Publication

NMSL Lab

Publication

Toward highly accessible Fe-N4 sites via rational design of metal chelated ionic liquids for ORR, OER and HER trifunctional electrocatalysis
Author
Arunprasath Sathyaseelan, Vijayakumar Elumalai, Muthukumar Perumalsamy, Noor Ul Haq Liyakath Ali, Aparna Sajeev, Sang-Jae Kim
Journal
Chemical Engineering Journal
Page
151235
Year
2024

Abstract

The development of efficient non-precious, atomically dispersed single-atom catalysts (SACs) is vital for advancing fuel cell and water electrolyzer technologies. Here, we rationally designed a metal-chelated ionic liquid (M-IL) as a cornerstone (single source) to synthesize highly efficient M-SAC electrocatalysts via a robust and straightforward approach for ORR, OER, and HER reactions. The effect of temperature, as well as various metals (Fe, Co, Cu, Ni), on the formation of the M-SAC catalyst, was meticulously investigated. Among the designed single-atom catalysts, IL-Fe-SAC-8 delivered superior methanol tolerance toward ORR with a higher half-wave potential (0.902 V vs. RHE) and lower potential values of −0.127 V and 1.511 V vs. RHE, achieving a benchmark current density of 10 mA cm−2 toward HER and OER reactions. Thanks to the optimal graphitization, abundant defects, enhanced surface area, and high atomic coordination (supported by HAADF & XANES) of IL-Fe-SAC-8. Furthermore, the flexible DMFC assembled using IL-Fe-SAC-8 cathode delivered 2.5 times higher power density than the Pt/C-based cathode. When we tested a bifunctional IL-Fe-SAC-8||IL-Fe-SAC-8 electrolyzer, it achieved 1.58 V to deliver 10 mA cm−2. Moreover, for the real-time demonstration, we powered an H-type membrane water electrolyzer (separated by AEM) with a windmill and measured the hydrogen and oxygen produced concerning wind speeds. Furthermore, the produced hydrogen gas is used to power the lab-scale hydrogen fuel cell vehicle. This overall study demonstrates a new pathway to prepare unexplored atomically dispersed catalysts through a single source and template-free approach for next-generation energy technologies.