Graphitic Carbon Nitride (g‐C₃N₄): An Interface Enabler for Solid‐State Lithium Metal Batteries

Abstract

Solid‐state Li metal batteries (SSLMBs) have attracted considerable interests due to their promising energy density as well as high safety. However, the realization of a well‐matched Li metal/solid‐state electrolyte (SSE) interface remains challenging. Herein, we report g‐C3N4 as a new interface enabler. We discover that introducing g‐C3N4 into Li metal can not only convert the Li metal/garnet‐type SSE interface from point contact to intimate contact but also greatly enhance the capability to suppress the dendritic Li formation because of the greatly enhanced viscosity, decreased surface tension of molten Li, and the in situ formation of Li3N at the interface. Thus, the resulting Li‐C3N4|SSE|Li‐C3N4 symmetric cell gives a significantly low interfacial resistance of 11 Ω cm2 and a high critical current density (CCD) of 1500 μA cm−2. In contrast, the same symmetric cell configuration with pristine Li metal electrodes has a much larger interfacial resistance (428 Ω cm2) and a much lower CCD (50 μA cm−2).

Progress and perspective of interface design in garnet electrolyte‐based all‐solid‐state batteries

“…68 First principle calculation shows that Li-Li 2 CO 3 only has 0.1 J m −2 of interfacial work of adhesion, W ad , whereas that for Li-LLZO is 0.67 J m −2 . Interestingly, the reported contact angle of Li-LLZO varies from 90°to 122°, 64,67,[69][70][71] possibly due to the difference and cleanliness of the surface. Therefore, a standardized measurement procedure, including the precise surface cleaning procedure is required to enable comparison in literature.…”

“…12 The most representative example is atomic layer deposition (ALD) of Al 2 O 3 on LLZO electrolyte. 64 The ALD method maximizes the contact between Al 2 O 3 and LLZO. Al 2 O 3 is lithiophilic, showing a much smaller contact angle with molten Li (Figure 10B).…”

DFT-Guided Design and Fabrication of Carbon-Nitride-Based Materials for Energy Storage Devices: A Review

“…27 c) and maintained a strong/intimate contact with the Garnet (Fig. 27 d) [ 165 ]. Lu et al also reported the application of mesoporous carbon nitride (MCN) and acetylene black (AB) as a support for in situ growth of Pt nanoparticles for an all-solid-state lithium air battery system.…”

“…Reproduced with permission from Ref. [ 165 ]. e Scheme of the configuration of the MCN-based electrode solid-state lithium-air battery.…”

Low-Temperature Multielement Fusible Alloy-Based Molten Sodium Batteries for Grid-Scale Energy Storage

“…Meanwhile, good wetting is still maintained after cell cycling as presented in Figure S7 , indicating the stable interface between liquid metals and current collectors. 43 In contrast, when stainless steel was adopted, the liquid metal will ball up on the current collector with poor wetting ( Figure S8 ). The voltage profiles in Figure S9 also show more obvious polarization with a larger overpotential.…”