Dynamical SEI Reinforced by Open‐Architecture MOF Film with Stereoscopic Lithiophilic Sites for High‐Performance Lithium–Metal Batteries

Wu, Qingping; Zheng, Yongjian; Guan, Xiang; Xu, Jun; Cao, Fahai; Li, Chilin

doi:10.1002/adfm.202101034

Cited by 62 publications

(57 citation statements)

References 48 publications

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“…The thus-derived B-Cu-Li, D-Cu-Li, and D-Cu@CuSe-Li electrodes were subject to symmetric cell testing. [43,44] Figure 3d presents the long-term plating/stripping voltage profiles of B-Cu-Li-, D-Cu-Li-, and D-Cu@CuSe-Li-based symmetric cells at 1 mA cm À2 / 1 mAh cm À2 . It is observed that D-Cu@CuSe-Li implements a stable cyclic performance over 1800 h, whereas B-Cu-Li and D-Cu-Li exhibit a considerable fluctuation even prior to 400 h cycling.…”

Section: Resultsmentioning

confidence: 99%

Synergizing Conformal Lithiophilic Granule and Dealloyed Porous Skeleton toward Pragmatic Li Metal Anodes

et al. 2022

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Li metal is regarded as one of the most promising anodes for next‐generation rechargeable batteries. Nonetheless, infinite volume change and severe dendrite growth impede its practicability. To date, unremitting efforts have been devoted to stabilizing Li metal anode via the rational design of 3D current collectors. In this sense, optimizing Li nucleation behavior plays a pivotal role in alleviating the dendrite formation. Herein, a practically viable route is devised by in situ crafting lithiophilic CuSe granules on the dealloyed Cu skeleton (D‐Cu@CuSe). Persuasive electrochemical analysis and systematic theoretical calculation disclose the underlying Li nucleation mechanism on the CuSe overlayer. Impressively, the D‐Cu@CuSe‐Li symmetric cell can sustain a stable plating/stripping operation over 1000 h at a high depth of discharge at 62.5%. More crucially, when paired with high‐loading sulfur cathodes, D‐Cu@CuSe‐Li||S batteries harvest advanced areal capacity and stable cycling performance even under stringent working conditions of low negative‐to‐positive (N/P) (≈2) and electrolyte‐to‐sulfur (8 μL mgs−1) ratios. Overall, a fresh perspective into rationalizing current collector design is afforded, which extends Li utilization and cycling durability in the pursuit of pragmatic Li metal anodes.

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Section: Resultsmentioning

confidence: 99%

Synergizing Conformal Lithiophilic Granule and Dealloyed Porous Skeleton toward Pragmatic Li Metal Anodes

et al. 2022

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“…To reinforce the view of PPy‐guided Li plating/stripping on PPHK@Cu, apparent Li + transference numbers ( t

_{Li^{+}}

) were estimated following the potentiostatic polarization method established by Evans et al., [23] which was also used in previous studies to index the charge transfer kinetics on lithium metal anodes [24] and MOF‐modified electrolyte [6b] . The symmetric cell of Li⊂PPHK@Cu measured a t

_{Li^{+}}

value of 0.56, which was higher than the value of 0.42 given by Li@bare‐Cu (Figure S24, Table S2).…”

Section: Resultsmentioning

confidence: 99%

A “Blockchain” Synergy in Conductive Polymer‐Filled Metal–Organic Frameworks for Dendrite‐Free Li Plating/Stripping with High Coulombic Efficiency

et al. 2022

Angew Chem Int Ed

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The performance of lithium-metal batteries is severely hampered by uncontrollable dendrite growth and volume expansion on the metal anodes. Inspired by the "blockchain" concept in data mining, here we utilize a conductive polymer-filled metal-organic framework (MOF) as the lithium host, in which polypyrrole (PPy) serves as the "chain" to interlink Li "blocks" stored in the MOF pores. While the N-rich PPy guides fast Li + infiltration/extrusion and serves as the nucleation sites for isotropic Li growth, the MOF pores compartmentalize bulk Li deposition for 3D matrix Li storage, leading to low-barrier and dendrite-free Li plating/stripping with superb Coulombic efficiency. The asfabricated lithium-metal anodes operate over 700 cycles at 5 mA cm À 2 in symmetric cells, and 800 cycles at 1 C in full cells with a per-cycle capacity loss of only 0.017 %. This work might open a new chapter for Li-metal anode construction by introducing the concept of "blockchain" management of Li plating/stripping.

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“…[ 24 ] In the following cycles, the charge/discharge curves of NHM overlap much better than NHS and NHP, suggesting good stability and significant reversibility of the NHM electrode for the insertion/extraction of Li + , corresponding to Figure S13, Supporting Information. [ 25 ] Meaningfully, the sloping voltage profiles suggest the pseudocapacitive lithium storage behavior, which could reduce the polarization of LIB and improve the stability of the electrodes. [ 22,26 ] These results with remitted capacity fading are attributed to the Tostadas‐shaped architecture of NHM built by the strong electrostatic adsorption of NHP on the NHS, which shortens the diffusion distance of Li ions, thus maintaining the sustainability in the repeated activation process of the NHM electrode.…”

Section: Resultsmentioning

confidence: 99%

Synthesis of Tostadas‐Shaped Metal‐Organic Frameworks for Remitting Capacity Fading of Li‐Ion Batteries

Cai

Wang

Cao

et al. 2021

Adv Funct Materials

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Electrode design strategies that aim to increase the electrochemical performance of Li‐ion batteries (LIBs) play a key role in tapping into the power of the energy transformations involved. Metal‐organic frameworks (MOFs) have attracted scientific interest as electrode materials for LIBs, while the utilization of pristine MOFs is hindered by limited conductivity and stability, partly due to their lack of hierarchically structured pores. Herein a hydrothermal‐mechanical synthesis is reported by combining the one‐pot chemical fabrication of Ni3(2,3,6,7,10,11‐hexaiminotriphenylene)2 sheets and particles, and the mechanical assembly of these building blocks to improve electrical conductivity is also described. The as‐prepared ensemble (denoted as NHM) exhibits a Tostadas‐shaped structure with enriched ultramicropores and micropores. The charge‐discharge profile of NHM gives a superior reversible capacity of 1280 mA h g−1 after 100 cycles at the rate of 0.1 A g−1, surpassing the state‐of‐art pristine MOFs‐based anodes. Moreover, NHM is capable of maintaining 392 mA h g−1 at 1 A g−1 after 1000 cycles, the completion of a stability test in coin cell‐powered light emitting diodes further visualizes the remitted capacity fading of NHM. This work breaks through the limitation of capacity for pristine MOFs, providing a new pathway for achieving better energy conversion and storage.

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Dynamical SEI Reinforced by Open‐Architecture MOF Film with Stereoscopic Lithiophilic Sites for High‐Performance Lithium–Metal Batteries

Cited by 62 publications

References 48 publications

Synergizing Conformal Lithiophilic Granule and Dealloyed Porous Skeleton toward Pragmatic Li Metal Anodes

Synergizing Conformal Lithiophilic Granule and Dealloyed Porous Skeleton toward Pragmatic Li Metal Anodes

A “Blockchain” Synergy in Conductive Polymer‐Filled Metal–Organic Frameworks for Dendrite‐Free Li Plating/Stripping with High Coulombic Efficiency

Synthesis of Tostadas‐Shaped Metal‐Organic Frameworks for Remitting Capacity Fading of Li‐Ion Batteries

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