An Atomically Dispersed Mn-Photocatalyst for Generating Hydrogen Peroxide from Seawater via the Water Oxidation Reaction (WOR)

In this work, we have fabricatedan aryl amino-substitutedgraphiticcarbon nitride (g-C3N4) catalyst with atomicallydispersed Mn capable of generating hydrogen peroxide (H2O2) directly from seawater. This new catalyst exhibitedexcellent reactivity, obtaining up to 2230 & mu;M H2O2 in 7 h from alkaline water and up to 1800 & mu;Mfrom seawater under identical conditions. More importantly, the catalystwas quickly recovered for subsequent reuse without appreciable lossin performance. Interestingly, unlike the usual two-electron oxygenreduction reaction pathway, the generation of H2O2 was through a less common two-electron water oxidation reaction(WOR) process in which both the direct and indirect WOR processesoccurred; namely, photoinduced h(+) directly oxidized H2O to H2O2 via a one-step 2e(-) WOR, and photoinduced h(+) first oxidized a hydroxide (OH-) ion to generate a hydroxy radical ((OH)-O-& BULL;), and H2O2 was formed indirectly by thecombination of two (OH)-O-& BULL;. We have characterized thematerial, at the catalytic sites, at the atomic level using electronparamagnetic resonance, X-ray absorption near edge structure, extendedX-ray absorption fine structure, high-resolution transmission electronmicroscopy, X-ray photoelectron spectroscopy, magic-angle spinningsolid-state NMR spectroscopy, and multiscale molecular modeling, combiningclassical reactive molecular dynamics simulations and quantum chemistrycalculations.

Zhang, Tong (author)
Jain, Noopur (author)
Ching, H. Y. Vincent (author)
Jaworski, Aleksander,1986-Stockholms universitet,Avdelningen för fysikalisk kemi(Swepub:su)ajawo (author)
Barcaro, Giovanni (author)
Monti, Susanna (author)
Silvestre-Albero, Joaquin (author)
Celorrio, Veronica (author)
Chouhan, Lata (author)
Rokicinska, Anna (author)
Debroye, Elke (author)
Kustrowski, Piotr (author)
Van Doorslaer, Sabine (author)
Van Aert, Sandra (author)
Bals, Sara (author)
Das, Shoubhik (author)
Stockholms universitetAvdelningen för fysikalisk kemi (creator_code:org_t)

In:Journal of the American Chemical Society145:30, s. 16584-165960002-78631520-5126

By the author/editor: Ren, Peng; Zhang, Tong; Jain, Noopur; Ching, H. Y. Vin ...; Jaworski, Aleksa ...; Barcaro, Giovann ...; show more...; Monti, Susanna; Silvestre-Albero ...; Celorrio, Veroni ...; Chouhan, Lata; Rokicinska, Anna; Debroye, Elke; Kustrowski, Piot ...; Van Doorslaer, S ...; Van Aert, Sandra; Bals, Sara; Das, Shoubhik; show less...

About the subject

NATURAL SCIENCES: NATURAL SCIENCES; and Chemical Science ...; and Physical Chemist ...

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