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Stabilizing Pt3Co intermetallic nanocrystals on Co3ZnC/Co in N-doped carbon for efficient oxygen reduction reaction and high-performance zinc-air batteries
Carbon ( IF 10.5 ) Pub Date : 2023-07-26 , DOI: 10.1016/j.carbon.2023.118321
Weiyi Shi , Jie Zhang , Xinran Dong , Jinwei Chen , Gang Wang , Ruilin Wang

Tremendous attention has been paid to the stabilization of Pt-based catalysts on desirable supports to reduce Pt loading in zinc-air batteries (ZABs). However, it is still challenging to design catalysts with efficient activity and stability because of the sluggish kinetic of oxygen reduction reaction (ORR) occurred at cathode. Here, we proposed an effective strategy to fabricate highly dispersed Pt3Co nanocrystals on zeolitic imidazolate frameworks-derived multicomponent support of Co3ZnC@Co in N-doped carbon. Especially, Pt3Co intermetallic can be simultaneously generated on the formed Co3ZnC@Co-NC after the two-step pyrolysis. The Co3ZnC@Co-NC is beneficial to enhance the anchoring ability, resulting in an improved stability for active Pt3Co nanocrystals. What's more, theoretical calculation reveals the unique composition of support could adjust the geometric configuration and electronic structure of Pt, resulting in a favorable ORR process. As expected, the optimal Pt3Co/Co3ZnC@Co-NC delivers the high half-wave potential (E1/2) of 0.90 V and only 11 mV of negative shift on E1/2 after 30000 cycles. When applied in air cathode, Pt3Co/Co3ZnC@Co-NC-based ZABs also exhibit considerable performance with peak power density of 172 mW cm−2, specific capacity of 809 mAh g−1, and long-term cycling stability. This work provides an insight for preparation of durable ORR catalysts for ZABs.



中文翻译:

在氮掺杂碳中稳定 Co3ZnC/Co 上的 Pt3Co 金属间纳米晶体,以实现高效的氧还原反应和高性能锌空气电池

人们对铂基催化剂在理想载体上的稳定性给予了极大的关注,以减少锌空气电池(ZAB)中的铂负载。然而,由于阴极发生的氧还原反应(ORR)动力学缓慢,设计具有高效活性和稳定性的催化剂仍然具有挑战性。在这里,我们提出了一种有效的策略,在 N 掺杂碳中的Co 3 ZnC@Co沸石咪唑酯骨架衍生的多组分载体上制造高度分散的 Pt 3 Co 纳米晶体。特别是,两步热解后形成的Co 3 ZnC@Co-NC上可以同时生成Pt 3 Co金属间化合物。3ZnC@Co-NC有利于增强锚定能力,从而提高活性Pt 3 Co纳米晶的稳定性。此外,理论计算表明,载体的独特组成可以调整Pt的几何构型和电子结构,从而产生有利的ORR过程。正如预期的那样,最佳的 Pt 3 Co/Co 3 ZnC@Co-NC 可提供 0.90 V 的高半波电势 (E 1/2 ),并且在 30000 次循环后E 1/2上仅产生 11 mV 的负移。当应用于空气阴极时,Pt 3 Co/Co 3 ZnC@Co-NC基ZAB也表现出相当好的性能,峰值功率密度为172 mW cm -2,比容量为809 mAh g -1,并且具有长期循环稳定性。这项工作为制备 ZAB 的耐用 ORR 催化剂提供了见解。

更新日期:2023-07-31
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