Fast-Charging MXene/TiN-Confined In2Se3 Anode with Dual Hydrogen-Bonding Synergy for High-Capacity Ammonium-Ion Storage

Adv Mater. 2025 Jun 27:e2509246. doi: 10.1002/adma.202509246. Online ahead of print.

Abstract

Aqueous ammonium-ion (NH4 +) based hybrid pseudocapacitors (NH-HPCs) integrate sustainability and cost-effectiveness, yet their cycling stability is critically challenged by sluggish NH4 + transport, particularly in MXene-based anodes. Herein, NH3-induced N-functionalization fabricates a MXene/TiN conductive substrate, enabling confined rotary hydrothermal growth of indium selenide (In2Se3) nanoparticles into an In2Se3@MXene/TiN heterostructure. Directional Ti─N bonds suppress MXene stacking and In2Se3 agglomeration while synergizing charge-redistribution-induced lattice strain with hierarchical 2-5 nm pore channels, enabling ultrafast NH4 + migration. Density functional theory (DFT) calculations confirm electron-deficient Ti sites and dual Se···H─N/Ti─N···H hydrogen bonds enhance NH4 + adsorption, where intensified charge polarization and optimized orbital hybridization boost ion storage kinetics and structural stability. The heterostructure anode delivers 1776.1 F g-1 at 1 A g-1 with 98.84% capacitance retention over 6000 cycles. In full-cell configuration (In2Se3@MXene/TiN//AC), the NH-HPC achieves 85.45 Wh kg-1 at 800 W kg-1-powering a commercial mini-fan for >4 min after 30 s charging. A modular pouch-cell version reaches 98.2 Wh kg-1 (800 W kg-1), demonstrating exceptional stability during bending/flame tests while operating light emitting diodes array (LEDs). This work highlights interfacial charge synergy in confined heterostructures for unprecedented NH4 + storage capacity and stability, advancing high-performance ammonium-ion energy storage.

Keywords: MXene; N‐functionalization; ammonium‐ion storage; indium selenide; interfacial charge synergy.