Photocatalytic selective H₂release from formic acid enabled by CO₂captured carbon nitride

The selective decomposition of formic acid (FA) traditionally needs to be carried out under high temperature with the noble metal-based catalysts. Meanwhile, it also encounters a separation of H₂and CO₂for pure H₂production. The photocatalytic FA dehydrogenation under mild conditions can meet a growing demand for sustainable H₂generation. Here, we reported a photocatalytic selective H₂release from FA decomposition at low temperature for pure H₂production by Pt/g-C₃N₄. Low-cost and easy-to-obtained urea was utilized to produce carbon nitride as the metal-free semiconductor photocatalyst, along with a photodeposition to obtain Pt/g-C₃N₄. The electrochemical evidences clearly demonstrate the photocatalytic activity of Pt/g-C₃N₄to produce H₂and CO₂in one-step FA decomposition. And, the impedance is the lowest under simulated solar light of 70 mW cm^-2with a faster electron transfer kinetic. Under simulated solar light, H₂production rate is up to 1.59 mmol · h^-1· g^-1for FA with concentration at 2.65 mol l^-1, 1700 000 times larger than that under visible light and 1928 times under ultraviolet (UV) light. DFT calculations further elucidate that nitrogen (N) active site at the g-C₃N₄has an excellent adsorption towards CO₂molecule capture. Then, H₂molecules are selectively released to simultaneously separate H₂and CO₂in solution. Platinum (Pt) at Pt/g-C₃N₄as the catalytic site contributes into the acceleration of H₂production.