A Single‐Site Platinum CO Oxidation Catalyst in Zeolite KLTL: Microscopic and Spectroscopic Determination of the Locations of the Platinum Atoms

Kistler, Joseph D.; Chotigkrai, Nutchapon; Xu, Pinghong; Enderle, Bryan; Praserthdam, Piyasan; Chen, Cong-Yan; Browning, Nigel D.; Gates, Bruce C.

doi:10.1002/anie.201403353

Cited by 269 publications

(242 citation statements)

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“…This issue of nanogold catalysts has been the foremost technical barrier for their practical applications and commercialization [21]. Inspired by our recent work on the excellent performance of singleatom catalysts of Pt 1 /FeO x [22,23] and Ir 1 /FeO x [24], and recent studies on this topic [9,[25][26][27][28][29][30][31][32][33][34][35][36][37][38], we, for the first time, demonstrate in this work that individual gold atoms (Au 1 ) dispersed onto iron oxides are much more sintering-resistant than their nanoparticle counterparts and show extremely high reaction stability in a wide temperature range for a few important catalytic reactions. Theoretical studies revealed that the positively charged and surface-anchored Au 1 atoms with high valent states formed significant covalent chemical bonds with the support, thus providing ultra-stability and remarkable catalytic performance.…”

Section: Introductionmentioning

confidence: 99%

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

et al. 2015

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Supported noble metal nanoparticles (including nanoclusters) are widely used in many industrial catalytic processes. While the finely dispersed nanostructures are highly active, they are usually thermodynamically unstable and tend to aggregate or sinter at elevated temperatures. This scenario is particularly true for supported nanogold catalysts because the gold nanostructures are easily sintered at high temperatures, under reaction conditions, or even during storage at ambient temperature. Here, we demonstrate that isolated Au single atoms dispersed on iron oxide nanocrystallites (Au 1 /FeO x ) are much more sinteringresistant than Au nanostructures, and exhibit extremely high reaction stability for CO oxidation in a wide temperature range. Theoretical studies revealed that the positively charged and surface-anchored Au 1 atoms with high valent states formed significant covalent metal-support interactions (CMSIs), thus providing the ultra-stability and remarkable catalytic performance. This work may provide insights and a new avenue for fabricating supported Au catalysts with ultra-high stability.

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Section: Introductionmentioning

confidence: 99%

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

et al. 2015

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“…Owing to significantly high efficiency of metal atom usage, low-coordination environment of metal centers, and strong metal-support interaction, single-atom catalysts have revealed remarkable activity in a variety of reactions, including oxidation, water gas shift and hydrogenation11121314151617181920212223242526272829. More importantly, when the size of metal catalysts is reduced into single-atom scale, the selectivity in certain reactions is much different compared with their nanocrystal or nanocluster counterparts272829.…”

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confidence: 99%

Atomic-level insights in optimizing reaction paths for hydroformylation reaction over Rh/CoO single-atom catalyst

et al. 2016

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Rh-based heterogeneous catalysts generally have limited selectivity relative to their homogeneous counterparts in hydroformylation reactions despite of the convenience of catalyst separation in heterogeneous catalysis. Here, we develop CoO-supported Rh single-atom catalysts (Rh/CoO) with remarkable activity and selectivity towards propene hydroformylation. By increasing Rh mass loading, isolated Rh atoms switch to aggregated clusters of different atomicity. During the hydroformylation, Rh/CoO achieves the optimal selectivity of 94.4% for butyraldehyde and the highest turnover frequency number of 2,065 h−1 among the obtained atomic-scale Rh-based catalysts. Mechanistic studies reveal that a structural reconstruction of Rh single atoms in Rh/CoO occurs during the catalytic process, facilitating the adsorption and activation of reactants. In kinetic view, linear products are determined as the dominating products by analysing reaction paths deriving from the two most stable co-adsorbed configurations. As a bridge of homogeneous and heterogeneous catalysis, single-atom catalysts can be potentially applied in other industrial reactions.

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“…Another commonly used imaging technique, high‐angle annular dark‐field scanning transmission electron microscopy (HAADF‐STEM), is also a poor choice, despite its easily interpretable image contrast, owing to the fact that it only uses a very small fraction of the incident electrons (those scattered to high angles), producing insufficient signals under the low‐electron‐dose conditions required to preserve the fragile structure of zeolites . Consequently, guest components in zeolites are mostly invisible by HAADF‐STEM, unless they are composed of heavy elements with a high loading …”

Section: Introductionmentioning

confidence: 99%

Direct Imaging of Atomically Dispersed Molybdenum that Enables Location of Aluminum in the Framework of Zeolite ZSM‐5

et al. 2019

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Integrated differential phase‐contrast scanning transmission electron microscopy (iDPC‐STEM) is capable of directly probing guest molecules in zeolites, owing to its sufficient and interpretable image contrast for both heavy and light elements under low‐dose conditions. This unique ability is demonstrated by imaging volatile organic compounds adsorbed in zeolite Silicalite‐1; iDPC‐STEM was then used to investigate molybdenum supported on various zeolites including Silicalite‐1, ZSM‐5, and mordenite. Isolated single‐Mo clusters were observed in the micropores of ZSM‐5, demonstrating the crucial role of framework Al in driving Mo atomically dispersed into the micropores. Importantly, the specific one‐to‐one Mo‐Al interaction makes it possible to locate Al atoms, that is, catalytic active sites, in the ZSM‐5 framework from the images, according to the positions of Mo atoms in the micropores.

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A Single‐Site Platinum CO Oxidation Catalyst in Zeolite KLTL: Microscopic and Spectroscopic Determination of the Locations of the Platinum Atoms

Cited by 269 publications

References 23 publications

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

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

Atomic-level insights in optimizing reaction paths for hydroformylation reaction over Rh/CoO single-atom catalyst

Direct Imaging of Atomically Dispersed Molybdenum that Enables Location of Aluminum in the Framework of Zeolite ZSM‐5

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