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An Atomically Dispe...
An Atomically Dispersed Mn-Photocatalyst for Generating Hydrogen Peroxide from Seawater via the Water Oxidation Reaction (WOR)
- Article/chapterEnglish2023
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LIBRIS-ID:oai:DiVA.org:su-221350
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https://urn.kb.se/resolve?urn=urn:nbn:se:su:diva-221350URI
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https://doi.org/10.1021/jacs.3c03785DOI
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Language:English
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Summary in:English
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Subject category:ref swepub-contenttype
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Subject category:art swepub-publicationtype
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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.
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Zhang, Tong
(author)
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Jain, Noopur
(author)
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Ching, H. Y. Vincent
(author)
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Jaworski, Aleksander,1986-Stockholms universitet,Avdelningen för fysikalisk kemi(Swepub:su)ajawo
(author)
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Barcaro, Giovanni
(author)
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Monti, Susanna
(author)
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Silvestre-Albero, Joaquin
(author)
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Celorrio, Veronica
(author)
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Chouhan, Lata
(author)
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Rokicinska, Anna
(author)
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Debroye, Elke
(author)
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Kustrowski, Piotr
(author)
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Van Doorslaer, Sabine
(author)
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Van Aert, Sandra
(author)
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Bals, Sara
(author)
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Das, Shoubhik
(author)
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Stockholms universitetAvdelningen för fysikalisk kemi
(creator_code:org_t)
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In:Journal of the American Chemical Society145:30, s. 16584-165960002-78631520-5126
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Ren, Peng
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Zhang, Tong
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Jain, Noopur
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Ching, H. Y. Vin ...
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Jaworski, Aleksa ...
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Barcaro, Giovann ...
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Monti, Susanna
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Silvestre-Albero ...
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Celorrio, Veroni ...
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Chouhan, Lata
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Rokicinska, Anna
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Debroye, Elke
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Kustrowski, Piot ...
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Van Doorslaer, S ...
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Van Aert, Sandra
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Bals, Sara
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Das, Shoubhik
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- NATURAL SCIENCES
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NATURAL SCIENCES
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Stockholm University