Mitigating cerium migration for perfluorosulfonic acid membranes using organic ligands

Technical Report · Wed Nov 09 04:00:00 EST 2022

DOI:https://doi.org/10.2172/2386899· OSTI ID:2386899

Agarwal, Tanya ^[1]; Gonzales, Ivana ^[2]; Adhikari, Santosh ^[3]; Park, Eun Joo ^[3]; Komini Babu, Siddharth ^[3]; Kim, Yu Seung ^[3]; Tian, Ding ^[4]; Bae, Chulsung ^[4]; Morales-Collazo, Oscar ^[5]; F. Brennecke, Joan ^[5]; Prasad, Ajay K. ^[6]; Advani, Suresh G. ^[6]; Sievert, Allen ^[7]; Hopkins, Timothy ^[7]; Park, Andrew ^[7]; Borup, Rodney L. ^[3]

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1. Los Alamos National Laboratory (LANL), Los Alamos, NM (United States); Univ. of Delaware, Newark, DE (United States)
2. Los Alamos National Laboratory (LANL), Los Alamos, NM (United States); Univ. of New Mexico, Albuquerque, NM (United States)
3. Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
4. Rensselaer Polytechnic Inst., Troy, NY (United States)
5. Univ. of Texas, Austin, TX (United States)
6. Univ. of Delaware, Newark, DE (United States)
7. The Chemours Company, Newark, DE (United States)

Improving the electrochemical stability of proton exchange membranes is a pressing priority for heavy-duty fuel cell vehicles. The lifetime of the most widely used perfluorosulfonic acid membranes is limited by reactive free radicals generated inside the system. Cerium has been found to reduce the chemical degradation of the membranes. However, cerium migration during fuel cell operation limits the chemical durability enhancement effect expected from the radical scavenging activity of cerium. Here we investigate a wide range of organic immobilizers for cerium, measuring their suitability concerning cerium retention, radical scavenging activity, and fuel cell performance. We report that partially fluorinated phosphonic acids enhance cerium retention up to 45 times and reduce fluoride emission rate by 38% compared to the commercial Nafion™ XL membrane pre-impregnated with cerium. The energetics of cerium-phosphonic acid complex systems by density functional theory calculations rationalizes effective cerium immobilization.

• Research Organization: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
• Sponsoring Organization: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Hydrogen Fuel Cell Technologies Office (HFTO); USDOE Advanced Research Projects Agency - Energy (ARPA-E); USDOE National Nuclear Security Administration (NNSA)
• DOE Contract Number: 89233218CNA000001; AR0001003; AC02-05CH11231
• OSTI ID: 2386899
• Report Number(s): LA-UR--22-28539
• Country of Publication: United States
• Language: English

Related Subjects

30 DIRECT ENERGY CONVERSION
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
cerium migration
chemical stability
durability
perfluorosulfonic acid
proton exchange membrane fuel cell
radical scavenger