Header

UZH-Logo

Maintenance Infos

Preparative History vs Driving Force in Water Oxidation Catalysis: Parameter Space Studies of Cobalt Spinels


Reith, Lukas; Lienau, Karla; Triana, Carlos A; Siol, Sebastian; Patzke, Greta R (2019). Preparative History vs Driving Force in Water Oxidation Catalysis: Parameter Space Studies of Cobalt Spinels. ACS Omega, 4(13):15444-15456.

Abstract

The development of efficient, stable, and economic water oxidation catalysts (WOCs) is a forefront topic of sustainable energy research. We newly present a comprehensive three-step approach to systematically investigate challenging relationships among preparative history, properties, and performance in heterogeneous WOCs. To this end, we studied (1) the influence of the preparative method on the material properties and (2) their correlation with the performance as (3) a function of the catalytic test method. Spinel-type Co3O4 was selected as a clear-cut model WOC and synthesized via nine different preparative routes. In search of the key material properties for high catalytic performance, these cobalt oxide samples were characterized with a wide range of analytical methods, including X-ray absorption spectroscopy, X-ray photoelectron spectroscopy, powder X-ray diffraction, Raman spectroscopy, BET surface area analysis, and transmission electron microscopy. Next, the corresponding catalytic water oxidation activities were assessed with the three most widely applied protocols to date, namely, photocatalytic, electrocatalytic, and chemical oxidation. The activity of the Co3O4 samples was found to clearly depend on the applied test method. Increasing surface area and disorder as well as a decrease in oxidation states arising from low synthesis temperatures were identified as key parameters for high chemical oxidation activity. Surprisingly, no obvious property–performance correlations were found for photocatalytic water oxidation. In sharp contrast, all samples showed similar activity in electrochemical water oxidation. The substantial performance differences between the applied protocols demonstrate that control and comprehensive understanding of the preparative history are crucial for establishing reliable structure–performance relationships in WOC design.

Abstract

The development of efficient, stable, and economic water oxidation catalysts (WOCs) is a forefront topic of sustainable energy research. We newly present a comprehensive three-step approach to systematically investigate challenging relationships among preparative history, properties, and performance in heterogeneous WOCs. To this end, we studied (1) the influence of the preparative method on the material properties and (2) their correlation with the performance as (3) a function of the catalytic test method. Spinel-type Co3O4 was selected as a clear-cut model WOC and synthesized via nine different preparative routes. In search of the key material properties for high catalytic performance, these cobalt oxide samples were characterized with a wide range of analytical methods, including X-ray absorption spectroscopy, X-ray photoelectron spectroscopy, powder X-ray diffraction, Raman spectroscopy, BET surface area analysis, and transmission electron microscopy. Next, the corresponding catalytic water oxidation activities were assessed with the three most widely applied protocols to date, namely, photocatalytic, electrocatalytic, and chemical oxidation. The activity of the Co3O4 samples was found to clearly depend on the applied test method. Increasing surface area and disorder as well as a decrease in oxidation states arising from low synthesis temperatures were identified as key parameters for high chemical oxidation activity. Surprisingly, no obvious property–performance correlations were found for photocatalytic water oxidation. In sharp contrast, all samples showed similar activity in electrochemical water oxidation. The substantial performance differences between the applied protocols demonstrate that control and comprehensive understanding of the preparative history are crucial for establishing reliable structure–performance relationships in WOC design.

Statistics

Citations

Dimensions.ai Metrics
2 citations in Web of Science®
1 citation in Scopus®
Google Scholar™

Altmetrics

Downloads

16 downloads since deposited on 07 Feb 2020
16 downloads since 12 months
Detailed statistics

Additional indexing

Item Type:Journal Article, refereed, original work
Communities & Collections:07 Faculty of Science > Department of Chemistry
08 Research Priority Programs > Solar Light to Chemical Energy Conversion
Dewey Decimal Classification:540 Chemistry
Scopus Subject Areas:Physical Sciences > General Chemistry
Physical Sciences > General Chemical Engineering
Language:English
Date:2019
Deposited On:07 Feb 2020 15:06
Last Modified:22 Apr 2020 22:54
Publisher:American Chemical Society (ACS)
ISSN:2470-1343
OA Status:Gold
Free access at:Publisher DOI. An embargo period may apply.
Publisher DOI:https://doi.org/10.1021/acsomega.9b01677
Project Information:
  • : FunderSNSF
  • : Grant IDCRSII2_160801
  • : Project TitlePhotocatalytic Processes at Solvated Interfaces
  • : FunderCOST Action MP1407
  • : Grant IDIZCNZ0-174856 C16.0075
  • : Project Title

Download

Gold Open Access

Download PDF  'Preparative History vs Driving Force in Water Oxidation Catalysis: Parameter Space Studies of Cobalt Spinels'.
Preview
Content: Published Version
Filetype: PDF
Size: 8MB
View at publisher