Cation-swapped homogeneous nanoparticles in perovskite oxides for high power density

Joo, Sangwook; Kwon, Oh Hun; Kim, Kyeounghak; Kim, Seona; Kim, Hyunmin; Shin, Jeeyoung; Jeong, Hu Young; Sengodan, Sivaprakash; Han, Jeong Woo; Kim, Guntae

doi:10.1038/s41467-019-08624-0

Cited by 144 publications

(111 citation statements)

References 35 publications

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“…A lower temperature was also reported by Steiger et al for LaFe0.8Ni0.2O3-δ with Ni nanoparticle exsolution by reduction at 873 K [35]. Joo et al reduced a cobalt doped Mn-based perovskite at 1023 K to achieve Co nanoparticle exsolution [36].…”

Section: Exsolution Propertiesmentioning

confidence: 71%

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Modifying the Surface Structure of Perovskite-Based Catalysts by Nanoparticle Exsolution

et al. 2020

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In heterogeneous catalysis, surfaces decorated with uniformly dispersed, catalytically-active (nano)particles are a key requirement for excellent performance. Beside standard catalyst preparation routines—with limitations in controlling catalyst surface structure (i.e., particle size distribution or dispersion)—we present here a novel time efficient route to precisely tailor catalyst surface morphology and composition of perovskites. Perovskite-type oxides of nominal composition ABO3 with transition metal cations on the B-site can exsolve the B-site transition metal upon controlled reduction. In this exsolution process, the transition metal emerges from the oxide lattice and migrates to the surface where it forms catalytically active nanoparticles. Doping the B-site with reducible and catalytically highly active elements, offers the opportunity of tailoring properties of exsolution catalysts. Here, we present the synthesis of two novel perovskite catalysts Nd0.6Ca0.4FeO3-δ and Nd0.6Ca0.4Fe0.9Co0.1O3-δ with characterisation by (in situ) XRD, SEM/TEM and XPS, supported by theory (DFT+U). Fe nanoparticle formation was observed for Nd0.6Ca0.4FeO3-δ. In comparison, B site cobalt doping leads, already at lower reduction temperatures, to formation of finely dispersed Co nanoparticles on the surface. These novel perovskite-type catalysts are highly promising for applications in chemical energy conversion. First measurements revealed that exsolved Co nanoparticles significantly improve the catalytic activity for CO2 activation via reverse water gas shift reaction.

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Section: Exsolution Propertiesmentioning

confidence: 71%

“…In comparison to our studied perovskites, other groups reported generally much higher reduction temperatures for nanoparticle exsolution. Gao [36].…”

Section: Exsolution Propertiesmentioning

confidence: 99%

Modifying the Surface Structure of Perovskite-Based Catalysts by Nanoparticle Exsolution

et al. 2020

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“…Only 0.011 mol of Fe was required using ALD, whereas 0.176 mol of Fe was necessary using the infiltration method ( fig. S4) (24). The effectiveness of topotactic exsolution using ALD is about 16 times higher than that using the previous infiltration owing to the features of regular and thin deposition of ALD.…”

Section: Topotactic Exsolution Via Aldmentioning

confidence: 95%

“…If only the value of the A/B ratio can be lowered, it would lead to a new equilibrium position to make particle exsolution much more dynamic. The topotactic exsolution can be used here as a way to lower the A/B ratio value (24). That is, the introduced guest cation B′ can be substituted into the B-site (substitution step in fig.…”

Section: Topotactic Exsolution Via Aldmentioning

confidence: 99%

“…We have previously shown that the different cosegregation tendency of transition metal dopants can be used for topotactic exsolution. That is, the cosegregation tendency of the depositing guest ion should be lower than that of the exsolving host ion (24,27,29). Therefore, we examined the cosegregation energies for single dopant elements of various transition metals as well as host Ti cation (Fig.…”

Section: Dft Calculationsmentioning

confidence: 99%

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Highly active dry methane reforming catalysts with boosted in situ grown Ni-Fe nanoparticles on perovskite via atomic layer deposition

et al. 2020

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With the need for more stable and active metal catalysts for dry reforming of methane, in situ grown nanoparticles using exsolution are a promising approach. However, in conventional exsolution, most nanoparticles remain underneath the surface because of the sluggish diffusion rate of cations. Here, we report the atomic layer deposition (ALD)–combined topotactic exsolution on La0.6Sr0.2Ti0.85Ni0.15O3-δ toward developing active and durable catalysts. The uniform and quantitatively controlled layer of Fe via ALD facilitates the topotactic exsolution, increasing finely dispersed nanoparticles. The introduction of Fe2O3 yields the formation of Ni-Fe alloy owing to the spontaneous alloy formation energy of −0.43 eV, leading to an enhancement of the catalytic activity for dry methane reforming with a prolonged stability of 410 hours. Overall, the abundant alloy nanocatalysts via ALD mark an important step forward in the evolution of exsolution and its application to the field of energy utilization.

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Manipulating and Optimizing the Hierarchically Porous Electrode Structures for Rapid Mass Transport in Solid Oxide Cells

Hou

Pan

et al. 2022

Adv Funct Materials

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Over the past decades, considerable efforts have been made to develop hierarchically porous electrodes for the high surface area, the fast velocity of fuels/products to/away from the reaction site, and the high loading of thermal-and/or electrochemical-catalysts. Manipulation of the hierarchical structure is one of the key steps for high performance in applications of efficient energy storage and conversion such as solid oxide cells. This review starts with a brief introduction to the basic concept of mass transport and how mass transport may affect performance. Then, the latest developments in enhancing the performance of cells through modification or optimization of the hierarchically porous electrode structures, including altering the geometry or morphology and increasing the triple-phase boundaries length of electrodes are summarized. Subsequently, the unique characteristics of microstructures that are critical to enhancing electrode performance and provide important insights into the mechanisms of performance (activity and durability) enhancement, aiming at achieving the rational design of better electrode architecture are highlighted. Finally, the remaining challenges for the knowledge-based design of highly efficient electrodes for electrochemical devices, together with possible directions and future perspectives for the development of highly efficient electrodes through optimization of microstructure are discussed.

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Cation-swapped homogeneous nanoparticles in perovskite oxides for high power density

Cited by 144 publications

References 35 publications

Modifying the Surface Structure of Perovskite-Based Catalysts by Nanoparticle Exsolution

Modifying the Surface Structure of Perovskite-Based Catalysts by Nanoparticle Exsolution

Highly active dry methane reforming catalysts with boosted in situ grown Ni-Fe nanoparticles on perovskite via atomic layer deposition

Manipulating and Optimizing the Hierarchically Porous Electrode Structures for Rapid Mass Transport in Solid Oxide Cells

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