Evolution of zincian malachite synthesis by low temperature co-precipitation and its catalytic impact on the methanol synthesis

[Display omitted] •Transient low-temperature protocol for zincian malachite co-precipitation developed.•Level of Zn-incorporation shifted to higher values (by 15%).•Higher surface areas, increased dispersions and catalytic activities obtained.•Increased interfacial contact suppresses rWGS.•New synth...

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Bibliographic Details
Published in:Applied catalysis. B, Environmental Environmental, 2019-07, Vol.249, p.218-226
Main Authors: Zwiener, Leon, Girgsdies, Frank, Brennecke, Daniel, Teschner, Detre, Machoke, Albert G.F., Schlögl, Robert, Frei, Elias
Format: Article
Language:English
Subjects:
Catalysis
Catalysts
Chemical synthesis
Co-precipitation
Coprecipitation
High temperature
Low temperature
Methanol
Methanol synthesis
Nitrous oxide
Temperature effects
Zinc
Zinc oxide
Zincian malachite
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Summary:[Display omitted] •Transient low-temperature protocol for zincian malachite co-precipitation developed.•Level of Zn-incorporation shifted to higher values (by 15%).•Higher surface areas, increased dispersions and catalytic activities obtained.•Increased interfacial contact suppresses rWGS.•New synthesis tool for any coprecipitated material. Low temperature co-precipitation enabled, for the first time, the preparation of phase pure zincian malachite precursors with Zn contents of up to 31 at.-%. The high Zn content was beneficial for maximizing the dispersion of Cu and oxygen defect sites on the ZnO surface. Further, an increase of the Zn loading from 10 to 31 at.-% doubled the specific surface areas obtained from N2O-RFC (Reactive Frontal Chromatography) and H2-TA (Transient Adsorption). As the Zn content was increased from 10 to 31 at.-%, the apparent activation energy for methanol formation was strongly decreased. Furthermore, water formation was reduced indicating a retardation of the rWGS in favor of methanol formation at high Zn loadings. Additionally, compared to high temperature co-precipitation, low temperature precipitated catalysts exhibited increased catalytic activities.
ISSN:0926-3373
1873-3883
DOI:10.1016/j.apcatb.2019.02.023