由于其獨特的結(jié)構(gòu)和電子特性,納米碳材料(NCMs)在多個領(lǐng)域引起了廣泛的研究興趣。納米碳材料的一系列特性,包括在許多條件下高的化學(xué)惰性、熱穩(wěn)定性和機(jī)械抗性,以及其他傳統(tǒng)材料無法比擬的輕質(zhì)性,使得NCMs適合作為多相催化材料的載體。在一些情況下,這類納米材料載體比常規(guī)載體有著更好的性能。由于NCMs是石墨類材料,其表面是惰性的,使得發(fā)生于NCMs載體上的副反應(yīng)得到適當(dāng)?shù)囊种?因而可能有利于催化過程。相對的,由于缺乏錨定位點,化學(xué)活性相的沉積則變得具有挑戰(zhàn)性。為了打破純NCMs材料的化學(xué)惰性,利用鹵素鹵化NCMs材料是可行途徑,也是其在催化和材料科學(xué)中應(yīng)用時的重要預(yù)處理方法。鹵素?fù)诫s到NCMs晶格后,造成NCMs電子和幾何結(jié)構(gòu)劇烈畸變,同時導(dǎo)致碳碳鍵的雜化狀態(tài)由sp2轉(zhuǎn)變?yōu)閟p3。這些變化會改變NCMs的結(jié)構(gòu)性能并調(diào)節(jié)其帶隙,也會顯著提高碳材料的電導(dǎo)率和載流子遷移率。此外,NCMs的固有特性(包括機(jī)械強(qiáng)度,分散性和磁性等)也能在鹵化過程中得到相應(yīng)的調(diào)控。因而,鹵代NCMs在諸如光催化、電化學(xué)傳感、儲能、生物醫(yī)藥等領(lǐng)域都有出色的表現(xiàn),并得到了廣泛應(yīng)用。然而,理解鹵素原子與NCMs間相互作用關(guān)...

【文章頁數(shù)】：135 頁

【學(xué)位級別】：博士

【文章目錄】：
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 (C_aX_b, X=F,Cl,Br,I;a≠b)
        1.3.2 Chlorinated NCM (C_aCl_b, a ≠ b)
        1.3.3 Brominated NCM (C_aBr_b, a ≠ b)
        1.3.4 Iodinated NCM (C_aI_b, 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



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