Aqueous Li-ion battery enabled by halogen conversion–intercalation chemistry in graphite

Yang, Changping; Chen, Ji; Ji, Xiao; Pollard, Travis P.; Lu, Xiaofeng; Sun, Chengjun; Hou, Singyuk; Liu, Qi; Liu, Cunming; Qing, Tingting; Wang, Yingqi; Borodin, Oleg; Ren, Yang; Xu, Kang; Wang, Chunsheng

doi:10.1038/s41586-019-1175-6

Cited by 630 publications

(514 citation statements)

References 53 publications

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“…Nonmetallic cations, e.g., proton (H + ), hydronium (H 3 O + ), and ammonium (NH 4 + ) ions, have rarely been regarded as charge carriers in aqueous battery chemistry for research and commercial applications, [ 1–3 ] where the mainstream attention located at the metal cations, such as Li + , Na + , Zn 2+ , and Al 3+ ions. [ 4–8 ] Most recently, Ji and co‐workers have pioneeringly reported several typical aqueous batteries utilizing H + and NH 4 + as charging carriers with outstanding electrochemical performance, especially for the ultrafast kinetics with high power density. [ 1,9 ] It could be ascribed to (1) nondiffusion‐controlled topochemistry between nonmetallic charging carriers and electrode framework during insertion/extraction process, resulting in pseudocapacitive‐dominated behavior; [ 1,9 ] (2) the lower molar mass and smaller hydrated ionic size of such non‐metallic charging carriers, which could result in fast diffusion in aqueous electrolytes.…”

Section: Figurementioning

confidence: 99%

Initiating Hexagonal MoO₃ for Superb‐Stable and Fast NH₄⁺ Storage Based on Hydrogen Bond Chemistry

et al. 2020

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Nonmetallic ammonium (NH4+) ions are applied as charge carriers for aqueous batteries, where hexagonal MoO3 is initially investigated as an anode candidate for NH4+ storage. From experimental and first‐principle calculated results, the battery chemistry proceeds with reversible building–breaking behaviors of hydrogen bonds between NH4+ and tunneled MoO3 electrode frameworks, where the ammoniation/deammoniation mechanism is dominated by nondiffusion‐controlled pseudocapacitive behavior. Outstanding electrochemical performance of MoO3 for NH4+ storage is delivered with 115 mAh g−1 at 1 C and can retain 32 mAh g−1 at 150 C. Furthermore, it remarkably exhibits ultralong and stable cyclic performance up to 100 000 cycle with 94% capacity retention and high power density of 4170 W kg−1 at 150 C. When coupled with CuFe prussian blue analogous (PBA) cathode, the full ammonium battery can deliver decent energy density 21.3 Wh kg−1 and the resultant flexible ammonium batteries at device level are also pioneeringly developed for potential realistic applications.

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Section: Figurementioning

confidence: 99%

Initiating Hexagonal MoO₃ for Superb‐Stable and Fast NH₄⁺ Storage Based on Hydrogen Bond Chemistry

et al. 2020

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“…Interestingly, with the progress in the development of water‐in‐salt electrolyte and the corresponding battery chemistry, aqueous LIBs are also possible to meet the Battery 500 Project target. A representative work is the aqueous LIBs that has been recently reported by Yang et al which achieves a stable operation potential of 4.2 V and energy density of 460 Wh kg −1 . It is great progress but worthy noting that the energy density calculation is based on the mass of anode and cathode.…”

Section: Introductionmentioning

confidence: 99%

Thick Electrode Batteries: Principles, Opportunities, and Challenges

Kuang

Chen

Kirsch

et al. 2019

Advanced Energy Materials

455

413

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Recent reviews on LBs have provided a good overview of the developments of high energy density LBs based on diverse battery chemistries. [3][4][5][6] It is believed that the energy density of current LBs can be improved up to 300-350 Wh kg −1 in a short time by using high-nickel (Ni) content cathodes, silicon (Si) dominant anodes, and higher voltage electrolytes, but further progress is needed to achieve an acceptable lifetime for practical application. [7] In regards to long term goals, continued research and development (R&D) of next-generation LBs is necessary to meet the Battery500 Project target of a cell-level specific energy of 500 Wh kg −1 , [8] which necessitates a combination of both innovative battery chemistries (such as lithium (Li)-sulfur (S), Li-O 2 , Li-CO 2 , and so on), and cell configurations (improved active material ratio and cell integration). [9] However, the majority of current research efforts are dedicated to the R&D of battery materials while battery configurational design is relatively overlooked. Interestingly, with the progress in the development of water-in-salt electrolyte and the corresponding battery chemistry, aqueous LIBs are also possible to meet the Battery 500 Project target. A representative work is the aqueous LIBs that has been recently reported by Yang et al. which achieves a stable operation potential of 4.2 V and energy density of 460 Wh kg −1 . [10] It is great progress but worthy noting that the energy density calculation is based on the mass of anode and cathode. When the mass of the electrolyte is included, the full-cell energy density is dropped to 304 Wh kg −1 , revealing the important role of battery configurational design.Structural engineering provides a feasible and universal way to further improve the energy density of LBs without changing the fundamental battery chemistries. Since the battery's energy only comes from the electrically active materials in the electrodes, the core principle for the novel structural design of batteries is to minimize the ratio of inactive components while maintaining or improving battery performance per mass or volume of active material. Common strategies include the optimization of battery packaging with thinner, more robust materials, the reduction of electrode porosity with a higher packing density and increased electrolyte uptake, and the utilization of thick electrodes. The first is relatively hard to improve in a short time and would require a breakthrough in battery packaging materials with carefully evaluated cost and safety parameters. As for the reduction of electrolyte, it is also difficult toThe ever-growing portable electronics and electric vehicle markets heavily influence the technological revolution of lithium batteries (LBs) toward higher energy densities for longer standby times or driving range. Thick electrode designs can substantially improve the electrode active material loading by minimizing the inactive component ratio at the device level, providing a great platform for enhancing the overall energy densi...

