Building Atomic Scale and Dense Fe─N4 Edge Sites of Highly Efficient Fe─N─C Oxygen Reduction Catalysts Using a Sacrificial Bimetallic Pyrolysis Strategy,Small

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Building Atomic Scale and Dense Fe─N4 Edge Sites of Highly Efficient Fe─N─C Oxygen Reduction Catalysts Using a Sacrificial Bimetallic Pyrolysis Strategy
Small ( IF 13.0 ) Pub Date : 2023-08-03 , DOI: 10.1002/smll.202304750
Zhaoyan Luo ₁ , Tingyi Zhou ₁ , Yi Guan ₂ , Lei Zhang ₁ , Qianling Zhang ₁ , Chuanxin He ₁ , Xueliang Sun ₂ , Xiangzhong Ren ₁

Affiliation

Replacing high-cost and scarce platinum (Pt) with transition metal and nitrogen co-doped carbon (M/N/C, M = Fe, Co, Mn, and so on) catalysts for the oxygen reduction reaction (ORR) in proton exchange membrane fuel cells has largely been impeded by the unsatisfactory ORR activity of M/N/C due to the low site utilization and inferior intrinsic activity of the M─N₄ active center. Here, these limits are overcome by using a sacrificial bimetallic pyrolysis strategy to synthesize Fe─N─C catalyst by implanting the Cd ions in the backbone of ZIF-8, leading to exposure of inaccessible FeN₄ edge sites (that is, increasing active site density (SD)) and high fast mass transport at the catalyst layer of cathode. As a result, the final obtained Fe(Cd)─N─C catalyst has an active site density of 33.01 µmol g⁻¹ (with 33.01% site utilization) over 5.8 times higher than that of Fe─N─C catalyst. Specially, the optimal catalyst delivers a high ORR performance with a half-wave potential of 0.837 (vs RHE) in a 0.1 m HClO₄ electrolyte, which surpasses most of Fe-based catalysts.

中文翻译：

使用牺牲双金属热解策略构建高效 Fe─N─C 氧还原催化剂的原子尺度和致密 Fe─N4 边缘位点

用过渡金属和氮共掺杂碳（M/N/C，M=Fe、Co、Mn等）催化剂代替高成本和稀缺的铂（Pt）用于质子交换中的氧还原反应（ORR）由于M─N ₄活性中心的位点利用率低和固有活性差，M/N/C的ORR活性不理想，极大地阻碍了膜燃料电池的发展。在这里，通过使用牺牲双金属热解策略来合成 Fe─N─C 催化剂，通过将 Cd 离子植入 ZIF-8 的主链中，从而克服了这些限制，导致难以接近的 FeN ₄边缘位点的暴露（即增加了活性位点）密度（SD））和阴极催化剂层的高快速传质。结果，最终获得的Fe(Cd)─N─C催化剂的活性中心密度为33.01 µmol g ^-1 (中心利用率为33.01%)，是Fe─N─C催化剂的5.8倍以上。特别是，优化的催化剂在0.1 m HClO ₄电解质中提供了高ORR性能，半波电位为0.837（vs RHE），超过了大多数铁基催化剂。

更新日期：2023-08-03

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