Li Yanru, Li Hongwei, Li Guixian, Wang Dongliang, Wang Shoudeng, Zhao Xinhong
School of Petrochemical Technology, Lanzhou University of Technology, Lanzhou, 730050, China.
Key Laboratory of Low Carbon Energy and Chemical Engineering of Gansu Province, Lanzhou, 730050, China.
Nanoscale. 2022 Oct 6;14(38):14199-14211. doi: 10.1039/d2nr04316e.
To enhance nanocatalyst performance and durability for the methanol oxidation reaction (MOR) in a direct methanol fuel cell, small-sized (2.1 nm) and structurally ordered PtCo intermetallic nanoparticles are uniformly anchored onto nitrogen-doped carbon nanotubes (N-CNTs) a low-temperature N-anchoring method, and the N-doping abilities of different N-containing reagents are compared. After investigating the microstructure of PtCo/N-CNTs and evaluating their catalytic activity for the MOR, the results show that N-doping facilitates the uniform loading of PtCo NPs and plays a crucial role in improving the electrocatalytic activity of PtCo NPs supported on CNTs. PtCo/N-CNT-M with melamine as the N dopant exhibits the highest MOR activity and stability among all N-CNT-supported PtCo NPs and Pt/N-CNT-M. Density functional theory calculations suggest that the doping of N enhances the binding energy of CNTs to PtCo NPs, and the MOR mechanism shows that the introduction of Co is the reason for the enhancement of MOR reaction kinetics. The excellent electrochemical performance of PtCo/N-CNT-M is mainly attributed to the synergistic effect of N and PtCo intermetallic nanoparticles. The combination of ordered alloy nanoparticles and high-performance carrier N-CNT-M described herein exhibits great potential for fuel cells and may provide an unequivocal direction for the optimization of catalyst performance.
为提高直接甲醇燃料电池中甲醇氧化反应(MOR)的纳米催化剂性能和耐久性,采用低温氮锚定法将小尺寸(2.1 nm)且结构有序的PtCo金属间化合物纳米颗粒均匀锚定在氮掺杂碳纳米管(N-CNTs)上,并比较了不同含氮试剂的氮掺杂能力。在研究了PtCo/N-CNTs的微观结构并评估其对MOR的催化活性后,结果表明,氮掺杂有助于PtCo纳米颗粒的均匀负载,并在提高负载在碳纳米管上的PtCo纳米颗粒的电催化活性方面起着关键作用。以三聚氰胺作为氮掺杂剂的PtCo/N-CNT-M在所有N-CNT负载的PtCo纳米颗粒和Pt/N-CNT-M中表现出最高的MOR活性和稳定性。密度泛函理论计算表明,氮的掺杂增强了碳纳米管与PtCo纳米颗粒的结合能,MOR机理表明,Co的引入是MOR反应动力学增强的原因。PtCo/N-CNT-M优异的电化学性能主要归因于N与PtCo金属间化合物纳米颗粒的协同效应。本文所述的有序合金纳米颗粒与高性能载体N-CNT-M的结合在燃料电池方面展现出巨大潜力,并可能为催化剂性能优化提供明确方向。