Boosting catalytic activity of Cu-Ce solid solution catalysts by flame spray pyrolysis with high Cu+ concentration and oxygen vacancies

Jiang, Jiechao; Hong, Yi; Jiang, Hao; Hu, Yanjie; Li, Chunzhong

doi:10.1016/j.cej.2023.144439

Cited by 17 publications

(3 citation statements)

References 57 publications

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“…The EPR spectrum of Ce-CuZn sample presents obvious oxygen vacancies peak at g || value of 1.99, which is much different with the other two samples (Fig. 2f ) 43 . Moreover, the type K peaks at g || values of 2.29 and 1.83 are ascribed to Cu 2+ /Zn 2+ dimer, which could be observed when two neighboring Ce 4+ ions with short separation distance are substituted by Cu 2+ /Zn 2+ ions 44 .…”

Section: Resultsmentioning

confidence: 71%

“…However, the Ce 3+ /(Ce 3+ +Ce 4+ ) ratio (34.8%) of Ce-CuZn is slightly lower than that over CuZn-Ce (36.4%), but higher than that over Ce-CuZn-IM (27.4%, Supplementary Table 1 ). This is because that the catalyst has two types of oxygen vacancies: I) generation from the reduction of Ce 4+ to Ce 3+ , and II) the replacement of Ce 4+ by Cu/Zn ions, resulting in the formation of oxygen vacancies 43 . Thus, the Ce-CuZn catalyst with slightly lower Ce 3+ /(Ce 3+ +Ce 4+ ) ratio could still exhibit higher O β /(O α + O β + O γ ) ratio due to the substitutional incorporation of Cu/Zn ions into the CeO 2 lattice.…”

Section: Resultsmentioning

confidence: 99%

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A Ce-CuZn catalyst with abundant Cu/Zn-OV-Ce active sites for CO2 hydrogenation to methanol

Ye,

Ma,

Mao

et al. 2024

Nat Commun

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CO2 hydrogenation to chemicals and fuels is a significant approach for achieving carbon neutrality. It is essential to rationally design the chemical structure and catalytic active sites towards the development of efficient catalysts. Here we show a Ce-CuZn catalyst with enriched Cu/Zn-OV-Ce active sites fabricated through the atomic-level substitution of Cu and Zn into Ce-MOF precursor. The Ce-CuZn catalyst exhibits a high methanol selectivity of 71.1% and a space-time yield of methanol up to 400.3 g·kgcat−1·h−1 with excellent stability for 170 h at 260 °C, comparable to that of the state-of-the-art CuZnAl catalysts. Controlled experiments and DFT calculations confirm that the incorporation of Cu and Zn into CeO2 with abundant oxygen vacancies can facilitate H2 dissociation energetically and thus improve CO2 hydrogenation over the Ce-CuZn catalyst via formate intermediates. This work offers an atomic-level design strategy for constructing efficient multi-metal catalysts for methanol synthesis through precise control of active sites.

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Section: Resultsmentioning

confidence: 71%

Section: Resultsmentioning

confidence: 99%

A Ce-CuZn catalyst with abundant Cu/Zn-OV-Ce active sites for CO2 hydrogenation to methanol

Ye,

Ma,

Mao

et al. 2024

Nat Commun

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“…25–27 As the Cu content continues to increase, some of the copper precipitates out, forming clustered copper species on the Cu/CuCeO x nanorods. 28 And no diffraction peaks corresponding to Cu can be found when the copper loading is below 30 wt%, which may be due to the high dispersion of Cu nanoparticles with too small particle sizes on the surface of the ceria support to be identified by the XRD (Fig. S2†).…”

Section: Resultsmentioning

confidence: 99%

Customized CO₂ electroreduction to methane or ethylene by manipulating H and CO adsorption on Cu/CeO_x catalysts

Yang,

Zhang,

Huang

et al. 2024

J. Mater. Chem. A

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Pd Single‐Atom Loaded Ce‐Zr Solid Solution Catalysts Prepared by Flame Spray Pyrolysis for Efficient CO Catalytic Oxidation

Zheng,

Zhang,

Jiang

et al. 2024

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Single‐atom catalysts (SACs) exhibit remarkable catalytic activity at each metal site. However, conventionally synthesized single‐atom catalysts often possess low metal loading, thereby constraining their overall catalytic performance. Here, a flame spray pyrolysis (FSP) method for the synthesis of a single‐atom catalyst with a high loading capacity of up to 1.4 wt.% in practice is reported. CeZrO2 acts as a carrier and provides a large number of anchoring sites, which promotes the high‐density generation of Pd, and the strong interaction between the metal and the support avoids atom aggregation. Pd‐CeZrO2 series catalysts have excellent CO oxidation performance. When 0.97 wt.% Pd is added, the catalytic activity is the highest, and the temperature can be reduced to 120 °C. This work presented here demonstrates that FSP, as an inherently scalable technique, allows for elevating the single‐atom loading to achieve an increase in its catalytic performance. The method presented here more options for the preparation of SACs.

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Boosting catalytic activity of Cu-Ce solid solution catalysts by flame spray pyrolysis with high Cu+ concentration and oxygen vacancies

Cited by 17 publications

References 57 publications

A Ce-CuZn catalyst with abundant Cu/Zn-OV-Ce active sites for CO2 hydrogenation to methanol

A Ce-CuZn catalyst with abundant Cu/Zn-OV-Ce active sites for CO2 hydrogenation to methanol

Customized CO₂ electroreduction to methane or ethylene by manipulating H and CO adsorption on Cu/CeO_x catalysts

Pd Single‐Atom Loaded Ce‐Zr Solid Solution Catalysts Prepared by Flame Spray Pyrolysis for Efficient CO Catalytic Oxidation

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Boosting catalytic activity of Cu-Ce solid solution catalysts by flame spray pyrolysis with high Cu+ concentration and oxygen vacancies

Cited by 17 publications

References 57 publications

A Ce-CuZn catalyst with abundant Cu/Zn-OV-Ce active sites for CO2 hydrogenation to methanol

A Ce-CuZn catalyst with abundant Cu/Zn-OV-Ce active sites for CO2 hydrogenation to methanol

Customized CO2 electroreduction to methane or ethylene by manipulating *H and *CO adsorption on Cu/CeOx catalysts

Pd Single‐Atom Loaded Ce‐Zr Solid Solution Catalysts Prepared by Flame Spray Pyrolysis for Efficient CO Catalytic Oxidation

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Customized CO₂ electroreduction to methane or ethylene by manipulating H and CO adsorption on Cu/CeO_x catalysts