Rational design of vitamin C/defective carbon van der Waals heterostructure for enhanced activity, durability and storage stability toward oxygen reduction reaction

IF 14 1区 化学 Q1 CHEMISTRY, APPLIED 能源化学 Pub Date : 2023-09-22 DOI:10.1016/j.jechem.2023.09.011
Ruiqi Cheng , Kaiqi Li , Huanxin Li , Tianshuo Zhao , Yibo Wang , Qingyue Xue , Jiao Zhang , Chaopeng Fu
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Abstract

Metal-free defective carbon materials with abundant active sites have been widely studied as low-cost and efficient oxygen reduction reaction (ORR) electrocatalysts in metal-air batteries. However, the active sites in defective carbon are easily subjected to serious oxidation or hydroxylation during ORR or storage, leading to rapid degradation of activity. Herein, we design a van der Waals heterostructure comprised of vitamin C (VC) and defective carbon (DC) to not only boost the activity but also enhance the durability and storage stability of the DC-VC electrocatalyst. The formation of VC van der Waals between DC and VC is demonstrated to be an effective strategy to protect the defect active sites from oxidation and hydroxylation degradation, thus significantly enhancing the electrochemical durability and storage anti-aging performance. Moreover, the DC-VC van der Waals can reduce the reaction energy barrier to facilitate the ORR. These findings are also confirmed by operando Fourier transform infrared spectroscopy and density functional theory calculations. It is necessary to mention that the preparation of this DC-VC electrocatalyst can be scaled up, and the ORR performance of the largely produced electrocatalyst is demonstrated to be very consistent. Furthermore, the DC-VC-based aluminum-air batteries display very competitive power density with good performance maintenance.

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维生素C/缺陷碳范德华异质结构的合理设计,提高氧还原反应的活性、耐久性和储存稳定性
具有丰富活性位点的无金属缺陷碳材料作为金属-空气电池中低成本、高效的氧还原反应(ORR)电催化剂已被广泛研究。然而,缺陷碳中的活性位点在ORR或储存过程中很容易发生严重的氧化或羟基化,导致活性的快速降解。在此,我们设计了一种由维生素C(VC)和缺陷碳(DC)组成的范德华异质结构,不仅提高了DC-VC电催化剂的活性,还提高了其耐久性和储存稳定性。在DC和VC之间形成VC范德华被证明是保护缺陷活性位点免受氧化和羟基化降解的有效策略,从而显著提高电化学耐久性和储存抗老化性能。此外,DC-VC范德华可以降低反应能垒以促进ORR。这些发现也得到了操作傅立叶变换红外光谱和密度泛函理论计算的证实。有必要提及的是,这种DC-VC电催化剂的制备可以按比例进行,并且大量生产的电催化剂的ORR性能被证明是非常一致的。此外,基于直流VC的铝空气电池显示出非常有竞争力的功率密度和良好的性能维护。
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CiteScore
23.60
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0.00%
发文量
2875
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