Effect of NH3 addition on the preparation of nitrogen-doped carbon nanomaterials by flame synthesis method

IF 5.5 3区材料科学 Q2 CHEMISTRY, MULTIDISCIPLINARY

Carbon Letters Pub Date : 2024-06-27 DOI:10.1007/s42823-024-00760-y

Hui Zhou, Yuhang Yang, Fen Qiao, Run Hong, Hanfang Zhang, Huaqiang Chu

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Abstract

Nitrogen-doped carbon nanomaterials (N-CNMs) were prepared using Ni(NO₃)₂ as a catalyst in the laminar diffusion flame. Doping the structure of carbon nanomaterials (CNMs) with nitrogen can significantly change the characteristics of CNMs. The purpose of this research is to study the effect of adding ammonia (NH₃) on the evolution of CNMs structure in the laminar flame of ethylene. Raman analysis shows that the intensity ratio (I_D/I_G) of the D-band and G-band of N-CNMs increases and then decreases after the addition of NH₃. The intensity ratio is a maximum of 0.99, which has a good degree of disorder and defect density. The binding distribution of nitrogen was analyzed by X-ray photoelectron spectroscopy (XPS), and a correlation was found between the amount of nitrogen and the morphology of N-CNMs. Nitrogen atoms predominantly present in the forms of pyrrolic-N, pyridinic-N, graphitized-N and oxidized-N, with a doping ratio of nitrogen atoms reaching up to 2.44 at.%. This study found that smaller nickel (Ni) nanoparticles were the main catalysts for carbon nanotubes (CNTs), and their synthesis followed the ‘hollow growth mechanism’ and carbon nanofibers (CNFs) were synthesized from larger Ni nanoparticles according to the ‘solid growth mechanism’. Furthermore, a growth mechanism for the synthesis of bamboo-like CNTs using a specific particle size of the Ni catalyst is proposed. It is noteworthy that the synthesis and modulation of high-performance N-CNMs by flame method represents a simple and efficient approach.

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添加 NH3 对火焰合成法制备掺氮碳纳米材料的影响

以 Ni(NO3)2 为催化剂，在层流扩散火焰中制备了掺氮碳纳米材料（N-CNMs）。在碳纳米材料（CNMs）结构中掺入氮元素可显著改变 CNMs 的特性。本研究旨在研究添加氨气（NH3）对乙烯层流火焰中 CNMs 结构演化的影响。拉曼分析表明，添加 NH3 后，N-CNMs 的 D 波段和 G 波段的强度比（ID/IG）先增大后减小。其强度比最大值为 0.99，具有良好的无序度和缺陷密度。通过 X 射线光电子能谱（XPS）分析了氮的结合分布，发现氮的数量与 N-CNMs 的形态之间存在相关性。氮原子主要以吡咯-N、吡啶-N、石墨化-N 和氧化-N 的形式存在，氮原子的掺杂率高达 2.44%。该研究发现，较小的镍纳米粒子是碳纳米管（CNTs）的主要催化剂，其合成遵循 "空心生长机制"，而碳纳米纤维（CNFs）则根据 "固体生长机制 "由较大的镍纳米粒子合成。此外，还提出了利用特定粒径的镍催化剂合成竹节状 CNTs 的生长机制。值得注意的是，利用火焰法合成和调制高性能 N-CNMs 是一种简单而高效的方法。

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来源期刊

Carbon Letters CHEMISTRY, MULTIDISCIPLINARY-MATERIALS SCIENCE, MULTIDISCIPLINARY

CiteScore

7.30

自引率

20.00%

发文量

118

期刊介绍： Carbon Letters aims to be a comprehensive journal with complete coverage of carbon materials and carbon-rich molecules. These materials range from, but are not limited to, diamond and graphite through chars, semicokes, mesophase substances, carbon fibers, carbon nanotubes, graphenes, carbon blacks, activated carbons, pyrolytic carbons, glass-like carbons, etc. Papers on the secondary production of new carbon and composite materials from the above mentioned various carbons are within the scope of the journal. Papers on organic substances, including coals, will be considered only if the research has close relation to the resulting carbon materials. Carbon Letters also seeks to keep abreast of new developments in their specialist fields and to unite in finding alternative energy solutions to current issues such as the greenhouse effect and the depletion of the ozone layer. The renewable energy basics, energy storage and conversion, solar energy, wind energy, water energy, nuclear energy, biomass energy, hydrogen production technology, and other clean energy technologies are also within the scope of the journal. Carbon Letters invites original reports of fundamental research in all branches of the theory and practice of carbon science and technology.