Catalyst synthesis and evaluation using an integrated atomic layer deposition synthesis–catalysis testing tool

Camacho-Bunquin, Jeffrey; Shou, Heng; Aich, Payoli; Beaulieu, David R.; Klotzsch, H.; Bachman, Stephen; Marshall, Christopher L.; Hock, Adam S.; Stair, Peter C.

doi:10.1063/1.4928614

Cited by 20 publications

(20 citation statements)

References 18 publications

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“…Volatile products of the ALD synthesis and catalytic reactions can be analyzed by both GC and mass spectrometry. 18 The approach presented in this report provides key insights into the mechanism of zinc grafting on hydroxylated supports, and the reactivity and stability of these alkyl-zinc and zinc oxide-type sites as a function of zinc dispersion and nuclearity. Additionally, this study presents the use of an organo-zinc pre-catalyst where the initial pre-catalyst ligand (ethyl, C2) is well differentiated from the reacting alkene/alkane (propylene and propene, both C3 species).…”

Section: Introductionmentioning

confidence: 96%

“…In this paper, we report the use of an Integrated Atomic Layer Deposition-Catalysis (I-ALD-CAT, Figure 2) 18 synthesis and catalyst reaction testing tool for the synthesis of isolated alkyl-zinc and zinc oxide-type sites via one-cycle ALD methods and immediate in situ evaluation of the reactivity of these sites at the atomic-scale/submonolayer level under propylene hydrogenation and propane dehydrogenation conditions. 18 The I-ALD-CAT toolthe first of its kindhas the capability of (1) ALD synthesis on a support loaded into a plug-flow reactor, a design element that allows for (2) immediate in situ catalyst performance evaluation under plugflow conditions without material exposure to air or moisture (Figure 2). .…”

Section: Introductionmentioning

confidence: 99%

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Single-site zinc on silica catalysts for propylene hydrogenation and propane dehydrogenation: Synthesis and reactivity evaluation using an integrated atomic layer deposition-catalysis instrument

Camacho-Bunquin

Aich

Ferrandon

et al. 2017

Journal of Catalysis

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Alkyl-zinc and zinc oxide-type sites were synthesized via atomic layer deposition on highsurface-area silica using an integrated atomic layer deposition-catalysis instrument (I-ALD-CAT). One-cycle ALD experiments using diethylzinc (DEZ) afforded Zn/SiO 2 systems that provided key insights into the reactivity and stability of Zn sites as a function of dispersion at the submonolayer level. The I-ALD-CAT tool design allowed for systematic comparison of the reactivity of different grafted zinc sites. Open-shell 16-electron, tricoordinate ethyl zinc-silica sites exhibit higher activity in propane hydrogenation-dehydrogenation compared to 18-electron, tetracoordinate zinc oxide-type centers. Silica surface saturation with Zn(II) sites (~75% of a monolayer) results in facile zinc agglomeration and catalyst deactivation under reaction conditions. Reduced DEZ dosing coupled with thermal substrate pretreatment techniques (e.g., dehydration under vacuum) resulted in increased Zn dispersion and produced Zn/SiO 2 catalysts with improved activity and stability under propylene hydrogenation (200°C) and propane dehydrogenation (550°C) conditions.

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Section: Introductionmentioning

confidence: 96%

Section: Introductionmentioning

confidence: 99%

Single-site zinc on silica catalysts for propylene hydrogenation and propane dehydrogenation: Synthesis and reactivity evaluation using an integrated atomic layer deposition-catalysis instrument

Camacho-Bunquin

Aich

Ferrandon

et al. 2017

Journal of Catalysis

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“…The fixed-bed offers an excellent gas-solid contact. This reactor geometry is highly suitable for the deposition of very thin films on high surface area materials [16]. Our setup is equipped with a magnetic suspension balance, which measures in situ the mass changes during the ALD.…”

Section: Introductionmentioning

confidence: 99%

Investigating the Trimethylaluminium/Water ALD Process on Mesoporous Silica by In Situ Gravimetric Monitoring

et al. 2018

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A low amount of AlOx was successfully deposited on an unordered, mesoporous SiO2 powder using 1–3 ALD (Atomic Layer Deposition) cycles of trimethylaluminium and water. The process was realized in a self-built ALD setup featuring a microbalanceand a fixed particle bed. The reactor temperature was varied between 75, 120, and 200 °C. The self-limiting nature of the deposition was verified by in situ gravimetric monitoring for all temperatures. The coated material was further analyzed by nitrogen sorption, inductively coupled plasma-optical emission spectroscopy, powder X-ray diffraction, high-resolution transmission electron microscopy, attenuated total reflection Fourier transformed infrared spectroscopy, and elemental analysis. The obtained mass gains correspond to average growth between 0.81–1.10 Å/cycle depending on substrate temperature. In addition, the different mass gains during the half-cycles in combination with the analyzed aluminum content after one, two, and three cycles indicate a change in the preferred surface reaction of the trimethylaluminium molecule from a predominately two-ligand exchange with hydroxyl groups to more single-ligand exchange with increasing cycle number. Nitrogen sorption isotherms demonstrate (1) homogeneously coated mesopores, (2) a decrease in surface area, and (3) a reduction of the pore size. The experiment is successfully repeated in a scale-up using a ten times higher substrate batch size.

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“…It combines an ALD manifold with a plug flow reactor system. The I-ALD-CAT was successfully used in synthesizing platinum active sites, Al 2 O 3 overcoats and in the activity evaluation of propylene hydrogenation under plug-flow conditions [240].…”

Section: Catalystmentioning

confidence: 99%

New development of atomic layer deposition: processes, methods and applications

Oviroh

Akbarzadeh

Pan

et al. 2019

Science and Technology of Advanced Materials

375

200

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Atomic layer deposition (ALD) is an ultra-thin film deposition technique that has found many applications owing to its distinct abilities. They include uniform deposition of conformal films with controllable thickness, even on complex three-dimensional surfaces, and can improve the efficiency of electronic devices. This technology has attracted significant interest both for fundamental understanding how the new functional materials can be synthesized by ALD and for numerous practical applications, particularly in advanced nanopatterning for microelectronics, energy storage systems, desalinations, catalysis and medical fields. This review introduces the progress made in ALD, both for computational and experimental methodologies, and provides an outlook of this emerging technology in comparison with other film deposition methods. It discusses experimental approaches and factors that affect the deposition and presents simulation methods, such as molecular dynamics and computational fluid dynamics, which help determine and predict effective ways to optimize ALD processes, hence enabling the reduction in cost, energy waste and adverse environmental impacts. Specific examples are chosen to illustrate the progress in ALD processes and applications that showed a considerable impact on other technologies.

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Catalyst synthesis and evaluation using an integrated atomic layer deposition synthesis–catalysis testing tool

Cited by 20 publications

References 18 publications

Single-site zinc on silica catalysts for propylene hydrogenation and propane dehydrogenation: Synthesis and reactivity evaluation using an integrated atomic layer deposition-catalysis instrument

Single-site zinc on silica catalysts for propylene hydrogenation and propane dehydrogenation: Synthesis and reactivity evaluation using an integrated atomic layer deposition-catalysis instrument

Investigating the Trimethylaluminium/Water ALD Process on Mesoporous Silica by In Situ Gravimetric Monitoring

New development of atomic layer deposition: processes, methods and applications

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