Structural Engineering of Carbon-Based Cathodes for Advanced Aqueous Zn-CO2 Batteries: From Macroscopic Architectures to Atomic-level Manipulation

Abstract

Aqueous Zn-CO2 batteries as a safe and green energy storge device, which can simultaneously achieve the electrochemical CO2 conversion for value-added chemicals production and energy storage, have attracted wide attention. Carbon-based cathodes have been widely explored due to their tunable characteristics, but the comprehensive summary on the multi-scale structural engineering is still lacking. This review first introduces the latest progress of Zn-CO2 batteries from battery mechanism, battery system to the cathode structural design. The structural engineering of carbon cathodes at both macroscopic level (e.g., morphology control, pore engineering, heterostructure, and interface engineering) and atomic level (including heteroatom doping, defect engineering, and single-atom site engineering) are systematically summarized. This review emphasized the importance of synergistic design integrating atomic-level manipulation and macroscopic design for performance optimization, which is promising to provide guidance for the rational structural design of carbon-based cathodes for high-performance Zn-CO2 batteries and other related energy storage devices.