Tailoring charge reconfiguration in dodecahedral Co2P@carbon nanohybrids by triple-doping engineering for promoted reversible oxygen catalysis,Journal of Materials Chemistry A

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Tailoring charge reconfiguration in dodecahedral Co2P@carbon nanohybrids by triple-doping engineering for promoted reversible oxygen catalysis
Journal of Materials Chemistry A ( IF 10.7 ) Pub Date : 2022-09-21 , DOI: 10.1039/d2ta04482j
Luhan Li ₁ , Lei Zhang ₁ , Zhicheng Nie ₁ , Wenyu Ma ₁ , Nianpeng Li _{1,

2} , Thomas Wågberg ₃ , Guangzhi Hu _{2,

3}

Affiliation

Simultaneously tuning the electronic structure of active sites and the microenvironment of the carbon matrix in metal phosphide/carbon nanohybrids is the most effective way to design and develop bi-functional electrocatalysts for electrochemically related energy storage devices. Inspired by this, a robust and advanced N/P co-doped carbon-based dodecahedron catalyst with confined Fe-doped Co₂P particles was successfully prepared through a multi-doping engineering strategy. Phytic acid molecules, which were used in the synthesis of the catalyst, not only contribute to the formation of the porous structure, but also act as a phosphorus source to form the corresponding metal phosphide and the P dopant in the carbon matrix. Thanks to the unique composition and structure-dependent merits, the microenvironment of the electrocatalyst was significantly modulated, thus promoting the advantageous local charge rearrangement and smooth mass/charge transfer processes during the oxygen-related electrocatalytic reactions. As a result, the resultant catalyst exhibited significantly enhanced reversible oxygen activity, as evidenced by an ultra-small potential gap of 0.655 V (half-wave potential of 0.895 V for the oxygen reduction reaction; η₁₀ of 320 mV for the oxygen evolution reaction), a remarkable specific capacity of 762 mA h g_Zn⁻¹, and high voltaic efficiency, exceeding most previous reports. This study provides a new synthetic approach for fabricating highly efficient bi-functional oxygen catalysts and can be handily extended to the synthesis of other heterogeneous electrocatalysts for sustainable energy storage.

中文翻译：

通过三重掺杂工程定制十二面体 Co2P@carbon 纳米杂化物中的电荷重构以促进可逆氧催化

同时调整金属磷化物/碳纳米杂化物中活性位点的电子结构和碳基质的微环境是设计和开发用于电化学相关储能装置的双功能电催化剂的最有效方法。受此启发，一种坚固且先进的 N/P 共掺杂碳基十二面体催化剂与受限的 Fe 掺杂 Co ₂通过多掺杂工程策略成功制备了 P 粒子。用于催化剂合成的植酸分子不仅有助于多孔结构的形成，而且还作为磷源在碳基体中形成相应的金属磷化物和P掺杂剂。由于独特的组成和结构相关的优点，电催化剂的微环境得到了显着调节，从而促进了与氧相关的电催化反应中有利的局部电荷重排和平稳的质量/电荷转移过程。结果，所得催化剂表现出显着增强的可逆氧活性，0.655 V 的超小电位间隙（氧还原反应的半波电位为 0.895 V；对于析氧反应，η _{10为 320 mV），762 mA hg}_Zn^-1的显着比容量和高电压效率，超过了大多数先前的报道。该研究为制造高效双功能氧催化剂提供了一种新的合成方法，并且可以方便地扩展到其他非均相电催化剂的合成，以实现可持续的储能。

更新日期：2022-09-21

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