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Stabilization of Carbon Chain and Application on Metal-free Catalyst

Periodic Reporting for period 1 - SCCAMC (Stabilization of Carbon Chain and Application on Metal-free Catalyst)

Okres sprawozdawczy: 2023-08-01 do 2025-07-31

The goal of this project is to stabilize carbon chains (also known as polyynes or carbon atomic nanowires) in solid materials and to investigate their electrochemical performance, with a focus on metal-free catalysts for the oxygen reduction reaction (ORR). Three objectives are addressed: O1: deposition of functionalized carbon chains; O2: nitrogen-doping capability of carbon chain-based materials; O3: electrochemical performance of carbon chain-based materials as metal-free catalysts for ORR.
In this project, we have developed new methods for synthesizing carbon chains, including a modified chemical coupling method and a modified physical arc-discharge method. A new sp–sp² hybrid carbon chain-based material has been synthesized through a liquid–liquid interfacial reaction at room temperature. This new carbon chain-based material has exhibited high stability under ambient conditions. Heat-treated carbon materials have undergone structural transformations and have demonstrated ORR performance as metal-free catalysts in alkaline electrolytes.
In addition, a collaboration activity has been carried out to facilitate knowledge transfer. Polyynes, as perfectly linear molecules, have been successfully encapsulated into carbon nanotubes. An irreversible one-dimensional Langmuir adsorption model has been proposed to explain the behavior of linear carbon chains encapsulated in carbon nanotubes.
1.A modified chemical coupling method has been developed for preparing highly concentrated polyynes. Polyynes up to C24H2 can be detected.
2.A modified physical arc-discharge method has been developed. By combining pulsed arc discharge in liquid with solvent recovery, polyynes and cyano polyynes can be prepared with higher purity and more than 80% solvent savings compared with conventional arc discharge.
3.A new sp–sp² hybrid carbon membrane has been synthesized at room temperature. The new material is stable under ambient condition.
4. An Island growth mode is proposed to explain the formation of new carbon materials.
5. The ORR performance of the thermal treated new carbon materials has been observed. The new material can be a metal-free catalyst for ORR in alkaline condition.
6. Size-selected polyynes have been successfully encapsulated into chirality-isolated single-walled carbon nanotubes.
7. An irreversible Langmuir adsorption model is proposed to explain the encapsulation behavior of polyynes in carbon nanotubes.
8. Laser irradiation has been applied as a novel way to enhance the encapsulation by an order of magnitude.
The research work carried out will enhance innovation capacity through new methodologies and knowledge. The modified chemical coupling method significantly improves the yield of polyynes with ease. The modified physical method for preparing both polyynes and cyano-polyynes greatly enhances product purity and reduces solvent consumption by over 80% through solvent recovery. These two methods will benefit all lab-scale research on polyynes. The preparation of solid carbon chain-based material at room temperature also offers energy-saving advantages compared to other carbon-based materials. The resulting new materials will create more opportunities for the academic community. Currently, stable carbon chain-based material has been achieved at lab scale (wafer-sized), with its basic structural information validated through standardized tests including Raman, SEM, and TEM. Key physical and chemical properties, as well as potential applications such as metal-free catalytic performance, have also been tested. Therefore, no immediate industrial or market opportunities can be identified. At the present stage, academic researchers are the target group and users. The new material has attracted interest among our collaborators and is expected to gain wider attention after publication.
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