Catalytic Resonance of Ammonia Synthesis by Dynamic Ruthenium Crystal Strain

Wittreich, Gerhard R.; Liu, Shizhong; Dauenhauer, Paul J.; Vlachos, Dionisios G.

doi:10.33774/chemrxiv-2021-b8kgr

Cited by 6 publications

(4 citation statements)

References 54 publications

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“…Their thermal stability (up to ~500 °C) may make them suitable for high temperature catalytic applications, such as methanol decomposition, CO oxidation, and ammonia synthesis and decomposition. [37] Programmable catalysis achieved by dynamic modulation of surface charge density is predicted to achieve faster catalytic rates with larger variations in charge condensation. [38,39,40] The alternation of insulating and semiconducting layers in nanolaminates imparts high capacitance (2 μF/cm 2 ) with the capability for fast response (1,000 Hz).…”

Section: Ir Of Co Adsorbed On Pt/c Ato Condensersmentioning

confidence: 99%

Alumina-Titania Nanolaminate Condensers for Hot Programmable Catalysis

Oh,

Walton,

Chalmers

et al. 2024

Preprint

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For programmable catalysis applications, nanolaminates composed of thin alternating layers of alumina and titania (ATO) were engineered using atomic layer deposition (ALD) as the dielectric material for a Pt-on-carbon catalytic condenser. Systematic investigation assessed synthesis parameters such as deposition temperature, alumina and titania layer thicknesses, the total number of layers (and interfaces), and the presence of a capping alumina layer on the maximum achievable charge accumulation in the Pt catalyst layer. The highest capacitance ATO configuration demonstrated a specific capacitance of ~1,200 nF/cm2 with working voltages of ±5 V, enabling the storage of 4×10^13 electrons or holes per cm2 at room temperature. Adsorption of carbon monoxide on the Pt/C-ATO device characterized by grazing incidence infrared spectroscopy showed changes in the surface binding energy of 13.1 ± 0.8 kJ/mol for an applied external voltage bias of ±1 V. The results enhance our understanding of nanolaminate structures and provide a method for increasing charge condensation strength for higher temperature surface chemistries.

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Section: Ir Of Co Adsorbed On Pt/c Ato Condensersmentioning

confidence: 99%

Alumina-Titania Nanolaminate Condensers for Hot Programmable Catalysis

Oh,

Walton,

Chalmers

et al. 2024

Preprint

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“…For example, catalytic synthesis of ammonia on ruthenium undergoing ± 4% dynamic crystal strain has been predicted by Vlachos and coworkers to exhibit negative gamma dynamics for the N* hydrogenation step when accounting for lateral interactions between adsorbed species, which can significantly change adsorption energies (𝛾 𝑁𝐻+𝐻/𝑁+2𝐻 = -1.8). [37] They simulated the dynamic performance of this system, observing a 10-fold rate increase at an applied waveform frequency of 2 kHz for this complex chemical mechanism. In another example, negative scaling relationships have been predicted to exist for the methane steam reforming reaction, which is responsible for the majority of greenhouse gas emissions from the Haber-Bosh process.…”

mentioning

confidence: 99%

Catalytic resonance theory: Negative dynamic surfaces for programmable catalysts

Gathmann¹,

Ardagh²,

Dauenhauer³

2022

Chem Catalysis

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“…[72,80] For reactions such as ammonia synthesis, energy input via surfaceprogrammed strain oscillations is predicted to accelerate the overall reaction and promote the reaction at lower pressure. [81] As reactions become more complex, programmed surface oscillations can significantly promote specific reaction pathways over others, providing dramatic potential for control of product selectivity. [82] Realizing these catalytic benefits will require understanding the new relationships that exist between molecules, surfaces, and complex programmed inputs.…”

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confidence: 99%

Up Up Down Down Left Right Left Right B A Start for the Catalytic Hackers of Programmable Materials

Dauenhauer

2023

Preprint

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The valuable information of catalysis for the past century has been the composition and structure of high-performing catalytic materials. But a new class of programmable catalysts that change the electronic characteristics of their active sites on the time scale of the surface reaction are changing the catalyst design process by requiring additional information describing the input program that directs the temporal changes in the catalyst surface. Catalyst programs vary in complexity associated with the number of combined waveforms required to optimize surface chemistry rates and selectivity to products. The path forward for writing and optimizing catalyst programs will combine together the methods of parameter screening, rational design based on molecular models, and machine learning. This new approach to catalysis will change the nature of catalysis science, with researchers pursuing dynamic catalytic programs with improved catalytic performance over static catalyst compositions.

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Catalytic Resonance of Ammonia Synthesis by Dynamic Ruthenium Crystal Strain

Cited by 6 publications

References 54 publications

Alumina-Titania Nanolaminate Condensers for Hot Programmable Catalysis

Alumina-Titania Nanolaminate Condensers for Hot Programmable Catalysis

Catalytic resonance theory: Negative dynamic surfaces for programmable catalysts

Up Up Down Down Left Right Left Right B A Start for the Catalytic Hackers of Programmable Materials

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