Pyridine N‐Modulated Adsorption Equilibrium of Highly Dispersed Atomic W‐P Clusters toward Advanced Potassium‐Ion Hybrid Capacitors

Improving the atomic utilization of storage sites and developing isotropic transport characteristics become crucial to enhance the performance of potassium‐ion hybrid capacitors (PIHCs), and the disordered strategy and coordination modulation of the electrodes can satisfy the above structure‐activity requirements. Herein, the highly dispersed atomic W‐P clusters are chosen as a platform for the electronic restructuring. Studies and calculations indicate that replacing O in W‐O2/P2 with pyridine N can modulate the electron distribution and electronegativity, and enrich the edge‐dangling bonds of the amorphous clusters (W‐N2/P2), resulting in proper adsorption equilibrium and high affinity for K+ storage. In addition, the clusters have isotropic and bulk‐phase‐indifferent fast ion storage, and in situ protection of carbon nanosheets can provide stable support for ion storage and electron transfer in the clusters. As an anode, the composite (W‐N/P@C) exhibits superior storage properties of K+ (reversible capacity of 181.6 mAh g−1 after 3000 cycles at 5.0 A g−1), with high energy density (163.7 Wh Kg−1) at the high‐power output (3500 W Kg−1) in PIHCs. This work systematically delineates the effects of disordered design and pyridine N‐coordination on energy storage, and provides new research ideas for studying high‐performance PIHCs. Disordered strategy and coordination modulation of electrodes can satisfy the structure‐activity requirements of potassium‐ion hybrid capacitors (PIHCs). Herein, N‐coordinated atomic W‐P clusters are uniformly encapsulated in N‐doped carbon nanosheets (W‐N/P@C). Pyridine N‐modulation optimizes the adsorption equilibrium and K+ affinity of the clusters. W‐N/P@C exhibits superior storage properties, as well as high energy density and high‐power output in PIHCs.