Synthesis of Lattice‐Contracted Cobalt Disulfide as an Outstanding Oxygen Reduction Reaction Catalyst via Self‐assembly Arrangement,ChemSusChem

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Synthesis of Lattice‐Contracted Cobalt Disulfide as an Outstanding Oxygen Reduction Reaction Catalyst via Self‐assembly Arrangement
ChemSusChem ( IF 7.5 ) Pub Date : 2021-01-06 , DOI: 10.1002/cssc.202002960
Hao Zhang ₁ , Zhiqiang Wang ₂ , Chenglong Ma ₁ , Zhenhua Zhou ₁ , Limei Cao ₁ , Xueqing Gong ₂ , Chunxiao Dong ₃ , Ji Yang ₄

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Identifying high‐performance non‐precious metal‐based catalysts at the cathode is a major challenge for future practical applications. Herein, a soft‐template route through a self‐assembly arrangement of sulfur sources was successfully developed, facilitating the anion exchange. In addition, compared with pristine cobalt disulfide synthesized without templates, the cobalt disulfide prepared using the new method presented a lattice shrinking phenomenon due to the hindrance of cobalt hydroxide crystal cell. Based on X‐ray absorption spectroscopy (XAS) and density functional theory (DFT) calculation, increased occupancy of e_g orbitals was verified for the cobalt disulfide after shrinkage, which was the main factor for enhancing the intrinsic activity of the catalyst. Besides the microscopic morphologic structure, elementary composition, and the valence state of the elements, the possible growth process of the cobalt disulfide was also discussed in detail. As catalyst for the oxygen reduction reaction, CoS₂ showed a similar half‐wave potential (0.81 vs. 0.84 V for Pt/C) and higher diffusion‐limiting current density (reaching 5.33 vs. 5.19 mA cm⁻² for Pt/C) than a commercial Pt/C catalyst. Hence, our results provide a rational design direction for this type of catalysts.

中文翻译：

自组装法合成格子缩合二硫化钴作为杰出的氧还原反应催化剂

在阴极处识别高性能的非贵金属基催化剂是未来实际应用的主要挑战。在此，成功开发了一种通过自组装硫源的软模板路线，从而促进了阴离子交换。此外，与没有模板合成的原始二硫化钴相比，使用新方法制备的二硫化钴由于氢氧化钴晶体晶胞的阻碍而呈现出晶格收缩现象。基于X射线吸收光谱（XAS）和密度泛函理论（DFT）计算，增加电子占用_克收缩后，对二硫化钴的轨道进行了验证，这是增强催化剂固有活性的主要因素。除了微观形态结构，元素组成和元素的价态外，还详细讨论了二硫化钴可能的生长过程。作为氧还原反应的催化剂，CoS ₂表现出相似的半波电势（Pt / C为0.81 vs. 0.84 V）和更高的扩散限制电流密度（Pt / C达到5.33 vs. 5.19 mA cm ^-2）比市售Pt / C催化剂要多。因此，我们的结果为这类催化剂提供了合理的设计方向。

更新日期：2021-03-07

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