Utilizing CO₂ as a Reactant for C₃ Oxygenate Production via Tandem Reactions

Abstract

One possible solution to closing the loop on carbon emissions is using CO 2 as the carbon source to generate highvalue, multicarbon products. In this Perspective, we describe four tandem reaction strategies for converting CO 2 into C 3 oxygenated hydrocarbon products (i.e., propanal and 1-propanol), using either ethane or water as the hydrogen source: (1) thermocatalytic CO 2assisted dehydrogenation and reforming of ethane to ethylene, CO, and H 2 , followed by heterogeneous hydroformylation, (2) one-pot conversion of CO 2 and ethane using plasma-activated reactions in combination with thermocatalysis, (3) electrochemical CO 2 reduction to ethylene, CO, and H 2 , followed by thermocatalytic hydroformylation, and (4) electrochemical CO 2 reduction to CO, followed by electrochemical CO reduction to C 3 oxygenates. We discuss the proof-of-concept results and key challenges for each tandem scheme, and we conduct a comparative analysis of the energy costs and prospects for net CO 2 reduction. The use of tandem reaction systems can provide an alternative approach to traditional catalytic processes, and these concepts can be further extended to other chemical reactions and products, thereby opening new opportunities for innovative CO 2 utilization technologies.

Membrane Electrode Assembly for Electrocatalytic CO2 Reduction: Principle and Application

“…Through this tandem strategy, CO 2 was firstly electrochemically reduced to ethylene, CO, and H 2 with Cu catalyst, followed by the thermochemical hydroformylation reaction to produce 1‐propanol and propanal via using Rh 1 Co 3 /MCM‐41 catalyst [124] . This kind of tandem system would be another promising method for C 2+ production from CO 2 [125] …”

“…[124] This kind of tandem system would be another promising method for C 2 + production from CO 2 . [125]…”

Bimetallic-Derived Catalytic Structures for CO2-Assisted Ethane Activation

“…Crucially, verifying potential CO 2 reduction in the new tandem processes requires a comprehensive CO 2 footprint analysis. 16 The intertwined nature of multiple interactions presents significant challenges in establishing structure−function correlations and can lead to structural heterogeneity, compromising the catalytic performance. Hence, self-constrained and precise synthesis strategies (e.g., strong electrostatic adsorption, atomic layer deposition, galvanic replacement, and thermal shock methods) can be employed to potentially produce uniform alloy or inverse interfacial structures with optimized site densities.…”

“…Additionally, integrating additional reaction chemistries (e.g., hydrocarboxylation: C 2 H 4 + CO + H 2 O → CH 3 CH 2 COOH) in the downstream reactor can expand value-added product types and improve the atom efficiency from CO 2 –ethane upgrading reactions. Crucially, verifying potential CO 2 reduction in the new tandem processes requires a comprehensive CO 2 footprint analysis …”

“…Ethane is often underutilized in conventional petrochemical processes, despite its substantial global supply from shale gas reserves . Recent developments have explored the simultaneous upgrading of ethane and CO 2 , enabling the synthesis of valuable gaseous (CO, H 2 , and olefins) and liquid (e.g., aromatics and oxygenates) chemicals that are essential to various industries worldwide. − A recent analysis of CO 2 footprint reveals the potential to achieve a net CO 2 reduction in the CO 2 –ethane reactions …”