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与CeO纳米酶杂交的铁单原子碳催化剂的ORR耐久性的改善。

Improvement in ORR Durability of Fe Single-Atom Carbon Catalysts Hybridized with CeO Nanozyme.

作者信息

Qiu Yiwei, Wu Yu, Wei Xiaoqian, Luo Xin, Jiang Wenxuan, Zheng Lirong, Gu Wenling, Zhu Chengzhou, Yamauchi Yusuke

机构信息

State Key Laboratory of Green Pesticide, International Joint Research Center for Intelligent Biosensing Technology and Health, College of Chemistry, Central China Normal University, Wuhan, 430079, People's Republic of China.

Faculty of Science and Engineering, Waseda University, 3-4-1 Okubo Shinjuku, Tokyo, 169-8555, Japan.

出版信息

Nano Lett. 2024 Jul 24;24(29):9034-9041. doi: 10.1021/acs.nanolett.4c02178. Epub 2024 Jul 11.

DOI:10.1021/acs.nanolett.4c02178
PMID:38990087
Abstract

FeNC catalysts are considered one of the most promising alternatives to platinum group metals for the oxygen reduction reaction (ORR). Despite the extensive research on improving ORR activity, the undesirable durability of FeNC is still a critical issue for its practical application. Herein, inspired by the antioxidant mechanism of natural enzymes, CeO nanozymes featuring catalase-like and superoxide dismutase-like activities were coupled with FeNC to mitigate the attack of reactive oxygen species (ROS) for improving durability. Benefiting from the multienzyme-like activities of CeO, ROS generated from FeNC is instantaneously eliminated to alleviate the corrosion of carbon and demetallization of metal sites. Consequently, FeNC/CeO exhibits better ORR durability with a decay of only 5 mV compared to FeNC (18 mV) in neutral electrolyte after 10k cycles. The FeNC/CeO-based zinc-air battery also shows minimal voltage decay over 140 h in galvanostatic discharge-charge cycling tests, outperforming FeNC and commercial Pt/C.

摘要

铁氮碳(FeNC)催化剂被认为是氧还原反应(ORR)中铂族金属最有前景的替代物之一。尽管在提高ORR活性方面进行了广泛研究,但FeNC不理想的耐久性仍是其实际应用中的关键问题。在此,受天然酶抗氧化机制的启发,具有过氧化氢酶样和超氧化物歧化酶样活性的CeO纳米酶与FeNC耦合,以减轻活性氧(ROS)的攻击,从而提高耐久性。受益于CeO的多酶样活性,FeNC产生的ROS被即时消除,以减轻碳的腐蚀和金属位点的脱金属。因此,在中性电解质中经过10000次循环后,FeNC/CeO表现出更好的ORR耐久性,与FeNC(18 mV)相比,衰减仅为5 mV。基于FeNC/CeO的锌空气电池在恒电流充放电循环测试中,在140小时内也显示出最小的电压衰减,优于FeNC和商业Pt/C。

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