贵金属团簇与碳纳米材料的表面修饰与物性调控
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摘要
目前,低维纳米结构如金属团簇、碳纳米管和石墨烯,成为物理学、化学、材料科学等多个学科的研究热点,对它们的深入研究有助于揭示和理解其独特的光学性质、电子结构和带隙特征,为微纳尺度的材料设计和改性提供科学依据。本论文采用密度泛函理论方法分别考察了有机分子吸附的零维Ag和Au纳米团簇的光吸收谱,Ru原子或团簇在一维碳纳米管内外表而的吸附行为,以及二维氢化石墨烯的能隙调控。
多聚物、生物分子和配体等有机分子吸附的贵金属纳米团簇,不仅能够阻止团簇继续生长还能改变金属团簇的表面结构,从而调控其物理化学性质,因此在生物传感、医学成像和治疗方面有较广泛的应用。本论文采用第一性原理研究了有机分子吸附的Ag38和Au38团簇的吸附结构、电子性质和光吸收谱,发现贵金属纳米团簇的光吸收谱受到机分子官能团类型和吸附浓度的调控。具有较浅d带深度的Au团簇比Ag团簇的结构和电子性质更容易受到有机分子的影响,且有机分子吸附对Au38团簇的紫外-可见光吸收谱的改变更大。具有高吸附能,转移电荷量大、对团簇结构改变明显的有机分子(如2-巯基吡啶)是贵金属团簇光吸收谱调控的理想有机分子。改变吸附分子数量同样能调控贵金属团簇的光吸收特性。随着三甲胺分子吸附数量增加,Ag38团簇的吸收光谱总体红移、并伴随吸收峰展宽现象；8个TMA分子吸附的Au38团簇在399nm处山现一个强度与紫外区主吸收峰相当的新吸收峰。我们的理论模拟加深了对有机金属团簇的光吸收行为的理解,也为实验上制备光敏感金属团簇基电子器件提供了参考。
与传统碳材料如石墨,无定形碳等相比,碳纳米管作为催化剂的载体,具有更高的催化活性和选择性。由于碳管内外表面曲率不同、电子结构差异,过渡金属担载在其内外表面时相互作用也不同,从而形成不同的金属/碳管复合物。我们采用第一性原理方法系统地研究了4d过渡金属(尤其是Ru)原子和团簇吸附在单壁或双壁碳纳米管上的几何结构、结合能和电子性质。过渡金属原子在碳管上的平衡吸附构型依赖于金属原子的价电子构型。因为曲率效应,所有过渡金属原子吸附在(6,6)管内外部时向碳管贡献不同量的电子,但是工者转移电荷的差值近似一个常数,即0.5个电子。电子态密度分析揭示出C原子的π电子和Ru的d电子存在杂化现象,这导致了电荷从金属转移向碳管。电荷转移量给出了对4d过渡金属电负性系统地依赖关系。当Ru原子或团簇吸附在双壁碳纳米管上时,电荷转移效应比单壁管略有加强。我们的理论结果对过渡金属和碳纳米管之间的相互作用提供了更深的理解,有助于解释在实验上观察到的碳纳米管内部和外部吸附的过渡金属纳米粒子不同的催化行为。
石墨烯作为一种原子厚度的二维材料,为纳米电子学和光电材料的发展提供了平台,然而零带隙的特征极大地限制了石墨烯在电子学和光子学领域的应用。因此石墨烯带隙的打开和调控成为石墨烯研究的一个重点,我们通过密度泛函理论重点调查了部分氢化石墨烯的电子态。氢化石墨烯构型包括随机去除孤立H原子、随机去除相邻H原子对、有序去除相邻H原子对三类。模拟结果发现随机去除相邻H原子对的氢化石墨烯构型更稳定。更有趣的是,这类构型的氢化石墨烯带隙随着H浓度下降而逐渐变小,在H覆盖度为67%时,带隙为零。带隙从0到4.66eV连续可变,为石墨烯材料电子结构的调控提供了一条新的途径,并增加了其在电子学和光子学方面的应用。
During the last decades, the exploration of low-dimensional nano structures such as metal clusters, carbon nanotubes and graphene, is a hot topic in the fields of physics, chemistry and many other subjects. Intensive investigations of these nanostructures is of key importance to reveal and understand their unique optical properties, electronic structures and band gap, which can help design the novel nano-materials that are technologically promising. In this dissertation, we studied from optical adsorption spectra of the zero-dimensional Ag38and Au38clusters adsorbed with organic molecules, the adsorption behavior of Ru atom or clusters inside and outside carbon nanotubes, to band gap tuning of the two-dimensional hydrogenated graphene.
