Carbon Dioxide as Feedstock in Selective Oxidation of Propane

Kang, Jungshik; Czaja, Andrew D.; Guliants, Vadim V.

doi:10.1002/ejic.201701049

Cited by 12 publications

(9 citation statements)

References 20 publications

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“…Na-promoted SiO 2 supports have also been employed in an attempt to anchor more monovanadate species with the surface Si−O−Na + . 120 Characterization results confirm the improved surface V density, but along with the formation of inactive Na metavanadate species that selectively produce CO instead of C 3 H 6 (Table 4).…”

Section: Oxidative Dehydrogenation Of Propane With Carbon Dioxidementioning

confidence: 57%

“…To alleviate CO 2 poisoning, a relatively higher but proper CO 2 partial pressure is necessary to ensure more oxidized metal species for the ODHP reaction. Na-promoted SiO 2 supports have also been employed in an attempt to anchor more monovanadate species with the surface Si–O–Na + . Characterization results confirm the improved surface V density, but along with the formation of inactive Na metavanadate species that selectively produce CO instead of C 3 H 6 (Table ).…”

Section: Oxidative Dehydrogenation Of Propane With Carbon Dioxidementioning

confidence: 89%

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Oxidative Dehydrogenation of Propane to Propylene with Soft Oxidants via Heterogeneous Catalysis

et al. 2021

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Oxidative dehydrogenation of propane to propylene can be achieved using conventional, oxygen-assisted dehydrogenation of propane (O2–ODHP) or via the use of soft oxidants, such as CO2, N2O, S-containing compounds, and halogens/halides. The major roles of soft oxidants include inhibiting overoxidation and improving propylene selectivity, which are considered to be current challenges in O2-assisted dehydrogenation. For both CO2– and N2O–ODHP reactions, significant efforts have been devoted to developing redox-active (e.g., chromium, vanadate, iron, etc.), nonredox-type main group metal oxide (e.g., group IIIA, gallium), and other transition metal/metal oxide catalysts (e.g., molybdenum, palladium platinum, rhodium, ruthenium, etc.), as well as zeolite-based catalysts with adjustable acid–base properties, unique pore structures, and topologies. Metal sulfides have shown promising performance in DHP, whereas the development of suitable catalysts has lagged for SO2- or S-assisted ODHP. Recently, significant efforts have been focused on homogeneous and heterogeneous ODHP using halogens (e.g., Br2, I2, Cl2, etc.) and hydrogen halides (e.g., HCl and HBr) for the development of facile processes for C3H6 synthesis. This Review aims to provide a critical, comprehensive review of recent advances in oxidative dehydrogenation of propane with these soft oxidants, particularly highlighting the current state of understanding of the following factors: (i) relationships between composition, structure, and catalytic performance, (ii) effects of the support, acidity, and promoters, (iii) reaction pathway and mechanistic insights, and (iv) the various roles of soft oxidants. Theoretical and computational insights toward understanding reaction mechanisms and catalyst design principles are also covered. Future research opportunities are discussed in terms of catalyst design and synthesis, deactivation and regeneration, reaction mechanisms, and alternative approaches.

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Section: Oxidative Dehydrogenation Of Propane With Carbon Dioxidementioning

confidence: 57%

Section: Oxidative Dehydrogenation Of Propane With Carbon Dioxidementioning

confidence: 89%

Oxidative Dehydrogenation of Propane to Propylene with Soft Oxidants via Heterogeneous Catalysis

et al. 2021

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“…[8][9][10][11][12][13] Although reaction with CO2 generally leads to lower conversion in comparison to commercialized dehydrogenation processes, the selectivity in a CO2-ODH reaction is significantly improved. 14,15 The mechanism for the ODH of light alkanes with CO2 has not been thoroughly explained, although different pathways have been proposed. It has been reported that the redox and acidbase properties of oxides can determine which of two pathways the reaction takes.…”

