Freestanding trimetallic Fe–Co–Ni phosphide nanosheet arrays as an advanced electrode for high‐performance asymmetric supercapacitors

Transition metal phosphides hold great promise for high performance battery-type electrode materials due to their superb electrical conductivity and high theoretical capacity. Unfortunately, the electrochemical properties of single metal or bimetallic phosphides are unsatisfactory owing to their low energy density and poor cyclic stability, and one feasible approach is to introduce heteroatoms to form trimetallic phosphides. Here, novel Fe-Co-Ni-P nanosheet arrays are in situ synthesized on a flexible carbon cloth substrate via an electrodeposition method followed by a phosphorization treatment. Due to the presence of abundant redox active sites, large specific surface area with mesoporous channels, desirable electrical conductivity, modified electronic structure, and synergistic effect of Fe, Co, and Ni ions, the as-prepared Fe-Co-Ni-P electrode displays significantly enhanced electrochemical performance when compared to bimetallic phosphides Fe-Co-P and Fe-Ni-P. Remarkably, the Fe-Co-Ni-P electrode exhibits a large specific capacity of 593.0 C g-1 at 1 A g-1, exceptional rate performance (80.3% capacity retention at 20 A g-1), and good cycling stability (84.2% capacity retention after 5000cycles). Besides, an asymmetric supercapacitor device with Fe-Co-Ni-P electrode as a positive electrode and a hierarchical porous carbon as a negative electrode shows a high energy density of 57.1 Wh kg-1 at a power density of 768.5 W kg-1 as well as excellent cyclability with 88.4% of initial capacity after 10,000cycles. This work manifests that the construction of trimetallic phosphides is an effective strategy to solve the shortcomings of single or bimetallic phosphides for high-performance supercapacitors.