氧化镁负载铁铅双金属催化剂制备单壁碳纳米管

　　

单壁碳纳米管（Single-walled
carbon nanotubes，SWNTs）凭借其卓越的电学、光学、热学和力学性能，在电子器件、生物医学、能源存储和复合材料等领域具有广阔的应用前景。由于SWNTs的的手性指数（n, m）直接决定了SWNTs的性能及其应用领域，制备具有窄手性分布的SWNTs是推动其在高端领域应用的关键。化学气相沉积（Chemical vapor
deposition，CVD）技术是目前催化制备高质量SWNTs的主流方法。其中，负载型金属催化剂的组成对SWNTs的手性指数（n, m）有显著的影响，所以负载型金属催化剂的设计和开发至关重要。由于传统的单金属催化剂由于存在奥斯特瓦尔德熟化作用，在载体表面上容易发生聚集，导致SWNTs的直径分布不均匀且生长密度较低。相比之下，双金属催化剂体系通过金属间协同作用，不仅显著提升催化活性，更能在苛刻的条件下维持优异的稳定性。基于此，本论文提出将低熔点助金属Pb引入Fe/MgO催化剂体系中，利用浸渍法制备了MgO负载的FePb双金属催化剂，探究了两种金属组分比例和生长温度对催化生长SWNTs的影响。实验结果表明，当Fe与Pb的金属摩尔比为1:1时，FePb/MgO双金属催化剂显著提升了（6, 5）手性SWNTs的丰度，且FePb/MgO双金属催化剂在800 ℃下实现了窄手性分布SWNTs的合成。为开发用于制备窄手性分布SWNTs的新型双金属催化体系提供了新的研究思路和实验基础。
Single-walled carbon nanotubes (SWNTs), with their exceptional electrical, optical, thermal, and mechanical properties, have vast potential applications in electronic devices, biomedicine, energy storage, and composite materials. Since the chirality indices (n, m) of SWNTs directly determine their properties and application domains, synthesizing SWNTs with narrow chirality distributions is crucial for advancing their applications in high-end fields. Chemical vapor deposition (CVD) is the primary method for catalytically synthesizing high-quality SWNTs. The composition of supported metal catalysts significantly influences the chirality indices (n, m) of SWNTs; thus, the design and development of supported metal catalysts are crucial. Traditional single-metal catalysts, due to the Ostwald ripening effect, tend to aggregate on the support surface, resulting in uneven diameter distributions and low growth densities of SWNTs. In contrast, bimetallic catalyst systems, through metal-metal synergistic interactions, significantly enhance catalytic activity and maintain excellent stability under harsh conditions. Based on this, this study proposes the introduction of low-melting-point promoter metal Pb into the Fe/MgO catalyst system, preparing MgO-supported FePb bimetallic catalysts via the impregnation method, and investigating the effects of the ratio of the two metal components and growth temperature on the catalytic growth of SWNTs. Experimental results show that when the molar ratio of Fe to Pb is 1:1, the FePb/MgO bimetallic catalyst significantly enhances the abundance of (6, 5) chiral SWNTs. Furthermore, the FePb/MgO bimetallic catalyst achieves the synthesis of SWNTs with narrow chirality distributions at 800 °C. This provides new research insights and experimental foundations for developing novel bimetallic catalytic systems for synthesizing SWNTs with narrow chirality distributions.

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