Monolayer supertubes of Carbon-Armored platinum nanocrystals enabling robust oxygen reduction electrocatalysis

Jing Ning; Jinxiang Zou; Ying Long; Xiaomeng Ren; Yangfei Cao; Tongtao Li; Angang Dong

doi:10.1016/j.jcis.2023.06.036

Monolayer supertubes of Carbon-Armored platinum nanocrystals enabling robust oxygen reduction electrocatalysis

J Colloid Interface Sci. 2023 Oct 15:648:719-726. doi: 10.1016/j.jcis.2023.06.036. Epub 2023 Jun 10.

Authors

Jing Ning¹, Jinxiang Zou¹, Ying Long¹, Xiaomeng Ren², Yangfei Cao³, Tongtao Li⁴, Angang Dong⁵

Affiliations

¹ Collaborative Innovation Center of Chemistry for Energy Materials, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Department of Chemistry, Fudan University, Shanghai 200438, China.
² PLA Naval Medical Center, 5 Panshan Rd, Shanghai 200052, China.
³ Collaborative Innovation Center of Chemistry for Energy Materials, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Department of Chemistry, Fudan University, Shanghai 200438, China. Electronic address: caoyangf@fudan.edu.cn.
⁴ Collaborative Innovation Center of Chemistry for Energy Materials, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Department of Chemistry, Fudan University, Shanghai 200438, China. Electronic address: ttli@fudan.edu.cn.
⁵ Collaborative Innovation Center of Chemistry for Energy Materials, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Department of Chemistry, Fudan University, Shanghai 200438, China. Electronic address: agdong@fudan.edu.cn.

PMID: 37321091
DOI: 10.1016/j.jcis.2023.06.036

Abstract

Self-assembled superstructures composed of nanocrystals (NCs) have shown immense potential for enhancing the performance in electrocatalytic applications. However, there has been limited research on the self-assembly of platinum (Pt) into low-dimensional superstructures as efficient electrocatalysts for oxygen reduction reaction (ORR). In this study, we designed a unique tubular superstructure composed of monolayer or sub-monolayer carbon-armored platinum nanocrystals (Pt NCs) using a template-assisted epitaxial assembly approach. The organic ligands on the surface of Pt NCs were in situ carbonized, resulting in few-layer graphitic carbon shells that encapsulate Pt NCs. Due to their monolayer assembly and tubular geometry, the Pt utilization of the supertubes was 1.5 times higher than that of conventional carbon-supported Pt NCs. As a result, such Pt supertubes exhibit remarkable electrocatalytic performance for the ORR in acidic media, with a high half-wave potential of 0.918 V and a high mass activity of 181 A g^-1_Pt at 0.9 V, which are comparable to commercial carbon-supported Pt (Pt/C) catalysts. Furthermore, the Pt supertubes demonstrate robust catalytic stability, as confirmed by long-term accelerated durability tests and identical-location transmission electron microscopy. This study presents a new approach to designing Pt superstructures for highly efficient and stable electrocatalysis.

Keywords: Oxygen reduction reaction; Platinum nanocrystals; Self-assembly; Superstructures; Supertubes.