In Situ Growth of α-MoC Nanoparticles on Bamboo-Structured Carbon Nanotubes as Proton-Feeding Centers of the Fe Site, Achieving Efficient Oxygen Reduction Reaction in Multiple Environments

IF 5.4 3区 材料科学 Q2 CHEMISTRY, PHYSICAL
Xianchang Cui, Fei He*, Yumeng Zhang, Yijun Gao, Shanshan Song, Linbo Cao, Xiao Zhang* and Piaoping Yang*, 
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Abstract

Oxygen reduction reaction (ORR) is a key component of the next generation energy storage system, and most of the current research on ORR catalysts focuses on promoting the rapid conversion process of oxygen-containing intermediates, but its reaction kinetics is also severely limited by the laborious and slow proto-coupled electron transfer (PCET) process. Therefore, it is imperative to develop a high-performance ORR catalyst that can simultaneously accelerate the rapid conversion of PCET and oxygen-containing intermediates. In this context, we purposely grew α-MoC nanoparticles (Fe-MoC@NCNT) in situ on Fe and N codoped bamboo-structured carbon nanotubes to realize the simultaneous promotion of rapid conversion of oxygen intermediates and PCET process. According to the theoretical study, the adjacent α-MoC nanoparticles accelerate the dissociation of water and can act as the proton supply center of Fe–N4 active site to promote the PCET process, while the oxygenated intermediates can achieve rapid transformation in the Fe–N4 active site in order to reduce the reaction barrier of the, ORR. Due to the synergistic effect of Fe–N4 active site and α-MoC, Fe-MoC@NCNT exhibits excellent ORR properties in both alkaline and neutral environments with half-wave potentials of 0.895 and 0.744 V, respectively. Using Fe-MoC@NCNT as the negative catalyst, the assembled aluminum-air battery has a high-power peak rate density of 285.7 mW cm–2. This work elucidates the method of constructing adjacent proton-supplying centers to optimize the ORR kinetics of single atomic sites and proposes ideas for the synthesis of low-cost and excellent performance ORR catalysts.

Abstract Image

α-MoC纳米颗粒在竹结构碳纳米管上原位生长,作为Fe位点的质子供给中心,在多种环境下实现高效的氧还原反应
氧还原反应(ORR)是下一代储能系统的关键组成部分,目前对ORR催化剂的研究大多集中在促进含氧中间体的快速转化过程,但其反应动力学也受到费力且缓慢的原耦合电子转移(PCET)过程的严重限制。因此,开发一种能同时加速PCET和含氧中间体快速转化的高性能ORR催化剂势在必行。在此背景下,我们有意在Fe和N共掺杂的竹结构碳纳米管上原位生长α-MoC纳米粒子(Fe-MoC@NCNT),以实现氧中间体快速转化和PCET工艺的同步推进。理论研究表明,邻近的α-MoC纳米颗粒加速了水的解离,可作为Fe-N4活性位点的质子供应中心,促进PCET过程,而氧化中间体可在Fe-N4活性位点实现快速转化,从而降低了反应屏障。由于Fe-N4活性位点与α-MoC的协同作用,Fe-MoC@NCNT在碱性和中性环境下均表现出优异的ORR性能,半波电位分别为0.895 V和0.744 V。使用Fe-MoC@NCNT作为负极催化剂,组装铝-空气电池的大功率峰值速率密度为285.7 mW cm-2。本工作阐明了构建相邻质子供应中心的方法来优化单原子位点的ORR动力学,并为合成低成本、高性能的ORR催化剂提出了思路。
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来源期刊
ACS Applied Energy Materials
ACS Applied Energy Materials Materials Science-Materials Chemistry
CiteScore
10.30
自引率
6.20%
发文量
1368
期刊介绍: ACS Applied Energy Materials is an interdisciplinary journal publishing original research covering all aspects of materials, engineering, chemistry, physics and biology relevant to energy conversion and storage. The journal is devoted to reports of new and original experimental and theoretical research of an applied nature that integrate knowledge in the areas of materials, engineering, physics, bioscience, and chemistry into important energy applications.
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