Stable Li‐Metal Deposition via a 3D Nanodiamond Matrix with Ultrahigh Young's Modulus

Abstract

The practical usage of high‐energy lithium metal batteries remains a great challenge mainly due to the formation of uneven lithium deposition and huge volume fluctuation on the anode side, which increases the potential risks of a cell short‐circuit. Herein, a nanodiamond‐Li composite anode (ND‐Li) is created using a facile thermal infusion strategy, which can mechanically confine active Li‐metal in the ND matrix and minimize the electrode volume change during electrochemical cycling with high areal capacities. The geometrically restrictive ND matrix with ultrahigh modulus can deform the uneven lithium deposition mechanically and confine the deposition to the ND matrix. Owing to the 3D rigid skeleton, low stripping/plating overpotential (≈60 mV) can be achieved for a ND‐Li anode under a high current density of 10 mA cm−2, whereas the overpotential of a bare Li foil anode is almost seven times larger than the ND‐Li matrix. When a ND‐Li anode pairs with a S cathode, a high capacity of 607.3 mAh g−1 at 1 C and stable long‐term cyclability over 500 cycles can be achieved.

Regulating the Catalytic Dynamics Through a Crystal Structure Modulation of Bimetallic Catalyst

“…Hence, the crystal or surface structure of solid catalysts should be varied to not only enable the nucleation‐preferred formation of discharge products but also make the interaction between discharge products and catalyst surface appropriate. We believe that these rationales based on the growth dynamics of products from ORR/OER can be valid for a lot of solid catalysts and energy materials for future battery systems ranging from metals to oxides or hybrid materials …”

Colossal Granular Lithium Deposits Enabled by the Grain‐Coarsening Effect for High‐Efficiency Lithium Metal Full Batteries

“…[7] Battery short-circuits induced by dendritic Li deposition can be relieved by employing functionalized separators, [8,9] artificial solid electrolyte interphases [10][11][12] and 3D composite anodes. [13][14][15] Li Coulombic efficiency (Li CE), defined as the ratio between the amount of Li stripped and Li plated at each cycle, is used as a truthful indicator to monitor the irreversible consumption of active Li. [16] Recently published works have demonstrated that low Li CE as a result of side reactions at the lithium metal surface and inefficient stripping process turns out to be the real culprit behind poor cyclability of practical full LMBs, but this issue is usually hidden when huge excess Li is used (e.g., thick Li metal anode > 300 µm).…”

Engineering Wavy‐Nanostructured Anode Interphases with Fast Ion Transfer Kinetics: Toward Practical Li‐Metal Full Batteries

“…Extensive studies have explored to suppress dendritic lithium deposition by mechanical confinements (e.g., using functional separators, [ 7–9 ] rigid 3D hosts, [ 10 ] and solid‐state electrolytes [ 11–13 ] ), lithiophilic substrate modifications, [ 14 ] and electrolyte optimizations. [ 15–17 ] However, recent quantitative experiments demonstrated that low lithium Coulombic efficiency (Li CE) is the real culprit behinds the poor cyclability in practical LMBs with limited negative to positive capacity (N/P) ratio and electrolyte amount to cathode capacity (E/C) ratio.…”