Impact of 1% Lanthanum Dopant on Carbonaceous Fuel Redox Reactions with an Iron-Based Oxygen Carrier in Chemical Looping Processes

Qin, Lang; Cheng, Zhuo; Guo, Mengqing; Xu, Mingyuan; Fan, Jonathan A.; Fan, Liang‐Shih

doi:10.1021/acsenergylett.6b00511

Cited by 83 publications

(42 citation statements)

References 21 publications

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“…The calculated α-Fe 2 O 3 bulk lattice parameters were a = b = 5.04 Å and c = 13.83 Å, in good agreement with the experimental values ( a = b = 5.038 Å and c = 13.772 Å). The α-Fe 2 O 3 (001) surface with Fe-O 3 -Fe- termination was chosen to model the iron oxide slab with a thickness of ~15 Å 29 . Fe 2 O 3 nanoparticles were modeled by a three-dimensional periodic arrangement with a large cubic cell of 5 × 5 × 5 nm 3 to minimize lateral interactions.…”

Section: Methodsmentioning

confidence: 99%

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

et al. 2019

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Chemical looping methane partial oxidation provides an energy and cost effective route for methane utilization. However, there is considerable CO2 co-production in current chemical looping systems, rendering a decreased productivity in value-added fuels or chemicals. In this work, we demonstrate that the co-production of CO2 can be dramatically suppressed in methane partial oxidation reactions using iron oxide nanoparticles embedded in mesoporous silica matrix. We experimentally obtain near 100% CO selectivity in a cyclic redox system at 750–935 °C, which is a significantly lower temperature range than in conventional oxygen carrier systems. Density functional theory calculations elucidate the origins for such selectivity and show that low-coordinated lattice oxygen atoms on the surface of nanoparticles significantly promote Fe–O bond cleavage and CO formation. We envision that embedded nanostructured oxygen carriers have the potential to serve as a general materials platform for redox reactions with nanomaterials at high temperatures.

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Section: Methodsmentioning

confidence: 99%

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

et al. 2019

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“…DFT calculations indicated that 1 % La dopant preferred to migrate to the outermost layer of the iron oxide surface with the least surface energy of 1.39 J/m 2 (Figure 14(c)), on which CH 4 adsorbed (0.12 eV vs . 0.06 eV) and dissociated more facilely compared with Fe sites in un‐doped Fe 2 O 3 (Figure 14(b)) [63] . Such the promotional influence on CH 4 conversion was also reported in 1 % Cu doped Fe 2 O 3 wherein Cu dopants was not enriched on the surface like La and was able to favor the formation the oxygen vacancies in Fe 2 O 3 , which significantly lowers the barrier of CH 4 activation by the path of CH x species adsorbed on the neighboring oxygen vacancies and H on Cu adsorption sites [64] .…”

Section: Oxygen Carriersmentioning

confidence: 99%

“… (a) Conversion of La‐doped and undoped Fe 2 O 3 for 5 min reduction at 1000 °C with CH 4 ; (b) Energy profile of CH 4 activation on the Fe 2 O 3 surface and on the 1 % La‐doped Fe 2 O 3 surface; (c) Optimized structure of α‐Fe 2 O 3 (001) surfaces with 1 % La dopant in four different sites. Purple, red, and blue balls represent Fe, O, and La atoms, respectively [63] . Reproduced with permission from Ref.…”

Section: Oxygen Carriersmentioning

confidence: 99%

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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“…Since metal oxides play a crucial role in the CLPOM, substantial research efforts have been devoted to the design and development of efficient oxygen carriers, which have high oxygen-carrying capacities, high selectivities toward syngas, and excellent redox reactivities [8]. Metal oxides such as nickel oxides [9][10][11], copper oxides [12], ferrite oxides [8,[13][14][15], and tungsten oxides [16] have been applied in CLPOM and have shown great potential.…”

Section: Introductionmentioning

confidence: 99%