Effect of atomic layer deposited zinc promoter on the activity of copper-on-zirconia catalysts in the hydrogenation of carbon dioxide to methanol

Aitor Arandia; Jihong Yim; Hassaan Warraich; Emilia Leppäkangas; René Bes; Aku Lempelto; Lars Gell; Hua Jiang; Kristoffer Meinander; Tiia Viinikainen; Simo Huotari; Karoliina Honkala; Riikka L. Puurunen

doi:10.1016/j.apcatb.2022.122046

Effect of atomic layer deposited zinc promoter on the activity of copper-on-zirconia catalysts in the hydrogenation of carbon dioxide to methanol

Aitor Arandia^*, Jihong Yim, Hassaan Warraich, Emilia Leppäkangas, René Bes, Aku Lempelto, Lars Gell, Hua Jiang, Kristoffer Meinander, Tiia Viinikainen, Simo Huotari, Karoliina Honkala, Riikka L. Puurunen

^*Corresponding author for this work

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Abstract

The development of active catalysts for carbon dioxide (CO₂) hydrogenation to methanol is intimately related to the creation of effective metal-oxide interfaces. In this work, we investigated how the order of addition of copper and zinc on zirconia influences the catalytic properties, the catalytic activity and selectivity toward methanol. Regarding the carbon dioxide conversion and methanol production, the catalysts on which the promoter (zinc) was atomically deposited after copper impregnation (i.e., ZnO/Cu/ZrO₂ and ZnO/Cu/ZnO/ZrO₂) were superior catalysts compared to the reverse copper-after-zinc catalyst (Cu/ZnO/ZrO₂). Temperature-programmed experiments and in situ diffuse reflectance infrared Fourier transform-spectroscopy (DRIFTS) experiments allowed us to elucidate the benefits of the zinc-after-copper pair to store CO₂ as carbonate species and further convert them into formate species, key intermediates in the formation of methanol. This research provides insights into the potential of atomic layer deposition in the development of tailored heterogeneous catalysts for efficient CO₂ valorization to methanol.

Original language	English
Article number	122046
Journal	Applied Catalysis B: Environmental
Volume	321
Early online date	22 Oct 2022
DOIs	https://doi.org/10.1016/j.apcatb.2022.122046
Publication status	Published - Feb 2023
MoE publication type	A1 Journal article-refereed

Keywords

Atomic layer deposition
Carbon dioxide
Copper
Hydrogenation
Methanol
Zinc oxide

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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10.1016/j.apcatb.2022.122046Licence: CC BY

CHEM_Arandia_et_al_Effect_of_atomic_layer_2022_Applied_Catalysis_BFinal published version, 16.4 MBLicence: CC BY

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Arandia, A., Yim, J., Warraich, H., Leppäkangas, E., Bes, R., Lempelto, A., Gell, L., Jiang, H., Meinander, K., Viinikainen, T., Huotari, S., Honkala, K., & Puurunen, R. L. (2023). Effect of atomic layer deposited zinc promoter on the activity of copper-on-zirconia catalysts in the hydrogenation of carbon dioxide to methanol. Applied Catalysis B: Environmental, 321, Article 122046. https://doi.org/10.1016/j.apcatb.2022.122046

@article{a2247120cba946a1a2581b531842289e,

title = "Effect of atomic layer deposited zinc promoter on the activity of copper-on-zirconia catalysts in the hydrogenation of carbon dioxide to methanol",

abstract = "The development of active catalysts for carbon dioxide (CO2) hydrogenation to methanol is intimately related to the creation of effective metal-oxide interfaces. In this work, we investigated how the order of addition of copper and zinc on zirconia influences the catalytic properties, the catalytic activity and selectivity toward methanol. Regarding the carbon dioxide conversion and methanol production, the catalysts on which the promoter (zinc) was atomically deposited after copper impregnation (i.e., ZnO/Cu/ZrO2 and ZnO/Cu/ZnO/ZrO2) were superior catalysts compared to the reverse copper-after-zinc catalyst (Cu/ZnO/ZrO2). Temperature-programmed experiments and in situ diffuse reflectance infrared Fourier transform-spectroscopy (DRIFTS) experiments allowed us to elucidate the benefits of the zinc-after-copper pair to store CO2 as carbonate species and further convert them into formate species, key intermediates in the formation of methanol. This research provides insights into the potential of atomic layer deposition in the development of tailored heterogeneous catalysts for efficient CO2 valorization to methanol.",

