Isolated Metalloid Tellurium Atomic Cluster on Nitrogen‐Doped Carbon Nanosheet for High‐Capacity Rechargeable Lithium‐CO₂ Battery

Abstract

Rechargeable Li‐CO2 battery represents a sustainable technology by virtue of CO2 recyclability and energy storage capability. Unfortunately, the sluggish mass transport and electron transfer in bulky high‐crystalline discharge product of Li2CO3, severely hinder its practical capacity and rechargeability. Herein, a heterostructure of isolated metalloid Te atomic cluster anchored on N‐doped carbon nanosheets is designed (TeAC@NCNS) as a metal‐free cathode for Li‐CO2 battery. X‐ray absorption spectroscopy analysis demonstrates that the abundant and dispersed Te active centers can be stabilized by C atoms in form of the covalent bond. The fabricated battery shows an unprecedented full‐discharge capacity of 28.35 mAh cm−2 at 0.05 mA cm−2 and long‐term cycle life of up to 1000 h even at a high cut‐off capacity of 1 mAh cm−2. A series of ex situ characterizations combined with theoretical calculations demonstrate that the abundant Te atomic clusters acting as active centers can drive the electron redistribution of carbonate via forming TeO bonds, giving rise to poor‐crystalline Li2CO3 film during the discharge process. Moreover, the efficient electron transfer between the Te centers and intermediate species is energetically beneficial for nucleation and accelerates the decomposition of Li2CO3 on the TeAC@NCNS during the discharge/charge process.

MOF‐Derived CoSe2 Nanoparticles/Carbonized Melamine Foam as Catalytic Cathode Enabling Flexible Li–CO2 Batteries with High Energy Efficiency and Stable Cycling

“…It is widely recognized that this dense discharge product layer would hinder efficient electron transfer between the cathode catalysts and CO 2 molecules and cause sluggish kinetics of CO 2 reduction reaction. [55] As expected, the discharge voltage of the Co/CMF cathode rapidly fades >2 mAh cm −2 (Figure 2c). The micromorphology of the Co/CMF cathode at a full discharge is shown in Figure S11 (Supporting Information).…”

Te Cluster Engineering for Tunable Optical Response

“…It can be clearly found that the absorption edge of the sample is located at the higher energy region than that of the Te‐foil, indicating a more positively charged state of central Te atoms due to the lower electronegativity of Te (χ Te = 2.1) than that of neighboring oxygen atoms (χ O = 3.5). [ 42 ] Figure 1f represents the Fourier transformed ( r space) extended X‐ray absorption fine structural (FT‐EXAFS) spectra of Cs 2 O‐containing sample and Te‐foil. Both the sample and the Te‐foil exhibit a similar prominent peak at 2.64 Å, corresponding to the Te─Te bond.…”

Revealing the Indispensable Role of In Situ Electrochemically Reconstructed Mn(II)/Mn(III) in Improving the Performance of Lithium‐Carbon Dioxide Batteries

“…The higher adsorption temperature proves that MOC@NCNF possesses stronger chemical adsorption for CO 2 , which is beneficial for promoting its activation during the discharge process. [40,41] Besides, good electrical conductivity is beneficial to facilitate the reaction kinetics of CORR and COER. Therefore, the fourprobe technique was performed to explore the impact of the introduction of MOC on electrical conductivity.…”

“…The higher adsorption temperature proves that MOC@NCNF possesses stronger chemical adsorption for CO 2 , which is beneficial for promoting its activation during the discharge process. [ 40,41 ]…”