Apparent Potential Difference Boosting Directional Electron Transfer for Full Solar Spectrum‐Irradiated Catalytic H2 Evolution

Abstract Directional charge transfer among nanolayers of graphitic carbon nitride ( g ‐C 3 N 4 ) is still inefficient because of the interlayer electrostatic potential barrier, which tremendously restricts the utilization of charges in conversion of solar energy into fuel. Herein, an apparent potential among nanolayers is introduced to boost interlayer electron transfer by curving planar g ‐C 3 N 4 nanosheets into carbon nitride square tubes (C 3 N 4 Ts), and Ni 2 P nanoparticles as electron acceptors are loaded on C 3 N 4 Ts (Ni 2 P/C 3 N 4 Ts) for highly efficient H 2 evolution. Study results present H 2 ‐evolution efficiency over the constructed Ni 2 P/C 3 N 4 Ts up to 19.25 mmol g −1 h −1 with a large number of visible H 2 bubbles, which is more than 1.9 and 2.6 times of that over g ‐C 3 N 4 supported 1 wt%Pt and 3 wt%Pd, respectively. Density functional theory (DFT) and characterizations reveal efficient directional transfer through C 3 N 4 T interlayer (001) to Ni 2 P (111) is achieved under the apparent potential difference of C 3 N 4 Ts, which therefore ensures the high H 2 ‐evolution performance of Ni 2 P/C 3 N 4 Ts. These results in the field of material engineering supply a novel strategy to boost directional charge transfer for solar energy conversion efficiency by introducing apparent potential difference.