Co0 − Coδ+ active pairs tailored by Ga-Al-O spinel for CO2-to-ethanol synthesis

An, Kang; Zhang, Siran; Wang, Hong; Li, Ningyan; Zhang, Ziyang; Liu, Yuan

doi:10.1016/j.cej.2022.134606

Cited by 25 publications

(16 citation statements)

References 62 publications

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“…The shifts of Al 2p BEs in Figure c revealed the change of Al compounds on the catalyst surface. A previous paper has proven that the binding energy of Al 3+ in Al 2 O 3 was higher than that in spinel . Compared with the HEO-X samples, HEO-XR catalysts displayed much higher BE values for Al 2p, demonstrating that a part of Al in HEO-X was converted into Al 2 O 3 during the reduction process.…”

Section: Resultsmentioning

confidence: 90%

“…A previous paper has proven that the binding energy of Al 3+ in Al 2 O 3 was higher than that in spinel. 86 Compared with the HEO-X samples, HEO-XR catalysts displayed much higher BE values for Al 2p, demonstrating that a part of Al in HEO-X was converted into Al 2 O 3 during the reduction process. It is noteworthy that BEs of Al in the three HEO-XS catalysts shifted to lower energy directions with different degree, which also indicated that Co was recombined with Al 2 O 3 to form CoAl 2 O 4 , thereby reducing the amount of Al 2 O 3 and the BEs of Al.…”

Section: Xpsmentioning

confidence: 90%

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Highly Stable Bimetal Ni–Co on Alumina-Covered Spinel Oxide Derived from High Entropy Oxide for CO₂ Methanation

Liu

Wang

Sun

et al. 2022

Ind. Eng. Chem. Res.

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Inhibiting the sintering of supported metal catalysts for CO 2 methanation is still a great challenge, especially at high temperature. Herein, the novel catalyst was prepared by using high entropy spinel oxide (Co 0.2 Ni 0.2 Mg 0.2 Zn 0.2 Mn 0.2 )Al 2 O 4 (HEO) as precursor, which was reduced in a hydrogen atmosphere to obtain Ni−Co alloys supported on Al 2 O 3 -covered (Mg 0.2 Zn 0.2 Mn 0.2 )-Al 1.2 O 2.4 spinel oxide with a core−shell structure. This catalyst exhibited excellent stability at 550 °C for 320 h. Characterization results showed that the formation of the core−shell structure due to uniform element dispersion of the HEO precursor led to a larger interface, closer contact, and stronger interaction between the core and shell, which ensured the stability of the shell Al 2 O 3 and further stabilized Ni−Co alloys. However, the catalyst derived from the mixed spinel oxide precursor was unable to achieve the core−shell structure support due to uneven element dispersion, which exhibited inferior stability. This study has successful extended the application of high entropy oxides.

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Section: Resultsmentioning

confidence: 90%

Section: Xpsmentioning

confidence: 90%

Highly Stable Bimetal Ni–Co on Alumina-Covered Spinel Oxide Derived from High Entropy Oxide for CO₂ Methanation

Liu

Wang

Sun

et al. 2022

Ind. Eng. Chem. Res.

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“…This result implies that Co can be dynamically balanced between Co 0 and Co δ + during the reaction. [16] When compared with Co/MAO (778.2 eV for Co 0 ), the binding energy of Co 0 in CoÀ CoO x / MAO exhibit slightly positive shifts (ca. 0.1 eV for Co 2p), suggesting that the electronic structure of Co was significantly changed and the decreased electron density of metallic Co in the Co 0 À Co δ + sites.…”

Section: Resultsmentioning

confidence: 98%

Co⁰−Co^δ+ Interface Double‐Site‐Mediated C−C Coupling for the Photothermal Conversion of CO₂ into Light Olefins

Ning

et al. 2023

Angewandte Chemie

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Solar-driven CO 2 hydrogenation into multicarbon products is a highly desirable, but challenging reaction. The bottleneck of this reaction lies in the CÀ C coupling of C 1 intermediates. Herein, we construct the CÀ C coupling centre for C 1 intermediates via the in situ formation of Co 0 À Co δ + interface double sites on MgAl 2 O 4 (CoÀ CoO x /MAO). Our experimental and theoretical prediction results confirmed the effective adsorption and activation of CO 2 by the Co 0 site to produce C 1 intermediates, while the introduction of the electron-deficient state of Co δ + can effectively reduce the energy barrier of the key CHCH* intermediates. Consequently, CoÀ CoO x /MAO exhibited a high C 2-4 hydrocarbons production rate of 1303 μmol g À 1 h À 1 ; the total organic carbon selectivity of C 2-4 hydrocarbons is 62.5 % under light irradiation with a high ratio ( � 11) of olefin to paraffin. This study provides a new approach toward the design of photocatalysts used for CO 2 conversion into C 2 + products.

