pre-adsorbed CO molecule on the Au site which is not observed in the conventional LH and ER mechanisms. Our findings give a clear description of the relationship between the support and the catalytic properties of Au and demonstrate the possible ways to engineer the catalytic performance of Au catalysts by rational doping.
机译：在理论上使用密度函数理论，通过系统地研究了在原始和氮气或硼（5,5）和（8,0）单壁碳纳米管（SWCNTs）上负载的单个Au原子上的O-2对掺杂（5,5）和（8,0）的单壁碳纳米管（SWCNT）的机理。阐明了优化的几何，吸附能量和电荷转移等基本方面，以分析CO和O-2的吸附性能。结果表明，与原始SWCNTS相比，硼和氮掺杂的SWCTS可以增强Au催化剂的结合强度和催化活性。此外，硼和氮掺杂掺杂或从Au原子中捐赠或释放电荷。 Au上过量的阳性或负电荷可以显着改变其与CO和O-2分子的相互作用。我们发现O-2比AU / B-SWCNTS上的CO更强，但在AU / SWCNTS和AU / N-SWCNT上弱于CO。掺杂SWCNT上的CO和O-2分子的吸附偏好给出了与掺杂剂配置密切相关的反应物的不同的共吸附模式。此外，计算表明，反应通过双分子朗米尔 - 欣斯伍德（BLH）机制或双分子素丝序（BER）机制进行，其具有相对低的能量屏障为0.22和0.28eV。过氧化物样（OOCO）复合物是BER和BLH机构中的反应途径中的关键中间体。从Ooco到最终产物CO2有两种不同的途径：一种两步途径，其中两个CO 2分子独立形成，并且通过第二CO分子促进第一CO分子的氧化的自我促进途径。障碍较低。除了传统的BLH和BER机制之外，还观察到三分子eley-rideal（TER）机制，这几乎是Au / B-SWCNTS的障碍过程。在三分子机制中，氧分子通过在常规LH和ER机制中未观察到的AU位点上的预吸附的CO分子激活。我们的研究结果清楚地描述了Au的支持和催化性能之间的关系，并证明了通过合理掺杂工程师催化性能的可能方法。

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    Ali Sajjad; Liu Tianfu; Lian Zan; Li Bo; Su Dang Sheng;

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    Chinese Acad Sci Inst Met Res Shenyang Natl Lab Mat Sci 72 Wenhua Rd Shenyang 110016 Liaoning Peoples R China;

    Chinese Acad Sci Inst Met Res Shenyang Natl Lab Mat Sci 72 Wenhua Rd Shenyang 110016 Liaoning Peoples R China;

    Chinese Acad Sci Inst Met Res Shenyang Natl Lab Mat Sci 72 Wenhua Rd Shenyang 110016 Liaoning Peoples R China;

    Chinese Acad Sci Inst Met Res Shenyang Natl Lab Mat Sci 72 Wenhua Rd Shenyang 110016 Liaoning Peoples R China;

    Chinese Acad Sci Inst Met Res Shenyang Natl Lab Mat Sci 72 Wenhua Rd Shenyang 110016 Liaoning Peoples R China;

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  • 正文语种 eng
  • 中图分类 工程材料学;
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