Journal
ACS APPLIED MATERIALS & INTERFACES
Volume 11, Issue 12, Pages 11298-11305Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsami.8b18375
Keywords
non-precious metal catalysts; electrocatalysts; triple phase boundary; interface reaction; oxygen reduction reaction
Funding
- EPSRC [EP/R021554/1, EP/N509899/1, EP/S018204/1]
- EU [CIG 631092]
- CSC
- EPSRC [EP/R021554/1, EP/N509899/1] Funding Source: UKRI
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The oxygen reduction reaction (ORR) in aqueous media plays a critical role in sustainable and clean energy technologies such as polymer electrolyte membrane and alkaline fuel cells. In this work, we present a new concept to improve the ORR performance by engineering the interface reaction at the electrocatalyst/electrolyte/oxygen triple-phase boundary using a protic and hydrophobic ionic liquid and demonstrate the wide and general applicability of this concept to several Pt-free catalysts. Two catalysts, Fe-N codoped and metal-free N-doped carbon electrocatalysts, are used as a proof of concept. The ionic liquid layer grafted at the nanocarbon surface creates a water-equilibrated secondary reaction medium with a higher O-2 affinity toward oxygen adsorption, promoting the diffusion toward the catalytic active site, while its protic character provides sufficient H+/H3O+ conductivity, and the hydrophobic nature prevents the resulting reaction product water from accumulating and blocking the interface. Our strategy brings obvious improvements in the ORR performance in both acid and alkaline electrolytes, while the catalytic activity of FeNC-nanocarbon outperforms commercial Pt-C in alkaline electrolytes. We believe that this research will pave new routes toward the development of high-performance ORR catalysts free of noble metals via careful interface engineering at the triple point.
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