Design principles for heterointerfacial alloying kinetics at metallic anodes in rechargeable batteries

Abstract

How surface chemistry influences reactions occurring thereupon has been a long-standing question of broad scientific and technological interest. Here, we consider the relation between the surface chemistry at interfaces and the reversibility of electrochemical transformations at rechargeable battery electrodes. Using Zn as a model system, we report that a moderate strength of chemical interaction between the deposit and the substrate—neither too weak nor too strong—enables highest reversibility and stability of the plating/stripping redox processes. Focused ion beam and electron microscopy were used to directly probe the morphology, chemistry, and crystallography of heterointerfaces of distinct natures. Analogous to the empirical Sabatier principle for chemical heterogeneous catalysis, our findings arise from competing interfacial processes. Using full batteries with stringent negative electrode–to–positive electrode capacity (N:P) ratios, we show that such knowledge provides a powerful tool for designing key materials in highly reversible battery systems based on Earth-abundant, low-cost metals such as Zn and Na.

Dynamic template directed construction of three-dimensional porous bismuth aerogels for high-rate Na-ion storage

“…Otherwise, when it approaches 0.5, a diffusion-controlled behavior occurs. 50 The b values of R 1 , R 2 , O 1 and O 2 were estimated to be 0.55, 0.59, 0.57 and 0.60, respectively, suggesting a dominant diffusion-controlled redox reaction. 51…”

“…Otherwise, when it approaches 0.5, a diffusion-controlled behavior occurs. 50 The b values of R 1 , R 2 , O 1 and O 2 were estimated to be 0.55, 0.59, 0.57 and 0.60, respectively, suggesting a dominant diffusion-controlled redox reaction. 51 To further explore the reasons for the excellent electrochemical performance of the 3DBS aerogel anode, the electrochemical impedance spectra (EIS) of 3DBS, 3DBNS and 3DBNW aerogels with a mass loading of 1 mg cm −2 were compared (Fig.…”

Metal Anodes with Ultrahigh Reversibility Enabled by the Closest Packing Crystallography for Sustainable Batteries

“…In the electrodepositing process of Zn on Cu, Cu–Zn alloys always form between Zn and Cu. [ 19 ] Among the variety of Cu–Zn alloys, only the CuZn 4 possesses the same hcp structure as Zn. [ 20 ] The low lattice mismatches among Cu(111), CuZn 4 (002), and Zn(002) make the CuZn 4 (002) the most possible buffer layer (Figure S10, Supporting Information).…”

Rational design and regulation of tremella-like selenium-doped MoS2 for highly reversible sodium storage

“…MoS 1.5 Se 0.5 @C delivers initial discharge and charge capacities of 780.7 and 603.5 mA h g −1 with 77.3% initial coulombic efficiency (ICE), which is the best among MoS 2 @C (598.8/316.1 mA h g −1 , 52.8%), MoS 1.8 Se 0.2 (670.0/402.6 mA h g −1 , 60.1%), MoS 1.5 Se 0.5 (662.3/438.5 mA h g −1 , 66.2%), MoSSe (677.2/423.2 mA h g −1 , 62.5%), MoS 1.8 Se 0.2 @C (776.4/537.2 mA h g −1 , 69.2%) and MoSSe@C (689.9/487.1 mA h g −1 , 70.6%). The irreversible capacity loss for the rst cycle is due to the formation of a solidliquid interface SEI layer, 34,35 while the enhanced ICE of 77.3% for MoS 1.5 Se 0.5 @C is due to improved stability resulting from carbon coating and an appropriate amount of Se doping. In order to investigate the inuence of different amounts of Se doping and carbon coating on electrochemical performance, the sodium storage performance of all samples was evaluated from their rate performance (Fig.…”