Theoretical Design and Structural Modulation of a Surface-Functionalized Ti3C2Tx MXene-Based Heterojunction Electrocatalyst for a Li–Oxygen Battery

过电位 电催化剂 材料科学 异质结 析氧 电池(电) 电化学 化学工程 电极 化学 光电子学 物理化学 功率(物理) 物理 量子力学 工程类
作者
Xingzi Zheng,Mengwei Yuan,Donghua Guo,Caiying Wen,Xingyu Li,Xianqiang Huang,Huifeng Li,Genban Sun
出处
期刊:ACS Nano [American Chemical Society]
卷期号:16 (3): 4487-4499 被引量:54
标识
DOI:10.1021/acsnano.1c10890
摘要

Two-dimensional MXene with high conductivity has metastable Ti atoms and inert functional groups on the surface, greatly limiting application in surface-related electrocatalytic reactions. A surface-functionalized nitrogen-doped two-dimensional TiO2/Ti3C2Tx heterojunction (N-TiO2/Ti3C2Tx) was fabricated theoretically, with high conductivity and optimized electrocatalytic active sites. Based on the conductive substrate of Ti3C2Tx, the heterojunction remained metallic and efficiently accelerated the transfer of Li+ and electrons in the electrode. More importantly, the precise regulation of active sites in the N-TiO2/Ti3C2Tx heterojunction optimized the adsorption for LiO2 and Li2O2, facilitating the sluggish kinetics with a lowest theoretical overpotential in both the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER). Employed as an electrocatalyst in a Li-oxygen battery (Li-O2 battery), it demonstrated a high specific capacity of 15 298 mAh g-1 and a superior cyclability with more than 200 cycles at 500 mA g-1, as well as the swiftly reduced overpotential. Furthermore, combined with the in situ differential electrochemical mass spectrometry, ex situ Raman spectra, and SEM tests, the N-TiO2/Ti3C2Tx heterojunction electrode presented a superior stability and reduced side reaction along with the high performance toward the ORR and OER. It provides an efficient insight for the design of high-performance electrocatalysts for metal-oxygen batteries.
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