Chemically Self-Charging Aqueous Zinc-Organic Battery

Abstract

Zn–organic batteries are attracting extensive attention, but their energy density is limited by the low capacity (<400 mAh g–1) and potential (<1 V vs Zn/Zn2+) of organic cathodes. Herein, we propose a long-life and high-rate Zn–organic battery that includes a poly­(1,5-naphthalenediamine) cathode and a Zn anode in an alkaline electrolyte, where the cathode reaction is based on the coordination reaction between K+ and the CN group (i.e., CN/C–N–K conversion). Interestingly, we find that the discharged Zn–organic battery can recover to its initial state quickly with the presence of O2, and the theoretical calculation demonstrates that the K–N bond in the discharged cathode can be easily broken by O2 via redox reaction. Accordingly, we design a chemically self-charging aqueous Zn–organic battery. Benefiting from the excellent self-rechargeability, the organic cathode exhibits an accumulated capacity of 16264 mAh g–1, which enables the Zn–organic battery to show a record high energy density of 625.5 Wh kg–1.

High‐Rate, Large Capacity, and Long Life Dendrite‐Free Zn Metal Anode Enabled by Trifunctional Electrolyte Additive with a Wide Temperature Range

“…[ 5 , 6 , 7 ] In the recent years, rechargeable aqueous zinc ion batteries (AZIBs) have lately drawn intensive attentions, mainly owing to their rich resources, cost‐effectiveness, environmental robustness, and high‐safety. [ 8 , 9 , 10 , 11 , 12 ] Furthermore, the zinc metal possesses a higher theoretical capacity density (5855 mAh cm –3 ) and low redox potential (−0.763 V vs standard hydrogen electrode). Unfortunately, the problem of interfacial parasitic reactions, corrosion, and formation of zinc dendrite during the Zn plating/stripping process have hindered their commercialized application, which leads to poor utilization, lower Coulombic efficiency (CE), and short cycling lifespans of zinc metal anodes.…”

Proton Chemistry Induced Long‐Cycle Air Self‐Charging Aqueous Batteries

“…Even at an extremely high rate of 150 A g −1 , the corresponding discharge capacity can still maintain 105 mAh g −1 . The superior rate capability of air self‐charging Pb/PTO batteries surpasses those of the previously reported air self‐charging AMBs (Figure S12) [5a–d, 17, 18] …”

Computational and data driven molecular material design assisted by low scaling quantum mechanics calculations and machine learning

“…, poly(1,5-NAPD)) cathode, a Zn-foil anode and an alkaline electrolyte, the binding energies of (1,5-NAPD) 7 with different ions (H + , Zn + , and K + ) were calculated by CIM-RI-MP2 with the def2-TZVPD basis set. 14 The high level CIM-DLPNO-CCSD(T) binding energies were also obtained for a molecular capsule with multiple hydrogen interactions. With this binding energy as a reference, the results show that several DFT functionals overestimate the binding energies.…”

“…† Several low-scaling strategies, such as density matrix-based, local correlation, and fragment-based methods, were used to predict the ground-state energies, structures, and molecular properties of large systems. For example, a local correlation cluster-in-molecule (CIM) method was used to predict the binding energies in aqueous zinc-organic batteries; 14 a divide-and-conquer method was developed to optimize the molecular geometries of conjugated oligomers; 15 density-functional perturbation theory (DFPT) was employed to compute the polarizabilities of large organic molecules; 16 a generalized energy-based fragmentation (GEBF) method was used to predict the infrared (IR) and nuclear magnetic resonance (NMR) spectra of large supramolecular coordination complexes. 17 …”