Verifying the Rechargeability of Li‐CO₂ Batteries on Working Cathodes of Ni Nanoparticles Highly Dispersed on N‐Doped Graphene

Abstract

Li‐CO2 batteries could skillfully combine the reduction of “greenhouse effect” with energy storage systems. However, Li‐CO2 batteries still suffer from unsatisfactory electrochemical performances and their rechargeability is challenged. Here, it is reported that a composite of Ni nanoparticles highly dispersed on N‐doped graphene (Ni‐NG) with 3D porous structure, exhibits a superior discharge capacity of 17 625 mA h g−1, as the air cathode for Li‐CO2 batteries. The batteries with these highly efficient cathodes could sustain 100 cycles at a cutoff capacity of 1000 mA h g−1 with low overpotentials at the current density of 100 mA g−1. Particularly, the Ni‐NG cathodes allow to observe the appearance/disappearance of agglomerated Li2CO3 particles and carbon thin films directly upon discharge/charge processes. In addition, the recycle of CO2 is detected through in situ differential electrochemical mass spectrometry. This is a critical step to verify the electrochemical rechargeability of Li‐CO2 batteries. Also, first‐principles computations further prove that Ni nanoparticles are active sites for the reaction of Li and CO2, which could guide to design more advantageous catalysts for rechargeable Li‐CO2 batteries.

Water Splitting–Biosynthetic Hybrid System for CO2 Conversion using Nickel Nanoparticles Embedded in N‐Doped Carbon Nanotubes

“…Figure 1d shows the XRD patterns of the as-prepared Ni@N-Cc omplex. [40,44] Electrochemical characterization of the Ni@N-C complex The content of Ni wasa sl ow as only 1.42 AE 0.65 at %.…”

“…[43] In addition, the de-convoluted C1ss pectrum can be fitted with three different types of carbon species in CÀC( 284.6 eV), CÀN( 285.8 eV), and C=O ( Figure S3;288.2 eV). [40,44] Electrochemical characterization of the Ni@N-C complex…”

Progress and Future Perspectives on Li(Na)–CO2 Batteries

“…[ 63] This work is instructive for developing highly efficient nonprecious metal cathodes for Li-CO 2 www.advsustainsys.com the conductive matrix (Mo 2 C/CNTs) prepared by a carbothermal reduction process. [64] They found that the Mo 2 C nanoparticles could stabilize the Li 2 C 2 O 4 intermediate reduction product of CO 2 on discharge and prevent its disproportionation to Li 2 CO 3 .…”

Reversible Hybrid Aqueous Li−CO2 Batteries with High Energy Density and Formic Acid Production

“…Furthermore, the reversible hybrid aqueous LiÀCO 2 battery showed superbr ate performance even at high currentd ensities. These advantages of the reversible hybrid aqueous LiÀCO 2 battery could be duet ot he new reaction mechanism derived from the integration of aL ia node and aqueous catholyte in the battery.I nr eported organic LiÀCO 2 batteries, the battery reaction mostly occurs as described in Equation (1): [21] Figure 2. The discharge voltage and HCOOH production of the reversible hybrid aqueousLi ÀCO 2 battery.a )Galvanostaticd ischarge voltagesa nd b) the corresponding FEsofH COOH and H 2 at different currents.c )Galvanostatic long-termdischarge curve at 5.56 mA cm À2 and corresponding product selectivity.…”