Section: Introductionmentioning

confidence: 99%

Elucidating the Role of CO₂ in the Soft Oxidative Dehydrogenation of Propane over Ceria-Based Catalysts

et al. 2018

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A mixed oxide support containing Ce, Zr and Al was synthesized using a physical grinding method and applied in the oxidative dehydrogenation of propane using CO2 as the oxidant. The activity of the support was compared with that of fully-formulated catalysts containing palladium. The Pd/CeZrAlOx material exhibited long-term stability and selectivity to propene (during continuous operation for 140 h) which is not normally associated with dehydrogenation catalysts. From temperature-programmed desorption of NH3 and CO2 it was found that the catalyst possessed both acidic and basic sites. In addition, temperature programmed reduction showed that palladium promoted both the reduction and re-oxidation of the support. When the role of CO2 was investigated in the absence of gas-phase oxidant, using a Temporal Analysis of Products (TAP) reactor, it was found that CO2 dissociates over the reduced catalyst leading to formation of CO and selective oxygen species. It is proposed that CO2 has the dual role of regenerating selective oxygen species, and shifting the equilibrium for alkane dehydrogenation by consuming H2 through the reverse water-gas-shift reaction. These two mechanistic functions have previously been considered to be mutually exclusive.

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“…Generally, vanadium oxide can form vanadate with alkali metals. Guliants et al varied the surface coverage of VO x species by using sodium on the silica surface [86]. They found that Na ?…”

Section: Vanadium-based Catalystsmentioning

confidence: 99%

Research progress of CO2 oxidative dehydrogenation of propane to propylene over Cr-free metal catalysts

Wang

et al. 2022

Rare Met.

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CO 2 -assisted oxidative dehydrogenation of propane (CO 2 -ODHP) is an attractive strategy to offset the demand gap of propylene due to its potentiality of reducing CO 2 emissions, especially under the demands of peaking CO 2 emissions and carbon neutrality. The introduction of CO 2 as a soft oxidant into the reaction not only averts the over-oxidation of products, but also maintains the high oxidation state of the redox-active sites. Furthermore, the presence of CO 2 increases the conversion of propane by coupling the dehydrogenation of propane (DHP) with the reverse water gas reaction (RWGS) and inhibits the coking formation to prolong the lifetime of catalysts via the reverse Boudouard reaction. An effective catalyst should selectively activate the C-H bond but suppress the C-C cleavage. However, to prepare such a catalyst remains challenging. Chromium-based catalysts are always applied in industrial application of DHP; however, their toxic properties are harmful to the environment. In this aspect, exploring environment-friendly and sustainable catalytic systems with Cr-free is an important issue. In this review, we outline the development of the CO 2 -ODHP especially in the last ten years, including the structural information, catalytic performances, and mechanisms of chromium-free metal-based catalyst systems, and the role of CO 2 in the reaction. We also present perspectives for future progress in the CO 2 -ODHP.

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Carbon Dioxide as Feedstock in Selective Oxidation of Propane

Cited by 12 publications

References 20 publications

Oxidative Dehydrogenation of Propane to Propylene with Soft Oxidants via Heterogeneous Catalysis

Oxidative Dehydrogenation of Propane to Propylene with Soft Oxidants via Heterogeneous Catalysis

Elucidating the Role of CO₂ in the Soft Oxidative Dehydrogenation of Propane over Ceria-Based Catalysts

Research progress of CO2 oxidative dehydrogenation of propane to propylene over Cr-free metal catalysts

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Carbon Dioxide as Feedstock in Selective Oxidation of Propane

Cited by 12 publications

References 20 publications

Oxidative Dehydrogenation of Propane to Propylene with Soft Oxidants via Heterogeneous Catalysis

Oxidative Dehydrogenation of Propane to Propylene with Soft Oxidants via Heterogeneous Catalysis

Elucidating the Role of CO2 in the Soft Oxidative Dehydrogenation of Propane over Ceria-Based Catalysts

Research progress of CO2 oxidative dehydrogenation of propane to propylene over Cr-free metal catalysts

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Elucidating the Role of CO₂ in the Soft Oxidative Dehydrogenation of Propane over Ceria-Based Catalysts