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

Directional charge transfer among nanolayers of graphitic carbon nitride (g‐C3N4) 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‐C3N4 nanosheets into carbon nitride square tubes (C3N4Ts), and Ni2P nanoparticles as electron acceptors are loaded on C3N4Ts (Ni2P/C3N4Ts) for highly efficient H2 evolution. Study results present H2‐evolution efficiency over the constructed Ni2P/C3N4Ts up to 19.25 mmol g−1 h−1 with a large number of visible H2 bubbles, which is more than 1.9 and 2.6 times of that over g‐C3N4 supported 1 wt%Pt and 3 wt%Pd, respectively. Density functional theory (DFT) and characterizations reveal efficient directional transfer through C3N4T interlayer (001) to Ni2P (111) is achieved under the apparent potential difference of C3N4Ts, which therefore ensures the high H2‐evolution performance of Ni2P/C3N4Ts. 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. An apparent potential difference among nanolayers of g‐C3N4 nanosheets is introduced to boost interlayer electron transfer by curving planar g‐C3N4 into carbon nitride square tubes, and Ni2P nanoparticles as electron acceptors are loaded on C3N4Ts for efficient H2 evolution with a large number of visible H2 bubbles.