Phosphorus Vacancy‐Engineered Ultrathin RuP Nanosheets for Accelerated and High‐Capacity N‐Ethylcarbazole Hydrogen Storage

Abstract Precisely constructing efficient and durable catalysts for liquid organic hydrogen carriers (LOHCs) is essential for large‐scale hydrogen storage and transport. In this work, we present a salt‐templated synthesis of ultrathin ruthenium phosphide nanosheets enriched with phosphorus vacancy (U‐RuPv). The catalyst exhibits remarkable catalytic performance for N‐ethylcarbazole (NEC) hydrogenation, achieving complete NEC conversion and a 98.11% yield of 12H‐NEC within 1.0 h at 180 °C and 7 MPa H 2 . The enhanced activity arises from abundant phosphorus vacancies on ultrathin RuP nanosheets, which modulate the electron configuration of adjacent Ru atoms, generating electron‐rich Ru σ+ (0<σ<3) active sites that promote efficient hydrogen activation and spillover. Density functional theory (DFT) calculations reveal that these vacancies induce local charge redistribution and a downward shift in the d‐band center, facilitating hydrogen desorption and NEC activation. This work highlights a dual‐engineering approach combining ultrathin nanoarchitectures and defect chemistry to advance LOHCs catalytic performance, offering new insights for catalyst design in hydrogen storage applications.