Journal
ACS CATALYSIS
Volume 9, Issue 12, Pages 11242-11254Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.9b03155
Keywords
Pt-based intermetallic nanostructures; activity origin; multifunctional electrocatalysis; free-standing catalysts; proton exchange membrane fuel cells
Categories
Funding
- National Research Foundation (NRF) of Korea - Ministry of Science and ICT [NRF-2015M1A2A2056560, NRF-2016M3D IA1900035, NRF-2017R1A2B2008464, NRF-2017R1A4A1015533, 2017M1A2A2092564]
- Korea Evaluation Institute of Industrial Technology (KEIT) - Ministry of Trade, Industry and Energy [10050509]
- KIST [2E28271]
- Ministry of Education, Pohang University of Science of Technology (POSTECH)
- UCRF at UNIST
- Ministry of Science & ICT (MSIT), Republic of Korea [2E28271] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)
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Pt-based intermetallic nanostructures have demonstrated higher electrocatalytic performances compared to random alloy structures. However, the origin of their enhanced catalytic properties remains elusive. Furthermore, a robust synthetic strategy for well-defined intermetallic nanostructures represents a challenge. Here, we reveal by combining theoretical and experimental results that the activity enhancement in intermetallic structures for the oxygen reduction reaction (ORR) originates from an intensified ligand effect. We prepared well-defined model nanocatalysts via confined nanospace-directed synthesis using mesoporous silica templates, which allows precise control over the size and shape of nanostructures. Importantly, this method can transform disordered alloy nanostructures into intermetallic analogues without agglomeration, enabling decoupling of an atomic ordering effect in catalysis. The prepared ordered intermetallic Pt3Co nanowires (O-Pt3Co NWs) can benefit from an intensified ligand effect, Pt-skin layer, and agglomeration-tolerant contiguous structure, which led to their enhanced ORR activity and durability compared to disordered alloy Pt3Co nanowires (D-Pt3Co NWs) and Pt/C catalysts. The multifunctionality of O-Pt3Co NWs is demonstrated with their higher activity and durability in the alkaline hydrogen evolution reaction and acidic methanol oxidation reaction than those of D-Pt3Co NWs and Pt/C catalysts. Furthermore, a proton exchange membrane fuel cell cathode based on O-Pt3Co NWs shows much better durability than a Pt/C-based one.
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