ZIF-67-derived CoO (tetrahedral Co2+)@nitrogen-doped porous carbon protected by oxygen vacancies-enriched SnO2 as highly active catalyst for oxygen reduction and Pt co-catalyst for methanol oxidation
ZIF-67-derived CoO (tetrahedral Co2+)@nitrogen-doped porous carbon protected by oxygen vacancies-enriched SnO2 as highly active catalyst for oxygen reduction and Pt co-catalyst for methanol oxidation
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ZIF-67衍生的CoO（四面体Co2）@富氧空位SnO2保护的氮掺杂多孔碳作为氧还原的高活性催化剂和甲醇氧化的Pt助催化剂
DOI：
10.1016/j.apcatb.2019.118043
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发表时间：
2019-12
期刊：
影响因子：
--
通讯作者：
Zou Jinlong
中科院分区：
文献类型：
--
作者：
Yu Yang;You Shijie;Du Jiannan;Xing Zipeng;Dai Ying;Chen Hun;Cai Zhuang;Ren Nanqi;Zou Jinlong
制备高效的甲醇氧化/氧还原催化剂(MOR/ORR)是使直接甲醇燃料电池更加经济的关键。本文以分子筛咪唑骨架-67(ZIF-67)为载体，制备了层次化的CoO@氮掺杂多孔碳@SnO2(COO@NPC@SnO2)多面体作为ORR活性催化剂和铂载体/MoR共催化剂。对于ORR，CoO@NPC@SnO2-1(Co@NPC与SnCl2·2H2O的质量比为1：1)的峰电位(0.82 V比RHE)比商业铂/C(10 wt.%)更正。在ORR过程中，外层SnO2壳层可以防止CoO核(活性四面体Co2+)的腐蚀。对于MOR，Pt-CoO@NPC@SnO2-1(5 wt.%)的质量活性(1518mA mgPT−1)远高于铂/C(496.8 mgPT−1)。PtCoO@NPC@SnO2-1对CO的高耐受性归因于强的金属(Pt)-金属氧化物(SnO2)相互作用，这种相互作用促进了OH−在SnO2上的吸附，从而去除Coad。因此，本研究提供了一种通过使用ZIF模板中的分级结构催化剂/助催化剂来提高ORR/MOR性能的策略。
Fabrication of efficient catalyst/co-catalyst for enhancing methanol oxidation and oxygen reduction reactions (MOR/ORR) is the key to make direct methanol fuel cells more economical. Here, hierarchical CoO@nitrogen-doped porous carbon@SnO2(CoO@NPC@SnO2) polyhedrons are prepared as active catalysts for ORR and Pt supports/co-catalysts for MOR using zeolitic imidazolate frameworks-67 (ZIF-67). For ORR, CoO@NPC@SnO2-1 (Co@NPC-to-SnCl2·2H2O mass ratio of 1: 1) exhibits a more positive peak potential (0.82 V vs. RHE) than that of commercial Pt/C (10 wt.%). Outer SnO2shells can prevent CoO cores (active tetrahedral Co2+) from corrosion during ORR. For MOR, Pt-CoO@NPC@SnO2-1 (5 wt.%) shows a much higher mass activity (1518 mA mgPt−1) than that of Pt/C (496.8 mA mgPt−1). High CO tolerance of Pt-CoO@NPC@SnO2-1 is attributed to strong metal (Pt)-metal oxides (SnO2) interactions, which facilitate adsorption of OH−on SnO2to remove COads. Therefore, this study provides a strategy to enhance ORR/MOR performance by using hierarchically-structured catalysts/co-catalysts from ZIF templates.
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