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Cage-confinement of gas-phase ferrocene in zeolitic imidazolate frameworks to synthesize high-loading and atomically dispersed Fe–N codoped carbon for efficient oxygen reduction reaction†
Journal of Materials Chemistry A ( IF 10.7 ) Pub Date : 2019-06-19 00:00:00 , DOI: 10.1039/c9ta04954a
Guanying Ye 1, 2, 3, 4 , Qian He 5, 6, 7, 8, 9 , Suqin Liu 1, 2, 3, 4, 10 , Kuangmin Zhao 1, 2, 3, 4 , Yuke Su 1, 2, 3, 4 , Weiwei Zhu 1, 2, 3, 4 , Rongjiao Huang 1, 2, 3, 4 , Zhen He 1, 2, 3, 4, 10
Journal of Materials Chemistry A ( IF 10.7 ) Pub Date : 2019-06-19 00:00:00 , DOI: 10.1039/c9ta04954a
Guanying Ye 1, 2, 3, 4 , Qian He 5, 6, 7, 8, 9 , Suqin Liu 1, 2, 3, 4, 10 , Kuangmin Zhao 1, 2, 3, 4 , Yuke Su 1, 2, 3, 4 , Weiwei Zhu 1, 2, 3, 4 , Rongjiao Huang 1, 2, 3, 4 , Zhen He 1, 2, 3, 4, 10
Affiliation
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Fe–N codoped carbon (Fe–N/C) has emerged as one of the most promising non-precious electrocatalysts for the oxygen reduction reaction (ORR). However, the fabrication of Fe–N/C with high Fe and N loadings while maintaining atomic dispersion of the loaded Fe is still challenging. Herein, we present a cage-confinement synthesis strategy that utilizes zeolitic imidazolate framework-8 (ZIF-8) with an ordered microporous structure to uniformly adsorb gas-phase ferrocene (FeCp) molecules at mildly elevated temperatures followed by carbonization to fabricate Fe–N/C with a high content of atomically dispersed Fe and abundant N. The content of FeCp molecules adsorbed in the nanocavities of ZIF-8 could be precisely controlled by the adsorption temperature and time, and confining the adsorbed FeCp in the nanocavities of ZIF-8 could effectively prevent the Fe atoms from aggregating and/or forming Fe compounds during the carbonization process. The Fe–N/C fabricated under optimal conditions has a high iron loading of 5.86 wt% and abundant N content of 10.51 at%. The as-prepared Fe–N/C exhibits a remarkable ORR catalytic performance in 0.1 M KOH with a half-wave potential (E1/2) of 0.85 V (vs. RHE) and excellent long-term durability (less than 10 mV change of E1/2 after 10 000 cycles of the CV test and 11% current density decay after a 40 000 s long-term ORR test). This work provides a simple and controllable synthesis strategy for fabricating high-content atomically dispersed Fe and N codoped carbon catalysts, which might also shed light on the design and synthesis of other single-atom metal doped carbon materials for energy storage and conversion applications.
中文翻译：
在沸石咪唑酸酯骨架中笼固限定气相二茂铁，以合成高负载和原子分散的Fe–N共掺杂碳，以有效地进行氧还原反应†
Fe-N共掺杂碳（Fe-N / C）已成为氧还原反应（ORR）中最有前途的非贵金属电催化剂之一。然而，在保持Fe原子弥散的同时制备高Fe和N负载的Fe–N / C仍具有挑战性。在这里，我们提出了一种笼罩限制合成策略，该策略利用具有有序微孔结构的沸石咪唑啉骨架8（ZIF-8）在温和升高的温度下均匀吸附气相二茂铁（FeCp）分子，然后碳化以制备Fe–N / C原子分散的Fe含量高，N含量高。ZIF-8纳米腔中吸附的FeCp分子的含量可以通过吸附温度和时间精确控制，将吸附的FeCp限制在ZIF-8的纳米腔中可以有效地防止碳化过程中Fe原子的聚集和/或形成Fe化合物。在最佳条件下制备的Fe–N / C具有5.86 wt％的高铁负载量和10.51 at％的丰富N含量。所制备的Fe–N / C在0.1 M KOH中显示出显着的ORR催化性能，具有半波电势（E 1/2）为0.85 V（与RHE相比），具有出色的长期耐久性（在经过1万次CV测试后，E 1/2的变化小于10 mV，并且在经过40 000 s的时间后电流密度衰减了11％学期的ORR测试）。这项工作为制造高含量原子分散的Fe和N共掺杂的碳催化剂提供了一种简单且可控的合成策略，这也可能为其他用于能量存储和转化应用的单原子金属掺杂的碳材料的设计和合成提供启示。
更新日期：2019-06-19
中文翻译：
在沸石咪唑酸酯骨架中笼固限定气相二茂铁，以合成高负载和原子分散的Fe–N共掺杂碳，以有效地进行氧还原反应†
Fe-N共掺杂碳（Fe-N / C）已成为氧还原反应（ORR）中最有前途的非贵金属电催化剂之一。然而，在保持Fe原子弥散的同时制备高Fe和N负载的Fe–N / C仍具有挑战性。在这里，我们提出了一种笼罩限制合成策略，该策略利用具有有序微孔结构的沸石咪唑啉骨架8（ZIF-8）在温和升高的温度下均匀吸附气相二茂铁（FeCp）分子，然后碳化以制备Fe–N / C原子分散的Fe含量高，N含量高。ZIF-8纳米腔中吸附的FeCp分子的含量可以通过吸附温度和时间精确控制，将吸附的FeCp限制在ZIF-8的纳米腔中可以有效地防止碳化过程中Fe原子的聚集和/或形成Fe化合物。在最佳条件下制备的Fe–N / C具有5.86 wt％的高铁负载量和10.51 at％的丰富N含量。所制备的Fe–N / C在0.1 M KOH中显示出显着的ORR催化性能，具有半波电势（E 1/2）为0.85 V（与RHE相比），具有出色的长期耐久性（在经过1万次CV测试后，E 1/2的变化小于10 mV，并且在经过40 000 s的时间后电流密度衰减了11％学期的ORR测试）。这项工作为制造高含量原子分散的Fe和N共掺杂的碳催化剂提供了一种简单且可控的合成策略，这也可能为其他用于能量存储和转化应用的单原子金属掺杂的碳材料的设计和合成提供启示。
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