Near 100% CO selectivity in nanoscaled iron-based oxygen carriers for chemical looping methane partial oxidation

Liu, Yan; Fan, Liang‐Shih; Cheng, Zhuo; Goetze, Josh W.; Kong, Fanhe; Fan, Jonathan A.

doi:10.1038/s41467-019-13560-0

Cited by 124 publications

(80 citation statements)

References 33 publications

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“…DFT calculations demonstrated that such a high CO selectivity of confined Fe species in garnet originated from enhanced oxygen vacancy formation energy (Eov) compared with Fe 2 O 3 , which resulted from the lattice oxygen shared by not only reducible Fe ions but also nonreducible Al and Y ones in a garnet structure [25] . Near 100 % CO selectivity was also achieved with higher conversion (Figure 4(a and b)) when decreasing the size of Fe 2 O 3 particles to nanoscale by embedding it into SBA‐15 mesoporous silica which was quite distinct with the previous work involving microscale Fe‐based OCs (Figure 4(c)) [26] . Such the superior selectivity was attributed to smaller average coordination number of surface Fe atoms in nano‐Fe 2 O 3 significantly favoring CH 4 adsorption and low‐coordinated lattice oxygen atoms on the surface of nanoparticle promoting Fe−O bond cleavage as well as CO formation, supported by DFT calculations (Figure 4(d and e)).…”

Section: Oxygen Carriersmentioning

confidence: 53%

“…Fe 2 O 3 @SBA‐15 oxygen carrier; (d) Calculated energies of CH 4 adsorption. E ad (kJ mol −1 ), on Fe atop site and O atop site of (Fe 2 O 3 ) n nanoparticles as a function of n. The adsorption trends are shown by the blue and red lines; (e) Energy profile of CH 4 partial oxidation on Fe 40 O 60 nanoparticle and Fe 2 O 3 (001) surface [26] . Reproduced with permission from Ref.…”

Section: Oxygen Carriersmentioning

confidence: 99%

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Recent Advances of Oxygen Carriers for Chemical Looping Reforming of Methane

et al. 2021

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This review discussed recent advances of oxygen carriers (OCs) for chemical looping reforming (CLR) of CH4 which aims to generate high‐quality syngas, an important chemical intermediate for the synthesis of chemicals and fuels. We firstly introduced CLR and that combined with CO2 and H2O splitting as well as clarified their advantages over conventional reforming processes. Then we reviewed the latest advances of metal‐based OCs, composite OCs including perovskites and hexaaluminates, and catalytic OCs, namely oxygen‐containing materials with catalytically metal sites, during the past five years. Specific discussion focused on the influence of composition, surface, and bulk structure of these OCs on conversion, selectivity, and lattice oxygen reactivity to summarize design and optimization strategies of the tailored OCs. Finally, a brief summary and an outlook on some of the scientific challenges and suggestions for future investigations on the development of outstanding OCs for CLR of CH4 are given.

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Section: Oxygen Carriersmentioning

confidence: 53%

Section: Oxygen Carriersmentioning

confidence: 99%

Recent Advances of Oxygen Carriers for Chemical Looping Reforming of Methane

et al. 2021

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“…Chemical looping processes are a promising route for improving energy efficiency, [1][2][3][4] leveraging renewable energy sources, [5][6][7][8][9][10][11] facilitating chemical conversions, [12][13][14][15][16][17][18][19][20] and reducing undesirable emissions across many sectors of the chemical industry. [21][22][23][24][25][26] In a chemical looping (CL) process, the overall reaction is separated into multiple (typically two) subreactions, each mediated by the redox chemistry of a "looped" active material.…”

Section: Introductionmentioning

confidence: 99%

High-Throughput Analysis of Materials for Chemical Looping Processes

Singstock¹,

Bartel²,

Holder³

et al. 2020

Preprint

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Chemical looping is a promising approach for improving the energy efficiency of many industrial chemical processes. However, a major limitation of modern chemical looping technologies is the lack of suitable active materials to mediate the involved subreactions. Identification of suitable materials has been historically limited by the scarcity of high-temperature (> 600 °C) thermochemical data to evaluate candidate materials. An accurate thermodynamic approach is demonstrated here to rapidly identify active materials which is applicable to a wide variety of chemical looping chemistries. Application of this analysis to chemical looping combustion correctly classifies 17/17 experimentally studied redox materials by their viability and identifies over 1,300 promising yet previously unstudied active materials. This approach is further demonstrated by analyzing redox pairs for mediating a novel chemical looping process for producing pure SO2 from raw sulfur and air which could provide a more efficient and lower emission route to sulfuric acid. 12 promising redox materials for this process are identified, two of which are supported by previous experimental studies of their individual oxidation and reduction reactions. This approach provides the necessary foundation for connecting process design with high-throughput materials discovery to accelerate the innovation and development of a wide-range of chemical looping technologies.

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“…Oxidants like O2, H2O and air have been widely used for regenerating OCs 16,17 , and thus the CLCS process lowers the requirement for extra purification and exhibits the potential of directly utilizing impure CO2. Different from well-known dry reforming of CO2 18,19 , the CLCS process takes advantage of producing syngas with controllable H2/CO ratio and pure CO 15,20 . In addition, the separately obtained syngas and CO products can be directly used for green acetic acid production 15 .…”

Section: Introductionmentioning

confidence: 99%

Polyfunctional perovskite oxides optimized for efficient CO2 splitting against oxidative impurity via chemical looping

Liao

Long

Chen

et al. 2020

Preprint

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Via redox chemistry, chemical looping reduction of CO2 to CO provides a promising strategy for mitigating carbon emissions. However, it’s still challenging to directly reduce CO2/O2 mixture gas due to lack of effective oxygen carriers towards reductive C–O bond scission in the presence of strongly oxidative gas. Here, we report an autocatalytic strategy of polyfunctional perovskite oxides to achieve enhanced C–O bond activation and superior performance of methane driven syngas generation. The self-generated Ni nanoparticles, through Ni cations migrating from the bulk lattice to the surface of LaFeO3 perovskite under fast methane reduction, are identified as catalytically active sites for enhancing C-H activation in the methane oxidation step. The reduced Ni-LaFeO3 oxygen carrier features multifunctional active sites with Ni species for accelerating C–O activation and oxygen vacancies for O2 adsorption in the step of CO2 splitting with the presence of abundant O2. At 800℃, the 5 at.% Ni-LaFeO3 perovskite stably exhibited high performances during 100 redox cycles: 98% CO selectivity in the methane oxidation step, and 98.5% CO2 conversion in the step of CO2 splitting even with the presence of 25 at.% O2. This efficient and durable perovskite underpins an economic utilization of impure CO2 from various carbon sources with no requirement for energy-costing purifications.

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Near 100% CO selectivity in nanoscaled iron-based oxygen carriers for chemical looping methane partial oxidation

Cited by 124 publications

References 33 publications

Recent Advances of Oxygen Carriers for Chemical Looping Reforming of Methane

Recent Advances of Oxygen Carriers for Chemical Looping Reforming of Methane

High-Throughput Analysis of Materials for Chemical Looping Processes

Polyfunctional perovskite oxides optimized for efficient CO2 splitting against oxidative impurity via chemical looping

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