Performance of Au/ZnO catalysts in CO2 reduction to methanol: Varying the Au loading / Au particle size

Chen, Shilong; Abdel‐Mageed, Ali M.; Hauble, Ashlee; Ishida, Tamao; Murayama, Toru; Parlinska-Wojtan, Magdalena; Behm, R. Jürgen

doi:10.1016/j.apcata.2021.118318

Cited by 20 publications

(10 citation statements)

References 43 publications

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“…The CO 2 RR is a typical gas-phase reaction that requires efficient capture and activation of CO 2 molecules to produce valuable chemicals . To achieve this, an effective photoelectrode should possess specific catalytically active sites for CO 2 reduction products and promote the diffusion of CO 2 molecules. , Several strategies, such as morphology manipulation, , particle size tuning, , and formation of multimetallic alloys, , have been implemented to improve the CO 2 reduction selectivity and suppress the competing HER. In addition to the catalyst itself, the properties of the photoelectrode/electrolyte interface are also critical to enhance the CO 2 reduction activity of the photoelectrode.…”

mentioning

confidence: 99%

Modulating the Cu₂O Photoelectrode/Electrolyte Interface with Bilayer Surfactant Simulating Cell Membranes for Boosting Photoelectrochemical CO₂ Reduction

Zhang

Liu

Wang

et al. 2023

J. Phys. Chem. Lett.

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The low solubility of CO2 molecules and the competition of the hydrogen evolution reaction (HER) in aqueous electrolytes pose significant challenges to the current photoelectrochemical (PEC) CO2 reduction reaction. In this study, inspired by the bilayer phospholipid molecular structure of cell membranes, we developed a Cu2O/Sn photocathode that was modified with the bilayer surfactant DHAB for achieving high CO2 permeability and suppressed HER. The Cu2O/Sn/DHAB photocathode stabilizes the *OCHO intermediate and facilitates the production of HCOOH. Our findings show that the Faradaic efficiency (FE) of HCOOH by the Cu2O/Sn/DHAB photoelectrode is 83.3%, significantly higher than that achieved with the Cu2O photoelectrode (FEHCOOH = 30.1%). Furthermore, the FEH2 produced by the Cu2O/Sn/DHAB photoelectrode is only 2.95% at −0.6 V vs RHE. The generation rate of HCOOH by the Cu2O/Sn/DHAB photoelectrode reaches 1.52 mmol·cm–2·h–1·L–1 at −0.7 V vs RHE. Our study provides a novel approach for the design of efficient photocathodes for CO2 reduction.

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mentioning

confidence: 99%

Modulating the Cu₂O Photoelectrode/Electrolyte Interface with Bilayer Surfactant Simulating Cell Membranes for Boosting Photoelectrochemical CO₂ Reduction

Zhang

Liu

Wang

et al. 2023

J. Phys. Chem. Lett.

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“…Thus, the bound SiAu 5 cluster lowers the activation energy barrier for CO oxidation, and the reaction occurs more readily compared with the Au 6 cluster process. In addition, we also noted that the reactivity and catalytical effects are also affected by supports for different metal oxide surfaces [ 5 , 9 , 20 ]. Moreover, experimental investigations are important for understanding CO oxidation on SiAu n clusters.…”

Section: Resultsmentioning

confidence: 99%

“…Among the various types of metal clusters, Au clusters have attracted much attention as size-tunable prototypes, because they have been shown to have significant catalytic activity [ 5 , 6 , 7 , 8 , 9 , 10 , 11 , 12 , 13 , 14 , 15 , 16 , 17 , 18 , 19 ]. Chen et al [ 20 ] showed that Au loading and the Au particle size have significant effects on the generation of methanol and CO; with an increase in the Au loading/Au particle size, the generation activity (Au-mass-normalized reaction rate, TOF) for methanol and CO decreases, while the selectivity for methanol generation increases. The decrease in activity is mainly due to the decrease in the dispersion of Au particles, which is the particle size effect.…”

Section: Introductionmentioning

confidence: 99%

Mechanisms for Catalytic CO Oxidation on SiAun (n = 1–5) Cluster

Zhang

Ren

2023

Molecules

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Significant progress has been made in understanding the reactivity and catalytic activity of gas-phase and loaded gold clusters for CO oxidation. However, little research has focused on mixed silicon/gold clusters (SiAun) for CO oxidation. In the present work, we performed density function theory (DFT) calculations for a SiAun (n = 1–5) cluster at the CAM-B3LYP/aug-cc-pVDZ-PP level and investigated the effects on the reactivity and catalytic activity of the SiAun cluster for CO oxidation. The calculated results show that the effect is very low for the activation barriers for the formation of OOCO intermediates on SiAu clusters, SiAu3 clusters, and SiAu5 clusters in the catalytic oxidation of CO and the activation energy barriers for the formation of OCO intermediates on OSiAu3, OSiAu4, and OSiAu5. Our calculations show that, compared with the conventional small Au cluster, the incorporation of Si enhances the catalytic performance towards CO oxidation.

