Dual-template strategy synthesis of hierarchically porous electrocatalysts for oxygen reduction reaction

Yuxin Xie , Xiaogang Yu , Zhaohang Jin , Qingbin Liu , Shizhen Liu , Yun Zhao , Zhonghua Xiang
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Abstract

Metal organic frameworks derived M-N-C catalysts have been discovered as promising alternatives to Pt-based catalysts in oxygen reduction reaction (ORR). However, the dominated micropores in their porous structures strongly restrain the mass transfer and lead to insufficient utilization of active sites. Here, we proposed a dual-template strategy to improve the catalytic performance of ZIF-8 derived M-N-C catalysts. Both the silica and sodium chloride templates created mesopores, which may intensified the mass transfer. Moreover, the molten sodium chloride connected the individual ZIF-8 crystals form highly graphitized carbon structure which had better stability and conductivity. The as-synthesized (FeCo)HPNC@NaCl catalyst exhibited similar ORR activity to commercial Pt/C under acidic conditions with half-wave potential of 0.808 V. The catalyst expressed high stability with 12 mV decrease of half-wave potential after 5000 cycles and 80% remained activity after 100000 s operation. Moreover, we tested the catalyst in fuel cell for practical application, achieving a high peak power density of 427 mW cm−2.

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双模板策略合成层次多孔氧还原反应电催化剂
金属有机骨架衍生的M-N-C催化剂已被发现是氧还原反应(ORR)中pt基催化剂的有前途的替代品。然而,其多孔结构中占主导地位的微孔强烈地抑制了传质,导致活性位点的利用不足。在这里,我们提出了双模板策略来提高ZIF-8衍生的M-N-C催化剂的催化性能。二氧化硅和氯化钠模板都产生了介孔,这可能会加剧传质。此外,熔融氯化钠连接单个ZIF-8晶体形成高度石墨化的碳结构,具有更好的稳定性和导电性。合成的(FeCo)HPNC@NaCl催化剂在酸性条件下表现出与商品Pt/C相似的ORR活性,半波电位为0.808 V。催化剂表现出较高的稳定性,循环5000次后半波电位降低12 mV,运行100000 s后仍保持80%的活性。此外,我们在燃料电池中测试了催化剂的实际应用,实现了427 mW cm−2的峰值功率密度。
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