Exploring Sodium‐Ion Storage Mechanism in Hard Carbons with Different Microstructure Prepared by Ball‐Milling Method

Huang, Lu; Ai, Fang-Xing; Jia, Yanlong; Tang, Chunyan; Zhang, Xinhe; Huang, Yunhui; Yang, Hanxi; Cao, Yuliang

doi:10.1002/smll.201802694

Cited by 155 publications

(86 citation statements)

References 54 publications

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“…Although hard carbon has been demonstrated to be an efficient anode for SIB and KIB, the storage mechanism has been difficult to understand because of the complex arrangements of short‐ranged graphene layers inside hard carbon. As a result, the storage mechanism of sodium in hard carbon is still under debate . For KIBs, we used the defect‐rich graphitic carbons for a mechanistic study.…”

Section: Resultsmentioning

confidence: 99%

Graphitic Nanocarbon with Engineered Defects for High‐Performance Potassium‐Ion Battery Anodes

Zhang

Ming

Zhao

et al. 2019

Adv Funct Materials

236

182

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The application of graphite anodes in potassium-ion batteries (KIB) is limited by the large variation in lattice volume and the low diffusion coefficient of potassium ions during (de)potassiation. This study demonstrates nitrogendoped, defect-rich graphitic nanocarbons (GNCs) as high-performance KIB anodes. The GNCs with controllable defect densities are synthesized by annealing an ethylenediaminetetraacetic acid nickel coordination compound. The GNCs show better performance than the previously reported thin-walled graphitic carbonaceous materials such as carbon nanocages and nanotubes. In particular, the GNC prepared at 600 °C shows a stabilized capacity of 280 mAh g −1 at 50 mA g −1 , robust rate capability, and long cycling life due to its high-nitrogen-doping, short-range-ordered, defect-rich graphitic structure. A high capacity of 189 mAh g −1 with a long cycle life over 200 cycles is demonstrated at a current density of 200 mA g −1 . Further, it is confirmed that the potassium ion storage mechanism of GNCs is different from that of graphite using multiple characterization methods. Specifically, the GNCs with numerous defects provide more active sites for the potassiation process, which results in a final discharge product with short-range order. This study opens a new pathway for designing graphitic carbonaceous materials for KIB anodes.

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Section: Resultsmentioning

confidence: 99%

Graphitic Nanocarbon with Engineered Defects for High‐Performance Potassium‐Ion Battery Anodes

Zhang

Ming

Zhao

et al. 2019

Adv Funct Materials

236

182

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“…However, the assignment of the aforementioned three storage mechanisms to the charge–discharge voltage profile is still controversial. For example, Liu et al and Cao et al attributed the plateau region to sodium intercalation into the graphene–graphene interlayers, whereas Tarascon and co‐workers observed a constant interlayer distance upon sodiation at the plateau, suggesting no intercalation in the graphitic domains . Concerning the analysis of sodium insertion into nanopores, most research groups have tried to use the pore size distribution, as measured by gas absorption techniques, of the pristine hard carbon.…”

Section: Introductionmentioning

confidence: 99%

Mechanism of Sodium Storage in Hard Carbon: An X‐Ray Scattering Analysis

Morikawa

Nishimura

Hashimoto

et al. 2019

Advanced Energy Materials

166

197

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Hard carbon is a standard anode material for Na‐ion batteries. However, its low crystallinity and diverse microstructures make obtaining a full understanding of the sodium storage mechanism challenging. Here, the results of a systematic ex situ small and wide angle X‐ray scattering study of a series of nanostructured hard carbons, which reveal clear evidence of sodium storage in the graphene–graphene interlayers and nanopores, are presented. Particularly, an emergence of a broad peak around q ≈ 2.0–2.1 Å−1 in the low voltage region is suggested to be an indicator that sodium is densely confined in the nanopores. Thus, classical X‐ray scattering techniques are demonstrated to be effective in elucidating the overall reaction scheme of Na insertion into hard carbon.