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“…This concept has been continuously developed into “hydrate‐melt electrolytes,” “water‐in‐bisalt (WiBS),” “water‐in‐ionomer,” and “hybrid aqueous/non‐aqueous electrolytes (HANE),” yielding outstanding ESWs up to 4.1 V ( Figure 1 ) and enabling a 3.2 V battery output voltage using Li 4 Ti 5 O 12 (LTO) and LiNi 0.5 Mn 1.5 O 4 (LNMO) as active electrode materials . By following an “inhomogeneous additive” approach, even 4.0 V aqueous LIBs were realized and further combined with a new halogen conversion–intercalation chemistry in graphite . The concept of highly concentrated electrolytes (HCE) and especially the high anodic limit of ≈5.1 V versus Li|Li + , demonstrated for HANE may open the pathway to aqueous‐based dual‐ion batteries (DIBs) .…”

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confidence: 99%

Development of Safe and Sustainable Dual‐Ion Batteries Through Hybrid Aqueous/Nonaqueous Electrolytes

Wrogemann

Künne

Heckmann

et al. 2020

Advanced Energy Materials

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In this study, a new dual‐ion battery (DIB) concept based on an aqueous/non‐aqueous electrolyte is reported, combining high safety in the form of a nonflammable water‐in‐salt electrolyte, a high cathodic stability by forming a protective interphase on the negative electrode (non‐aqueous solvent), and improved sustainability by using a graphite‐based positive electrode material. Far beyond the anodic stability limit of water, the formation of a stage‐2 acceptor‐type graphite intercalation compound (GIC) of bis(trifluoromethanesulfonyl) imide (TFSI) anions from an aqueous‐based electrolyte is achieved for the first time, as confirmed by ex‐situ X‐ray diffraction. The choice of negative electrode material shows a huge impact on the performance of the DIB cell chemistry, i.e., discharge capacities up to 40 mAh g−1 are achieved even at a high specific current of 200 mA g−1. In particular, lithium titanium phosphate (LiTi2(PO4)3; LTP) and lithium titanium oxide (Li4Ti5O12; LTO) are evaluated as negative electrodes, exhibiting specific advantages for this DIB setup. In this work, a new DIB storage concept combining an environmentally friendly, transition‐metal‐free, abundant graphite positive electrode material, and a nonflammable water‐based electrolyte is established, thus paving the path toward a sustainable and safe alternative energy storage technology.

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Aqueous Li-ion battery enabled by halogen conversion–intercalation chemistry in graphite

Cited by 630 publications

References 53 publications

Initiating Hexagonal MoO₃ for Superb‐Stable and Fast NH₄⁺ Storage Based on Hydrogen Bond Chemistry

Initiating Hexagonal MoO₃ for Superb‐Stable and Fast NH₄⁺ Storage Based on Hydrogen Bond Chemistry

Thick Electrode Batteries: Principles, Opportunities, and Challenges

Development of Safe and Sustainable Dual‐Ion Batteries Through Hybrid Aqueous/Nonaqueous Electrolytes

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Aqueous Li-ion battery enabled by halogen conversion–intercalation chemistry in graphite

Cited by 630 publications

References 53 publications

Initiating Hexagonal MoO3 for Superb‐Stable and Fast NH4+ Storage Based on Hydrogen Bond Chemistry

Initiating Hexagonal MoO3 for Superb‐Stable and Fast NH4+ Storage Based on Hydrogen Bond Chemistry

Thick Electrode Batteries: Principles, Opportunities, and Challenges

Development of Safe and Sustainable Dual‐Ion Batteries Through Hybrid Aqueous/Nonaqueous Electrolytes

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Product

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Initiating Hexagonal MoO₃ for Superb‐Stable and Fast NH₄⁺ Storage Based on Hydrogen Bond Chemistry

Initiating Hexagonal MoO₃ for Superb‐Stable and Fast NH₄⁺ Storage Based on Hydrogen Bond Chemistry