Mapping Support Interactions in Copper Catalysts

Rishika Chatterjee, Sebastian Kuld, Roy van den Berg, Aling Chen, Wenjie Shen, Jakob Munkholt Christensen, Anker Degn Jensen, Jens Sehested*

*Corresponding author for this work

Research output: Contribution to journalJournal articleResearchpeer-review

Abstract

Intrinsic activity is often reported as a Turnover Frequency (TOF) of an active phase and is determined from an overall activity and a specific active surface area. The latter parameter is often determined by selective chemisorption techniques, but (strong) metal-support interactions, (S)MSI, between the metal and the carrier in an interplay with the nature of the probe molecules may distort the measurements. Here, a double-area-estimation approach is used for fast and accurate evaluation of (S)MSI effects in supported Cu catalysts: Firstly, baselines for the Temperature Programmed Desorption of Hydrogen (H2-TPD) and Reactive Frontal Chromatography by Nitrous oxide (N2O-RFC) methods commonly used to titrate Cu areas were established by comparison with Brunauer-Emmett-Teller (BET) surface areas using a series of pure Cu catalysts. Pure unsupported Cu samples, free from support interactions, were used to determine the stoichiometries between the probe molecules, H2 and N2O, and Cu surface atoms. This resulted in values of 2.08 ± 0.14:1 (Cu:O) and 2.81 ± 0.09:1 (Cu:H2). Cu on a wide range of support materials were subsequently analyzed by H2-TPD and N2O-RFC and benchmarked according to the unsupported Cu reference. This was done to study metal support interactions and increase the understanding of the nature of the interactions between Cu and different carriers.
Original languageEnglish
JournalTopics in catalysis
Volume62
Issue number7-11
Pages (from-to)649-659
ISSN1022-5528
DOIs
Publication statusPublished - 2019

Keywords

  • Strong metal support interactions (SMSI)
  • Temperature Programmed Desorption of Hydrogen ( H2-TPD)
  • Reactive frontal Chromatography by Nitrous oxide ( N2O-RFC)

Cite this

Chatterjee, R., Kuld, S., van den Berg, R., Chen, A., Shen, W., Christensen, J. M., ... Sehested, J. (2019). Mapping Support Interactions in Copper Catalysts. Topics in catalysis, 62(7-11), 649-659. https://doi.org/10.1007/s11244-019-01150-9
Chatterjee, Rishika ; Kuld, Sebastian ; van den Berg, Roy ; Chen, Aling ; Shen, Wenjie ; Christensen, Jakob Munkholt ; Jensen, Anker Degn ; Sehested, Jens. / Mapping Support Interactions in Copper Catalysts. In: Topics in catalysis. 2019 ; Vol. 62, No. 7-11. pp. 649-659.
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Chatterjee, R, Kuld, S, van den Berg, R, Chen, A, Shen, W, Christensen, JM, Jensen, AD & Sehested, J 2019, 'Mapping Support Interactions in Copper Catalysts', Topics in catalysis, vol. 62, no. 7-11, pp. 649-659. https://doi.org/10.1007/s11244-019-01150-9

Mapping Support Interactions in Copper Catalysts. / Chatterjee, Rishika; Kuld, Sebastian; van den Berg, Roy; Chen, Aling; Shen, Wenjie; Christensen, Jakob Munkholt; Jensen, Anker Degn; Sehested, Jens.

In: Topics in catalysis, Vol. 62, No. 7-11, 2019, p. 649-659.

Research output: Contribution to journalJournal articleResearchpeer-review

TY - JOUR

T1 - Mapping Support Interactions in Copper Catalysts

AU - Chatterjee, Rishika

AU - Kuld, Sebastian

AU - van den Berg, Roy

AU - Chen, Aling

AU - Shen, Wenjie

AU - Christensen, Jakob Munkholt

AU - Jensen, Anker Degn

AU - Sehested, Jens

PY - 2019

Y1 - 2019

N2 - Intrinsic activity is often reported as a Turnover Frequency (TOF) of an active phase and is determined from an overall activity and a specific active surface area. The latter parameter is often determined by selective chemisorption techniques, but (strong) metal-support interactions, (S)MSI, between the metal and the carrier in an interplay with the nature of the probe molecules may distort the measurements. Here, a double-area-estimation approach is used for fast and accurate evaluation of (S)MSI effects in supported Cu catalysts: Firstly, baselines for the Temperature Programmed Desorption of Hydrogen (H2-TPD) and Reactive Frontal Chromatography by Nitrous oxide (N2O-RFC) methods commonly used to titrate Cu areas were established by comparison with Brunauer-Emmett-Teller (BET) surface areas using a series of pure Cu catalysts. Pure unsupported Cu samples, free from support interactions, were used to determine the stoichiometries between the probe molecules, H2 and N2O, and Cu surface atoms. This resulted in values of 2.08 ± 0.14:1 (Cu:O) and 2.81 ± 0.09:1 (Cu:H2). Cu on a wide range of support materials were subsequently analyzed by H2-TPD and N2O-RFC and benchmarked according to the unsupported Cu reference. This was done to study metal support interactions and increase the understanding of the nature of the interactions between Cu and different carriers.

AB - Intrinsic activity is often reported as a Turnover Frequency (TOF) of an active phase and is determined from an overall activity and a specific active surface area. The latter parameter is often determined by selective chemisorption techniques, but (strong) metal-support interactions, (S)MSI, between the metal and the carrier in an interplay with the nature of the probe molecules may distort the measurements. Here, a double-area-estimation approach is used for fast and accurate evaluation of (S)MSI effects in supported Cu catalysts: Firstly, baselines for the Temperature Programmed Desorption of Hydrogen (H2-TPD) and Reactive Frontal Chromatography by Nitrous oxide (N2O-RFC) methods commonly used to titrate Cu areas were established by comparison with Brunauer-Emmett-Teller (BET) surface areas using a series of pure Cu catalysts. Pure unsupported Cu samples, free from support interactions, were used to determine the stoichiometries between the probe molecules, H2 and N2O, and Cu surface atoms. This resulted in values of 2.08 ± 0.14:1 (Cu:O) and 2.81 ± 0.09:1 (Cu:H2). Cu on a wide range of support materials were subsequently analyzed by H2-TPD and N2O-RFC and benchmarked according to the unsupported Cu reference. This was done to study metal support interactions and increase the understanding of the nature of the interactions between Cu and different carriers.

KW - Strong metal support interactions (SMSI)

KW - Temperature Programmed Desorption of Hydrogen ( H2-TPD)

KW - Reactive frontal Chromatography by Nitrous oxide ( N2O-RFC)

U2 - 10.1007/s11244-019-01150-9

DO - 10.1007/s11244-019-01150-9

M3 - Journal article

VL - 62

SP - 649

EP - 659

JO - Topics in Catalysis

JF - Topics in Catalysis

SN - 1022-5528

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ER -

Chatterjee R, Kuld S, van den Berg R, Chen A, Shen W, Christensen JM et al. Mapping Support Interactions in Copper Catalysts. Topics in catalysis. 2019;62(7-11):649-659. https://doi.org/10.1007/s11244-019-01150-9