Modulating the Interfacial Water Network of Dual-Site Pd/FeO x /C Catalyst for Efficient Formate Electrooxidation.
Yongjia LiKaixin ZhangYingjie JiZheng TangYebo YaoXia LiuDewei WangXiaoxuan WangLanlan ShiKaiqi NieZhiyu YangJiangzhou XieYi-Ming YanPublished in: ACS applied materials & interfaces (2023)
The rational design of electrocatalysts for formate oxidation reaction (FOR) in alkaline media is crucial to promote the practical applications of direct formate fuel cells (DFFCs). The FOR kinetic on palladium (Pd) based electrocatalysts is strongly hindered by unfavorably adsorbed hydrogen (H ad ) as the major intermediate species blocking the active sites. Herein, we report a strategy of modulating the interfacial water network of dual-site Pd/FeO x /C catalyst to significantly enhance the desorption kinetics of H ad during FOR. Aberration-corrected electron microscopy and synchrotron characterizations revealed the successful construction of Pd/FeO x interfaces on carbon support as a dual-site electrocatalyst for FOR. Electrochemical tests and in situ Raman spectroscopy results showed that H ad could be effectively removed from the active sites of the as-designed Pd/FeO x /C catalyst. CO-stripping voltammetry and density functional theory calculations (DFT) demonstrated that the introduced FeO x could effectively accelerate the dissociative adsorption of water molecules on active sites, which accordingly generates adsorbed hydroxyl species (OH ad ) to facilitate the removal of H ad during FOR. This work provides a novel route to develop advanced FOR catalysts for fuel cell applications.
Keyphrases
- density functional theory
- ionic liquid
- molecular dynamics
- metal organic framework
- raman spectroscopy
- room temperature
- highly efficient
- reduced graphene oxide
- visible light
- signaling pathway
- single cell
- electron transfer
- induced apoptosis
- gold nanoparticles
- electron microscopy
- carbon dioxide
- genetic diversity
- mass spectrometry
- molecular docking
- high resolution
- cell proliferation