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“…This type of damaged structure certainly can be employed as an electrode for the reversible Na‐storage process with carbonate‐based electrolytes owing more number of defects in their layered structure. [ 46 ] In the case of more mechanical damage in the graphite structure, it can be easily milled and renewed as a hard carbon that can intercalate both Li and Na‐ions reversibly. [ 47,48 ] Undoubtedly, the hard carbon is one of the promising anodes for Na‐ion batteries and high power anode for Li‐ion capacitors; thus, the transformation of damaged graphite to hard carbon paving a route to prepare this kind of commercialized carbonaceous materials from the spent LIBs.…”

Section: Research Progress Of the Graphite Reuse In Lab‐scale: Energymentioning

confidence: 99%

An Urgent Call to Spent LIB Recycling: Whys and Wherefores for Graphite Recovery

Natarajan

Aravindan

2020

Advanced Energy Materials

201

120

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diffuse between their layers, though only at prismatic surfaces as well as it is also possible via defect sites for the basal planes. The term "intercalation in graphite" refers to the incorporation of atomic or molecular layers of a guest species between the ordered graphite layers, and this process would be reversible and "topotactic" that endorses the different interlayer distance without changing the carbon atomic arrangement within the layer. The mechanism involved in the intercalation process is generally identified as "staging" where the lithium prefers to reside in the distant graphene layers first rather than picking the neighbor graphene layers as shown in Figure 1; however, Li-ions pick the gap of neighboring graphene layers to form a Li-C 6-Li-C 6 chain along the c-direction if the graphite is intercalated fully with a spacing of 0.430 nm. [3,4,6-8] As well, it is also proven that both hexagonal and rhombohedral graphitic phases could able to intercalate the lithium reversibly almost in the same storage capacities. Commercial graphite possesses a larger number of rhombohedral units, and that kind of graphene planes as a host will be more favorable to intercalate lithium. Many efforts have been made to clarify the intercalation mechanism of lithium into the graphite from various perspectives. The occurrence of solid electrolyte interphase (SEI) formation is necessary for safe operation (since LiC 6 is known to be the strong reducing agent) of the cell regardless of any electrode/electrolyte contact and plays a decisive role in the capacity of the material. [9] It is well-known that the excess charge consumption for the graphite-based electrodes during the first cycle surpasses the theoretical capacity of 372 mAh g-1 as a result of this passive layer formation, i.e., SEI, also attributed to the corrosion-like reactions of Li x C 6. The intercalated compounds are unstable similar to metallic lithium in the electrolytes which surface is protected by this formation of SEI layer that pays the excess charge consumption in the first cycle of the intercalation/deintercalation process. Generally, non-graphitic carbons which have not c-direction in the crystallographic order can be categorized as high (x > 1 in Li x C 6) and low (x = 0.5-0.8 in Li x C 6) specific charge carbons based on their reversible lithium storage properties. From the category of low-specific charge carbons, coke and turbostratic kind of carbons gain much attention for the Li-intercalation owing to their structural properties, which could overwhelm the development of Li x (solv) y C 6. Also, the coke-containing electrode unveiled the reversible Li-intercalation at ≈1.2 V versus Li during the first cycle, distinguishes from the insertion potential of graphite because of the disordered structure. High specific Spent lithium-ion batteries (LIBs) are a key source for securing tons of raw materials that are valuable materials for LIB applications. However, the massive emerging volume of spent LIBs urgently needs a new management strategy to recy...

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Exploring Sodium‐Ion Storage Mechanism in Hard Carbons with Different Microstructure Prepared by Ball‐Milling Method

Cited by 155 publications

References 54 publications

Graphitic Nanocarbon with Engineered Defects for High‐Performance Potassium‐Ion Battery Anodes

Graphitic Nanocarbon with Engineered Defects for High‐Performance Potassium‐Ion Battery Anodes

Mechanism of Sodium Storage in Hard Carbon: An X‐Ray Scattering Analysis

An Urgent Call to Spent LIB Recycling: Whys and Wherefores for Graphite Recovery

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