Staging Na/K-ion de-/intercalation of graphite retrieved from spent Li-ion batteries: <i>in operando</i> X-ray diffraction studies and an advanced anode material for Na/K-ion batteries

Liang, Hao‐Jie; Hou, Bao‐Hua; Li, Wenhao; Ning, Qiu‐Li; Yang, Xu; Gu, Zhen‐Yi; Nie, Xue‐Jiao; Guang, Wang; Wu, Xing‐Long

doi:10.1039/c9ee02759a

Cited by 199 publications

(112 citation statements)

References 48 publications

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“…The intercalation and de‐intercalation of [Na‐G 4 ] + is a diffusion‐controlled process, and the apparent diffusion coefficient was calculated by the Randles–Sevcik equation and was found to be 1.733×10 −7 and 1.156×10 −7 cm 2 s −1 based on cathodic and anodic peak current, respectively (Figure 3c). However, the values are higher than the reported value of 1–6×10 −10 cm 2 s −1 , which may be due to lower concentration of electrolyte [30] . The contributions of diffusion‐limited intercalation and pseudocapacitive intercalation in sodium storage were qualitatively calculated by using the power‐law equation ( i = av b ), which gives the relationship between measured current i [A] and scan rate v [mV s −1 ] from CV profiles.…”

Section: Resultsmentioning

confidence: 99%

Highly Reversible Na‐Intercalation into Graphite Recovered from Spent Li–Ion Batteries for High‐Energy Na‐Ion Capacitor

et al. 2020

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High‐performance Na‐ion capacitor (NIC) was constructed with graphite recovered from spent Li‐ion batteries (LIBs) as battery‐type negative electrode and high‐surface‐area activated carbon as a supercapacitor component. Unlike Li‐insertion into graphite, Na‐insertion into graphite is extremely limited; hence, a “solvent‐co‐intercalation” mechanism was proposed for high reversibility using ether family solvents. First, the Na‐insertion properties were assessed in the half‐cell assembly with 0.5 m NaPF6 in tetraethylene glycol dimethyl ether as an electrolyte solution and compared with the commercial graphite. The NIC comprised pre‐sodiated graphite as a negative electrode and commercial activated carbon as a cathode. This fascinating NIC configuration displayed the maximum energy density of 59.93 Wh kg−1 with exceptional cyclability of 5000 cycles at ambient temperature with approximately 98 % retention. Interestingly, the electrode aging process in the presence of electrolyte resulted in approximately 19 % higher energy density than the routine electrode heat treatment. Further, the electrochemical activity of the NIC at various temperatures was studied, and it was found that the graphite recovered from spent LIBs could be effectively reused towards the construction of high‐performance charge storage devices with exceptional performance.

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Section: Resultsmentioning

confidence: 99%

Highly Reversible Na‐Intercalation into Graphite Recovered from Spent Li–Ion Batteries for High‐Energy Na‐Ion Capacitor

et al. 2020

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“…Liang et al [ 29 ] performed the calcination at different temperatures to evaluate the spent LIBs graphite as an anode for Na and K‐ion batteries. The optimized electrodes exhibited a good specific capacity of 162 and 320 mAh g –1 , respectively, for Na and K‐ion battery applications (Figure 3i–n).…”

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

195

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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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“…[24] In the subsequent charging process,t he peak change is reversible, and the (002) peak of the natural graphite appeared at the end of charge (2.0 V). As shown in Figure 2b,c, the color intensity change is highly reversible,i ndicating the superior cycling stability of natural graphite electrode.I na ddition, the new peaks that appeared during charge/discharge process can be indexed as (00l)a nd (00l + 1) according to Braggsl aw following the equations: [37][38][39]…”

Section: Angewandte Chemiementioning

confidence: 99%

“…Thediffusion coefficient of the K + -DEGDME complex in an atural graphite electrode (measured by GITT) is about 10 À9 cm 2 s À1 (Figure 5c)d uring charge/discharge processes, implying fast K + -solvent complex diffusion kinetics.T he diffusion coefficient of the K + -DEGDME complex in an atural graphite electrode is higher than that of the K + ( % 10 À11 cm 2 s À1 ). [39] Theh igh K + -DEGDME complex diffusion coefficient could be attributed to the DEGDME molecules that surround the Ki ons being nearly flat, which completely solvate the Ki ons in the interlayer space of graphite,r esulting in weak interaction between K + and the graphite layers,similar to that in Na + -solvent co-intercalation processes. [50] Theh igh K + -solvent complex diffusion coefficient is responsible for the superior rate performance of the natural graphite electrode in DEGDME-based electrolyte.…”

Section: Angewandte Chemiementioning

confidence: 99%

Understanding High‐Rate K⁺‐Solvent Co‐Intercalation in Natural Graphite for Potassium‐Ion Batteries

Liu

et al. 2020

Angewandte Chemie

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Graphite shows great potential as an anode material for rechargeable metal‐ion batteries because of its high abundance and low cost. However, the electrochemical performance of graphite anode materials for rechargeable potassium‐ion batteries needs to be further improved. Reported herein is a natural graphite with superior rate performance and cycling stability obtained through a unique K+‐solvent co‐intercalation mechanism in a 1 m KCF3SO3 diethylene glycol dimethyl ether electrolyte. The co‐intercalation mechanism was demonstrated by ex situ Fourier transform infrared spectroscopy and in situ X‐ray diffraction. Moreover, the structure of the [K‐solvent]+ complexes intercalated with the graphite and the conditions for reversible K+‐solvent co‐intercalation into graphite are proposed based on the experimental results and first‐principles calculations. This work provides important insights into the design of natural graphite for high‐performance rechargeable potassium‐ion batteries.

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Staging Na/K-ion de-/intercalation of graphite retrieved from spent Li-ion batteries: in operando X-ray diffraction studies and an advanced anode material for Na/K-ion batteries

Abstract: The exhausted graphite from spent Li-ion batteries is recycled and reused as a favorable anode for Na/K-ion batteries, and the insights into structural de-/intercalation model are realized.

Cited by 199 publications

References 48 publications

Highly Reversible Na‐Intercalation into Graphite Recovered from Spent Li–Ion Batteries for High‐Energy Na‐Ion Capacitor

Highly Reversible Na‐Intercalation into Graphite Recovered from Spent Li–Ion Batteries for High‐Energy Na‐Ion Capacitor

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

Understanding High‐Rate K⁺‐Solvent Co‐Intercalation in Natural Graphite for Potassium‐Ion Batteries

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Staging Na/K-ion de-/intercalation of graphite retrieved from spent Li-ion batteries: in operando X-ray diffraction studies and an advanced anode material for Na/K-ion batteries

Abstract: The exhausted graphite from spent Li-ion batteries is recycled and reused as a favorable anode for Na/K-ion batteries, and the insights into structural de-/intercalation model are realized.

Cited by 199 publications

References 48 publications

Highly Reversible Na‐Intercalation into Graphite Recovered from Spent Li–Ion Batteries for High‐Energy Na‐Ion Capacitor

Highly Reversible Na‐Intercalation into Graphite Recovered from Spent Li–Ion Batteries for High‐Energy Na‐Ion Capacitor

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

Understanding High‐Rate K+‐Solvent Co‐Intercalation in Natural Graphite for Potassium‐Ion Batteries

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Understanding High‐Rate K⁺‐Solvent Co‐Intercalation in Natural Graphite for Potassium‐Ion Batteries