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.
Li et al. (Tue,) studied this question.