Abstract:Lithium metal with high theoretical capacity (3860 mAh/g) and low operational voltage (-3.04 V vs. standard hydrogen electrode) reflects to be one of the most high energy density anodes for energy storage devices. While, its high chemical activity to continuously react with electrolytes causing low coulombic efficiency and formation of lithium dendrites leading safety concern limits practical applications. To conquer these challenges, amorphous Li 3 PO 4 thin films with thickness of 0-200 nm are directly coate… Show more
“…Lithium interfaces must be assembled below 500 K. At this temperature, the predicted ∆E * is too still high for the reaction to occur within reasonable timescales. The high activation energy associated with P-O bond cleavage is likely the reason Li 3 PO 4 has also been used as coating layers for lithium metal [64], even though Li 3 PO 4 is also thermodynamically unstable against Li metal [27].…”
Detailed understanding of solid-solid interface structure-function relationships is critical for the improvement and wide deployment of all-solid-state batteries. The interfaces between lithium phosphorous oxynitride (LiPON) solid electrolyte material and lithium metal anode, and between LiPON and Li CoO cathode, have been reported to generate solid-electrolyte interphase (SEI)-like products and/or disordered regions. Using electronic structure calculations and crystalline LiPON models, we predict that LiPON models with purely P-N-P backbones are kinetically inert towards lithium at room temperature. In contrast, transfer of oxygen atoms from low-energy Li CoO (104) surfaces to LiPON is much faster under ambient conditions. The mechanisms of the primary reaction steps, LiPON structural motifs that readily reacts with lithium metal, experimental results on amorphous LiPON to partially corroborate these predictions, and possible mitigation strategies to reduce degradations are discussed. LiPON interfaces are found to be useful case studies for highlighting the importance of kinetics-controlled processes during battery assembly at moderate processing temperatures.
“…Lithium interfaces must be assembled below 500 K. At this temperature, the predicted ∆E * is too still high for the reaction to occur within reasonable timescales. The high activation energy associated with P-O bond cleavage is likely the reason Li 3 PO 4 has also been used as coating layers for lithium metal [64], even though Li 3 PO 4 is also thermodynamically unstable against Li metal [27].…”
Detailed understanding of solid-solid interface structure-function relationships is critical for the improvement and wide deployment of all-solid-state batteries. The interfaces between lithium phosphorous oxynitride (LiPON) solid electrolyte material and lithium metal anode, and between LiPON and Li CoO cathode, have been reported to generate solid-electrolyte interphase (SEI)-like products and/or disordered regions. Using electronic structure calculations and crystalline LiPON models, we predict that LiPON models with purely P-N-P backbones are kinetically inert towards lithium at room temperature. In contrast, transfer of oxygen atoms from low-energy Li CoO (104) surfaces to LiPON is much faster under ambient conditions. The mechanisms of the primary reaction steps, LiPON structural motifs that readily reacts with lithium metal, experimental results on amorphous LiPON to partially corroborate these predictions, and possible mitigation strategies to reduce degradations are discussed. LiPON interfaces are found to be useful case studies for highlighting the importance of kinetics-controlled processes during battery assembly at moderate processing temperatures.
“…To overcome challenges in Li-S batteries, various methods have been thoroughly explored for Li anode or S cathode separately, with little attention to the cofunction hosts for both Li and S. [13][14][15] For Li anode, there are some strategies to improve the cycling performance, including the design of stable artificial solid electrolyte interphase (SEI), [16][17][18] rational engineering of interfacial layer, [19][20][21][22][23] the use of vertically aligned channels, 24,25 the introduction of 3D scaffolds as the current collectors, [26][27][28][29][30] and so on. 31 3D porous scaffolds are the current research hotspot in Li anode for improving the Li plating/stripping behavior by accommodating volume change and reducing current density.…”
Lithium‐sulfur (Li‐S) batteries with high energy density are promising candidates for next‐generation energy storage systems. Practical application of Li‐S batteries is hindered by shuttle effect of polysulfides and Li dendrites growth. Herein, a self‐supporting cofunction host is constructed with 3D hierarchical graphene modified by N‐doped nanoarrays, for both Li anode and S cathode to improve their performances simultaneously. Attributed to high conductivity, strong affinity, and optimized Li‐ion transport pathway of N‐doped nanoarrays, cofunction host provide excellent Li and S load, which facilitates uniform Li deposition and enhanced S conversion. Particularly, an extra graphene barrier is specialized for S cathode to inhibit the shuttle effect. As a result, Li anode shows long cycle life with outstanding Li‐plating behavior, and S cathode shows high capacity and ultrahigh capacity retention with good immobilization of polysulfides. More importantly, the integrated Li‐S battery shows long cycle stability and good flexibility, which is important for future application.
“…Artificial SEI layer constructing before cell cycling was also proposed to protect the surface. [24][25][26][27][28][29] However, the volume changes of lithium metal during the cycling inevitably generate the stress which will destroy the above passivation layers. Thus, the conductive threedimensional (3D) framework structures for lithium deposition, like the porous Cu current collectors and threedimensional graphene framework, attract great attention because they can lower the local electrode current density and accommodate the large volume changes [30][31][32][33][34][35][36].…”
Lithium metal is considered to be the most promising anode material for the next-generation rechargeable batteries. However, the uniform and dendrite-free deposition of Li metal anode is hard to achieve, hindering its practical applications. Herein, a lightweight, free-standing and nitrogen-doped carbon nanofiber-based 3D structured conductive matrix (NCNF), which is characterized by a robust and interconnected 3D network with high doping level of 9.5 at%, is prepared by electrospinning as the current collector for Li metal anode. Uniform Li nucleation with reduced polarization and dendrite-free Li deposition are achieved because the NCNF with high nitrogen-doping level and high conductivity provide abundant and homogenous metallic Li nucleation and deposition sites. Excellent cycling stability with high coulombic efficiency are realized. The Li plated NCNF was paired with LiFePO 4 to assemble the full battery, also showing high cyclic stability.
scite is a Brooklyn-based organization that helps researchers better discover and understand research articles through Smart Citations–citations that display the context of the citation and describe whether the article provides supporting or contrasting evidence. scite is used by students and researchers from around the world and is funded in part by the National Science Foundation and the National Institute on Drug Abuse of the National Institutes of Health.