Perovskite nanocomposites as effective CO
            <sub>2</sub>
            -splitting agents in a cyclic redox scheme

Zhang, Junshe; Haribal, Vasudev; Li, Fanxing

doi:10.1126/sciadv.1701184

Cited by 110 publications

(105 citation statements)

References 49 publications

Supporting

Mentioning

100

Contrasting

Unclassified

Order By: Relevance

“…When decreasing the reaction temperature to 800°C, it still exhibits a good CO selectivity of 93% and ideal H 2 /CO ratio as shown in Entry 2. It is evident that LSAF6428 is among the best materials so far for the selective conversion of methane to syngas with an extraordinary stability 36,37 . The versatility of OCs using different types of oxidants is another parameter for the potential application.…”

Section: Resultsmentioning

confidence: 99%

In situ encapsulation of iron(0) for solar thermochemical syngas production over iron-based perovskite material

Huang

Chen

et al. 2018

Commun Chem

View full text Add to dashboard Cite

Methane-to-syngas conversion plays an important role in industrial gas-to-liquid technologies, which is commercially fulfilled by energy-intensive reforming methods. Here we present a highly selective and durable iron-based La 0.6 Sr 0.4 Fe 0.8 Al 0.2 O 3-δ oxygen carrier for syngas production via a solar-driven thermochemical process. It is found that a dynamic structural transformation between the perovskite phase and a Fe 0 @oxides core-shell composite occurs during redox cycling. The oxide shell, acting like a micro-membrane, avoids direct contact between methane and fresh iron(0), and prevents coke deposition. This core-shell intermediate is regenerated to the original perovskite structure either in oxygen or more importantly in H 2 O-CO 2 oxidant with simultaneous generation of another source of syngas. Doping with aluminium cations reduces the surface oxygen species, avoiding overoxidation of methane by decreasing oxygen vacancies in perovskite matrix. As a result, this material exhibits high stability with carbon monoxide selectivity above 95% and yielding an ideal syngas of H 2 /CO ratio of 2/1.

show abstract

Section: Resultsmentioning

confidence: 99%

In situ encapsulation of iron(0) for solar thermochemical syngas production over iron-based perovskite material

Huang

Chen

et al. 2018

Commun Chem

View full text Add to dashboard Cite

show abstract

“…Compared to CeO 2 , a considerably higher CO generation efficiency was reported for the Pr 0.5 Sr 0.5 MnO 3−δ perovskite material [217]. [219]. Notably, almost complete CO 2 to CO conversion was reported in the temperature range of 900-980 • C.…”

Section: Solar Fuelsmentioning

confidence: 96%

Perovskites in the Energy Grid and CO2 Conversion: Current Context and Future Directions

et al. 2020

View full text Add to dashboard Cite

CO2 emissions from the consumption of fossil fuels are continuously increasing, thus impacting Earth’s climate. In this context, intensive research efforts are being dedicated to develop materials that can effectively reduce CO2 levels in the atmosphere and convert CO2 into value-added chemicals and fuels, thus contributing to sustainable energy and meeting the increase in energy demand. The development of clean energy by conversion technologies is of high priority to circumvent these challenges. Among the various methods that include photoelectrochemical, high-temperature conversion, electrocatalytic, biocatalytic, and organocatalytic reactions, photocatalytic CO2 reduction has received great attention because of its potential to efficiently reduce the level of CO2 in the atmosphere by converting it into fuels and value-added chemicals. Among the reported CO2 conversion catalysts, perovskite oxides catalyze redox reactions and exhibit high catalytic activity, stability, long charge diffusion lengths, compositional flexibility, and tunable band gap and band edge. This review focuses on recent advances and future prospects in the design and performance of perovskites for CO2 conversion, particularly emphasizing on the structure of the catalysts, defect engineering and interface tuning at the nanoscale, and conversion technologies and rational approaches for enhancing CO2 transformation to value-added chemicals and chemical feedstocks.

