Browsing by Author "Babu, Siddharth Komini"
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Item Biosourced Antioxidants for Chemical Durability Enhancement of Perfluorosulfonic Acid Membrane(Advanced Functional Materials, 2024-01-02) Agarwal, Tanya; Adhikari, Santosh; Babu, Siddharth Komini; Prasad, Ajay K.; Advani, Suresh G.; Borup, Rodney L.The chemical durability of perfluorosulfonic acid (PFSA) membranes is a topic of growing interest to meet Department of Energy (DOE) durability targets for heavy-duty vehicle (HDV) applications. State-of-the-art membranes like Nafion, rely on the use of cerium, heteropolyacids, and other inorganic additives to increase PFSA chemical durability. A less explored avenue for the oxidative stabilization of PFSA and hydrocarbon membranes is the use of organic antioxidants. No reversible organic antioxidant has been demonstrated to date which can enhance membrane lifetime by factors comparable to cerium. Here, ellagic acid (EA) is demonstrated as a promising radical scavenger for PFSA's. It is found that the incorporation of EA enhances the chemical durability of Nafion by 160%. EA, when incorporated with cerium as an electron donorenhances Nafion durability by at least 80% compared to a membrane incorporated with just cerium in DOE-defined durability tests. EA is found to be reversible in acidic conditions like those of fuel cells and its reversibility could be further enhanced by the use of suitable co-antioxidants.Item Fluoroalkyl phosphonic acid radical scavengers for proton exchange membrane fuel cells(Journal of Materials Chemistry A, 2023-04-06) Agarwal, Tanya; Adhikari, Santosh; Kim, Yu Seung; Babu, Siddharth Komini; Tian, Ding; Bae, Chulsung; Pham, Nguyet N. T.; Lee, Seung Geol; Prasad, Ajay K.; Advani, Suresh G.; Sievert, Allen; Rasika, Wipula Priya Liyanage; Hopkins, Timothy E.; Park, Andrew; Borup, RodRadical-induced degradation of proton exchange membranes limits the durability of proton-exchange membrane fuel cells. Cerium is widely used as a radical scavenger, but the migration of cerium ions to the catalyst layer has been an unresolved issue, reducing its effectiveness over time. Here, we report phosphonic acids as a promising class of radical scavengers, showing competent radical scavenging activity compared to cerium without the migration issue. The ex situ Fenton test shows that the fluoride emission rate for Nafion membrane incorporated with fluoroalkyl phosphonic acid ranged from 0.22 to 0.37 μg F cm−2 h−1, lower than that of the cerium-incorporated Nafion™ membrane (0.39 μg F cm−2 h−1). The in situ open circuit voltage hold test confirmed that a phosphonic acid-incorporated Nafion™ membrane has a 58% lower fluoride emission rate compared to the baseline. Density functional theory calculations indicate that the activation energy of the hydroxyl radical scavenging reaction of an alkyl phosphonic acid is only 0.68 eV, suggesting an effective radical scavenging pathway.