Ta-TiOx nanoparticles as radical scavengers to improve the durability of Fe-N-C oxygen reduction catalysts

被引:142
|
作者
Xie, Hua [1 ]
Xie, Xiaohong [2 ]
Hu, Guoxiang [3 ]
Prabhakaran, Venkateshkumar [2 ]
Saha, Sulay [4 ,5 ]
Gonzalez-Lopez, Lorelis [1 ]
Phakatkar, Abhijit H. [6 ]
Hong, Min [1 ]
Wu, Meiling [1 ]
Shahbazian-Yassar, Reza [6 ]
Ramani, Vijay [4 ,5 ]
Al-Sheikhly, Mohamad, I [1 ]
Jiang, De-en [7 ]
Shao, Yuyan [2 ]
Hu, Liangbing [1 ]
机构
[1] Univ Maryland, Dept Mat Sci & Engn, College Pk, MD 20742 USA
[2] Pacific Northwest Natl Lab, Richland, WA 99352 USA
[3] CUNY, Queens Coll, Dept Chem & Biochem, Queens, NY 11367 USA
[4] Washington Univ, Ctr Solar Energy & Energy Storage, St Louis, MO 63110 USA
[5] Washington Univ, Dept Energy Environm & Chem Engn, St Louis, MO 63110 USA
[6] Univ Illinois, Dept Mech & Ind Engn, Chicago, IL 60607 USA
[7] Univ Calif Riverside, Dept Chem, Riverside, CA 92521 USA
基金
美国国家科学基金会;
关键词
TOTAL-ENERGY CALCULATIONS; NONNOBLE METAL-CATALYSTS; IRON-BASED CATALYSTS; HYDROGEN-PEROXIDE; ACIDIC MEDIA; FUEL; CARBON; H2O2; ELECTROREDUCTION; DEGRADATION;
D O I
10.1038/s41560-022-00988-w
中图分类号
TE [石油、天然气工业]; TK [能源与动力工程];
学科分类号
0807 ; 0820 ;
摘要
Low-cost catalysts for oxygen reduction, such as Fe-N-C materials, often suffer from poor stability in fuel cells due to the generation of oxidizing radical species. Here the authors locate Ta-TiOx additives in the vicinity of Fe-N-C catalysts and show that they can successfully scavenge radicals, improving durability. Highly active and durable platinum group metal-free catalysts for the oxygen reduction reaction, such as Fe-N-C materials, are needed to lower the cost of proton-exchange membrane fuel cells. However, their durability is impaired by the attack of oxidizing radicals such as center dot OH and HO2 center dot that form from incomplete reduction of O-2 via H2O2. Here we demonstrate that Ta-TiOx nanoparticle additives protect Fe-N-C catalysts from such degradation via radical scavenging. The 5 nm Ta-TiOx nanoparticles were uniformly synthesized on a Ketjenblack substrate using a high-temperature pulse technique, forming the rutile TaO2 phase. We found that Ta-TiOx nanoparticles suppressed the H2O2 yield by 51% at 0.7 V in an aqueous rotating ring disk electrode test. After an accelerated durability test, a fuel cell prepared with the scavengers showed a current density decay of 3% at 0.9 ViR-free (internal resistance-compensated voltage); a fuel cell without scavengers showed 33% decay. Thus, addition of Ta-TiOx provides an active defence strategy to improve the durability of oxygen reduction reaction catalysts.
引用
收藏
页码:281 / 289
页数:9
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