show abstract

“…On the other hand, existing thermochemical approaches for CO 2 -splitting require high temperatures and are often subjected to limited CO 2 -to-CO conversion [10,[25][26][27][28][29][30][31] . Sr and Fe-containing perovskite nanocomposites have exhibited exceptional efficacy for both CO 2 -splitting and methane partial oxidation (POx), with >98% CO yield and 96% syngas selectivity in respective steps [32] . However, these materials require high operating temperatures (>950 o C), which do not allow for efficient use of the waste heat.…”

Section: Introductionmentioning

confidence: 99%

Modified Ceria for “Low‐Temperature” CO₂Utilization: A Chemical Looping Route to Exploit Industrial Waste Heat

Haribal

Wang

Dudek

et al. 2019

Advanced Energy Materials

Self Cite

View full text Add to dashboard Cite

Efficient CO 2-utilization is key to limit global climate change. Carbon monoxide, which is a crucial feedstock for chemical synthesis, can be produced by splitting CO 2. However, existing thermochemical routes are energy-intensive requiring high operating temperatures. We report a Hybrid Redox Process (HRP) involving CO 2-to-CO conversion using a lattice oxygen-deprived redox catalyst at relatively low temperatures (<700 °C). The lattice oxygen of the redox catalyst, restored during CO 2-splitting, is subsequently used to convert methane to syngas. Operated at temperatures significantly lower than a number of industrial waste heat sources, this cyclic redox process allows for efficient waste heat-utilization to convert CO 2. To enable the low temperature operation, we report lanthanum modified ceria (1:1 Ce: La) promoted by rhodium (0.5 wt. %) as an effective redox catalyst. Near-complete CO 2 conversion with a syngas yield of up to 83% at low temperatures were achieved using Rh-promoted LaCeO 4-x. While La improves low-temperature bulk redox properties of ceria, Rh considerably enhances the surface catalytic properties for methane-activation. Density Functional Theory calculations further illustrate the underlying functions of La-substitution. The highly effective redox catalyst and HRP scheme provide a potentially attractive route for chemical production using CO 2 , industrial waste heat, and methane, with appreciably lowered CO 2 emissions.

show abstract

Perovskite nanocomposites as effective CO ₂ -splitting agents in a cyclic redox scheme

Abstract: A methane-to-syngas selectivity of 96% and a CO yield of nearly 100% in CO2 splitting were achieved over perovskite nanocomposites in a cyclic redox scheme.

Cited by 110 publications

References 49 publications

In situ encapsulation of iron(0) for solar thermochemical syngas production over iron-based perovskite material

In situ encapsulation of iron(0) for solar thermochemical syngas production over iron-based perovskite material

Perovskites in the Energy Grid and CO2 Conversion: Current Context and Future Directions

Modified Ceria for “Low‐Temperature” CO₂Utilization: A Chemical Looping Route to Exploit Industrial Waste Heat

Contact Info

Product

Resources

About

Perovskite nanocomposites as effective CO 2 -splitting agents in a cyclic redox scheme

Abstract: A methane-to-syngas selectivity of 96% and a CO yield of nearly 100% in CO2 splitting were achieved over perovskite nanocomposites in a cyclic redox scheme.

Cited by 110 publications

References 49 publications

In situ encapsulation of iron(0) for solar thermochemical syngas production over iron-based perovskite material

In situ encapsulation of iron(0) for solar thermochemical syngas production over iron-based perovskite material

Perovskites in the Energy Grid and CO2 Conversion: Current Context and Future Directions

Modified Ceria for “Low‐Temperature” CO2Utilization: A Chemical Looping Route to Exploit Industrial Waste Heat

Contact Info

Product

Resources

About

Perovskite nanocomposites as effective CO ₂ -splitting agents in a cyclic redox scheme

Modified Ceria for “Low‐Temperature” CO₂Utilization: A Chemical Looping Route to Exploit Industrial Waste Heat