Promoting Photocatalytic Hydrogen Evolution Activity of Graphitic Carbon Nitride with Hole-Transfer Agents.

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作者:Indra Arindam, Beltrán-Suito Rodrigo, Müller Marco, Sivasankaran Ramesh P, Schwarze Michael, Acharjya Amitava, Pradhan Bapi, Hofkens Johan, Brückner Angelika, Thomas Arne, Menezes Prashanth W, Driess Matthias
Visible light-driven photocatalytic reduction of protons to H(2) is considered a promising way of solar-to-chemical energy conversion. Effective transfer of the photogenerated electrons and holes to the surface of the photocatalyst by minimizing their recombination is essential for achieving a high photocatalytic activity. In general, a sacrificial electron donor is used as a hole scavenger to remove photogenerated holes from the valence band for the continuation of the photocatalytic hydrogen (H(2) ) evolution process. Here, for the first time, the hole-transfer dynamics from Pt-loaded sol-gel-prepared graphitic carbon nitride (Pt-sg-CN) photocatalyst were investigated using different adsorbed hole acceptors along with a sacrificial agent (ascorbic acid). A significant increment (4.84†times) in H(2) production was achieved by employing phenothiazine (PTZ) as the hole acceptor with continuous H(2) production for 3†days. A detailed charge-transfer dynamic of the photocatalytic process in the presence of the hole acceptors was examined by time-resolved photoluminescence and in†situ electron paramagnetic resonance studies.

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