Surface oxygenation induced strong interaction between Pd catalyst and functional support for zinc–air batteries
Surface oxygenation induced strong interaction between Pd catalyst and functional support for zinc–air batteries
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表面氧化引起锌空气电池的钯催化剂和功能载体之间的强相互作用
DOI：
10.1039/d1ee03972e
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发表时间：
2022
影响因子：
32.5
通讯作者：
Gu, Meng
中科院分区：
文献类型：
--
作者：
Zhang, Wei;Chang, Jinfa;Wang, Guanzhi;Li, Zhao;Wang, Maoyu;Zhu, Yuanmin;Li, Boyang;Zhou, Hua;Wang, Guofeng;Gu, Meng
由于铂族金属（PGM）催化剂的电子结构优化和高利用率，利用强金属-载体相互作用（SMSI）效应来提高催化剂对氧还原反应（ORR）的活性是有前景的。与传统碳载体相比，金属氧化物作为铂族金属的替代载体可促进固有活性并提高耐久性。然而，需要解决金属/载体界面处的受限质量和电子转移。在此，为了增强金属/载体界面的相互作用并提高PGM的利用效率，将超低负载的Pd嵌入表面氧化的PdNiMnO多孔薄膜中。 Mn掺杂的目的是通过一种简便的阳极氧化工艺促进表面氧化，该工艺在Pd和载体之间形成充分暴露的界面，增强Pd/氧化载体界面处的SMSI效应，从而提高ORR性能。此外，含镍氧化催化剂既作为析氧反应（OER）的活性成分，又作为稳定Pd的功能载体，使PdNiMnO成为锌空气液流电池（ZAFB）的双功能催化剂。作为概念验证，ZAFB (PdNiMnO) 显示出 211.6 mW cm−2 的最大功率密度和超过 2000 小时的出色循环稳定性，在 10 mA cm−2 的电流密度下最小电压间隙为 0.69 V，优于最先进的催化剂。
Employing the strong metal-support interaction (SMSI) effect for promoting the catalyst's activity toward the oxygen reduction reaction (ORR) is promising due to the electronic structure optimization and high utilization efficiency of platinum group metal (PGM) catalysts. Metal oxides as alternative supports for PGMs facilitate intrinsic activity and improve durability as compared to conventional carbon supports. However, the restricted mass and electron transfer at the metal/support interface need to be addressed. Herein, to strengthen the interaction at the metal/support interfaces and improve the utilization efficiency of PGM, an ultralow loading of Pd was embedded in a surface-oxygenated PdNiMnO porous film. The Mn-doping was designed to promote surface oxygenation using a facile anodization process that created sufficiently exposed interfaces between Pd and the support, strengthening the SMSI effects at the Pd/oxygenated support interface for enhancing ORR performance. Furthermore, the Ni-containing oxygenated catalyst served as both the active component for the oxygen evolution reaction (OER) and the functional support for stabilizing Pd, making PdNiMnO a bifunctional catalyst for zinc–air flow batteries (ZAFB). As a proof-of-concept, the ZAFB (PdNiMnO) shows a maximal power density of 211.6 mW cm−2 and outstanding cycling stability for over 2000 h with a minimal voltage gap of 0.69 V at a current density of 10 mA cm−2, superior to the state-of-the-art catalysts.