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2.2.2. Thermal decomposition of carbon dioxide
The thermal decomposition of carbon dioxide into carbon monoxide and oxygen is considered to be a potential route for
carbon dioxide capture and utilization. However, carbon dioxide decomposition is limited by its thermodynamic
equilibrium. To achieve a high conversion, high-density energy inputs such as a very high temperature (> 1727 oC) are
necessary in a fixed-bed reactor. Integrating the TDCD and POM reactions in a dense CMR shows a remarkable advance in
utilization of carbon dioxide to supply oxygen for the POM reaction [70,73,79–81]. As shown in Fig. 6(a), a dense
CMR based on a disk-like SrCo0.4Fe0.5Zr0.1O3−δ membrane was designed for the coupling of the TDCD and POM reactions.
The TDCD reactions take place on one side of the membrane in the presence of a supported lead (Pb)-based catalyst, and
methane reacts with oxygen (which permeates from the TDCD side) over a supported nickel (Ni)-based catalyst on the
other side of the membrane. At 900 oC, the carbon monoxide selectivity and carbon dioxide conversion reached 100% and
15.8%, respectively [70]. For given external conditions, the decomposition of carbon dioxide benefits from the increase of
oxygen permeation flux [81]. Normally, the oxygen permeation flux can be promoted by decreasing the thickness of the
membrane (i.e., when bulk diffusion is the rate-determining step). Zhang et al. [79] performed coupling reactions using an
SCFA thin tubular membrane with a reduced thickness, which gave it a higher oxygen flux than a disk-like membrane. At
950 oC, the carbon dioxide conversion reached approximately 17%, which is higher than the conversion obtained when
using a disc-like membrane at the same operation temperature.
Having the POM occur on the opposite side of the membrane to the TDCD can increase the driving force and promote
carbon dioxide decomposition. However, the membrane in this case was actually in a much more complicated environment,
as one side was exposed to CO2/CO while the other side was exposed to CH4/CO/H2. As discussed in the previous section,
a compromise between high oxygen permeability and sufficient chemical stability is necessary in a membrane reactor.
Therefore, a triple-layer composite structure (porous/dense/porous) for the TDCD and POM coupling reaction was
proposed [73] (Fig. 6(b)). SBFM and La0.8Sr0.2MnO3--yttria-stabilized zirconia (LSM-YSZ) were fabricated as porous
layers on the dense SCFNb membrane, and were closed to the POM and TDCD sides, respectively. The functions of
reduction resistance, carbon dioxide resistance, and high permeability were segregated to the SBFM, LSM-YSZ, and
SCFNb layers, respectively. The essence of this design is that each of the layers plays its respective function and
synergistically contributes to improve the stability and conversion. This novel reactor attained a 20.58% carbon dioxide
conversion at 900 oC, and could be steadily operated for more than 500 h [73]. ...

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