Interfacial Active Sites for CO2 Assisted Selective Cleavage of C–C/C–H Bonds in Ethane

Simultaneously upgrading CO2 and light alkanes into value‐added products

“…Copyright 2019, Wiley‐VCH Verlag GmbH & Co. (C)–(F) and (H) were adapted from Ref. 18 with permission. Copyright 2020, Elsevier.…”

“…Diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) is widely applied for the in situ analysis of surface intermediates and for determining the surface termination with appropriate probe molecules (e.g., CO and N 2 O). For example, as illustrated in Figure 1H, DRIFTS results following CO adsorption suggest that the FeO x species interact with the Pd(111) facets of supported Pd particles, given the more suppression of its characteristic peak (~1925 cm −1 ) with the doping of FeO x species 18 …”

“…The CO 2 ‐assisted DR and ODH of ethane have been extensively studied over a wide range of catalysts, including monometallic, bimetallic, and metal carbide catalysts 16‐19,30‐33 . The effect of oxide support has also been investigated over reducible and irreducible oxides for both DR 34 and ODH 35 .…”

“…For example, it has been suggested that oxygen species are essential for the effective activation of the CH bond in alkanes, 33,40 although it is still less understood whether and how the electronic and geometric properties of the oxygen species generated from CO 2 dissociation would affect the selective cleavage of CC/CH bonds of alkanes. Using Pd–Fe bimetallic catalysts as a case study, Xie et al 18 investigated the properties of oxygen species at different interfacial sites and their roles in controlling the activity and selectivity of SU‐CO 2 Et over bimetallic PdFe x /CeO 2 catalysts. As demonstrated in Figure 2B, flow reactor experiments displayed that the 1.0%Pd/CeO 2 catalyst showed a high initial ethane conversion (~34%) with nearly 100% selectivity to CO and was subsequently deactivated to ~5% at the pseudo‐steady (PS) state.…”

“…In this Perspective, we discuss recent advances of CO 2 ‐assited dehydrogenation, aromatization, and hydroformylation reactions. Depending on the selective bond cleavage of light alkanes, the gaseous products can be syngas (CO and H 2 ) and olefins from the CO 2 ‐assisted dry reforming (DR, both CC and CH bond scission) and oxidative dehydrogenation (ODH, CH bond scission only) pathways, respectively 16‐19 . Moreover, the gaseous product stream (CO, H 2 , and olefins) can be further upgraded into value‐added liquid products, such as aromatics (e.g., benzene, toluene, and xylenes [BTX]) via a tandem aromatization process 20 or oxygenates via a downstream hydroformylation process using tandem reactors 21 .…”