Rapid Charge Transfer Endowed by Heteroatom Doped Z-Scheme Van Der Waals Heterojunction for Boosting Photocatalytic Hydrogen Evolution.

Constructing heterojunctions between phase interfaces represents a crucial strategy for achieving excellent photocatalytic performance, but the absence of sufficient interface driving force and limited charge transfer pathway leads to unsatisfactory charge separation processes. Herein, a doping-engineering strategy is introduced to construct a In─N bond-bridged InS nanocluster modified S doped carbon nitride (CN) nanosheets Z-Scheme van der Waals (VDW) heterojunctions (InS/CNS) photocatalyst, and the preparation process just by one-step pyrolysis using the pre-coordination confinement method. Specifically, S atoms doping enhances the bond strength of In─N and forms high-quality interfacial In─N linkage which serves as the atomic-level interfacial "highway" for improving the interfacial electrons migration, decreasing the charge recombination probability.

Design of a Single-Atom In-N-S site to Modulate Exciton Behavior in Carbon Nitride for Enhanced Photocatalytic Performance.

Rational tailoring of the local coordination environment of single atoms has demonstrated a significant impact on the electronic state and catalytic performance, but the development of catalysts beyond noble/transition metals is profoundly significant and highly desired. Herein, the main-group metal indium (In) single atom is immobilized on sulfur-doped porous carbon nitride nanosheets (In@CNS) in the form of three nitrogen atoms coordinated with one sulfur atom (In-N-S). Both theoretical calculations and advanced characterization investigations clearly elucidated that the single-atomic In-N-S structures on In@CNS are powerful in promoting the dissociation of excitons into more free carriers as well as the charge separation, synergistically elevating electron concentration by 2.