通过 N、S 掺杂碳壳封装 Fe5C2 促进氧还原反应：利用横向和轴向协同作用,ACS Sustainable Chemistry & Engineering

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通过 N、S 掺杂碳壳封装 Fe5C2 促进氧还原反应：利用横向和轴向协同作用
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2024-03-07 , DOI: 10.1021/acssuschemeng.4c00286
Lang Xiao ₁ , Wanqing Yu ₁ , Jing Liu ₁ , Shankui Luan ₁ , Shengchang Li ₁ , Xuejing Cui ₁ , Luhua Jiang ₁

Affiliation

在此，通过自组装超分子结构和受控热解开发了一种新型氧还原反应（ORR）电催化剂，该催化剂由封装Fe ₅ C ₂纳米颗粒的N,S共掺杂碳壳组成。所得的Fe ₅ C ₂ @SNC催化剂表现出优异的电催化性能，具有0.86 V的高半波电位（E _1/2），与商业Pt/C相当。独特的核壳结构有助于实现出色的稳定性，在连续计时电流分析法测试 20 小时后，电流维持率为 89%。在锌空气电池应用中，该催化剂实现了 222 mW cm ^–2的峰值功率密度，超过了相应的 Pt/C 催化剂。结合实验和密度泛函理论计算，Fe ₅ C _{2 @SNC中轴向Fe}₅ C ₂纳米粒子和横向SO _x功能化Fe-N _x碳平面的协同效应已被全面揭示。硫的吸电子性质导致电荷重新分布，特别是在靠近 SO _x基团的 N 位点上。此外，轴向Fe ₅ C _{2纳米粒子精确调节了Fe}₅ C ₂ @SNC催化剂的d带中心，优化了氧中间体的吸附并增强了ORR活性。这项工作强调了通过可控核壳结构对协同催化的理解和利用，为开发用于能量转换和存储应用的高效稳定的电催化剂提供了有效的方法。

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Boosting Oxygen Reduction Reaction via N, S-Doped Carbon Shell-Encapsulated Fe5C2: Leveraging Lateral and Axial Synergy

Herein, a novel oxygen reduction reaction (ORR) electrocatalyst, consisting of an N,S-codoped carbon shell encapsulating Fe₅C₂ nanoparticles, is developed through self-assembled supramolecular structures and controlled pyrolysis. The resulting Fe₅C₂@SNC catalyst exhibits exceptional electrocatalytic performance, with a high half-wave potential (E_1/2) of 0.86 V, comparable to that of commercial Pt/C. The distinctive core–shell structure contributes to excellent stability, demonstrating an 89% current maintenance after 20 h of continuous chronoamperometry testing. In Zn-air battery applications, the catalyst achieved a peak power density of 222 mW cm^–2, surpassing that of its Pt/C counterpart. Combining the experiments and density functional theory calculations, the synergistic effects of axial Fe₅C₂ nanoparticles and laterally SO_x-functionalized Fe–N_x carbon planes within Fe₅C₂@SNC have been comprehensively unveiled. The electron-withdrawing nature of sulfur leads to charge redistribution, particularly on N sites proximal to the SO_x group. Additionally, the axial Fe₅C₂ nanoparticles have precisely modulated the d-band center of the Fe₅C₂@SNC catalyst, optimizing oxygen intermediate adsorption and enhancing the ORR activity. This work highlights the understanding and harnessing of synergistic catalysis via a controllable core–shell structure, providing an effective way for developing highly efficient and stable electrocatalysts for energy conversion and storage applications.

更新日期：2024-03-07

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