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氮掺杂与结构设计对用于氧还原反应的无金属碳化物衍生碳电催化剂的协同效应

Synergistic Effect of Nitrogen Doping and Textural Design on Metal-Free Carbide-Derived Carbon Electrocatalysts for the ORR.

作者信息

Pérez-Román Berta, Recio F Javier, López-Sánchez Jesús, Pascual Laura, Mazo M Alejandra, Rubio-Marcos Fernando

机构信息

Instituto de Cerámica y Vidrio (ICV-CSIC), C/Kelsen 5, 28049 Madrid, Spain.

Escuela de Doctorado UAM, C/Francisco Tomás y Valiente 2, 28049 Madrid, Spain.

出版信息

ACS Appl Mater Interfaces. 2025 Sep 24;17(38):53388-53401. doi: 10.1021/acsami.5c10307. Epub 2025 Sep 9.

Abstract

The oxygen reduction reaction (ORR) is critical to energy conversion technologies and requires efficient catalysts for superior performance. Herein, nitrogen-doped carbide-derived carbon (N-CDC) catalysts are prepared using novel engineered molecular architectures based on polymer-derived ceramic technology. The obtained catalyst materials show a surface N concentration of >5 wt % and a hierarchically porous structure, resulting in a specific surface area of over 2000 m g. Subsequently, the electrocatalytic activity toward the ORR is studied in different media (acid, neutral, and alkaline conditions) using a rotating ring-disk electrode. The N-CDC catalysts demonstrate clear improvements in performance due to nitrogen doping in neutral and acidic media, while textural properties are crucial for the ORR activity in alkaline media. Specifically, a superior onset potential (0.8 V vs RHE) and enhanced kinetics (58 mV dec) are achieved in 0.1 M KOH. This work opens new avenues in the field of electrocatalysis, highlighting the potential of N-CDC materials and their significant advantage for the controlled synthesis of hierarchical porous and doped materials.

摘要

氧还原反应(ORR)对于能量转换技术至关重要,并且需要高效催化剂以实现卓越性能。在此,基于聚合物衍生陶瓷技术,利用新型工程化分子结构制备了氮掺杂碳化物衍生碳(N-CDC)催化剂。所获得的催化剂材料表面氮浓度大于5 wt%,且具有分级多孔结构,导致比表面积超过2000 m²/g。随后,使用旋转环盘电极在不同介质(酸性、中性和碱性条件)下研究了对ORR的电催化活性。由于在中性和酸性介质中进行了氮掺杂,N-CDC催化剂的性能有明显改善,而结构性质对于碱性介质中的ORR活性至关重要。具体而言,在0.1 M KOH中实现了优异的起始电位(相对于可逆氢电极0.8 V)和增强的动力学(58 mV/dec)。这项工作为电催化领域开辟了新途径,突出了N-CDC材料的潜力及其在可控合成分级多孔和掺杂材料方面的显著优势。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/21ea/12464907/8bea841518c4/am5c10307_0001.jpg

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