Fe-Ni/Mo2C@nitrogen-doped碳纳米盒中镍诱导的反向电荷转移促进可逆氧电催化

IF 14 1区 化学 Q1 CHEMISTRY, APPLIED
Zhicheng Nie , Lei Zhang , Qiliang Zhu , Zhifan Ke , Yingtang Zhou , Thomas Wågberg , Guangzhi Hu
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引用次数: 2

摘要

金属和载体之间的相互作用在氧催化中是至关重要的,因为它控制着这两个实体之间的电荷转移,影响载体金属的电子结构,影响反应中间体的吸附能,并最终影响催化性能。在本研究中,我们在金属/碳纳米杂化体系中发现了一种独特的电荷转移反转现象。具体来说,电子从金属基转移到n掺杂的碳上,而碳载体在引入镍后相互向金属畴提供电子。这使得Ni-Fe/Mo2C@nitrogen-doped碳催化剂具有优异的电催化性能,在碱性条件下,对氧还原反应(ORR)具有0.91 V的半波电位,对氧析反应(OER)在10 mA cm−2下具有290 mV的低过电位。此外,Fe-Ni/Mo2C@carbon异质结催化剂在锌空气电池中表现出高比容量(794 mA h gZn−1)和优异的循环稳定性(200 h)。理论计算表明,Mo2C有效地抑制了Fe向载体的电荷转移,而Ni的二次掺杂导致电荷转移逆转,导致Fe-Ni合金区电子积累。这种局部电子结构调制显著降低了氧催化过程中的能垒,提高了ORR和OER的催化效率。因此,我们的研究结果强调了操纵金属和载体之间电荷转移逆转的潜力,作为开发高活性和耐用双功能氧电极的有希望的策略。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Reversed charge transfer induced by nickel in Fe-Ni/Mo2C@nitrogen-doped carbon nanobox for promoted reversible oxygen electrocatalysis

Reversed charge transfer induced by nickel in Fe-Ni/Mo2C@nitrogen-doped carbon nanobox for promoted reversible oxygen electrocatalysis

The interaction between metal and support is critical in oxygen catalysis as it governs the charge transfer between these two entities, influences the electronic structures of the supported metal, affects the adsorption energies of reaction intermediates, and ultimately impacts the catalytic performance. In this study, we discovered a unique charge transfer reversal phenomenon in a metal/carbon nanohybrid system. Specifically, electrons were transferred from the metal-based species to N-doped carbon, while the carbon support reciprocally donated electrons to the metal domain upon the introduction of nickel. This led to the exceptional electrocatalytic performances of the resulting Ni-Fe/Mo2C@nitrogen-doped carbon catalyst, with a half-wave potential of 0.91 V towards oxygen reduction reaction (ORR) and a low overpotential of 290 mV at 10 mA cm−2 towards oxygen evolution reaction (OER) under alkaline conditions. Additionally, the Fe-Ni/Mo2C@carbon heterojunction catalyst demonstrated high specific capacity (794 mA h gZn−1) and excellent cycling stability (200 h) in a Zn-air battery. Theoretical calculations revealed that Mo2C effectively inhibited charge transfer from Fe to the support, while secondary doping of Ni induced a charge transfer reversal, resulting in electron accumulation in the Fe-Ni alloy region. This local electronic structure modulation significantly reduced energy barriers in the oxygen catalysis process, enhancing the catalytic efficiency of both ORR and OER. Consequently, our findings underscore the potential of manipulating charge transfer reversal between the metal and support as a promising strategy for developing highly-active and durable bi-functional oxygen electrodes.

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CiteScore
23.60
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