Achieving the robust immobilization of CoP nanoparticles in cellulose nanofiber network-derived carbon via chemical bonding for a stable potassium ion storage

Abstract

Potassium-ion batteries (KIBs) are currently being investigated as a potential alternative to lithium-ion batteries (LIBs) because of the natural abundance of K resources. Presently, it is crucial yet challenging to explore suitable anode materials for stable K-storage. Herein, a novel robust CoP–carbon composite with highly dispersed CoP nanoparticles (NPs) immobilized in natural cellulose nanofiber network (CNF)-derived carbon (denoted as CoP@CNFC) is synthesized via chemical bonding through a facile hydrothermal and subsequent in situ phosphidation approach. The designed structure can provide diverse merits, including fast reaction kinetics, sufficient active sites and effective accommodation for K⁺ insertion/extraction; thus, CoP@CNFC delivers desired electrochemical performance, including considerable reversible capacity, enhanced rate capability and excellent cycling stability. Additionally, the electrochemical reaction mechanism of CoP@CNFC was clearly revealed by ex situ characterizations and theoretical simulations of cyclic voltammetry (CV) and solid electrolyte interface (SEI) profiles based on first-principles calculations. The achieved deep elucidation of the reversible process of K⁺ insertion and extraction on the surface/interface of the active material during the discharge and charge states clearly highlights its significance for stable K-storage. This work promotes the facile design and deep understanding of nanostructured high-capacity electrodes of transition metal phosphates for rechargeable KIBs.