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Conversion-type transition-metal phosphide anode materials with high theoretical capacity usually suffer from low-rate capability and severe capacity decay, which are mainly caused by their inferior electronic conductivities and large volumetric variations together with the poor reversibility of discharge product (Li3P), impeding their practical applications. Herein, guided by density functional theory calculations, these obstacles are simultaneously mitigated by confining amorphous FeP nanoparticles into ultrathin 3D interconnected P-doped porous carbon nanosheets (denoted as FeP@CNs) via a facile approach, forming an intriguing 3D flake-CNs-like configuration. As an anode for lithium-ion batteries (LIBs), the resulting FeP@CNs electrode not only reaches a high reversible capacity (837 mA h g-1 after 300 cycles at 0.2 A g-1) and an exceptional rate capability (403 mA h g-1 at 16 A g-1) but also exhibits extraordinary durability (2500 cycles, 563 mA h g-1 at 4 A g-1, 98% capacity retention). By combining DFT calculations, in situ transmission electron microscopy, and a suite of ex situ microscopic and spectroscopic techniques, we show that the superior performances of FeP@CNs anode originate from its prominent structural and compositional merits, which render fast electron/ion-transport kinetics and abundant active sites (amorphous FeP nanoparticles and structural defects in P-doped CNs) for charge storage, promote the reversibility of conversion reactions, and buffer the volume variations while preventing pulverization/aggregation of FeP during cycling, thus enabling a high rate and highly durable lithium storage. Furthermore, a full cell composed of the prelithiated FeP@CNs anode and commercial LiFePO4 cathode exhibits impressive rate performance while maintaining superior cycling stability. This work fundamentally and experimentally presents a facile and effective structural engineering strategy for markedly improving the performance of conversion-type anodes for

Conversion-type transition-metal phosphide anode materials with high theoretical capacity usually suffer from low-rate capability and severe capacity decay, which are mainly caused by their inferior electronic conductivities and large volumetric variations together with the poor reversibility of discharge product (Li3P), impeding their practical applications. Herein, guided by density functional theory calculations, these obstacles are simultaneously mitigated by confining amorphous FeP nanoparticles into ultrathin 3D interconnected P-doped porous carbon nanosheets (denoted as FeP@CNs) via a facile approach, forming an intriguing 3D flake-CNs-like configuration. As an anode for lithium-ion batteries (LIBs), the resulting FeP@CNs electrode not only reaches a high reversible capacity (837 mA h g-1 after 300 cycles at 0.2 A g-1) and an exceptional rate capability (403 mA h g-1 at 16 A g-1) but also exhibits extraordinary durability (2500 cycles, 563 mA h g-1 at 4 A g-1, 98% capacity retention). By combining DFT calculations, in situ transmission electron microscopy, and a suite of ex situ microscopic and spectroscopic techniques, we show that the superior performances of FeP@CNs anode originate from its prominent structural and compositional merits, which render fast electron/ion-transport kinetics and abundant active sites (amorphous FeP nanoparticles and structural defects in P-doped CNs) for charge storage, promote the reversibility of conversion reactions, and buffer the volume variations while preventing pulverization/aggregation of FeP during cycling, thus enabling a high rate and highly durable lithium storage. Furthermore, a full cell composed of the prelithiated FeP@CNs anode and commercial LiFePO4 cathode exhibits impressive rate performance while maintaining superior cycling stability. This work fundamentally and experimentally presents a facile and effective structural engineering strategy for markedly improving the performance of conversion-type anodes for