keywords = "Atomic layer deposition, Carbon dioxide, Copper, Hydrogenation, Methanol, Zinc oxide",

author = "Aitor Arandia and Jihong Yim and Hassaan Warraich and Emilia Lepp{\"a}kangas and Ren{\'e} Bes and Aku Lempelto and Lars Gell and Hua Jiang and Kristoffer Meinander and Tiia Viinikainen and Simo Huotari and Karoliina Honkala and Puurunen, {Riikka L.}",

note = "Funding Information: The work at Aalto University has been financially supported by the Academy of Finland (COOLCAT consortium, decision no. 329977 and 329978 ; ALDI consortium, decision no. 331082 ). This work made use of Aalto University Bioeconomy, OtaNano and RawMatters infrastructure. Hannu Revitzer (Aalto University) is thanked for the ICP-OES analysis, Aalto workshop people (especially Seppo J{\"a}{\"a}skel{\"a}inen) for working on the reactor modifications. The DFT calculations were made possible by computational resources provided by the CSC — IT Center for Science, Espoo, Finland ( https://www.csc.fi/en/ ) and computer capacity from the Finnish Grid and Cloud Infrastructure (urn:nbn:fi:research-infras-2016072533). The University of Helsinki acknowledges support from Academy of Finland (project 295696 ) as well as ESRF for beamtime and Blanka Detlefs and Christoph Sahle for expert support. Preliminary XANES measurements were performed using the Helsinki Center for X-ray Spectroscopy Hel-XAS instrument under the proposal number 2021–0011. ",

year = "2023",

month = feb,

doi = "10.1016/j.apcatb.2022.122046",

language = "English",

volume = "321",

journal = "Applied Catalysis B: Environmental",

issn = "0926-3373",

publisher = "Elsevier BV",

}

Arandia, A, Yim, J, Warraich, H, Leppäkangas, E, Bes, R, Lempelto, A, Gell, L, Jiang, H , Meinander, K , Viinikainen, T, Huotari, S, Honkala, K & Puurunen, RL 2023, 'Effect of atomic layer deposited zinc promoter on the activity of copper-on-zirconia catalysts in the hydrogenation of carbon dioxide to methanol', Applied Catalysis B: Environmental, vol. 321, 122046. https://doi.org/10.1016/j.apcatb.2022.122046

TY - JOUR

T1 - Effect of atomic layer deposited zinc promoter on the activity of copper-on-zirconia catalysts in the hydrogenation of carbon dioxide to methanol

AU - Arandia, Aitor

AU - Yim, Jihong

AU - Warraich, Hassaan

AU - Leppäkangas, Emilia

AU - Bes, René

AU - Lempelto, Aku

AU - Gell, Lars

AU - Jiang, Hua

AU - Meinander, Kristoffer

AU - Viinikainen, Tiia

AU - Huotari, Simo

AU - Honkala, Karoliina

AU - Puurunen, Riikka L.

N1 - Funding Information: The work at Aalto University has been financially supported by the Academy of Finland (COOLCAT consortium, decision no. 329977 and 329978 ; ALDI consortium, decision no. 331082 ). This work made use of Aalto University Bioeconomy, OtaNano and RawMatters infrastructure. Hannu Revitzer (Aalto University) is thanked for the ICP-OES analysis, Aalto workshop people (especially Seppo Jääskeläinen) for working on the reactor modifications. The DFT calculations were made possible by computational resources provided by the CSC — IT Center for Science, Espoo, Finland ( https://www.csc.fi/en/ ) and computer capacity from the Finnish Grid and Cloud Infrastructure (urn:nbn:fi:research-infras-2016072533). The University of Helsinki acknowledges support from Academy of Finland (project 295696 ) as well as ESRF for beamtime and Blanka Detlefs and Christoph Sahle for expert support. Preliminary XANES measurements were performed using the Helsinki Center for X-ray Spectroscopy Hel-XAS instrument under the proposal number 2021–0011.

