Metal‐Doped PdH(111) Catalysts for CO<sub>2</sub> Reduction

Ai, Changzhi; Vegge, Tejs; Hansen, Heine Anton

doi:10.1002/cssc.202200008

Cited by 11 publications

(22 citation statements)

References 43 publications

(74 reference statements)

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“…All information on surface structures with adsorbates on all unique sites can be found in our database. 38 Binding energies of adsorbates of HOCO*, CO*, OH* and H* on the most stable sites of all PdH x candidates are shown in Figure 3b and the corresponding data can be found in Table S3. It can be seen that the binding energies of all adsorbates gradually increase as the concentration of H goes up from 0 to 1, especially for the adsorbate CO*.…”

Section: Resultsmentioning

confidence: 99%

“…pressure is 5562 Pa. 35 The partial pressure of both CO 2 and H 2 are under standard pressure 101325 Pa. 10,35 Further details for the calculations for Gibbs free energy and the kinetic model can be found in our previous work and the supporting information. 34 small range, approximately 0.2 Å from 0 to 1 for H concentration, which is less than 5% of the lattice constants of PdH. 36 Besides, previous work reported the strain of PdH only has a small impact on the performance of CO 2 RR and HER.…”

Section: All Cluster Expansion (Ce) Calculations In This Work Are Per...mentioning

confidence: 96%

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Impact of Hydrogen Concentration for CO2 reduction on PdHx

Chang

Tygesen

et al. 2023

Preprint

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Pd hydride has shown much better electrochemical CO2 reduction reaction (CO2RR) performance compared to metal Pd implying that H in the PdHx surface plays a vital role in affecting the performance. Some experiments show phase transformation from metal Pd to PdHx via in-situ X-ray diffraction and electrochemical method. However, studying the stable atomic structures and reaction mechanisms at different H concentrations is experimentally very difficult. Most previous experimental and com- putational studies only focus on the comparison of CO2RR performance of pure metal Pd (0% H concentration) and Pure PdH (100% H concentration). However, there is also no systematical theoretical study about the H concentration effect of PdHx (from 0% to 100%) on CO2RR and the hydrogen evolution reaction (HER), and the atomic structure of the active substoichiometric PdHx catalyst have not been identi- fied. Based on density functional theory (DFT) calculations, active learning cluster expansion equipped with Monte Carlo simulated annealing is carried out to search for stable PdHx(111) surface configurations in this work. We identify 12 stable PdHx(111) configurations from the converged DFT convex hull and theoretically investigate the evolution of the H concentration of the stable structures as a function of applied potential. After automatically finding unique adsorption sites and calculating the binding energies of adsorbates, we analyze their free energy diagram, activity volcano and selectivity toward CO and H2. Finally, we identify the atomic structure of the PdHx phase most likely to produce syngas. It’s activity can be attributed to the fact that H segregation breaks the linear relation between COOH and CO adsorbates.

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Section: Resultsmentioning

confidence: 99%

Section: All Cluster Expansion (Ce) Calculations In This Work Are Per...mentioning

confidence: 96%

Impact of Hydrogen Concentration for CO2 reduction on PdHx

Chang

Tygesen

et al. 2023

Preprint

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“…Microkinetic modeling of ENRR is performed along the DFT-predicted most favorable ENRR pathways on TMNO(100) with and without N-vacancy using the methods described in the Section 2 and elsewhere. 77,85,86 On perfect TMNO(100), CrNO, HfNO, and VNO lie close to the regions where log(i 0 ) is maximum. Figure 11a shows that a catalyst that has an N 2 HBE of ∼−2 eV and an N 2 BE of ∼−1.6 would be ideal for optimum ENRR.…”

Section: Microkinetic Modelingmentioning

confidence: 87%

A Density Functional Theory Study of Electrochemical Nitrogen Reduction to Ammonia on the (100) Surface of Transition-Metal Oxynitrides

Ologunagba

Kattel

2022

J. Phys. Chem. C

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The electrochemical nitrogen (N 2 ) reduction reaction (ENRR) to produce ammonia (NH 3 ) under ambient conditions is attractive compared to the energy-and carbon-intensive industrialized Haber−Bosch process. However, efficient catalysts are needed to break an N�N bond in an N 2 molecule to convert it to NH 3 . Transition-metal oxynitrides (TMNOs) have shown promising ENRR activities at low potentials. Here, density functional theory (DFT) calculations are performed to study the ENRR activity of TMNO(100) surfaces for TM = Co,

