A universal strategy is developed to construct a cascade Z‐Scheme system, in which an effective energy platform is the core to direct charge transfer and separation, blocking the unexpected type‐II charge transfer pathway. The dimension‐matched (001)TiO2‐g‐C3N4/BiVO4 nanosheet heterojunction (T‐CN/BVNS) is the first such model. The optimized cascade Z‐Scheme exhibits ≈19‐fold photoactivity improvement for CO2 reduction to CO in the absence of cocatalysts and costly sacrificial agents under visible‐light irradiation, compared with BVNS, which is also superior to other reported Z‐Scheme systems even with noble metals as mediators. The experimental results and DFT calculations based on van der Waals structural models on the ultrafast timescale reveal that the introduced T as the platform prolongs the lifetimes of spatially separated electrons and holes and does not compromise their reduction and oxidation potentials.

Die rationale Entwicklung effizienter Photokatalysatoren mit günstiger Ladungstrennung und breiter spektraler Absorption ist entscheidend für eine ökonomische Umwandlung von Solarenergie in chemische Energie. F. Q. Bai, J. Tang, L. Q. Jing et al. zeigen in ihrer Zuschrift auf S. 10989 H‐verbrückte ZnPc/BiVO4‐Nanokomposite als ultradünnen, räumlich angepassten 2D/2D‐Heteroübergang zur effizienten photokatalytischen CO2‐Reduktion über eine breite Region des sichtbaren Lichts.

Cascade charge transfer was realized by aH -bond linked zinc phthalocyanine/BiVO 4 nanosheet (ZnPc/BVNS) composite,w hichs ubsequently works as an efficient widevisible-light-driven photocatalyst for converting CO 2 into CO and CH 4 ,a ss hown by product analysis and 13 Ci sotopic measurement. The optimizedZ nPc/BVNS nanocomposite exhibits ac a. 16-fold enhancement in the quantum efficiency compared with the reported BiVO 4 nanoparticles at the excitation of 520 nm with an assistance of 660 nm photons. Experimental and theoretical results showt he exceptional activities are attributed to the rapid charge separation by acascade Z-scheme charge transfer mechanismformed by the dimension-matched ultrathin (ca. 8nm) heterojunction nanostructure.T he central Zn 2+ in ZnPc could accept the excited electrons from the ligand and then provideacatalytic function for CO 2 reduction. This Z-scheme is also feasible for other MPc,s uch as FePc and CoPc, together with BVNS.

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Graphene-modulated ZnPc/BiVO4 Z-scheme heterojunctions for efficient visible-light catalytic CO2 conversion are achieved by increasing the optimized amount of highly dispersed ZnPc.