Surface mobility and impact of precursor dosing during atomic layer deposition of platinum:<i>in situ</i>monitoring of nucleation and island growth

Dendooven, Jolien; Daele, Michiel Van; Solano, Eduardo; Ramachandran, Ranjith Karuparambil; Minjauw, Matthias; Resta, Andrea; Vlad, Alina; Garreau, Y.; Coati, Alessandro; Portale, Giuseppe; Detavernier, Christophe

doi:10.1039/d0cp03563g

Cited by 25 publications

(23 citation statements)

References 76 publications

(102 reference statements)

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“… 7 , 9 Fundamental insight into the reaction mechanisms also aids in understanding aspects such as nucleation and island growth, which are of interest for the controlled growth of nanoparticles. 9 , 17 , 20 …”

Section: Introductionmentioning

confidence: 99%

Surface Chemistry during Atomic Layer Deposition of Pt Studied with Vibrational Sum-Frequency Generation

2022

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A detailed understanding of the growth of noble metals by atomic layer deposition (ALD) is key for various applications of these materials in catalysis and nanoelectronics. The Pt ALD process using MeCpPtMe 3 and O 2 gas as reactants serves as a model system for the ALD processes of noble metals in general. The surface chemistry of this process was studied by in situ vibrational broadband sum-frequency generation (BB-SFG) spectroscopy, and the results are placed in the context of a literature overview of the reaction mechanism. The BB-SFG experiments provided direct evidence for the presence of CH 3 groups on the Pt surface after precursor chemisorption at 250 °C. Strong evidence was found for the presence of a C=C containing complex ( e.g ., the form of Cp species) and for partial dehydrogenation of the surface species during the precursor half-cycle. The reaction kinetics of the precursor half-cycle were followed at 250 °C, showing that the C=C coverage saturated before the saturation of CH 3 . This complex behavior points to the competition of multiple surface reactions, also reflected in the temperature dependence of the reaction mechanism. The CH 3 saturation coverage decreased significantly with temperature, while the C=C coverage remained constant after precursor chemisorption on the Pt surface for temperatures from 80 to 300 °C. These SFG results have resulted in a better understanding of the Pt ALD process and also highlight the surface chemistry during thin-film growth as a promising field of study for the BB-SFG community.

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Section: Introductionmentioning

confidence: 99%

Surface Chemistry during Atomic Layer Deposition of Pt Studied with Vibrational Sum-Frequency Generation

2022

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“…Among the many strategies in this line, one can enhance ECA by further increasing the ratio of surface platinum atoms that are catalytically active, for example, by optimizing catalyst geometry, especially given that ALD can be utilized to synthesize atomic scale catalyst down to single‐atom active sites. [ 73,74 ] With innovations on ALD chemicals, especially the Pt ALD precursors, [ 75,76 ] and deeper understanding and innovation of ALD deposition processes, [ 77,78 ] ORR activity normalized by mass or cost are expected to be improved further.…”

Section: Resultsmentioning

confidence: 99%

Direct Integration of Strained‐Pt Catalysts into Proton‐Exchange‐Membrane Fuel Cells with Atomic Layer Deposition

Wang

Dull

et al. 2021

Advanced Materials

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(2 of 10)www.advmat.de www.advancedsciencenews.com Comparing Rotating Disk Electrode and Membrane Electrode AssemblyCatalysts were deposited with ALD onto glassy carbon electrodes and carbon-loaded GDL, for catalytic performance evaluation under RDE and MEA, respectively. Acid-leaching conditions were tested to achieve reproducible results. When no pretreatment is applied in the RDE measurement, it is equivalent to pretreating the as-deposited electrode with strong acid (electrolyte pH = 1). Cobalt oxide quickly dissolves, which

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“…In order to extract the real space parameters such as the nanoparticle shape, size, and areal density from the q-space scattering data, we adopted an analysis approach, based on a geometrical model. 2 IsGISAXS 3 software was used to calculate the simulated 2D GISAXS patterns, using the extracted morphological parameters as input for the simulation. Then the measured data was compared to the simulated data to validate the proposed strategy.…”

Section: Gisaxs Data Analysismentioning

confidence: 99%

Selective Vapor-Phase Doping of Pt Nanoparticles into Phase-Controlled Nanoalloys

et al. 2022

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Bimetallic nanoparticles (BMNPs) are frontrunners in various fields including heterogeneous catalysis, medicinal applications, and medical imaging. Tailoring their properties requires adequate control over their structure and composition, which still presents a non-trivial endeavor. We present a flexible strategy to deposit phase-controlled BMNPs by vapor-phase "titration" of a secondary metal to a pre-deposited monometallic nanoparticle (NP) host. The strategy is exemplified for archetypal Pt−Sn BMNPs but transferrable to other BMNPs which alloy noble and non-noble metals. When exposing Pt NPs on a SiO 2 support to discrete TDMASn (tetrakis(dimethylamino)tin) vapor pulses from 150 to 300 °C, TDMASn selectively decomposes on Pt NPs. This leads to saturated infiltration of Sn into Pt NPs through reactive solid-state diffusion, resulting in the formation of Pt−Sn BMNPs with phase/composition control via the substrate temperature. An additional H 2 pulse after each TDMASn pulse removes the surface ligands and excess Sn on the surface as SnH 4 , preserving the small sizes of the pre-deposited Pt NPs. This approach provides a single-step, selective "vapor-phase conversion" of Pt NPs into Pt x Sn y BMNPs with great potential for catalysis. Hereto, a proof of concept is provided by converting wet impregnated Pt NPs into Pt−Sn BMNPs on high surface area supports.

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Surface mobility and impact of precursor dosing during atomic layer deposition of platinum:in situmonitoring of nucleation and island growth

Abstract: The increasing interest in atomic layer deposition (ALD) of Pt for the controlled synthesis of supported nanoparticles for catalysis demands an in-depth understanding of the nucleation controlled growth behaviour. We...

Cited by 25 publications

References 76 publications

Surface Chemistry during Atomic Layer Deposition of Pt Studied with Vibrational Sum-Frequency Generation

Surface Chemistry during Atomic Layer Deposition of Pt Studied with Vibrational Sum-Frequency Generation

Direct Integration of Strained‐Pt Catalysts into Proton‐Exchange‐Membrane Fuel Cells with Atomic Layer Deposition

Selective Vapor-Phase Doping of Pt Nanoparticles into Phase-Controlled Nanoalloys

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