Photocatalytic oxygen reduction to hydrogen peroxide over copper doped graphitic carbon nitride hollow microsphere: The effect of Cu(I)-N active sites

Add time:08/20/2019    Source:sciencedirect.com

H2O2 is produced industrially by the anthraquinone method, in which energy consumption is high because of its multistep hydrogenation and oxidation reactions. In this work, hollow copper-doped graphitic carbon nitride (g-C3N4) microspheres with outstanding photocatalytic H2O2 production ability are prepared. The characterization results demonstrate that Cu+ is not present as the oxide but instead inserts at the interstitial position through coordinative Cu(I)-N bonds. These Cu(I)-N active sites can act as chemical adsorption sites to activate molecular O2. Moreover, as an “electron transfer bridge”, Cu(I)-N active sites promote electron transfer from the catalyst to the adsorbed O2 molecules. The as-prepared copper-doped g-C3N4 displays much higher H2O2 equilibrium concentration and formation rate than neat g-C3N4 prepared by calcination does, as well as excellent structural stability. Density functional theory simulations show that Cu(I)-N active sites can adsorb the O2 molecules with high adsorption energy and elongate the OO bond. Charge density difference results confirm the electron transfer from the Cu+ doping sites to the O2 molecules. The Mulliken charge is −0.51 when the O2 adsorbed on Cu+ doping sites. This electron-rich environment is beneficial to the H+ attack to form H2O2.

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