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Simultaneously Realizing Rapid Electron Transfer and Mass Transport in Jellyfish-Like Mott-Schottky Nanoreactors for Oxygen Reduction Reaction

机译:同时实现水母样Mott-Schottky纳米反应器中用于氧还原反应的快速电子转移和质量传输

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摘要

Fundamental understanding of constructing elevated catalysts to realize fast electron transfer and rapid mass transport in oxygen reduction reaction (ORR) chemistry by interface regulation and structure design is important but still ambiguous. Herein, a novel jellyfish-like Mott-Schottky-type electrocatalyst is developed to realize fast electron transfer and decipher the structure-mass transport connection during ORR process. Both spectroscopy techniques and density functional theory calculation demonstrate electrons spontaneously transfer from Fe to N-doped graphited carbon at the heterojunction interface, thus accelerating electron transfer from electrode to reactant. Dynamic analysis indicates unique structure can significantly improve mass transport of oxygen-species due to two factors: one is electrolyte streaming effect caused by tentacle-like carbon nanotubes; the other is effective collision probability in the semi-closed cavity. Therefore, this Mott-Schottky-type catalyst delievers superior ORR performance with high onset potential, positive half wave potential, and large current density. It also exhibits low overpotential when serving as an air cathode in Zn-air batteries. This work deepens understanding of the two key factors-electron transfer and mass transport-on determining the kinetic reaction of ORR process and offers a new avenue in constructing efficient Mott-Schottky electrocatalysts.
机译:对通过界面调节和结构设计来构造高级催化剂以实现氧还原反应(ORR)化学中的快速电子转移和快速质量转移的基本理解很重要,但仍不明确。在此,开发了一种新型的水母状Mott-Schottky型电催化剂,以实现快速的电子转移并在ORR过程中破译结构-质量传输连接。光谱技术和密度泛函理论计算均表明电子在异质结界面处自发地从Fe转移到N掺杂的石墨碳,从而加速了电子从电极到反应物的转移。动力学分析表明,由于以下两个因素,独特的结构可以显着改善氧气种类的质量传输:一是触手状碳纳米管引起的电解质流动效应;二是触手状碳纳米管引起的电解质流动效应。另一个是在半封闭腔中的有效碰撞概率。因此,这种Mott-Schottky型催化剂除垢剂具有较高的ORR性能,具有高的起始电势,正半波电势和大电流密度。当用作Zn-空气电池中的空气阴极时,它还表现出低过电位。这项工作加深了对决定ORR过程动力学反应的两个关键因素-电子转移和传质的理解,并为构建有效的Mott-Schottky电催化剂提供了一条新途径。

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