卤化碳基纳米材料多功能催化剂的计算研究
发布时间：2023-08-11 17:54
由于其独特的结构和电子特性,纳米碳材料(NCMs)在多个领域引起了广泛的研究兴趣。纳米碳材料的一系列特性,包括在许多条件下高的化学惰性、热稳定性和机械抗性,以及其他传统材料无法比拟的轻质性,使得NCMs适合作为多相催化材料的载体。在一些情况下,这类纳米材料载体比常规载体有着更好的性能。由于NCMs是石墨类材料,其表面是惰性的,使得发生于NCMs载体上的副反应得到适当的抑制,因而可能有利于催化过程。相对的,由于缺乏锚定位点,化学活性相的沉积则变得具有挑战性。为了打破纯NCMs材料的化学惰性,利用卤素卤化NCMs材料是可行途径,也是其在催化和材料科学中应用时的重要预处理方法。卤素掺杂到NCMs晶格后,造成NCMs电子和几何结构剧烈畸变,同时导致碳碳键的杂化状态由sp2转变为sp3。这些变化会改变NCMs的结构性能并调节其带隙,也会显著提高碳材料的电导率和载流子迁移率。此外,NCMs的固有特性(包括机械强度,分散性和磁性等)也能在卤化过程中得到相应的调控。因而,卤代NCMs在诸如光催化、电化学传感、储能、生物医药等领域都有出色的表现,并得到了广泛应用。然而,理解卤素原子与NCMs间相互作用关...
【文章页数】：135 页
【学位级别】：博士
【文章目录】：
摘要
ABSTRACT
Chapter 1 Introduction
1.1 Background and overview
1.2 Carbon nanostructures for catalyst and catalyst support
1.2.1 Graphene
1.2.2 Carbon-nanotubes
1.3 Halogenation, a versatile way to tune the properties of NCMs
1.3.1 Halogenated NCMs (CaXb, X=F,Cl,Br,I;a≠b)
1.3.2 Chlorinated NCM (CaClb, a ≠ b)
1.3.3 Brominated NCM (CaBrb, a ≠ b)
1.3.4 Iodinated NCM (CaIb, a ≠ b)
1.4 Nitrogen and boron doping further tune the properties of the halogenated-NCMs
1.4.1 Nitrogen dopant in halogenated-NCMs
1.4.2 Boron dopant in halogenated-NCMs
1.5 Halogenated-NCM as metal free catalyst for Li-S Batteries
1.6 Metal supported halogenated NCM for oxygen reduction reaction (ORR)
1.7 Significance of the dissertation and design route
1.7.1 Research problems and design route
1.7.2 Significance of the dissertation and purpose
1.8 Thesis outline and research flow chart
Chapter 2 Theoretical tools
2.1 Methodology and theoretical tools
2.1.1 Density functional theory (DFT)
2.1.2 Schrodinger equation
2.1.3 Born-Oppenheimer approximation
2.1.4 Honenberg-Kohn theorem
2.1.5 Kohn-Sham equations
2.1.6 Exchange and correlation
2.1.7 Plane wave functions and Brillouin zone samplings
2.2 Computational methods
2.3 Instruments
Chapter 3 Halogenation of graphene triggered by heteroatom doping
3.1 Introduction
3.2 Computational methods
3.3 Results and discussion
3.3.1 Halogen adsorption on pristine graphene
3.3.2 Halogen adsorption on boron and nitrogen-doped graphene
3.3.3 Halogen dissociation and dissociation barrier
3.4 Summary
Chapter 4 Halogenated graphene as cathodes for high performance Li-S batteries
4.1 Introduction
4.2 Computational methods
4.3 Results and discussion
4.3.1 Halogen doped graphene with sulfur containing clusters
4.3.2 Halogen-boron dual doped graphene with sulfur containing clusters
4.4 Summary
Chapter 5 Halogen-doped SWNT supported iron single atom catalysts for smallmolecules adsorption and oxygen reduction reaction
5.1 Introduction
5.2 Computational methods
5.3 Results and discussion
5.3.1 Geometric structures of Fe on SWNT and X-SWNT
5.3.2 Adsorption of small molecules on Fe-X-SWNT
5.4 ORR performance on Fe-SWNT and Fe-X-SWNT
5.4.1 ORR reaction pathway on Fe-SWNT and Fe-X-SWNT
5.5 Summary
Chapter 6 Conclusion and perspectives
6.1 Conclusion
6.2 Perspectives
References
Acknowledgements
Author's academic achievements during Ph.D.study
Publications
Conference attended
Author's Profile
本文编号：3841489
【文章页数】：135 页
【学位级别】：博士
【文章目录】：
摘要
ABSTRACT
Chapter 1 Introduction
1.1 Background and overview
1.2 Carbon nanostructures for catalyst and catalyst support
1.2.1 Graphene
1.2.2 Carbon-nanotubes
1.3 Halogenation, a versatile way to tune the properties of NCMs
1.3.1 Halogenated NCMs (CaXb, X=F,Cl,Br,I;a≠b)
1.3.2 Chlorinated NCM (CaClb, a ≠ b)
1.3.3 Brominated NCM (CaBrb, a ≠ b)
1.3.4 Iodinated NCM (CaIb, a ≠ b)
1.4 Nitrogen and boron doping further tune the properties of the halogenated-NCMs
1.4.1 Nitrogen dopant in halogenated-NCMs
1.4.2 Boron dopant in halogenated-NCMs
1.5 Halogenated-NCM as metal free catalyst for Li-S Batteries
1.6 Metal supported halogenated NCM for oxygen reduction reaction (ORR)
1.7 Significance of the dissertation and design route
1.7.1 Research problems and design route
1.7.2 Significance of the dissertation and purpose
1.8 Thesis outline and research flow chart
Chapter 2 Theoretical tools
2.1 Methodology and theoretical tools
2.1.1 Density functional theory (DFT)
2.1.2 Schrodinger equation
2.1.3 Born-Oppenheimer approximation
2.1.4 Honenberg-Kohn theorem
2.1.5 Kohn-Sham equations
2.1.6 Exchange and correlation
2.1.7 Plane wave functions and Brillouin zone samplings
2.2 Computational methods
2.3 Instruments
Chapter 3 Halogenation of graphene triggered by heteroatom doping
3.1 Introduction
3.2 Computational methods
3.3 Results and discussion
3.3.1 Halogen adsorption on pristine graphene
3.3.2 Halogen adsorption on boron and nitrogen-doped graphene
3.3.3 Halogen dissociation and dissociation barrier
3.4 Summary
Chapter 4 Halogenated graphene as cathodes for high performance Li-S batteries
4.1 Introduction
4.2 Computational methods
4.3 Results and discussion
4.3.1 Halogen doped graphene with sulfur containing clusters
4.3.2 Halogen-boron dual doped graphene with sulfur containing clusters
4.4 Summary
Chapter 5 Halogen-doped SWNT supported iron single atom catalysts for smallmolecules adsorption and oxygen reduction reaction
5.1 Introduction
5.2 Computational methods
5.3 Results and discussion
5.3.1 Geometric structures of Fe on SWNT and X-SWNT
5.3.2 Adsorption of small molecules on Fe-X-SWNT
5.4 ORR performance on Fe-SWNT and Fe-X-SWNT
5.4.1 ORR reaction pathway on Fe-SWNT and Fe-X-SWNT
5.5 Summary
Chapter 6 Conclusion and perspectives
6.1 Conclusion
6.2 Perspectives
References
Acknowledgements
Author's academic achievements during Ph.D.study
Publications
Conference attended
Author's Profile
本文编号：3841489
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