Tunability of the Superconductivity of NbSe2 Films Grown by Two-Step Vapor Deposition.

Layered metallic transition-metal dichalcogenides (TMDCs) are ideal platforms for exploring their fascinating electronic properties at two-dimensional limits, such as their charge density wave (CDW) and superconductivity. Therefore, developing ways to improve the crystallization quality of TMDCs is urgently needed. Here we report superconductively tunable NbSe2 grown by a two-step vapor deposition method. By optimizing the sputtering conditions, superconducting NbSe2 films were prepared from highly crystalline Nb films. The bilayer NbSe2 films showed a superconducting transition temperature that was up to 3.1 K. Similar to the salt-assisted chemical vapor deposition (CVD) method, superconducting monolayer NbSe2 crystals were also grown from a selenide precursor, and the growth strategy is suitable for many other TMDCs. Our growth method not only provides a way to improve the crystalline quality of TMDC films, but also gives new insight into the growth of monolayer TMDCs. It holds promise for exploring two-dimensional TMDCs in fundamental research and device applications.

Ultrastable Anode/Electrolyte Interface in Solid-State Lithium-Metal Batteries Using LiCux Nanowire Network Host.

High interfacial resistance and uncontrollable lithium (Li) dendrite are major challenges in solid-state Li-metal batteries (SSLMBs), as they lead to premature short-circuiting and failure of SSLMBs. Here, we report the synthesis of a composite anode comprising a three-dimensional LiCux nanowire network host infiltrated with Li (Li* anode) with low interfacial impedance and superior electrochemical performance. The Li* anode is fabricated by dissolving Cu foil into molten Li followed by solidification. The Li* anode exhibits good wettability with Li6.4La3Zr1.4Ta0.6O12 (LLZTO) and high mechanical strength, rendering low Li*/LLZTO interfacial impedance, homogeneous deposition of Li, and suppression of Li dendrites. Consequently, the Li* anode-based symmetric cells and full cells with LiNi0.88Co0.1Al0.02O2 (NCA), LiFePO4 (LFP), and FeF2 cathodes deliver remarkable electrochemical performance. Specifically, the Li*/LLZTO/Li* symmetrical cell achieves a remarkably long cycle lifetime of 10 000 h with 0.1 mA·cm-2; the Li*/LLZTO/NCA full cell maintains capacity retention of 73.4% after 500 cycles at 0.5C; and all-solid-state Li*/LLZTO/FeF2 full cell achieves a reversible capacity of 147 mAh·g-1 after 500 cycles at 100 mA·g-1. This work demonstrates potential design tactics for an ultrastable Li*/garnet interface to enable high-performance SSLMBs.

In Situ Imaging Polysulfides Electrochemistry of Li-S Batteries in a Hollow Carbon Nanotubule Wet Electrochemical Cell.

Understanding polysulfide electrochemistry is critical for mitigation of the polysulfide shuttle effect in Li-S batteries. However, in situ imaging polysulfides evolution in Li-S batteries has not been possible. Herein, we constructed a hollow carbon nanotubule (CNT) wet electrochemical cell that permits real-time imaging of polysulfide evolutions in Li-S batteries in a Cs-corrected environmental transmission electron microscope. Upon discharge, sulfur was electrochemically reduced to long-chain polysulfides, which dissolved into the electrolyte instantly and were stabilized by Py14+ cations solvation. Metastable polysulfides prove to be problematic for Li-S batteries, therefore, destabilizing the Py14+-solvated polysulfides by adding low polarized solvents into the electrolyte to weaken the interaction between Py14+ cation and long-chain polysulfides renders a rapid polysulfides-to-Li2S transition, thus efficiently mitigating polysulfide formation and improving the performance of Li-S batteries dramatically. Moreover, the CNT wet electrochemical cell proves to be a universal platform for in situ probing electrochemistry of various batteries.

A High-Performance Carbonate-Free Lithium|Garnet Interface Enabled by a Trace Amount of Sodium.

Garnet-type solid-state electrolytes (SSEs) are promising for the realization of next-generation high-energy-density Li metal batteries. However, a critical issue associated with the garnet electrolytes is the poor physical contact between the Li anode and the garnet SSE and the resultant high interfacial resistance. Here, it is reported that the Li|garnet interface challenge can be addressed by using Li metal doped with 0.5 wt% Na (denoted as Li*) and melt-casting the Li* onto the garnet SSE surface. A mechanistic study, using Li6.4 La3 Zr1.4 Ta0.6 O12 (LLZTO) as a model SSE, reveals that Li2 CO3 resides within the grain boundaries of newly polished LLZTO pellet, which is difficult to remove and hinders the wetting process. The Li* melt can phase-transfer the Li2 CO3 from the LLZTO grain boundary to the Li*'s top surface, and therefore facilitates the wetting process. The obtained Li*|LLZTO demonstrates a low interfacial resistance, high rate capability, and long cycle life, and can find applications in future all-solid-state batteries (e.g., Li*|LLZTO|LiFePO4 ).