2D/2D BOB/CN is applied for NFA degradation for the first time with high efficiency and stability, and the charge separation mechanism is demonstrated by EPR, in situ XPS and theoretical calculations.

Regulating bulk polymeric carbon nitride (PCN) into nanostructured PCN has long been proven effective in enhancing its photocatalytic activity. However, simplifying the synthesis of nanostructured PCN remains a considerable challenge and has drawn widespread attention. This work reported the one-step green and sustainable synthesis of nanostructured PCN in the direct thermal polymerization of the guanidine thiocyanate precursor via the judicious introduction of hot water vapor’s dual function as gas-bubble templates along with a green etching reagent. By optimizing the temperature of the water vapor and polymerization reaction time, the as-prepared nanostructured PCN exhibited a highly boosted visible-light-driven photocatalytic hydrogen evolution activity. The highest H₂ evolution rate achieved was 4.81mmol∙g⁻¹∙h⁻¹, which is over four times larger than that of the bulk PCN (1.19 mmol∙g⁻¹∙h⁻¹) prepared only by thermal polymerization of the guanidine thiocyanate precursor without the assistance of bifunctional hot water vapor. The enhanced photocatalytic activity might be attributed to the enlarged BET specific surface area, increased active site quantity, and highly accelerated photo-excited charge-carrier transfer and separation. Moreover, the sustainability of this environmentally friendly hot water vapor dual-function mediated method was also shown to be versatile in preparing other nanostructured PCN photocatalysts derived from other precursors such as dicyandiamide and melamine. This work is expected to provide a novel pathway for exploring the rational design of nanostructured PCN for highly efficient solar energy conversion.

Precise regulation and control solar-light-driven charges photoexcited on photocatalysts for separation-transfer and target redox reactions is an attractive and challenging pathway toward sustainability. Herein, 0D/2D-3D Pt/In₂S₃ Schottky junction was fabricated for simultaneous selective phenylcarbinol conversion into value-added aldehydes and production of clean energy H₂ by directly utilizing photoexcited holes and electrons in one reaction system under mild reaction conditions. In contrast to pure water splitting and pure In₂S₃, the reaction thermodynamics and kinetics of H₂ evolution on the Pt/In₂S₃ were significantly enhanced. The optimized 0.3% Pt/In₂S₃ exhibited the highest and most stable photocatalytic activity with 22.1 mmol g⁻¹ h⁻¹ of H₂ production rate and almost 100% selectivity of benzaldehyde production. Notably, this dual-function photocatalysis also exhibited superiority in contrast to sacrificial-agent H₂ evolution reactions such as lactic acid, Na₂S, methanol and triethanolamine. The turnover frequency (TOF) could reach up to ~2394 h⁻¹. The Pt clusters anchored at the electron location and strong metal-support interactions (SMSI) between Pt and In₂S₃ synergistically improved the spatial charge separation and directional transportation (~90.1% of the charge transport efficiency could be achieved over the Pt/In₂S₃ hybrid), and thus result in significant enhancement of photocatalytic H₂ evolution with simultaneous benzaldehyde production.