The organic molecules such as polymers, biomolecules and organic ligands, adsorbing on noble metal clusters, not only can avoid the metal clusters aggregating to bigger, but also modify their surface geometry and electronic structures, which can tune their physical and chemical properties. We have investigated the adsorption structures, electronic properties and optical adsorption spectra of the Ag38and Au38clusters adsorbed with different organic molecules by first-principles calculations. Optical adsorption spectra of the noble metal clusters varies with metal elements, functional groups of organic molecules and concentration of adsorption molecules. Due to the d band of Au closer to Fermi level, geometry structures and electronic properties of the Au38cluster are more easily affected by adsorbing organic molecules, which leads to more distinctive optical adsorption spectra comparing with pure gold clusters. Optical adsorption spectra of the noble metal clusters is tuned by such organic molecules, which has higher adsorption energy, leads to stronger surface modifications and transfers more charge to metal clusters, such as2-Pyridinethiol molecule. Adsorption concentration of organic molecules is another important fact to tune optical adsorption spectra of noble mtal cluster. Increasing the numbers of trimethylamine molecules results in the overall red-shift of optical adsorption spectra and the broadening of adsorption peaks for Ag38cluster. After adsorbed with eight TMA molecules, there appears a new adsorption peak at399nm in the visible region for Au38cluster. The simulations of Ag38and Au38clusters can help understand the optical adsorption behavior of noble metal clusters adsorbed with organic molecules, and provide reference to synthesize light-sensitive metal clusters.
First-principles calculations were performed to investigate the binding energies, geometric structures, and electronic properties of4d transition metal TM (particularly, Ru), atoms, and clusters adsorbed outside/inside the single-walled or double-walled carbon nanotubes. The equilibrium adsorption structures of the TM atoms depend on the valence electron configuration of the metal atoms. Due to curvature effect, all TM atoms adsorbed inside and outside (6,6) carbon nanotubes donate different amounts of electrons to the nanotube, with a nearly constant difference of about0.5electrons/TM atom. The analysis of electronic density of states revealed hybridization between the n electrons from C and the d electrons from Ru, which results in charge transfer from metal to carbon. The amount of charge transfer shows systematical trend with the electronegativity of4d TMs. When Ru atom or cluster adsorbs on double-walled nanotubes, the effect of charge transfer is slightly enhanced with regard to the single-walled nanotubes.
The electronic states of partially hydrogenated graphene (HG) structures are studied by the density functional theory calculations. Several types of HG configurations, including randomly removing of H pair, randomly removing individual H atoms, and ordered H pairs removal, are investigated. We find that the configurations with randomly removingHpairs aremost energetically favorable. More interestingly, the band gap for such configurations decrease with H concentration and approaches zero around67%H coverage. The ability to continuously tune the band gap of hydrogenated graphene from0to4.66eV by different H coverage provides a new pathway for engineering the electronic structure of graphene materials and enhances their applications in electronics and photonics.
多聚物、生物分子和配体等有机分子吸附的贵金属纳米团簇,不仅能够阻止团簇继续生长还能改变金属团簇的表面结构,从而调控其物理化学性质,因此在生物传感、医学成像和治疗方面有较广泛的应用。本论文采用第一性原理研究了有机分子吸附的Ag38和Au38团簇的吸附结构、电子性质和光吸收谱,发现贵金属纳米团簇的光吸收谱受到机分子官能团类型和吸附浓度的调控。具有较浅d带深度的Au团簇比Ag团簇的结构和电子性质更容易受到有机分子的影响,且有机分子吸附对Au38团簇的紫外-可见光吸收谱的改变更大。具有高吸附能,转移电荷量大、对团簇结构改变明显的有机分子(如2-巯基吡啶)是贵金属团簇光吸收谱调控的理想有机分子。改变吸附分子数量同样能调控贵金属团簇的光吸收特性。随着三甲胺分子吸附数量增加,Ag38团簇的吸收光谱总体红移、并伴随吸收峰展宽现象；8个TMA分子吸附的Au38团簇在399nm处山现一个强度与紫外区主吸收峰相当的新吸收峰。我们的理论模拟加深了对有机金属团簇的光吸收行为的理解,也为实验上制备光敏感金属团簇基电子器件提供了参考。
与传统碳材料如石墨,无定形碳等相比,碳纳米管作为催化剂的载体,具有更高的催化活性和选择性。由于碳管内外表面曲率不同、电子结构差异,过渡金属担载在其内外表面时相互作用也不同,从而形成不同的金属/碳管复合物。我们采用第一性原理方法系统地研究了4d过渡金属(尤其是Ru)原子和团簇吸附在单壁或双壁碳纳米管上的几何结构、结合能和电子性质。过渡金属原子在碳管上的平衡吸附构型依赖于金属原子的价电子构型。因为曲率效应,所有过渡金属原子吸附在(6,6)管内外部时向碳管贡献不同量的电子,但是工者转移电荷的差值近似一个常数,即0.5个电子。电子态密度分析揭示出C原子的π电子和Ru的d电子存在杂化现象,这导致了电荷从金属转移向碳管。电荷转移量给出了对4d过渡金属电负性系统地依赖关系。当Ru原子或团簇吸附在双壁碳纳米管上时,电荷转移效应比单壁管略有加强。我们的理论结果对过渡金属和碳纳米管之间的相互作用提供了更深的理解,有助于解释在实验上观察到的碳纳米管内部和外部吸附的过渡金属纳米粒子不同的催化行为。
