Boosting Visible-Light-Driven H2 Evolution of Covalent Triazine Framework from Water by Modifying Ni(II) Pyrimidine-2-thiolate Cocatalyst

Covalent triazine frameworks (CTFs) have recently emerged as prospective photoactive materials coupled with Pt or Pd cocatalyst for the hydrogen evolution. Herein, we report visible-light driven hydrogen generation catalyzed by heterogeneous systems combining CTF photosensitizers and a noble-metal-free cocatalyst for the first time. CTF-HC2 was doped with two-dimensional Ni(II) pyrimidine-2-thiolate ([Ni(pymt)(2)](n)) to yield a series of x-[Ni(pymt)(2)](n)/CTF-HC2 (x=3, 6, 9, 12, 15, 18 and 24 wt %) composites. Illuminated with lambda>420 nm, [Ni(pymt)(2)](n)/CTF-HC2 materials display excellent photocatalytic performance for H-2 generation from water. The highest hydrogen evolution rate is up to 3472 mu mol h(-1) g(-1), which is 68 times of bare CTF-HC2 (51 mu mol h(-1) g(-1)) and 1.16 times of CTF-HC2 doped 2.0 wt % Pt (2991 mu mol h(-1) g(-1)). The efficient and recyclable heterogeneous photocatalytic H-2 production from water under visible light has been established.

Automated summary

The study presents a novel visible-light driven hydrogen generation method utilizing CTF photosensitizers and noble-metal-free cocatalysts. Composite materials prepared by dopant Ni and pyrimidine-2-thiolate in CTF-HC2 exhibit excellent photocatalytic performance for hydrogen generation, achieving high efficiency and recyclability under visible light.