Constructing a Triangle Ensemble of Pt Clusters for Enhanced Direct-Pathway Electrocatalysis of Formic Acid Oxidation
Cheng Li,
Zheng Tang,
Lanlan Shi,
Yongjia Li,
Yingjie Ji,
Kaixin Zhang,
Zhiyu Yang,
Yi-Ming Yan
Affiliations
Cheng Li
State Key Lab of Organic-Inorganic Composites, Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing 100029, China
Zheng Tang
State Key Lab of Organic-Inorganic Composites, Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing 100029, China
Lanlan Shi
State Key Lab of Organic-Inorganic Composites, Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing 100029, China
Yongjia Li
State Key Lab of Organic-Inorganic Composites, Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing 100029, China
Yingjie Ji
State Key Lab of Organic-Inorganic Composites, Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing 100029, China
Kaixin Zhang
State Key Lab of Organic-Inorganic Composites, Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing 100029, China
Zhiyu Yang
State Key Lab of Organic-Inorganic Composites, Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing 100029, China
Yi-Ming Yan
State Key Lab of Organic-Inorganic Composites, Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing 100029, China
The pursuit of operational advancements in direct formic acid fuel cells (DFAFCs) necessitates the development of high-performance platinum (Pt)-based catalysts for formic acid electrooxidation (FAOR). However, FAOR on Pt-based catalysts follows a dual pathway mechanism, in which the direct pathway is a preferred route due to its efficient dehydrogenation process. Conversely, the indirect pathway results in the generation of adsorbed CO species, a process that deleteriously poisons the active sites of the catalyst, with CO species only being oxidizable at higher potentials, causing a significant compromise in catalyst performance. Herein, we have successfully synthesized Pt-C3N4@CNT, where three Pt clusters are precisely dispersed in a triplet form within the C3N4 by virtue of the unique structure of C3N4. The mass activity for the direct pathway (0.44 V) delivered a current density of 1.91 A mgPt−1, while the indirect pathway (0.86 V) had no obvious oxidation peak. The selectivity of Pt-C3N4@CNT catalysts for the direct pathway of FAOR was improved due to the special structure of C3N4, which facilitates the dispersion of Pt tri-atoms in the structure and the electronic interaction with Pt. In this study, we provide a new strategy for the development of highly active and selective catalysts for DFAFCs.
