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Photoenzymatic catalysis is an efficient strategy for selectively converting CO 2 into valuable chemicals. However, the sluggish reaction kinetics, resulting from low visible light utilization and rapid recombination of photogenerated carriers, severely inhibit the yields of target products. Herein, we present a novel artificial photosynthesis platform of 2D/2D MXene/crystalline COF-367 heterostructure for efficient conversion of CO 2 into HCOOH. This platform is extremely sensitive to solar light (λ ≤ 750 nm), with rapid charge separation and transfer due to the well-designed abundant ultrathin 2D/2D hetero-interfaces. Remarkably, Ti 3 C 2 /COF-367 achieves an impressive yield of 83.38% for coenzyme NADH regeneration with absence of electron mediator. Furthermore, it demonstrates a cascade ultra-high production rate of HCOOH at 1.88 mmol g−1 h−1 with almost 100 % selectivity. This work represents the first example of MXene to promote charge transfer in COFs-based photoenzymatic synergistic catalytic system, and provides insights into the development of organic/inorganic hybrids for CO 2 photoreduction. [Display omitted] • First example of MXene to promote charge transfer in COFs-based photoenzymatic catalytic system. • Ultrathin highly crystalline imine-linked COF-367 nanosheets were synthesized. • Abundant ultrathin 2D/2D hetero-interfaces for rapid charge separation/transfer. • Impressive NADH regeneration yield of 83.38% without electron mediator. • Ultra-high HCOOH production rate of 1.88 mmol g−1 h−1 with high selectivity. [ABSTRACT FROM AUTHOR]

An ultrathin layered 2D/2D van der Waals heterojunction of ReS 2 /high-crystalline g-C 3 N 4 is reported to significantly improve photocatalytic H 2 production attribute to its efficient charge transport, strong visible light harvesting, and suppressed recombination of photogenerated carriers. [Display omitted] • Ultrathin layered 2D/2D van der Waals heterojunction of ReS 2 /high-crystalline g-C 3 N 4. • Efficient charge transport of highly crystalline g-C 3 N 4 by eliminating deep defects. • Strong visible light harvesting, and excellent conductivity of ReS 2 nanoflakes. • Synergistic effect of rapid charge separation and transfer in 2D/2D heterojunction. • Superior photocatalytic H 2 -evolution efficiency of 3.46 mmol g−1h−1. Fabricating efficient nanocatalysts with excellent visible light response, coupled with rapid charge separation and transfer efficiency is still the most challenge for solar-driven hydrogen (H 2) evolution. Herein, an ultrathin layered 2D/2D van der Waals heterojunction of ReS 2 /high-crystalline g-C 3 N 4 (CCN) is constructed for the first time to significantly boost photocatalytic H 2 production. The as-prepared optimized 15% ReS 2 /CCN exhibits the highest H 2 -evolution rate of 3.46 mmol g−1h−1 under visible light irradiation, a 2.7 fold enhancements over that of pristine CCN and is also much higher than ReS 2 alone. The excellent photocatalytic performance of ReS 2 /CCN is mainly attributed to the efficient charge transport of highly crystalline CCN by eliminating deep defects, the strong visible light harvesting of ReS 2 nanoflakes, as well as the synergistic effect of an ultrathin layered 2D/2D heterojunction to rapidly enable charge-separation while inhibiting the charge recombination. This work provides an efficient photocatalyst for H 2 energy production, and sheds light on fundamental insight to a rational design of photo/electro nanocatalysts or heterojunction materials toward highly efficient photocatalyst. [ABSTRACT FROM AUTHOR]