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“…Twenty-two transition metal elements are doped into the PdH(111) surface with different doping configurations, and Ti-doped Pd hydride shows high CO 2 RR and HER activity. 31 Based on this information, the Ti−Pd alloy hydride system with a higher complexity is also likely to accommodate very active candidates. Subsequently, the chemical composition of the alloy hydride Pd x Ti 1−x H y (111) surface is searched by the cluster expansion method equipped with Monte Carlo simulated annealing according to the compound stability.…”

Section: Introductionmentioning

confidence: 99%

“…Substantial efforts have been made in Pd-based hydride systems to establish relationships between the structures and the electrochemical performance. , Our previous systematic doping study builds the relationship between transition metal doping and CO 2 RR activity. Twenty-two transition metal elements are doped into the PdH(111) surface with different doping configurations, and Ti-doped Pd hydride shows high CO 2 RR and HER activity . Based on this information, the Ti–Pd alloy hydride system with a higher complexity is also likely to accommodate very active candidates.…”

Section: Introductionmentioning

confidence: 99%

Graph Neural Network-Accelerated Multitasking Genetic Algorithm for Optimizing Pd_xTi_1–xH_y Surfaces under Various CO₂ Reduction Reaction Conditions

Ai,

Han,

Yang

et al. 2024

ACS Appl. Mater. Interfaces

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Palladium (Pd) hydride-based catalysts have been reported to have excellent performance in the CO2 reduction reaction (CO2RR) and hydrogen evolution reaction (HER). Our previous work on doped PdH and Pd alloy hydrides showed that Ti-doped and Ti-alloyed Pd hydrides could improve the performance of the CO2 reduction reaction compared with pure Pd hydride. Compositions and chemical orderings of the surfaces with only one adsorbate under certain reaction conditions are linked to their stability, activity, and selectivity toward the CO2RR and HER, as shown in our previous work. In fact, various coverages, types, and mixtures of the adsorbates, as well as state variables such as temperature, pressure, applied potential, and chemical potential, could impact their stability, activity, and selectivity. However, these factors are usually fixed at common values to reduce the complexity of the structures and the complexity of the reaction conditions in most theoretical work. To address the complexities above and the huge search space, we apply a deep learning-assisted multitasking genetic algorithm to screen for Pd x Ti1–x H y surfaces containing multiple adsorbates for CO2RR under different reaction conditions. The ensemble deep learning model can greatly speed up the structure relaxations and retain a high accuracy and low uncertainty of the energy and forces. The multitasking genetic algorithm simultaneously finds globally stable surface structures under each reaction condition. Finally, 23 stable structures are screened out under different reaction conditions. Among these, Pd0.56Ti0.44H1.06 + 25%CO, Pd0.31Ti0.69H1.25 + 50%CO, Pd0.31Ti0.69H1.25 + 25%CO, and Pd0.88Ti0.12H1.06 + 25%CO are found to be very active for CO2RR and suitable to generate syngas consisting of CO and H2.

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Metal‐Doped PdH(111) Catalysts for CO₂ Reduction

Abstract: PdH-based catalysts hold promise for both CO 2 reduction to CO and the hydrogen evolution reaction. Density functional theory is used to systematically screen for stability, activity, and selectivity of transition metal dopants in PdH. The transition metal elements Sc,

Cited by 11 publications

References 43 publications

Impact of Hydrogen Concentration for CO2 reduction on PdHx

Impact of Hydrogen Concentration for CO2 reduction on PdHx

A Density Functional Theory Study of Electrochemical Nitrogen Reduction to Ammonia on the (100) Surface of Transition-Metal Oxynitrides

Graph Neural Network-Accelerated Multitasking Genetic Algorithm for Optimizing Pd_xTi_1–xH_y Surfaces under Various CO₂ Reduction Reaction Conditions

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Metal‐Doped PdH(111) Catalysts for CO2 Reduction

Abstract: PdH-based catalysts hold promise for both CO 2 reduction to CO and the hydrogen evolution reaction. Density functional theory is used to systematically screen for stability, activity, and selectivity of transition metal dopants in PdH. The transition metal elements Sc,

Cited by 11 publications

References 43 publications

Impact of Hydrogen Concentration for CO2 reduction on PdHx

Impact of Hydrogen Concentration for CO2 reduction on PdHx

A Density Functional Theory Study of Electrochemical Nitrogen Reduction to Ammonia on the (100) Surface of Transition-Metal Oxynitrides

Graph Neural Network-Accelerated Multitasking Genetic Algorithm for Optimizing PdxTi1–xHy Surfaces under Various CO2 Reduction Reaction Conditions

Contact Info

Product

Resources

About

Metal‐Doped PdH(111) Catalysts for CO₂ Reduction

Graph Neural Network-Accelerated Multitasking Genetic Algorithm for Optimizing Pd_xTi_1–xH_y Surfaces under Various CO₂ Reduction Reaction Conditions