Exploring the effect of surface chemistry and particle size of boron-doped diamond powder as catalyst and catalyst support for the oxygen reduction reaction

Exploring the effect of surface chemistry and particle size of boron-doped diamond powder as catalyst and catalyst support for the oxygen reduction reaction
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DOI:
10.1016/j.electacta.2023.142121
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发表时间:
2023-02
影响因子:
6.6
通讯作者:
G. Alemany-Molina;Beatriz Martínez-Sánchez;Atsushi Gabe;Takeshi Kondo;D. Cazorla-Amorós;E. Morallón-
G. Alemany-Molina;Beatriz Martínez-Sánchez;Atsushi Gabe;Takeshi Kondo;D. Cazorla-Amorós;E. Morallón-
中科院分区:
材料科学2区
文献类型:
--
作者:
G. Alemany-Molina;Beatriz Martínez-Sánchez;Atsushi Gabe;Takeshi Kondo;D. Cazorla-Amorós;E. Morallón-

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近年来,基于导电掺硼金刚石粉(BDDP)的电极由于其优异的物理和化学稳定性,在水和有机电解质中的宽电位窗口,相对较大的比表面积以及与掺硼金刚石薄膜电极相比的通用性而受到越来越多的关注。由于这些材料在燃料电池(特别是汽车)启停过程中产生的高正电位下具有较高的耐腐蚀性,因此被提议作为替代阴极催化剂载体。在本研究中,我们提出了三种不同粒径和不同表面氧含量的BDDP载体,作为不同铁种的载体,在碱性溶液中进行氧还原反应。用氮化碳(C3N4)或酞菁(Pc)作为铁的锚定点对BDDP支架进行改性。观察到的不同电催化性能证实了BDDP载体的表面化学对FePc样品金属位活性的强烈影响,而对于fe - c3n4样品,BDDP载体的粒径是决定作用。此外,DFT计算用于获得FePc与金刚石表面相互作用的一些见解。
The interest for the electrodes based on conductive boron-doped diamond powder (BDDP) is increasing in recent years due to their excellent physical and chemical stability, the wide potential window in both aqueous and organic electrolytes, the relatively large specific surface area, and their versatility in comparison to boron-doped diamond thin film electrodes. These materials have been proposed as alternative cathode catalyst support due to their high corrosion resistance when subjected to the highly positive potentials originated during the start-stop operations in fuel cells, especially in automobiles. In this work, we present three BDDP supports with different particle sizes and different surface oxygen contents as supports of different iron species for oxygen reduction reaction in alkaline solution. BDDP supports were modified with carbon nitride (C3N4) or phthalocyanines (Pc) as anchoring points for iron. The different electrocatalytic performance observed confirmed the strong influence of the surface chemistry of the BDDP supports on the activity of the metallic sites for FePc samples while, for Fe-C3N4samples, the determining effect was the particle size of the BDDP support. Additionally, DFT calculations were used to obtain some insights about the interaction of the FePc with the diamond surface.