Direct Z-scheme designs perform well in light-to-fuel conversion. Here, an active and stable ternary Z-scheme core-shell heterojunction for photocatalytic hydrogen evolution (PHE) is fabricated consisting of hexagonal 2D α-Fe₂O₃ (as photocatalyst II) and 2D nitrogen-doped graphene (NGr as photocatalyst I) functionalized with the Pt single-atoms (SAs) cocatalyst. Under visible light, the 2D/2D α-Fe₂O₃ @NGr₃Pt_SAs (NGr shell thickness of 3 nm and Pt loading of 0.5 wt%) achieves a remarkable PHE of 6.4 µmol ${\mathrm{mg}}_{\mathrm{cat}}^{-1}$ h^–1, which is 16.4- and 3.28-times higher than those of free NGr (0.39 µmol ${\mathrm{mg}}_{\mathrm{cat}}^{-1}$ h^–1) and binary α-Fe₂O₃ @NGr₃ (1.95 µmol ${\mathrm{mg}}_{\mathrm{cat}}^{-1}$ h^–1), thus outperforming the currently-advanced PHE catalysts. The outstanding performance is due to the superiority of a direct 2D/2D Z-scheme core-shell fabrication, including a large surface area for light harvesting, facile charge separation and transfer, and the workability of Pt SAs sites. Theoretical investigations provide additional insight into the mechanistic process of the ternary system for PHE reactions.

直接 Z 方案设计在光燃料转换中表现良好。在这里，制备了一种用于光催化析氢 (PHE) 的活性稳定的三元 Z 型核壳异质结，由六方二维 α-Fe 2 O 3（作为光催化剂 II）和_二维氮_掺杂石墨烯（NGr 作为光催化剂 I）组成用 Pt 单原子 (SAs) 助催化剂功能化。在可见光下，2D/2D α-Fe ₂ O ₃ @NGr ₃ Pt _SAs（NGr 壳厚度为 3 nm，Pt 负载量为 0.5 wt%）实现了 6.4 µmol 的显着 PHE${\mathrm{毫克}}_{\mathrm{猫}}^{-\mathrm{1个}}$h ^–1，比游离 NGr (0.39 µmol) 高 16.4 和 3.28 倍${\mathrm{毫克}}_{\mathrm{猫}}^{-\mathrm{1个}}$h ^–1 ) 和二元α-Fe ₂ O ₃ @NGr ₃ (1.95 µmol${\mathrm{毫克}}_{\mathrm{猫}}^{-\mathrm{1个}}$h ^–1 )，因此优于目前先进的 PHE 催化剂。出色的性能归功于直接 2D/2D Z 型核壳制造的优越性，包括用于光收集的大表面积、简便的电荷分离和转移以及 Pt SAs 位点的可加工性。理论研究为 PHE 反应的三元系统的机理过程提供了额外的见解。