Probing surface-adsorbate interactions through active particle dynamics

Greydanus, Benjamin; Saleheen, Mohammad; Wu, Haichao; Heyden, Andreas; Medlin, J. Will; Schwartz, Daniel K.

doi:10.1016/j.jcis.2022.01.053

Cited by 13 publications

(16 citation statements)

References 43 publications

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“…As previously reported, the qualitative aspects of active motion were observed to be activity-dependent. 13 While for the most active Pt particles a ballistic MSD regime was readily observed, as the particle activity decreased with changing metal compositions, the MSD at short lag times became increasingly linear as expected; indeed, for the least active PdAu 25:75 particles, the MSD at short lag times was indistinguishable from linear. However, the apparent mobility in this regime was measurably greater than for passive particles in the absence of fuel, which allowed for the quantitative determination of the active velocity from the long lag-time behavior, as described in the Materials section.…”

Section: Activity Of Synthesized Activesupporting

confidence: 55%

“…As previously reported, three adsorption isotherms for furfural on Pt were constructed at different temperatures (294, 303, and 311 K). Per the Van’t Hoff relation, the natural log of furfural concentration at the same coverages was plotted against reciprocal temperature to yield the enthalpy of adsorption of furfural on Pt as a function of coverage . This technique was complemented with another method – using the measured adsorption equilibrium constant and an estimate of the entropy of adsorption to extract enthalpies from adsorption isotherms .…”

Section: Resultsmentioning

confidence: 99%

“…As previously reported, furfural and other organic adsorbates systematically attenuated active motion for Pt-coated particles. 13 This reduction in active motion was attributed to physical occlusion of the metal active sites by adsorbed furfural that blocked access of the H 2 O 2 fuel. It was found that this attenuation of velocity could be quantitively linked to the adsorbed coverage of furfural and the adsorption process could be modeled using a Langmuir isotherm, enabling extraction of salient parameters of the adsorption process including the affinity and the maximum saturation coverage.…”

Section: Quantitative Analysis Of Adsorbate-attenuated Active Motionmentioning

confidence: 99%

“…The Pt sites rapidly decompose H 2 O 2 , creating an asymmetric chemical gradient that acts to propel the particle . In a previous work, the dependence of active motion on solute concentration was used to quantify adsorption on available metal surface sites . Furfural adsorption was studied on a Pt surface to determine key aspects of binding including the affinity, concentration-dependent coverage, and enthalpy of adsorption for furfural on Pt.…”

Section: Introductionmentioning

confidence: 99%

“…12 In a previous work, the dependence of active motion on solute concentration was used to quantify adsorption on available metal surface sites. 13 Furfural adsorption was studied on a Pt surface to determine key aspects of binding including the affinity, concentrationdependent coverage, and enthalpy of adsorption for furfural on Pt. Here, we investigate the use of other metal compositions including Pd and Pd-containing alloys.…”

Section: Introductionmentioning

confidence: 99%

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Elucidating the Influence of Metal Surface Composition on Organic Adsorbate Binding Using Active Particle Dynamics

2023

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The adsorption strengths of organic compounds on metal surfaces are sensitive to the metal composition, and they play a central role in many catalytic reactions, helping to control the coverage of the reactant and altering the overall reaction rate. While adsorption energies are straightforward to measure and calculate in vacuum and gas-phase environments, adsorption energetics can be dramatically altered by the presence of solvent in liquid-phase reactions. However, the effects of metal composition on binding strengths in a liquid environment are less well understood, primarily due to the difficulty of accurate in situ measurements of organic binding on metal surfaces in the liquid phase. Here, we utilize the motion of active particles in water to probe the adsorption energies of an organic adsorbate (furfural) on a range of metal surfaces (pure Pd, pure Pt, and four PdAu alloy compositions) to elucidate the effect of metal composition. Janus particles with catalytic caps of particular metal compositions all exhibited active motion resulting from consumption of H 2 O 2 ; adsorbate binding was inferred through the decrease in the velocity of active motion and was modeled by a Langmuir adsorption isotherm. The measured adsorption affinities were used to extract the adsorption enthalpy of furfural on the different metals. The Pd surface was found to bind furfural more strongly than the Pt surface by some 10 kJ/mol. Furthermore, the adsorption of furfural on the alloys was found to increase monotonically in magnitude with Pd content. The data reported herein aid the development of accurate understanding of organic adsorption in the presence of solvent and the role of the metal surface in tuning adsorption strengths to optimize catalytic processes in the liquid phase.

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Section: Activity Of Synthesized Activesupporting

confidence: 55%

Section: Resultsmentioning

confidence: 99%

Section: Quantitative Analysis Of Adsorbate-attenuated Active Motionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Elucidating the Influence of Metal Surface Composition on Organic Adsorbate Binding Using Active Particle Dynamics

2023

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Non‐Reciprocity, Metastability, and Dynamic Reconfiguration in Co‐Assembly of Active and Passive Particles

Al Harraq,

Patel,

Lee

et al. 2024

Advanced Science

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Living organisms often exhibit non‐reciprocal interactions where the forces acting on the objects are not equal in magnitude or opposite in direction. The combination of reciprocal and non‐reciprocal interactions between synthetic building blocks remains largely unexplored. Here, out‐of‐equilibrium assemblies of non‐motile isotropic passive and metal‐patched motile active particles are formed by overlapping bulk interactions with directed self‐propulsion. An external alternating current (AC) electric field generates concurrent dipolar and induced‐charge electrophoretic forces between the particles which are evaluated using microscopy. The interaction force measurements allow to determine the degree of reciprocity in interactions, which is tunable by designing the active particle and its trajectory. While linearly‐propelled active particles evade assembly with passive particles, helically propelled active particles form active‐passive clusters with dynamic reconfiguration and long‐lived metastability. Large clusters display programmable fluctuations and reconfigurability by controlling the fraction of active particles. The study establishes principles of integrating reciprocal and non‐reciprocal interactions in guided colloidal assembly of reconfigurable metastable structures.

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Evaluation of Glebionis coronaria L. flower extract as a novel green inhibitor for mild steel corrosion in acidic environment

El-Hashemy,

Almehmadi

2024

Biomass Conv. Bioref.

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Probing surface-adsorbate interactions through active particle dynamics

Cited by 13 publications

References 43 publications

Elucidating the Influence of Metal Surface Composition on Organic Adsorbate Binding Using Active Particle Dynamics

Elucidating the Influence of Metal Surface Composition on Organic Adsorbate Binding Using Active Particle Dynamics

Non‐Reciprocity, Metastability, and Dynamic Reconfiguration in Co‐Assembly of Active and Passive Particles

Evaluation of Glebionis coronaria L. flower extract as a novel green inhibitor for mild steel corrosion in acidic environment

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