Transition-Metal Single Atom Anchored on MoS2 for Enhancing Photocatalytic Hydrogen Production of g-C3N4 Photocatalysts

Single-atom catalyst technology with near-100% atomicutilizationand a well-defined coordination structure has provided new ideas fordesigning high-performance photocatalysts, which is also beneficialfor reducing the usage of noble metal cocatalysts. Herein, a seriesof single-atomic MoS2-based cocatalysts where monoatomicRu, Co, or Ni modify MoS2 (SA-MoS2) for enhancingthe photocatalytic hydrogen production performance of g-C3N4 nanosheets (NSs) are rationally designed and synthesized.The 2D SA-MoS2/g-C3N4 photocatalystswith Ru, Co, or Ni single atoms show similar enhanced photocatalyticactivity, and the optimized Ru-1-MoS2/g-C3N4 photocatalyst has the highest hydrogen productionrate of 11115 mu mol/h/g, which is about 37 and 5 times higherthan that of pure g-C3N4 and MoS2/g-C3N4 photocatalysts, respectively. Experimentaland density functional theory calculation results reveal that theenhanced photocatalytic performance is mainly attributed to the synergisticeffect and intimate interface between SA-MoS2 with well-definedcoordination single-atomic structures and g-C3N4 NSs, which is conducive to the rapid interfacial charge transport,and the unique single-atomic structure of SA-MoS2 withmodified electronic structure and appropriate hydrogen adsorptionperformance offers abundant reactive sites for enhancing the photocatalytichydrogen production performance. This work provides new insight intoimproving the cocatalytic hydrogen production performance of MoS2 by a single-atomic strategy.