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“…Diese Unterschiede wurden im Sinne einer kleinen Schottky‐Barriere interpretiert, deren Größe von Metall und Oxidträger abhängt. Die Bildung dieser Punktdefekte wurde auch mit der Aktivität bei der Methanolbildung an Au/ZnO‐Katalysatoren in Verbindung gebracht, die mit einer negativen Aufladung von Au‐Spezies unter den Reaktionsbedingungen einhergeht [43b,44,47] . Angesichts der leichten Aufladung von Au‐Spezies während der CO 2 ‐Hydrierung an Cu 93 Au 7 /ZnO‐Katalysatoren kann dieser Zusammenhang im vorliegenden Fall nicht ausgeschlossen werden, allerdings mit Unterschieden, die auf die Anwesenheit von Wasser an der Grenzfläche zurückzuführen sind.…”

Section: Ergebnisse Und Diskussionunclassified

Niedrige Temperatur Hydrierung von CO₂ zu Methanol in Wasser auf ZnO‐geträgerten CuAu‐Nanolegierungen

Mosrati,

Ishida,

Mac

et al. 2023

Angewandte Chemie

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Optimizing processes and materials for the valorization of CO2 to hydrogen carriers or platform chemicals is a key step for mitigating global warming and for the sustainable use of renewables. We report here on the hydrogenation of CO2 in water on ZnO‐supported CuAu nanoalloys, based on ≤ 7 mol% Au. CuxAuy/ZnO catalysts were characterized using 197Au Mössbauer, in‐situ X‐ray absorption (Au LIII‐ and Cu K‐edges), and ambient pressure X‐ray photoelectron spectroscopy (APXP), together with X‐ray diffraction and high‐resolution electron microscopy. At 200 °C, the conversion of CO2 showed a significant increase by 34 times (from 0.1 to 3.4 %) upon increasing Cu93Au7 loading from 1 to 10 wt.%, while maintaining methanol selectivity at 100%. Limited CO selectivity (4‐6%) was observed upon increasing temperature up to 240 °C but associated with a ~3‐fold increase in CO2 conversion. Based on APXPS during CO2 hydrogenation in an H2O‐rich mixture, Cu segregates preferentially to the surface in mainly metallic state, while slightly charged Au submerges deeper into the subsurface region. These results and detailed structural analyses are topics of present contribution.

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Performance of Au/ZnO catalysts in CO2 reduction to methanol: Varying the Au loading / Au particle size

Cited by 20 publications

References 43 publications

Modulating the Cu₂O Photoelectrode/Electrolyte Interface with Bilayer Surfactant Simulating Cell Membranes for Boosting Photoelectrochemical CO₂ Reduction

Modulating the Cu₂O Photoelectrode/Electrolyte Interface with Bilayer Surfactant Simulating Cell Membranes for Boosting Photoelectrochemical CO₂ Reduction

Mechanisms for Catalytic CO Oxidation on SiAun (n = 1–5) Cluster

Niedrige Temperatur Hydrierung von CO₂ zu Methanol in Wasser auf ZnO‐geträgerten CuAu‐Nanolegierungen

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Performance of Au/ZnO catalysts in CO2 reduction to methanol: Varying the Au loading / Au particle size

Cited by 20 publications

References 43 publications

Modulating the Cu2O Photoelectrode/Electrolyte Interface with Bilayer Surfactant Simulating Cell Membranes for Boosting Photoelectrochemical CO2 Reduction

Modulating the Cu2O Photoelectrode/Electrolyte Interface with Bilayer Surfactant Simulating Cell Membranes for Boosting Photoelectrochemical CO2 Reduction

Mechanisms for Catalytic CO Oxidation on SiAun (n = 1–5) Cluster

Niedrige Temperatur Hydrierung von CO2 zu Methanol in Wasser auf ZnO‐geträgerten CuAu‐Nanolegierungen

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Modulating the Cu₂O Photoelectrode/Electrolyte Interface with Bilayer Surfactant Simulating Cell Membranes for Boosting Photoelectrochemical CO₂ Reduction

Modulating the Cu₂O Photoelectrode/Electrolyte Interface with Bilayer Surfactant Simulating Cell Membranes for Boosting Photoelectrochemical CO₂ Reduction

Niedrige Temperatur Hydrierung von CO₂ zu Methanol in Wasser auf ZnO‐geträgerten CuAu‐Nanolegierungen