PY - 2023/2

Y1 - 2023/2

N2 - The development of active catalysts for carbon dioxide (CO2) hydrogenation to methanol is intimately related to the creation of effective metal-oxide interfaces. In this work, we investigated how the order of addition of copper and zinc on zirconia influences the catalytic properties, the catalytic activity and selectivity toward methanol. Regarding the carbon dioxide conversion and methanol production, the catalysts on which the promoter (zinc) was atomically deposited after copper impregnation (i.e., ZnO/Cu/ZrO2 and ZnO/Cu/ZnO/ZrO2) were superior catalysts compared to the reverse copper-after-zinc catalyst (Cu/ZnO/ZrO2). Temperature-programmed experiments and in situ diffuse reflectance infrared Fourier transform-spectroscopy (DRIFTS) experiments allowed us to elucidate the benefits of the zinc-after-copper pair to store CO2 as carbonate species and further convert them into formate species, key intermediates in the formation of methanol. This research provides insights into the potential of atomic layer deposition in the development of tailored heterogeneous catalysts for efficient CO2 valorization to methanol.

AB - The development of active catalysts for carbon dioxide (CO2) hydrogenation to methanol is intimately related to the creation of effective metal-oxide interfaces. In this work, we investigated how the order of addition of copper and zinc on zirconia influences the catalytic properties, the catalytic activity and selectivity toward methanol. Regarding the carbon dioxide conversion and methanol production, the catalysts on which the promoter (zinc) was atomically deposited after copper impregnation (i.e., ZnO/Cu/ZrO2 and ZnO/Cu/ZnO/ZrO2) were superior catalysts compared to the reverse copper-after-zinc catalyst (Cu/ZnO/ZrO2). Temperature-programmed experiments and in situ diffuse reflectance infrared Fourier transform-spectroscopy (DRIFTS) experiments allowed us to elucidate the benefits of the zinc-after-copper pair to store CO2 as carbonate species and further convert them into formate species, key intermediates in the formation of methanol. This research provides insights into the potential of atomic layer deposition in the development of tailored heterogeneous catalysts for efficient CO2 valorization to methanol.

KW - Atomic layer deposition

KW - Carbon dioxide

KW - Copper

KW - Hydrogenation

KW - Methanol

KW - Zinc oxide

UR - http://www.scopus.com/inward/record.url?scp=85140323413&partnerID=8YFLogxK

U2 - 10.1016/j.apcatb.2022.122046

DO - 10.1016/j.apcatb.2022.122046

M3 - Article

AN - SCOPUS:85140323413

SN - 0926-3373

VL - 321

JO - Applied Catalysis B: Environmental

JF - Applied Catalysis B: Environmental

M1 - 122046

ER -

Effect of atomic layer deposited zinc promoter on the activity of copper-on-zirconia catalysts in the hydrogenation of carbon dioxide to methanol

Abstract

Keywords

UN SDGs

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ALDI: Reactive flow in porous media: modelling and experiments in atomic layer deposition context

Renable Carbon Cycle - Uusiutuva hiilikierto: Conversion of CO2 to Fuels with Tailored Heterogeneous Catalysts

Bioeconomy Research Infrastructure

OtaNano

Raw Materials Research Infrastructure

Researchers from Aalto University Report Details of New Studies and Findings in the Area of Chemicals and Chemistry (Effect of Atomic Layer Deposited Zinc Promoter On the Activity of Copper-on-zirconia Catalysts In the Hydrogenation of Carbon ...)

Cite this

Effect of atomic layer deposited zinc promoter on the activity of copper-on-zirconia catalysts in the hydrogenation of carbon dioxide to methanol

Abstract

Keywords

UN SDGs

Access to Document

Other files and links

Fingerprint

Projects

ALDI: Reactive flow in porous media: modelling and experiments in atomic layer deposition context

Renable Carbon Cycle - Uusiutuva hiilikierto: Conversion of CO2 to Fuels with Tailored Heterogeneous Catalysts

Equipment

Bioeconomy Research Infrastructure

OtaNano

Raw Materials Research Infrastructure

Press/Media

Researchers from Aalto University Report Details of New Studies and Findings in the Area of Chemicals and Chemistry (Effect of Atomic Layer Deposited Zinc Promoter On the Activity of Copper-on-zirconia Catalysts In the Hydrogenation of Carbon ...)

Cite this