Mesoporous CuFe 2 O 4 Photoanodes for Solar Water Oxidation: Impact of Surface Morphology on the Photoelectrochemical Properties**

Einert, Marcus; Waheed, Arslan; Moritz, Dominik C.; Lauterbach, Stefan; Kundmann, Anna; Daemi, Sahar; Schlaad, Helmut; Osterloh, Frank E.; Hofmann, Jan P.

doi:10.1002/chem.202300277

Title: Mesoporous CuFe ₂ O ₄ Photoanodes for Solar Water Oxidation: Impact of Surface Morphology on the Photoelectrochemical Properties**

Journal Article · Tue Mar 14 00:00:00 EDT 2023 · Chemistry - A European Journal

DOI:https://doi.org/10.1002/chem.202300277· OSTI ID:1961487

^[1]; Waheed, Arslan ^[1];

^[1]; Lauterbach, Stefan ^[2];

^[3]; Daemi, Sahar ^[3]; Schlaad, Helmut ^[4];

^[3];

^[1]

Department of Materials and Earth Sciences Surface Science Laboratory Technical University of Darmstadt Otto-Bernd-Strasse 3 63287 Darmstadt Germany
Institute for Applied Geosciences Geomaterial Science Technical University of Darmstadt Schnittspahnstrasse 9 64287 Darmstadt Germany
Department of Chemistry University of California One Shields Avenue Davis, CA 95616 USA
Institute of Chemistry University of Potsdam Karl-Liebknecht-Strasse 24–25 14476 Potsdam Germany

Abstract Metal oxide‐based photoelectrodes for solar water splitting often utilize nanostructures to increase the solid‐liquid interface area. This reduces charge transport distances and increases the photocurrent for materials with short minority charge carrier diffusion lengths. While the merits of nanostructuring are well established, the effect of surface order on the photocurrent and carrier recombination has not yet received much attention in the literature. To evaluate the impact of pore ordering on the photoelectrochemical properties, mesoporous CuFe ₂ O ₄ (CFO) thin film photoanodes were prepared by dip‐coating and soft‐templating. Here, the pore order and geometry can be controlled by addition of copolymer surfactants poly(ethylene oxide)‐ block ‐poly(propylene oxide)‐ block ‐poly(ethylene oxide) (Pluronic® F‐127), polyisobutylene‐ block ‐poly(ethylene oxide) (PIB‐PEO) and poly(ethylene‐ co ‐butylene)‐ block ‐poly(ethylene oxide) (Kraton liquid™‐PEO, KLE). The non‐ordered CFO showed the highest photocurrent density of 0.2 mA/cm ² at 1.3 V vs. RHE for sulfite oxidation, but the least photocurrent density for water oxidation. Conversely, the ordered CFO presented the best photoelectrochemical water oxidation performance. These differences can be understood on the basis of the high surface area, which promotes hole transfer to sulfite (a fast hole acceptor), but retards oxidation of water (a slow hole acceptor) due to electron‐hole recombination at the defective surface. This interpretation is confirmed by intensity‐modulated photocurrent (IMPS) and vibrating Kelvin probe surface photovoltage spectroscopy (VKP‐SPS). The lowest surface recombination rate was observed for the ordered KLE‐based mesoporous CFO, which retains spherical pore shapes at the surface resulting in fewer surface defects. Overall, this work shows that the photoelectrochemical energy conversion efficiency of copper ferrite thin films is not just controlled by the surface area, but also by surface order.

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Research Organization:: Univ. of California, Davis, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: DOE-SC0015329; SC0015329

OSTI ID:: 1961487

Alternate ID(s):: OSTI ID: 1971569; OSTI ID: 2000439

Journal Information:: Chemistry - A European Journal, Journal Name: Chemistry - A European Journal Vol. 29 Journal Issue: 24; ISSN 0947-6539

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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solgel
water oxidation

Title: Mesoporous CuFe 2 O 4 Photoanodes for Solar Water Oxidation: Impact of Surface Morphology on the Photoelectrochemical Properties**

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Title: Mesoporous CuFe ₂ O ₄ Photoanodes for Solar Water Oxidation: Impact of Surface Morphology on the Photoelectrochemical Properties**