Installation talk at Aalto University by Prof. Riikka Puurunen
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This document summarizes the history and development of atomic layer deposition (ALD) and its applications in catalysis. It discusses key milestones in ALD including early work in 1974 and patents in 1990. It also examines using ALD to engineer catalysts by depositing thin films on high surface area powders. Experimental results are presented on optimizing the location of zinc promoters deposited by ALD to improve methanol production from carbon dioxide hydrogenation.
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Installation talk at Aalto University by Prof. Riikka Puurunen
- 1. Catalysis meets atomic layer deposition (ALD) Riikka Puurunen 0 2 4 6 8 10 12 1 2 3 CO 2 conversion, % a Zr Zn/Zr Cu/Zr Zn/Cu/Zr Cu/Zn/Zr Zn/Cu/Zn/Zr 450 K 500 K 550 K No measured activity STY methanol
- 2. Riikka Puurunen, Aalto University, 26.10.2022 Catalyst: “makes things happen” Catalysis, 1835 (Greek) 𝜅𝛼𝜏𝛼´ (down) 𝜆𝜐𝜎𝜄𝜍´ (solution, loosening) Berzelius, 1779-1848
- 3. Riikka Puurunen, Aalto University, 26.10.2022 Catalysis and catalysts: examples Fe, promoters (K) Pt, Pd, Rh, CeO2-x nitrogen hydrogen ammonia (“fixed nitrogen”)
- 4. Riikka Puurunen, Aalto University, 26.10.2022 What is ALD? Van Ommen, Goulas, Puurunen, “Atomic layer deposition” in Kirk-Othmer Encyclopedia of Chemical Technology, 2021, https://doi.org/10.1002/0471238 961.koe00059 Wikimedia Commons Growth per cycle (GPC) Based on repeated self- terminating reactions
- 5. Riikka Puurunen, Aalto University, 26.10.2022 ALD: selected milestones 1974 Atomic layer epitaxy (ALE) patent 1974-11-29 “framework hypothesis” → 1965 “molecular layering” 1965 1983 ALE-electroluminescent display demonstrator * 1990: International conference on atomic layer epitaxy (knowledge of molecular layering) 1990 ALE catalyst patent 1990-01-16 1990* 2018 Millennium Technology Prize Dr. Tuomo Suntola 2013**** 2018 vph-ald.com **** 2013 Virtual Project on the History of ALD 2007 ALD MOSFET with “high-k” to production, Intel 2001** *** 2005 J. Appl. Phys. Review (Puurunen) ** 2001: International conference series on “atomic layer deposition” 2005*** Essays: on ALE:Chem. Vap. Deposition 20 (2014) 332-344.; on ML: Chem. Vap. Deposition 21 (2015) 216-240.
- 6. Riikka Puurunen, Aalto University, 26.10.2022 Active ALD process development 2010 2022 Puurunen, J. App. Phys. 97 (2005) 121301. https://doi.org/10.1063/1.1940727 Miikkulainen, Leskelä, Ritala, Puurunen, J. Appl. Phys. 113 (2013) 021301. https://doi.org/10.1063/1.4757907 https://www.atomiclimits.com/alddatabase/, accessed 2022-10-19.
- 7. Riikka Puurunen, Aalto University, 26.10.2022 ALD for microelectronics & heterogeneous catalysts: 3-D ~seconds ~minutes, hours Area ~ 10-1 m2 Area ~ 103 m2 Conformal film? e.g. 100 m2/g Microelectronics: wafers Catalysts: powders Time Amount adsorbed ideal ALD + non-ideal continuous component “fast” “slow” Uniformly distributed species?
