BioChem - DOS

Iron oxide-promoted photochemical oxygen reduction to hydrogen peroxide (H2O2)

EES catalysis

Freese, Thomas; Meijer, Jelmer T.; Brands, Maria B.; Alachouzos, Georgios; Stuart, Marc C. A.; Tarozo, Rafael; Gerlach, Dominic; Smits, Joost; Rudolf, Petra; Reek, Joost N. H.; Feringa, Ben L.

<▼1><P>Hydrogen peroxide (H<SUB>2</SUB>O<SUB>2</SUB>) is a valuable green oxidant with a wide range of applications. Furthermore, it is recognized as a possible future energy carrier achieving safe operation, storage and transportation. The photochemical production of H<SUB>2</SUB>O<SUB>2</SUB> serves as a promising alternative to the waste- and energy-intensive anthraquinone process. Following the 12 principles of Green Chemistry, we demonstrate a facile and general approach to sustainable catalyst development utilizing earth-abundant iron and biobased sources only. We developed several iron oxide (FeO<SUB><I>x</I></SUB>) nanoparticles (NPs) for successful photochemical oxygen reduction to H<SUB>2</SUB>O<SUB>2</SUB> under visible light illumination (445 nm). Achieving a selectivity for H<SUB>2</SUB>O<SUB>2</SUB> of >99%, the catalyst material could be recycled for up to four consecutive rounds. An apparent quantum yield (AQY) of 0.11% was achieved for the photochemical oxygen reduction to H<SUB>2</SUB>O<SUB>2</SUB> with visible light (445 nm) at ambient temperatures and pressures (9.4&#x2013;14.8 mmol g<SUP>&#x2212;1</SUP> L<SUP>&#x2212;1</SUP>). Reaching productivities of H<SUB>2</SUB>O<SUB>2</SUB> of at least 1.7 ± 0.3 mmol g<SUP>&#x2212;1</SUP> L<SUP>&#x2212;1</SUP> h<SUP>&#x2212;1</SUP>, production of H<SUB>2</SUB>O<SUB>2</SUB> was further possible <I>via</I> sunlight irradiation and in seawater. Finally, a detailed mechanism has been proposed on the basis of experimental investigation of the catalyst's properties and computational results.</P></▼1><▼2><P>A sustainable catalyst development utilizing earth-abundant iron oxide (FeO<SUB><I>x</I></SUB>) nanoparticles for photochemical oxygen reduction to hydrogen peroxide (H<SUB>2</SUB>O<SUB>2</SUB>) was achieved, generating a valuable green oxidant and future energy carrier.</P></▼2>

2024

RSC

2753-801x

2

1

pp.262-275

10.1039/d3ey00256j

http://click.ndsl.kr/servlet/OpenAPIDetailView?keyValue=05787966&target=NART&cn=NART128388492