Identifying and Engineering Active Sites at the Surface of Porous Single-Crystalline Oxide Monoliths to Enhance Catalytic Activity and Stability

Lin, Guoqing; Li, Hao; Xie, Kui

doi:10.31635/ccschem.021.202000740

Cited by 9 publications

(4 citation statements)

References 34 publications

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“…We begin with the growth of the mother phase of AlF 3 single crystals, cut them into substrates and then treat them in O 2 /Ar atmosphere to grow PSC α‐Al 2 O 3 monolith at 500–700 Torr at 1000–1100 °C [7] . The contamination of transition metal could be negligible.…”

Section: Resultsmentioning

confidence: 99%

Porous Single‐crystalline Centimeter‐sized α‐Al₂O₃ Monoliths for Selective and Durable Non‐oxidative Dehydrogenation of Ethane

Li,

Zhang

et al. 2023

Angew Chem Int Ed

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Alpha alumina (α‐Al2O3) are inert materials with outstanding thermal, chemical and mechanical stability. Herein, we fabricate porous single‐crystalline (PSC) α‐Al2O3 monoliths at centimeter scale to endow them with high catalytic activity while maintaining their stability. We reduce PSC α‐Al2O3 monoliths to create oxygen vacancies in lattice and stabilize them by the ordered lattice to construct unsaturated Al−O coordination structures for enhancing the catalytic activity. The generation of oxygen vacancy at 18e wyckoff position contributes to the unsaturated Al−O coordination. As a case study, we demonstrate the outstanding performance with conversion (≈34 %) and selectivity (≈95 %) toward non‐oxidative dehydrogenation of ethane to ethylene at 700 °C. We achieve the outstanding performance without obvious degradation even after a continuous operation over 1000 hours at 700 °C.

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Section: Resultsmentioning

confidence: 99%

Porous Single‐crystalline Centimeter‐sized α‐Al₂O₃ Monoliths for Selective and Durable Non‐oxidative Dehydrogenation of Ethane

Li,

Zhang

et al. 2023

Angew Chem Int Ed

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“…The single-crystalline skeletons with diameter at the nanoscale significantly reduce the formation of defects that produces recombination centers and results in the scattering of electrons/holes within the materials. The porous architectures not only reduce light scattering to enhance light absorption but also increase the effectiveness of charge utilization by providing sufficient accessible surface areas in the three-dimensional percolation architectures. − …”

Section: Functionalities and Applicationsmentioning

confidence: 99%

Porous Single Crystals at the Macroscale: From Growth to Application

Xie

2023

Acc. Chem. Res.

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Conspectus Porous materials have wide applications in the fields of catalysis, separation, and energy conversion and storage. Porous materials contain pores that are specifically designed to achieve expectant performance. The solid phases in porous materials are normally completely continuous to form the basic porous frame while the pores are fluid phase within the solid phase. Single crystals are macroscopic materials in three spatial dimensions with the constituent atoms, ions, molecules, or molecular assemblies arranged in an orderly repeating pattern with the ordered structures. The growth of single crystals is indeed a process to arrange these constituents in three dimensions into a repeating pattern within the materials. Today the applications of single crystals are exponentially growing in wide fields, and single crystals are therefore unacknowledged as the pillars of our modern technology. Introducing porosity into single crystals would be expected to create a new kind of porous material in which the basic porous frames are single-crystalline and free of grain boundaries. The structural symmetry is completely maintained within the basic porous frames which are a continuous solid phase, but it is completely lost inside the pores. The porous architecture is free of grain boundaries, and the fully interconnected skeletons are in single-crystalline states within the basic porous frames. Single crystals with porosities can therefore be considered to be a new kind of porous material, but they are single-crystal-like because the structural symmetry is maintained only in the skeletons and completely lost within the pores. We therefore call them porous single crystals or consider them in porous single-crystalline states to stand out with their structural features. Porous single crystals at the macroscale combine the advantages of porous materials and single crystals to incorporate both porosity and structural coherence in a porous architecture, leading to invaluable opportunities to alter the material’s properties by controlling the unique structural features to enhance its performance. However, the growth of single crystals in three dimensions reduces the formation of porosities, leading to a fundamental challenge for introducing porosity into single crystals in a traditional process of crystal growth. In this Account, we report the rational design, growth methodology, and microstructural engineering of porous single crystals in a solid–solid transformation. We rationally design a high-density mother phase in a single-crystalline state and transform it into a low-density new phase in a single-crystalline state to introduce porosities into single crystals even incorporating the removal of specific compositions from the mother phase during the growth of porous single crystals. The porosity can be tailored by controlling the change in relative densities from the mother phase to the porous single crystals while the pore size can be engineered by controlling the fabrication conditions. Considering the unique structura...

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“…9 In addition, it has been reported that platinum ions of atomic size are dispersed in the lattice on the twisted surface of Mn 2 O 3 and Mn 3 O 4 to construct isolated active sites, so as to achieve the effect of single-atom catalysis, and oxidized CO at 65 °C. 10 However, due to the high price of these noble metal catalysts, researchers have begun to use relatively cheap transition metal substitutes, such as metal oxides, spinels, perovskites, Hopcalite and alloys. Siderite is the most widely used commercial catalyst.…”

Section: Introductionmentioning

confidence: 99%

Enhanced CO oxidation with cobalt-impregnated porous single-crystal manganese oxides

Jiang

et al. 2023

Catal. Sci. Technol.

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Identifying and Engineering Active Sites at the Surface of Porous Single-Crystalline Oxide Monoliths to Enhance Catalytic Activity and Stability

Cited by 9 publications

References 34 publications

Porous Single‐crystalline Centimeter‐sized α‐Al₂O₃ Monoliths for Selective and Durable Non‐oxidative Dehydrogenation of Ethane

Porous Single‐crystalline Centimeter‐sized α‐Al₂O₃ Monoliths for Selective and Durable Non‐oxidative Dehydrogenation of Ethane

Porous Single Crystals at the Macroscale: From Growth to Application

Enhanced CO oxidation with cobalt-impregnated porous single-crystal manganese oxides

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Identifying and Engineering Active Sites at the Surface of Porous Single-Crystalline Oxide Monoliths to Enhance Catalytic Activity and Stability

Cited by 9 publications

References 34 publications

Porous Single‐crystalline Centimeter‐sized α‐Al2O3 Monoliths for Selective and Durable Non‐oxidative Dehydrogenation of Ethane

Porous Single‐crystalline Centimeter‐sized α‐Al2O3 Monoliths for Selective and Durable Non‐oxidative Dehydrogenation of Ethane

Porous Single Crystals at the Macroscale: From Growth to Application

Enhanced CO oxidation with cobalt-impregnated porous single-crystal manganese oxides

Contact Info

Product

Resources

About

Porous Single‐crystalline Centimeter‐sized α‐Al₂O₃ Monoliths for Selective and Durable Non‐oxidative Dehydrogenation of Ethane

Porous Single‐crystalline Centimeter‐sized α‐Al₂O₃ Monoliths for Selective and Durable Non‐oxidative Dehydrogenation of Ethane