The catalytic reduction of CO 2 by propane may occur via dry reforming to produce syngas (CO + H 2 ) or oxidative dehydrogenation to yield propylene. Utilizing propane and CO 2 as coreactants presents several advantages over conventional methane dry reforming or direct propane dehydrogenation, including lower operating temperatures and less coke formation. Thus, it is of great interest to identify catalytic systems that can either effectively break the C C bond to generate syngas or selectively break C H bonds to produce propylene. In this study, several precious and nonprecious bimetallic catalysts supported on reducible CeO 2 were investigated using flow reactor studies at 823 K to identify selective catalysts for CO 2 -assisted reforming and dehydrogenation of propane.
K E Y W O R D SCeO 2 , CO 2 soft oxidant, propane, propylene, synthesis gas
| INTRODUCTIONCarbon dioxide management is a prominent issue facing society that requires a diverse portfolio of innovative technologies. High atmospheric concentrations of CO 2 contribute to adverse effects that impact human health and the climate. The need to reduce CO 2 is evident, and the International Panel on Climate Change has stated that climate stabilization (no more than a 2 C rise from preindustrial levels) will require a combination of mitigation, utilization, and even negative emission technologies. 1 Thus, one key approach will be to transform abundant CO 2 into a useful feedstock for processes that not only produce high value products but also match the scale necessary to impact anthropogenic emissions.The two most relevant reactions for the catalytic conversion of CO 2 to CO are reverse water gas shift (RWGS) and dry reforming of methane (DRM). The CO product can be utilized as feedstock for Fischer-Tropsch reactions or methanol synthesis. These two reduction chemistries are not without obstacles, beginning with the challenge that CO 2 is the most thermodynamically stable carbon/oxygen-based molecule (ΔG F = −394 kJ mol −1 ). 2 Current implementation of RWGS has limited feasibility since efforts to obtain large amounts of renewable and CO 2 -free hydrogen are still under development. 3 Furthermore, high coke deposition rates at the reaction temperatures required for DRM hinders further significant improvements in catalyst stability. 4,5 A viable alternative is to utilize other light hydrocarbons, such as ethane or propane, as feedstock for CO 2 reduction. In addition to reforming, these light alkanes contain the C C bond that can be advantageously utilized to build olefins. 6 Thus, the reduction of CO 2 via light alkanes offers two distinct reaction pathways: dry reforming and oxidative dehydrogenation. Specifically, it is of interest to explore the use of propane due to its increasing abundance, competitive pricing, and the demand for propylene, which is one of the most diverse petrochemical building blocks used in the production of various chemicals such as fibers and textiles for a variety of applications.Currently, propylene is primarily coproduced by...