Machine Learning Prediction of H Adsorption Energies on Ag Alloys

Hoyt, Robert A.; Montemore, Matthew M.; Fampiou, Ioanna; Chen, Wei; Tritsaris, Georgios A.; Kaxiras, Efthimios

doi:10.1021/acs.jcim.8b00657

Cited by 53 publications

(40 citation statements)

References 43 publications

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“…13,18,19 As this is similar to the behavior of nanoclusters (small particles with only a few atoms), 20 alloy surfaces with localized ensembles have been called "embedded nanoclusters". 21 In this work, we show how localized clusters of atoms embedded in the surface of a host can defy intuition and link this counterintuitive behavior to hybridization and splitting of sharp dstate peaks in these systems. By studying many dopants and several hosts, we also elucidate trends in the behavior of these systems, which allows us to develop correlations between electronic structure and adsorption energies for single atom alloys and embedded nanoclusters.…”

Section: Introductionmentioning

confidence: 89%

When More Is Less: Nonmonotonic Trends in Adsorption on Clusters in Alloy Surfaces

Monasterial¹,

Hinderks²,

Viriyavaree³

et al. 2020

Preprint

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Single-atom alloys can be effective catalysts and have been compared to supported single-atom catalysts. To rationally design single-atom alloys and other surfaces with localized ensembles, it is crucial to understand variations in reactivity when varying the dopant and the ensemble size. Here, we examined hydrogen adsorption on surfaces embedded with localized clusters and discovered general trends. Counterintuitively, increasing the amount of a more reactive metal sometimes makes a surface site less reactive. This behavior is due to the hybridization and splitting of sharp peaks in the electronic density of states of many of these surfaces, making them analogous to free-standing nanoclusters. Further, single-atom alloys have qualitatively different behavior than larger ensembles. Specifically, the adsorption energy is U-shaped when plotted against the dopant’s group for single atom alloys. Additionally, adsorption energies on single atom alloys correlate more strongly with the dopant’s p-band center than the d-band center. <br>

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Section: Introductionmentioning

confidence: 89%

When More Is Less: Nonmonotonic Trends in Adsorption on Clusters in Alloy Surfaces

Monasterial¹,

Hinderks²,

Viriyavaree³

et al. 2020

Preprint

View full text Add to dashboard Cite

show abstract

“…Some calculations reconstructed significantly, which led to unphysical configurations and difficulty in reaching geometric convergence. As done in previous work, 10,30 these calculations were removed.…”

Section: Methodsmentioning

confidence: 99%

“…While comparing to previous models is difficult due to differing data sets, our errors are in the ranges achieved by other models, but less data is required. 10,12 Error distributions are given in Figure S1. We attribute the relatively low error on a quite heterogeneous dataset to our strategy of decoupling the predictions of the surface properties, which were fit separately for each metal, from the prediction of the adsorption energies, which were fit separately for each adsorbate and site.…”

Section: Modelsmentioning

confidence: 99%

General Screening of Surface Alloys for Catalysis

Montemore

Nwaokorie²,

Kayode³

2020

Preprint

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Intensive research in catalysis has resulted in design parameters for many important catalytic reactions; however, designing new catalysts remains difficult, partly due to the time and expense needed to screen a large number of potential catalytic surfaces. Here, we create a general, efficient model that can be used to screen surface alloys for many reactions without any quantum-based calculations. This model allows the prediction of the adsorption energies of a variety of species (explicitly shown for C, N, O, OH, H, S, K, F) on metal alloy surfaces that include combinations of nearly all of the d-block metals. We find that a few simple structural features, chosen using data-driven techniques and physical understanding, can be used to predict electronic structure properties. These electronic structure properties are then used to predict adsorption energies, which are in turn used to predict catalytic performance. This framework is interpretable and gives insight into how underlying structural features affect adsorption and catalytic performance. We apply the model to screen more than 10<sup>7</sup> unique surface sites on approximately 10<sup>6</sup> unique surfaces for 7 important reactions. We identify novel surfaces with high predicted catalytic performance, and demonstrate challenges and opportunities in catalyst development using surface alloys. This work shows the utility of a general, reusable model that can be applied in new contexts without requiring new data to be generated.<br>

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“…12,17,18 As this is similar to the behavior of nanoclusters (small particles with only a few atoms), 19 alloy surfaces with localized ensembles have been called "embedded nanoclusters". 20 In this work, we show how localized clusters of atoms embedded in the surface of a host can defy intuition and link this counterintuitive behavior to the narrow d-state peaks in these systems. By studying many dopants and several hosts, we also elucidate trends in the behavior of these systems, which allows us to develop predictive correlations for single atom alloys and embedded nanoclusters.…”

mentioning

confidence: 88%

When More Is Less: Nonmonotonic Trends in Adsorption on Clusters in Alloy Surfaces

Monasterial¹,

Hinderks²,

Viriyavaree³

et al. 2020

Preprint

Self Cite

View full text Add to dashboard Cite

<div> <div> <div> <p>Single-atom alloys can be effective catalysts and have been compared to supported single-atom catalysts. To rationally design single-atom alloys and other surfaces with localized ensembles, it is crucial to understand variations in reactivity when varying the dopant and the ensemble size. Here, we examined hydrogen adsorption on surfaces embedded with localized clusters and discovered general trends. Counterintuitively, increasing the amount of a more reactive metal sometimes makes a surface site less reactive. This behavior is due to the localized electronic states in many of these surfaces, making them similar to free-standing nanoclusters. Further, single-atom alloys have qualitatively different behavior than larger ensembles. Specifically, the adsorption energy is U-shaped when plotted against the dopant’s group for single atom alloys. Additionally, adsorption energies on single atom alloys correlate more strongly with the dopant’s p-band center than the d-band center. </p> </div> </div> </div>

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Machine Learning Prediction of H Adsorption Energies on Ag Alloys

Cited by 53 publications

References 43 publications

When More Is Less: Nonmonotonic Trends in Adsorption on Clusters in Alloy Surfaces

When More Is Less: Nonmonotonic Trends in Adsorption on Clusters in Alloy Surfaces

General Screening of Surface Alloys for Catalysis

When More Is Less: Nonmonotonic Trends in Adsorption on Clusters in Alloy Surfaces

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