Ga-Promoted CuCo-Based Catalysts for Efficient CO2 Hydrogenation to Ethanol: The Key Synergistic Role of Cu-CoGaOx Interfacial Sites

Zhang, Guangcheng; Fan, Guoli; Zheng, Lirong; Li, Feng

doi:10.1021/acsami.2c07252

Cited by 32 publications

(13 citation statements)

References 70 publications

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“…It was reported that surface oxygen vacancies are responsible for improving CO 2 adsorption. 60 Therefore, for present CoFe/ ZrO 2 catalysts, the surface-dominant FeO x component with high concentrations of oxygen vacancies may be the main active species for CO 2 hydrogenation.…”

Section: ■ Results and Discussionmentioning

confidence: 98%

Crucial Role of Surface FeO_x Components on Supported Fe-Based Nanocatalysts for CO₂ Hydrogenation to Light Olefins

Zhao

Fan

et al. 2023

Ind. Eng. Chem. Res.

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Currently, Fe-based catalysts show excellent catalytic performance in the hydrogenation of CO 2 to produce light olefins. Despite numerous studies, the identification of the role of catalytically active components over Fe-based catalysts for CO 2 hydrogenation is not quite clear. In this work, a series of ZrO 2supported cobalt-doped Fe-based catalysts were fabricated by a microliquid film reactor-assisted coprecipitation method. It was demonstrated that appropriately strong interactions between Fecontaining species and the ZrO 2 support in catalyst precursors could facilitate the generation of a defective FeO x component upon reduction treatment and inhibit the carburization of metallic iron during the reaction. Among all Fe-based catalysts, the catalyst bearing a (Co + Fe)/ZrO 2 mass ratio of 3:7 and a Co/Fe molar ratio of 1:9 achieved a highest light olefins selectivity of about 38% at 49% CO 2 conversion under reaction conditions (i.e., 320 °C, 2.0 MPa, and 4800 mL•g cat −1 •h −1 ), along with a high Fe time yield to light olefins of 9.2 μmol COd 2 •g Fe −1•s −1 and a low CO selectivity of 4.7%. Comprehensive structural characterization and catalytic CO 2 hydrogenation experiments clarified that the surface-dominant defect-rich FeO x component as catalytically active species substantially played a crucial role in governing the hydrogenation of CO 2 , mainly owing to their enhanced adsorption and binding ability for CO 2 and the CO intermediate. This study offers a new strategy to design Fe-based catalysts and provides deep insight into the role of iron oxide species for CO 2 hydrogenation to produce light olefins.

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Section: ■ Results and Discussionmentioning

confidence: 98%

Crucial Role of Surface FeO_x Components on Supported Fe-Based Nanocatalysts for CO₂ Hydrogenation to Light Olefins

Zhao

Fan

et al. 2023

Ind. Eng. Chem. Res.

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“…Zhang et al developed a Ga-promoted CuCo catalyst for ethanol production by CO 2 hydrogenation, 173 Overall, despite researchers' best efforts to optimize ethanol production, the yield remains quite low, failing to reach 10%. Ethanol production by CO 2 hydrogenation is thus a complex task and requires substantial purification work to obtain a refined product, leading to significantly higher costs than standard ethanol production methods.…”

Section: Ethanol Synthesismentioning

confidence: 99%

“…Zhang et al developed a Ga-promoted CuCo catalyst for ethanol production by CO 2 hydrogenation, using a CuCoGaAl layered double hydroxide precursor. Using a Ga/Co molar ratio of 0.4, they were able to achieve 23.8% ethanol selectivity and 17.8% CO 2 conversion, outperforming most noble-metal catalysts previously explored in literature.…”

Section: Thermochemical Reactionsmentioning

confidence: 99%

“…Introducing Ga into the catalyst structure was demonstrated to improve interactions between Cu and Co, leading to the formation of Cu-CoGaO x and Cu + -CoGaO x interfacial structures in large amounts. They also showed that defectives Cu-CoGaO x and Cu + -CoGaO x structures lead to favored generation of CO and CH x intermediates, promoting the CH x -CO coupling reactions for higher ethanol generation 173. Similarly, Kang et al developed a CoGa 1.0 Al 1.0 O 4 /SiO 2 catalyst to achieve 20.1% ethanol selectivity 174.…”

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confidence: 99%

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New Insights on Catalytic Valorization of Carbon Dioxide by Conventional and Intensified Processes

Olivier

Desgagnés

Mercier

et al. 2023

Ind. Eng. Chem. Res.

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Carbon capture is an emerging technology that is often mentioned as a potential solution to the global warming crisis. However, most of the captured carbon is now treated as waste, discarded, and not used in any meaningful way. On the other hand, from a sustainable development point of view, CO 2 valorization could be a very appealing approach that offers an economic potential when this compound is recycled into valuable chemical products. In this regard, this state-of-the-art review encompasses a wide range of different processes to achieve the conversion of CO 2 into a large variety of products. It does not focus solely on a specific reaction or method, but rather brings different aspects together to provide a far more complete portrait of this emerging subject. Several methods and approaches are discussed, namely thermochemical, electrochemical, photochemical, photoelectrochemical, biochemical, and plasma-assisted conversion. The current state of CO 2 valorization, as well as emerging alternatives and stimulating prospects, was examined, while bearing in mind the realities that limit the application of such technologies. Special emphasis was placed on the optimization of reaction conditions and the development of materials that ensure the best possible production of valuable and environmentally friendly compounds from CO 2 . This review also highlights the challenges related to the application of CO 2 valorization at an industrial scale, which are also important in directing further research in this domain and assessing the prospects of these technologies. Due to the growing number of published papers on the subject, and the limited number of papers offering such a large perspective, we thus believe that this review will be a valuable addition to guide all researchers involved in the field of CO 2 valorization, but also for industrial and political leaders interested in investing in and developing these promising new technologies.

