Ultrastable single-atom gold catalysts with strong covalent metal-support interaction (CMSI)

Qiao, Botao; Liang, Jia; Wang, Aiqin; Xu, Chao; Li, Jun; Zhang, Tao; Liu, Jingyue Jimmy

doi:10.1007/s12274-015-0796-9

Cited by 464 publications

(415 citation statements)

References 77 publications

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“…Activity for various reactions has so far been demonstrated for metals including Ir [483], Au [484], Pt [485][486][487][488], and this has motivated theoretical studies aimed at understanding how it is that a single atom can function as a catalyst [489]. Unfortunately, the complexity of the "FeO x " support, usually a reduced α-Fe 2 O 3 , means that the termination of the oxide is not known.…”

Section: Metalsmentioning

confidence: 99%

Iron oxide surfaces

Parkinson

2016

Surface Science Reports

499

463

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The current status of knowledge regarding the surfaces of the iron oxides, magnetite (Fe 3 O 4 ), maghemite (γ-Fe 2 O 3 ), hematite (α-Fe 2 O 3 ), and wüstite (Fe 1-x O) is reviewed. The paper starts with a summary of applications where iron oxide surfaces play a major role, including corrosion, catalysis, spintronics, magnetic nanoparticles (MNPs), biomedicine, photoelectrochemical water splitting and groundwater remediation. The bulk structure and properties are then briefly presented; each compound is based on a close-packed anion lattice, with a different distribution and oxidation state of the Fe cations in interstitial sites. The bulk defect chemistry is dominated by cation vacancies and interstitials (not oxygen vacancies) and this provides the context to understand iron oxide surfaces, which represent the front line in reduction and oxidation processes. The atomic-scale structure of the low-index surfaces of iron oxides is the major focus of this review. Fe 3 O 4 is the most studied iron oxide in surface science, primarily because its stability range corresponds nicely to the ultra-high vacuum environment, and because it is an electrical conductor, which makes it straightforward to study with the most commonly used surface science methods such as photoemission spectroscopies (XPS, UPS) and scanning tunneling microscopy (STM). The impact of the surfaces on the measurement of bulk properties such as magnetism, the Verwey transition and the (predicted) half-metallicity is discussed.The best understood iron oxide surface at present is probably Fe 3 O 4 (100); the structure is known with a high degree of precision and the major defects and properties are well characterised. A major factor in this is that a termination at the Fe oct -O plane can be reproducibly prepared by a variety of methods, as long as the surface is annealed in 10 Such straightforward preparation of a monophase termination is generally not the case for other iron oxide surfaces. All available evidence suggests the oft-studied (√2×√2)R45° reconstruction results from a rearrangement of the cation lattice in the outermost unit cell in which two octahedral cations are replaced by one tetrahedral interstitial, a motif conceptually similar to well-known Koch-Cohen defects in Fe (0001) is the most studied hematite surface, but 2 difficulties preparing stoichiometric surfaces under UHV conditions have hampered a definitive determination of the structure. There is evidence for at least three terminations: a bulk-like termination at the oxygen plane, a termination with half of the cation layer, and a termination with ferryl groups. When the surface is reduced the so-called "bi-phase" structure is formed, which eventually transforms to a Fe 3 O 4 (111)-like termination. The structure of the bi-phase surface is controversial; a largely accepted model of coexisting Fe 1-x O and α-Fe 2 O 3 (0001) islands was recently challenged and a new structure based on a thin film of Fe 3 O 4 (111) on α-Fe 2 O 3 (0001) was proposed. The merits of the compet...

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Section: Metalsmentioning

confidence: 99%

Iron oxide surfaces

Parkinson

2016

Surface Science Reports

499

463

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“…[7][8][9][10][11] A step toward increasing complexity of such catalysts involves the synthesis of pairs of metal centers on supports, and these offer prospects of new properties associated with the neighboring metal centers. There are still only a small number of catalysts in this class.…”

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confidence: 99%

Tracking Rh Atoms in Zeolite HY: First Steps of Metal Cluster Formation and Influence of Metal Nuclearity on Catalysis of Ethylene Hydrogenation and Ethylene Dimerization

Yang

Browning

et al. 2016

J. Phys. Chem. Lett.

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The initial steps of rhodium cluster formation from zeolite-supported mononuclear Rh(C2H4)2 complexes in H2 at 373 K and 1 bar were investigated by infrared and extended X-ray absorption fine structure spectroscopies and scanning transmission electron microscopy (STEM). The data show that ethylene ligands on the rhodium react with H2 to give supported rhodium hydrides and trigger the formation of rhodium clusters. STEM provided the first images of the smallest rhodium clusters (Rh2) and their further conversion into larger clusters. The samples were investigated in a plug-flow reactor as catalysts for the conversion of ethylene + H2 in a molar ratio of 4:1 at 1 bar and 298 K, with the results showing how the changes in catalyst structure affect the activity and selectivity; the rhodium clusters are more active for hydrogenation of ethylene than the single-site complexes, which are more selective for dimerization of ethylene to give butenes.

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“…In contrast to Pt/FeO x for catalyzing the CO oxidation, the single Pt atoms on the support of titanium nitride exhibited alternative selectivity of catalysis: the methanol and formic acid molecules enable to be electro-catalytically oxidized. [ 56 ] Towards addressing the supprot issue, the concept of electronic metalsupport interactions (EMSI) [ 21 ] and strong covalent metal-support interaction (CMSI) [ 57 ] have been proposed for single-atom catalysts.…”

Section: Perspectivementioning

confidence: 99%

Single Atom Excels as the Smallest Functional Material

Zhang

Zheng

2016

Adv Funct Materials

114

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The emerging single‐atom field spans single‐atom catalysis in chemistry and single‐atom manipulation in physics up to the state‐of‐the‐art characterization via imaging and spectroscopy. These interdisciplinary progresses have been interacted closely with the development of materials science, underscoring the principle that the single atom excels as the smallest functional material. This simple concept not only permits to reinvent our understanding of the nature of materials, but also promises unambiguously to have a great impact on other physical sciences.

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Ultrastable single-atom gold catalysts with strong covalent metal-support interaction (CMSI)

Cited by 464 publications

References 77 publications

Iron oxide surfaces

Iron oxide surfaces

Tracking Rh Atoms in Zeolite HY: First Steps of Metal Cluster Formation and Influence of Metal Nuclearity on Catalysis of Ethylene Hydrogenation and Ethylene Dimerization

Single Atom Excels as the Smallest Functional Material

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