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

Abstract

The grand challenge in artificial photosynthesis is to produce liquid solar fuels from water and carbon dioxide. Unfortunately, current materials solutions for a 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, 3] 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, and A. Nilsson, J. Phys. Chem. Lett. 8, 285–290 (2017).

[2] M. Hannula, H. Ali-Löytty, K. Lahtonen, E. Sarlin, J. Saari, and M. Valden, Chem. Mater. 30, 1199–1208 (2018).

[3] H. Ali-Löytty, M. Hannula, J. Saari, L. Palmolahti, B.D. Bhuskute, R. Ulkuniemi, T. Nyyssönen, K. Lahtonen, and M. Valden, ACS Appl. Mater. Interfaces 11, 2758–2762 (2019).

Original language	English
Publication status	Published - 25 Mar 2021
Publication type	Not Eligible
Event	Physics Days 2021 - Online Duration: 24 Mar 2021 → 26 Mar 2021 https://www.jyu.fi/en/congress/physicsdays2021

Conference

Conference	Physics Days 2021
Period	24/03/21 → 26/03/21
Internet address	https://www.jyu.fi/en/congress/physicsdays2021

Cite this

@conference{44c9f83aa7404df591acccaed1b3d605,

title = "In situ electrochemical APXPS analysis of ALD grown Cu catalyst for CO2 reduction",

abstract = "The grand challenge in artificial photosynthesis is to produce liquid solar fuels from water and carbon dioxide. Unfortunately, current materials solutions for a 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, 3] 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, and A. Nilsson, J. Phys. Chem. Lett. 8, 285–290 (2017). [2] M. Hannula, H. Ali-L{\"o}ytty, K. Lahtonen, E. Sarlin, J. Saari, and M. Valden, Chem. Mater. 30, 1199–1208 (2018). [3] H. Ali-L{\"o}ytty, M. Hannula, J. Saari, L. Palmolahti, B.D. Bhuskute, R. Ulkuniemi, T. Nyyss{\"o}nen, K. Lahtonen, and M. Valden, ACS Appl. Mater. Interfaces 11, 2758–2762 (2019). ",

author = "Harri Ali-L{\"o}ytty and Lauri Palmolahti and Markku Hannula and Jesse Saari and Kimmo Lahtonen and Hsin-Yi Wang and Markus Soldemo and Anders Nilsson and Mika Valden",

year = "2021",

month = mar,

day = "25",

language = "English",

note = "Physics Days 2021 ; Conference date: 24-03-2021 Through 26-03-2021",

url = "https://www.jyu.fi/en/congress/physicsdays2021",

}

TY - CONF

T1 - In situ electrochemical APXPS analysis of ALD grown Cu catalyst for CO2 reduction

AU - Ali-Löytty, Harri

AU - Palmolahti, Lauri

AU - Hannula, Markku

AU - Saari, Jesse

AU - Lahtonen, Kimmo

AU - Wang, Hsin-Yi

AU - Soldemo, Markus

AU - Nilsson, Anders

AU - Valden, Mika

PY - 2021/3/25

Y1 - 2021/3/25

N2 - The grand challenge in artificial photosynthesis is to produce liquid solar fuels from water and carbon dioxide. Unfortunately, current materials solutions for a 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, 3] 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, and A. Nilsson, J. Phys. Chem. Lett. 8, 285–290 (2017). [2] M. Hannula, H. Ali-Löytty, K. Lahtonen, E. Sarlin, J. Saari, and M. Valden, Chem. Mater. 30, 1199–1208 (2018). [3] H. Ali-Löytty, M. Hannula, J. Saari, L. Palmolahti, B.D. Bhuskute, R. Ulkuniemi, T. Nyyssönen, K. Lahtonen, and M. Valden, ACS Appl. Mater. Interfaces 11, 2758–2762 (2019).

AB - The grand challenge in artificial photosynthesis is to produce liquid solar fuels from water and carbon dioxide. Unfortunately, current materials solutions for a 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, 3] 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, and A. Nilsson, J. Phys. Chem. Lett. 8, 285–290 (2017). [2] M. Hannula, H. Ali-Löytty, K. Lahtonen, E. Sarlin, J. Saari, and M. Valden, Chem. Mater. 30, 1199–1208 (2018). [3] H. Ali-Löytty, M. Hannula, J. Saari, L. Palmolahti, B.D. Bhuskute, R. Ulkuniemi, T. Nyyssönen, K. Lahtonen, and M. Valden, ACS Appl. Mater. Interfaces 11, 2758–2762 (2019).

M3 - Abstract

T2 - Physics Days 2021

Y2 - 24 March 2021 through 26 March 2021

ER -

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

Abstract

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