石墨烯作为一种原子厚度的二维材料,为纳米电子学和光电材料的发展提供了平台,然而零带隙的特征极大地限制了石墨烯在电子学和光子学领域的应用。因此石墨烯带隙的打开和调控成为石墨烯研究的一个重点,我们通过密度泛函理论重点调查了部分氢化石墨烯的电子态。氢化石墨烯构型包括随机去除孤立H原子、随机去除相邻H原子对、有序去除相邻H原子对三类。模拟结果发现随机去除相邻H原子对的氢化石墨烯构型更稳定。更有趣的是,这类构型的氢化石墨烯带隙随着H浓度下降而逐渐变小,在H覆盖度为67%时,带隙为零。带隙从0到4.66eV连续可变,为石墨烯材料电子结构的调控提供了一条新的途径,并增加了其在电子学和光子学方面的应用。
During the last decades, the exploration of low-dimensional nano structures such as metal clusters, carbon nanotubes and graphene, is a hot topic in the fields of physics, chemistry and many other subjects. Intensive investigations of these nanostructures is of key importance to reveal and understand their unique optical properties, electronic structures and band gap, which can help design the novel nano-materials that are technologically promising. In this dissertation, we studied from optical adsorption spectra of the zero-dimensional Ag38and Au38clusters adsorbed with organic molecules, the adsorption behavior of Ru atom or clusters inside and outside carbon nanotubes, to band gap tuning of the two-dimensional hydrogenated graphene.
The organic molecules such as polymers, biomolecules and organic ligands, adsorbing on noble metal clusters, not only can avoid the metal clusters aggregating to bigger, but also modify their surface geometry and electronic structures, which can tune their physical and chemical properties. We have investigated the adsorption structures, electronic properties and optical adsorption spectra of the Ag38and Au38clusters adsorbed with different organic molecules by first-principles calculations. Optical adsorption spectra of the noble metal clusters varies with metal elements, functional groups of organic molecules and concentration of adsorption molecules. Due to the d band of Au closer to Fermi level, geometry structures and electronic properties of the Au38cluster are more easily affected by adsorbing organic molecules, which leads to more distinctive optical adsorption spectra comparing with pure gold clusters. Optical adsorption spectra of the noble metal clusters is tuned by such organic molecules, which has higher adsorption energy, leads to stronger surface modifications and transfers more charge to metal clusters, such as2-Pyridinethiol molecule. Adsorption concentration of organic molecules is another important fact to tune optical adsorption spectra of noble mtal cluster. Increasing the numbers of trimethylamine molecules results in the overall red-shift of optical adsorption spectra and the broadening of adsorption peaks for Ag38cluster. After adsorbed with eight TMA molecules, there appears a new adsorption peak at399nm in the visible region for Au38cluster. The simulations of Ag38and Au38clusters can help understand the optical adsorption behavior of noble metal clusters adsorbed with organic molecules, and provide reference to synthesize light-sensitive metal clusters.
First-principles calculations were performed to investigate the binding energies, geometric structures, and electronic properties of4d transition metal TM (particularly, Ru), atoms, and clusters adsorbed outside/inside the single-walled or double-walled carbon nanotubes. The equilibrium adsorption structures of the TM atoms depend on the valence electron configuration of the metal atoms. Due to curvature effect, all TM atoms adsorbed inside and outside (6,6) carbon nanotubes donate different amounts of electrons to the nanotube, with a nearly constant difference of about0.5electrons/TM atom. The analysis of electronic density of states revealed hybridization between the n electrons from C and the d electrons from Ru, which results in charge transfer from metal to carbon. The amount of charge transfer shows systematical trend with the electronegativity of4d TMs. When Ru atom or cluster adsorbs on double-walled nanotubes, the effect of charge transfer is slightly enhanced with regard to the single-walled nanotubes.
The electronic states of partially hydrogenated graphene (HG) structures are studied by the density functional theory calculations. Several types of HG configurations, including randomly removing of H pair, randomly removing individual H atoms, and ordered H pairs removal, are investigated. We find that the configurations with randomly removingHpairs aremost energetically favorable. More interestingly, the band gap for such configurations decrease with H concentration and approaches zero around67%H coverage. The ability to continuously tune the band gap of hydrogenated graphene from0to4.66eV by different H coverage provides a new pathway for engineering the electronic structure of graphene materials and enhances their applications in electronics and photonics.
引文
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