Heteroatom dopant strategy triggered high-potential plateau to non-graphitized carbon with highly disordered microstructure for high-performance sodium ion storage

IF 14.9 1区 化学 Q1 Energy
Peilin Zhang , Chen Huang , Mingzhen Xiu , Siyu Zhu , Weiwei Wang , Bo Zhu , Likang Qin , Yizhong Huang , Luyang Chen
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引用次数: 2

Abstract

Non-graphitized carbon (NGC) has been extensively utilized as carbonaceous anode in sodium-ion batteries (SIBs). However, more optimization to achieve competitive capacity and stability is still challenging for SIBs. In the study, the dopant strategy is utilized to construct nitrogen/sulfur-doped non-graphitized carbon (N-NGC or S-NGC) shell decorated on three-dimensional graphene foam (GF) as a self-support electrode. The highly disordered microstructures of heteroatom doped carbons are produced by applying a low-temperature pyrolysis treatment to precursors containing nitrogen and sulfur. The DFT calculations of Na-ion adsorption energies at diverse heteroatom sites show marginal-S, pyrrolic N and pyridinic N with more intensive Na-ion adsorption ability than middle-S, CO and pristine carbon. The N-NGC with dominant small graphitic regions delivers adsorption ability to Na-ion, while the S-NGC with significant single carbon lattice stripes demonstrates redox reaction with Na-ion. Evidently, in comparison with only adsorption-driven slope regions at high potential for N-NGC, the redox reaction-generated potential-plateau enables non-graphitized S-NGC superior discharge/charge capacity and cycle-stability in the slope region. This work could provide deep insight into the rational design of non-graphitized carbon with rich microstructure and composition.

Abstract Image

杂原子掺杂策略触发了结构高度无序的非石墨化碳的高电位平台,实现了高性能的钠离子存储
非石墨化碳(NGC)已被广泛用作钠离子电池(SIBs)的碳质阳极。然而,对系统重要性银行来说,实现竞争能力和稳定性的更多优化仍然具有挑战性。在本研究中,利用掺杂策略构建了修饰在三维石墨烯泡沫(GF)上的氮/硫掺杂非石墨化碳(N-NGC或S-NGC)壳作为自支撑电极。通过对含有氮和硫的前体进行低温热解处理,产生了杂原子掺杂碳的高度无序微观结构。对不同杂原子位置的钠离子吸附能的DFT计算表明,边缘-S、吡咯N和吡啶N比中间-S、CO和原始碳具有更强的钠离子吸收能力。具有主要小石墨区的N-NGC对钠离子具有吸附能力,而具有显著单碳晶格条纹的S-NGC表现出与钠离子的氧化还原反应。显然,与N-NGC在高电势下仅吸附驱动的斜坡区域相比,氧化还原反应产生的电势平台使非石墨化的S-NGC在斜坡区域具有优异的放电/充电容量和循环稳定性。这项工作可以为具有丰富微观结构和成分的非石墨化碳的合理设计提供深入的见解。
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来源期刊
Journal of Energy Chemistry
Journal of Energy Chemistry CHEMISTRY, APPLIED-CHEMISTRY, PHYSICAL
CiteScore
19.10
自引率
8.40%
发文量
3631
审稿时长
15 days
期刊介绍: The Journal of Energy Chemistry, the official publication of Science Press and the Dalian Institute of Chemical Physics, Chinese Academy of Sciences, serves as a platform for reporting creative research and innovative applications in energy chemistry. It mainly reports on creative researches and innovative applications of chemical conversions of fossil energy, carbon dioxide, electrochemical energy and hydrogen energy, as well as the conversions of biomass and solar energy related with chemical issues to promote academic exchanges in the field of energy chemistry and to accelerate the exploration, research and development of energy science and technologies. This journal focuses on original research papers covering various topics within energy chemistry worldwide, including: Optimized utilization of fossil energy Hydrogen energy Conversion and storage of electrochemical energy Capture, storage, and chemical conversion of carbon dioxide Materials and nanotechnologies for energy conversion and storage Chemistry in biomass conversion Chemistry in the utilization of solar energy
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