In situ electrochemical APXPS analysis of ALD grown Cu catalyst for CO2 reduction

Harri Ali-Löytty, Lauri Palmolahti, Markku Hannula, Jesse Saari, Kimmo Lahtonen, Hsin-Yi Wang, Markus Soldemo, Anders Nilsson, Mika Valden

Tutkimustuotos: AbstraktiScientific

Abstrakti

The grand challenge in artificial photosynthesis is to produce liquid solar fuels from water and carbon dioxide. Unfortunately, current materials solutions for a photocatalytic (PEC) solar fuel reactor lack efficiency, selectivity towards liquid fuel products, and long-term stability. Cu based catalysts are so far the most promising materials for the carbon dioxide reduction reaction (CO2RR), whereas the selectivity of Cu catalyst towards liquid products is strongly affected by the exact chemical composition and structure. Recently, Eilert et al. suggested, based on in situ electrochemical APXPS measurements on Cu foil, that the high activity of oxide-derived copper towards CO2RR stems from subsurface oxygen that was proposed to increase the CO binding energy and thus enhance the production of methanol and multicarbon products [1]. This contradicts the alternative hypothesis that assigns the activity to Cu2O on the surface, albeit no copper oxide should be stable at reductive CO2RR conditions.

In this work, ALD grown Cu oxide thin film was analyzed in situ by electrochemical APXPS at the HIPPIE beamline, MAX IV Laboratory. The results, highlighted in Figure 1, show similar oxygen species on reduced ALD Cu oxide thin film to what was assigned to subsurface oxygen in Ref. [1]. Therefore, the ALD grown Cu oxide thin film combined with ALD TiO2 [2–4] forms a promising catalyst coating for photocathodes in solar fuel cells to produce methanol and multicarbon products from carbon dioxide, water, and sunlight.

[1] A. Eilert, F. Cavalca, F.S. Roberts, J. Osterwalder, C. Liu, M. Favaro, E.J. Crumlin, H. Ogasawara, D. Friebel, L.G.M. Pettersson, A. Nilsson, J. Phys. Chem. Lett. 8 (2017) 285–290.

[2] M. Hannula, H. Ali-Löytty, K. Lahtonen, E. Sarlin, J. Saari, M. Valden, Improved Stability of Atomic Layer Deposited Amorphous TiO2 Photoelectrode Coatings by Thermally Induced Oxygen Defects, Chem. Mater. 30 (2018) 1199–1208.

[3] M. Hannula, H. Ali-Löytty, K. Lahtonen, J. Saari, A. Tukiainen, M. Valden, Highly efficient charge separation in model Z-scheme TiO2/TiSi2/Si photoanode by micropatterned titanium silicide interlayer, Acta Mater. 174 (2019) 237–245.

[4] H. Ali-Löytty, M. Hannula, J. Saari, L. Palmolahti, B.D. Bhuskute, R. Ulkuniemi, T. Nyyssönen, K. Lahtonen, M. Valden, Diversity of TiO2: Controlling the Molecular and Electronic Structure of Atomic-Layer-Deposited Black TiO2, ACS Appl. Mater. Interfaces. 11 (2019) 2758–2762.
AlkuperäiskieliEnglanti
TilaJulkaistu - 29 kesäk. 2020
OKM-julkaisutyyppiEi OKM-tyyppiä
TapahtumaThe AVS 20th International Conference on Atomic Layer Deposition (ALD 2020)/the 7th International Atomic Layer Etching Workshop (ALE 2020), ALD/ALE 2020 Virtual Meeting (2020) -
Kesto: 29 kesäk. 20201 heinäk. 2020
https://ald2020.avs.org/

Conference

ConferenceThe AVS 20th International Conference on Atomic Layer Deposition (ALD 2020)/the 7th International Atomic Layer Etching Workshop (ALE 2020), ALD/ALE 2020 Virtual Meeting (2020)
Ajanjakso29/06/201/07/20
www-osoite

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