- 8. Riikka Puurunen, Aalto University, 26.10.2022 Case 1: ALD conformality modelling Yim, Verkama et al. Phys. Chem. Chem. Phys. 24 (2022) 8645-8660. https://doi.org/10.1039/D1CP04758B Ylilammi, Ylivaara, Puurunen, J. Appl. Phys. 123 (2018) 205301; DOI:10.1063/1.5028178 GPC pillarhall.com
- 9. Riikka Puurunen, Aalto University, 26.10.2022 Case 2: CO2 hydrogenation to methanol Effect of Zn promoter location (ALD) Support - ZrO2 Cu/ZnO/Zr ZnO/Cu/Zr ZnO/Zr Cu/Zr ZnO/Cu/ZnO/Zr ZnO (by ALD) Cu (by impregnation) Arandia et al., Appl. Catal. B, in press (2022), https://doi.org/10.1016/j.apcatb.2022.122046 0 2 4 6 8 10 12 1 2 3 CO 2 conversion, % a Zr Zn/Zr Cu/Zr Zn/Cu/Zr Cu/Zn/Zr Zn/Cu/Zn/Zr 450 K 500 K 550 K No measured activity STY methanol 0 100 200 300 425 450 475 500 525 550 575 c 0 1 2 3 4 425 450 475 500 525 550 575 b b 450 K 500 K 550 K STY methanol mmolCH3OH gCu -1h-1 mmolCH3OH gcat -1h-1 Conditions: 30 bar, H2/CO2/N2 (71/23/6, v/v/v); GHSV = 7500 h-1 0 100 200 300 425 450 475 500 525 550 575 c 0 1 2 3 4 425 450 475 500 525 550 575 b b 450 K 500 K 550 K STY methanol mmolCH3OH gCu -1h-1 mmolCH3OH gcat -1h-1 Space time yield
- 10. Riikka Puurunen, Aalto University, 26.10.2022 Future? 1. Contribute to by-catalysis- enabled green transition 2. Increase fundamental understanding of ALD More openness in science and education … Note: More ALD capacity needed!
- 11. Riikka Puurunen, Aalto University, 26.10.2022 Acknowledgements and credits https://pxhere. com/en/photo/ 1488167, CC0 https://en.wikipedia.org/wiki/ J%C3%B6ns_Jacob_Berzel ius#/media/File:J%C3%B6n s_Jacob_Berzelius_x_Joha n_Way.jpg, CC0 Millennium Prize Organization 2018 By Riikka Puurunen and Tuomo Suntola - Own work 2014, CC BY-SA 4.0, https://commons.wiki media.org/w/index.p hp?curid=74884900 By Riikka L. Puurunen, J. Ruud van Ommen, Aristeidis Goulas - Own work 2020, CC BY 4.0, https://commons.wiki media.org/w/index.ph p?curid=97744756 By Aristeidis Goulas, J. Ruud van Ommen, Riikka L. Puurunen - Own work 2020, CC BY 4.0, https://commons.wikim edia.org/w/index.php?c urid=97939221 0 2 4 6 8 10 12 1 2 3 CO 2 conversion, % a Zr Zn/Zr Cu/Zr Zn/Cu/Zr Cu/Zn/Zr Zn/Cu/Zn/Zr 450 K 500 K 550 K No measured activity STY methanol Arandia et al., Appl. Catal. B, in press (2022), https://doi.org/10 .1016/j.apcatb.20 22.122046 CC BY 4.0 From Suntola’s collections. Published in: Puurunen, Chem. Vap. Deposition 20 (2014) 332-344. https://doi.org/10.100 2/cvde.201402012 (c) Author, CC BY-NC 3.0 By J. Ruud van Ommen, Fenne B.M. van Ommen, Riikka L. Puurunen - Own work 2020, CC BY 4.0, https://commons.wikime dia.org/w/index.php?curi d=102275667 From Puurunen’s collections Credit: Aitor Arandia … and many illustrations by RLP (handmade & other)… Aalto - Catalysis group Photo: Matti Reinikainen, 2022 Funding: Neste Virtual Project on the History of ALD logo by Riikka Puurunen, 2013 Collaborators through years