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“…Chemical conversion of CO 2 to high-value-added carbon compounds is an effective way to achieve the carbon cycle. − The thermal catalytic CO 2 hydrogenation reaction has evoked considerable attention, which produces various chemicals including CO, CH 4 , CH 3 OH, olefins, etc. − Among the reported process, the CO 2 methanation reaction (CO 2 + 4H 2 ↔ CH 4 + 2H 2 O) has been considered a promising way since CH 4 can be directly stored and distributed using already existing natural gas pipeline networks. − This is a thermodynamically exothermic reaction (Δ G 298K = −113 kJ·mol –1 and Δ H 298K = −165 kJ·mol –1 ), and a low reaction temperature is favorable to reduce the formation of the byproduct CO . Although great advances have been achieved in noble-metal catalysts (e.g., Ru, , Rh, , and Pd) at low temperatures, they are limited by the low reserve and high price.…”

Section: Introductionmentioning

confidence: 99%

Synergistic Catalysis at the Ni/ZrO_2–x Interface toward Low-Temperature CO₂ Methanation

Wang

Cui

et al. 2023

ACS Appl. Mater. Interfaces

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The CO2 methanation reaction, which achieves the carbon cycle and gains value-added chemicals, has attracted much attention, but the design and exploitation of highly active catalysts remain a big challenge. Herein, zirconium dioxide-supported Ni catalysts toward low-temperature CO2 methanation are obtained via structural topological transformation of NiZrAl-layered double hydroxide (LDH) precursors, which have the feature of an interfacial structure (Ni–O–Zr3+–Vö) between Ni nanoparticles and ZrO2–x support (0 < x < 1). The optimized catalyst (Ni/ZrO2–x -S2) exhibits exceptional CO2 conversion (∼72%) at a temperature as low as 230 °C with a ∼100% selectivity to CH4, without obvious catalyst deactivation within a 110 h reaction at a high gas hourly space velocity of 30,000 mL·g–1·h–1. Markedly, the space–time yield of CH4 reaches up to ∼0.17 ·gcat –1·h–1, which is superior to previously reported Ni catalysts evaluated under similar reaction conditions. Both in situ/operando investigations (diffuse reflectance infrared Fourier transform spectroscopy and X-ray absorption fine structure) and catalytic evaluations substantiate the interfacial synergistic catalysis at the Ni/ZrO2–x interface: the Zr3+–Vö facilitates the activation adsorption of CO2, while the H2 molecule experiences dissociation at the metallic Ni sites. This work demonstrates that the metal–support interface effect plays a key role in improving the catalytic behavior toward CO2 methanation, which can be extended to other high-performance heterogeneous catalysts toward structure-sensitive systems.

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Ga-Promoted CuCo-Based Catalysts for Efficient CO₂ Hydrogenation to Ethanol: The Key Synergistic Role of Cu-CoGaO_x Interfacial Sites

Cited by 32 publications

References 70 publications

Crucial Role of Surface FeO_x Components on Supported Fe-Based Nanocatalysts for CO₂ Hydrogenation to Light Olefins

Crucial Role of Surface FeO_x Components on Supported Fe-Based Nanocatalysts for CO₂ Hydrogenation to Light Olefins

New Insights on Catalytic Valorization of Carbon Dioxide by Conventional and Intensified Processes

Synergistic Catalysis at the Ni/ZrO_2–x Interface toward Low-Temperature CO₂ Methanation

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Ga-Promoted CuCo-Based Catalysts for Efficient CO2 Hydrogenation to Ethanol: The Key Synergistic Role of Cu-CoGaOx Interfacial Sites

Cited by 32 publications

References 70 publications

Crucial Role of Surface FeOx Components on Supported Fe-Based Nanocatalysts for CO2 Hydrogenation to Light Olefins

Crucial Role of Surface FeOx Components on Supported Fe-Based Nanocatalysts for CO2 Hydrogenation to Light Olefins

New Insights on Catalytic Valorization of Carbon Dioxide by Conventional and Intensified Processes

Synergistic Catalysis at the Ni/ZrO2–x Interface toward Low-Temperature CO2 Methanation

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Ga-Promoted CuCo-Based Catalysts for Efficient CO₂ Hydrogenation to Ethanol: The Key Synergistic Role of Cu-CoGaO_x Interfacial Sites

Crucial Role of Surface FeO_x Components on Supported Fe-Based Nanocatalysts for CO₂ Hydrogenation to Light Olefins

Crucial Role of Surface FeO_x Components on Supported Fe-Based Nanocatalysts for CO₂ Hydrogenation to Light Olefins

Synergistic Catalysis at the Ni/ZrO_2–x Interface toward Low-Temperature CO₂ Methanation