Mastering Surface Sulfidation of MnP-MnO2 Heterostructure to Facilitate Efficient Polysulfide Conversion in Li─S Batteries.

The development of lithium-sulfur (Li─S) batteries has been hampered by the shuttling effect of lithium polysulfides (LiPSs). An effective method to address this issue is to use an electrocatalyst to accelerate the catalytic conversion of LiPSs. In this study, heterogeneous MnP-MnO2 nanoparticles are uniformly synthesized and embedded in porous carbon (MnP-MnO2/C) as core catalysts to improve the reaction kinetics of LiPSs. In situ characterization and density functional theory (DFT) calculations confirm that the MnP-MnO2 heterostructure undergo surface sulfidation during the charge/discharge process, forming the MnS2 phase. Surface sulfidation of the MnP-MnO2 heterostructure catalyst significantly accelerated the SRR and Li2S activation, effectively inhibiting the LiPSs shuttling effect. Consequently, the MnP-MnO2/C@S cathode achieves outstanding rate performance (10 C, 500 mAh g-1) and ultrahigh cycling stability (0.017% decay rate per cycle for 2000 cycles at 5 C). A pouch cell with MnP-MnO2/C@S cathode delivers a high energy density of 429 Wh kg-1. This study may provide a new approach to investigating the surface sulfidation of electrocatalysts, which is valuable for advancing high-energy-density Li-S batteries.

Three-Phase-Heterojunction Cu/Cu2O-Sb2O3 Catalyst Enables Efficient CO2 Electroreduction to CO and High-Performance Aqueous Zn-CO2 Battery.

Zn-CO2 batteries are excellent candidates for both electrical energy output and CO2 utilization, whereas the main challenge is to design electrocatalysts for electrocatalytic CO2 reduction reactions with high selectivity and low cost. Herein, the three-phase heterojunction Cu-based electrocatalyst (Cu/Cu2O-Sb2O3-15) is synthesized and evaluated for highly selective CO2 reduction to CO, which shows the highest faradaic efficiency of 96.3% at -1.3 V versus reversible hydrogen electrode, exceeding the previously reported best values for Cu-based materials. In situ spectroscopy and theoretical analysis indicate that the Sb incorporation into the three-phase heterojunction Cu/Cu2O-Sb2O3-15 nanomaterial promotes the formation of key *COOH intermediates compared with the normal Cu/Cu2O composites. Furthermore, the rechargeable aqueous Zn-CO2 battery assembled with Cu/Cu2O-Sb2O3-15 as the cathode harvests a peak power density of 3.01 mW cm-2 as well as outstanding cycling stability of 417 cycles. This research provides fresh perspectives for designing advanced cathodic electrocatalysts for rechargeable Zn-CO2 batteries with high-efficient electricity output together with CO2 utilization.