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“…35 With regard to CoP-CN, the Co 2p spectrum (Figure S8c) comprises the doublet signals of 778.5− 793.8 and 781.8−797.7 eV, consistent with the partially charged Co δ+ and Co 2+ species, respectively. 36,37 In the P 2p spectrum (Figure S8d), the 2p 3/2 and 2p 1/2 signals locating at 128.5 and 129.6 eV are attributed to partially charged P δ− in metal phosphides, 38 while the peak at 133.1 eV indicates the generation of oxidized phosphide species due to air exposure. 39 The coexistence of Co δ+ and P δ− species reveals the formation of CoP.…”

Section: ■ Results and Discussionmentioning

confidence: 99%

CoP-Embedded Graphitic N-Doped C Nanosheets in Ohmic Contact with S-Deficient CdS Nanocrystals Triggering Efficient Visible-Light Photocatalytic H₂ Evolution

Wang²,

Wang

et al. 2023

ACS Appl. Nano Mater.

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Photocatalytic water splitting using semiconductor-based catalysts is a promising avenue to gain H2 fuel from renewable solar energy. Nonetheless, developing earth-abundant and visible-light-responsive photocatalysts for efficient H2 production still remains a huge challenge. In this work, unique two-dimensional hierarchitectures of S-deficient CdS integrated with ultrafine CoP nanocrystals embedding in graphitic N-doped C (CoP-CN) nanosheets are fabricated for the first time. Noticeably, the graphitic CN electron mediator not only enhances the photocatalytic stability of CdS/CoP-CN composites by protecting CoP from external corrosion but also induces the formation of an ohmic junction to boost electron extraction from CdS to CoP efficiently. Meanwhile, the S vacancies in CdS serve as electron traps to further enhance the separation of photogenerated carriers. Such unique CdS/CoP-CN hierarchical hybrid nanosheets exhibited an extraordinary visible-light-induced (λ > 400 nm) photocatalytic H2-evolving performance, delivering a high apparent quantum yield (26.3% at 420 nm) and an excellent H2 generation rate of 54.01 mmol·g–1·h–1, much superior to those of a CdS/CoP Schottky junction, Pt-loaded CdS, and a vast amount of CdS-based photocatalysts ever reported. In addition, the outstanding H2-evolving durability of CdS/CoP-CN composites was verified by cycling and long-term photocatalytic tests. The findings presented here are anticipated to enlighten the rational design and synthesis of highly active photocatalysts with an ohmic junction for application in energy and environment-related domains.

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Co0 − Coδ+ active pairs tailored by Ga-Al-O spinel for CO2-to-ethanol synthesis

Cited by 25 publications

References 62 publications

Highly Stable Bimetal Ni–Co on Alumina-Covered Spinel Oxide Derived from High Entropy Oxide for CO₂ Methanation

Highly Stable Bimetal Ni–Co on Alumina-Covered Spinel Oxide Derived from High Entropy Oxide for CO₂ Methanation

Co⁰−Co^δ+ Interface Double‐Site‐Mediated C−C Coupling for the Photothermal Conversion of CO₂ into Light Olefins

CoP-Embedded Graphitic N-Doped C Nanosheets in Ohmic Contact with S-Deficient CdS Nanocrystals Triggering Efficient Visible-Light Photocatalytic H₂ Evolution

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Co0 − Coδ+ active pairs tailored by Ga-Al-O spinel for CO2-to-ethanol synthesis

Cited by 25 publications

References 62 publications

Highly Stable Bimetal Ni–Co on Alumina-Covered Spinel Oxide Derived from High Entropy Oxide for CO2 Methanation

Highly Stable Bimetal Ni–Co on Alumina-Covered Spinel Oxide Derived from High Entropy Oxide for CO2 Methanation

Co0−Coδ+ Interface Double‐Site‐Mediated C−C Coupling for the Photothermal Conversion of CO2 into Light Olefins

CoP-Embedded Graphitic N-Doped C Nanosheets in Ohmic Contact with S-Deficient CdS Nanocrystals Triggering Efficient Visible-Light Photocatalytic H2 Evolution

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Highly Stable Bimetal Ni–Co on Alumina-Covered Spinel Oxide Derived from High Entropy Oxide for CO₂ Methanation

Highly Stable Bimetal Ni–Co on Alumina-Covered Spinel Oxide Derived from High Entropy Oxide for CO₂ Methanation

Co⁰−Co^δ+ Interface Double‐Site‐Mediated C−C Coupling for the Photothermal Conversion of CO₂ into Light Olefins

CoP-Embedded Graphitic N-Doped C Nanosheets in Ohmic Contact with S-Deficient CdS Nanocrystals Triggering Efficient Visible-Light Photocatalytic H₂ Evolution