Metastability of palladium carbide nanoparticles during hydrogen release from liquid organic hydrogen carriers

Schuster, R.; Bertram, Manon; Runge, Henning; Geile, Simon; Chung, Simon; Vonk, Vedran; Noei, Heshmat; Poulain, Agnieszka; Lykhach, Yaroslava; Stierle, Andreas; Libuda, Jörg

doi:10.1039/d0cp05606e

Cited by 6 publications

(4 citation statements)

References 53 publications

(75 reference statements)

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“…A crucial aspect in LOHC development is selection of the proper catalytic system for the hydrogenation and dehydrogenation reactions. Various catalysts have been used for both the hydrogenation and dehydrogenation reactions, including precious metals platinum (Pt) [3], palladium (Pd) [4] and ruthenium (Ru) [5], supported on alumina (Al 2 O 3 ), carbide (C) and silica (SiO 2 ), to achieve chemical routes with high selectivity under sufficiently mild reaction conditions [6]. To understand the performance of Ru-based catalysts, the hexagonal close-packed (hcp) phase of Ru, the dominant phase in bulk Ru, has been studied extensively, both experimentally and theoretically using first-principles methods [7,8].…”

Section: Introductionmentioning

confidence: 99%

Computational Insights into Ru, Pd and Pt fcc Nano-Catalysts from Density Functional Theory Calculations: The Influence of Long-Range Dispersion Corrections

Ungerer

Leeuw

2022

Catalysts

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Ruthenium, palladium and platinum fall within the group of noble metals that are widely used in catalysis, especially for the electrocatalytic production of hydrogen. The dominant phase of the bulk Ru metal is hexagonal close-packed (hcp), which has been studied extensively. However, significantly less attention has been paid to the face-centred cubic (fcc) phases, which have been observed in nanoparticles. In this study, we have carried out density functional theory calculations with long-range dispersion corrections [DFT-D2, DFT-D3 and DFT-D3-(BJ)] to investigate the lattice parameters, surface energies and work functions of the (001), (011) and (111) surfaces of Ru, Pd and Pt in the fcc phase. When investigating the surface properties of the three metals, we observed that the DFT-D2 method generally underestimated the lattice parameters by up to 2.2% for Pt and 2.8% for Ru. The surface energies followed the observed trend (111) < (001) < (011) for both Ru and Pd with all three methods, which is comparable to experimental data. For Pt the same trend was observed with DFT-D2 and DFT-D3(BJ), but it deviated to Pt (111) < Pt (011) < Pt (001) for the DFT-D3 method. DFT-D2 overestimated the surface energies for all three Miller Indexes by 82%, 73%, and 60%, when compared to experimental values. The best correlation for the surface energies was obtained with the DFT-D3 and DFT-D3(BJ) methods, both of which have deviate by less than 15% deviation for all surfaces with respect to experiment. The work function followed the trend of Φ (111) < Φ (001) < Φ (011) for all three metals and calculated by all three methods. Five different types of Ru, Pd and Pt nanoparticles were considered, including icosahedral, decahedral, cuboctahedral, cubic and spherical particles of different sizes. The bulk, surface and nanoparticle calculations showed that the DFT-D2 method for Pt overestimated the exchange-correlation, leading to higher energy values that can be contributed erroneously to a more stable structure. The calculations showed that as soon as the surface-to-bulk ratio > 1, the energy per atom resembles bulk energy values.

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Section: Introductionmentioning

confidence: 99%

Computational Insights into Ru, Pd and Pt fcc Nano-Catalysts from Density Functional Theory Calculations: The Influence of Long-Range Dispersion Corrections

Ungerer

Leeuw

2022

Catalysts

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“…Therefore, optimization studies for LOHC-based hydrogen storage and transportation systems are actively conducted worldwide, and demonstration projects are underway to integrate LOHC systems with existing hydrogen infrastructure. However, continuous research and development efforts are needed due to the relatively low hydrogen density and availability compared to other hydrogen storage compounds (such as methanol and ammonia) [124,[128][129][130][131][132][133][134][135]. Various LOHCs based on substances including benzene and toluene have been researched, and their characteristics are summarized in Table 5 [126].…”

Section: Liquid Organic Hydrogen Carriermentioning

confidence: 99%

Chemical material as a hydrogen energy carrier: A review

Kim,

Yang

2024

Energ. Stor. Conv.

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In light of climate change imperatives, there arises a critical need for technological advancements and research endeavors towards clean energy alternatives to replace conventional fossil fuels. Additionally, the development of high-capacity energy storage solutions for global transportability becomes paramount. Hydrogen emerges as a promising environmentally sustainable energy carrier, devoid of carbon dioxide emissions and possessing a high energy density per unit mass. Its versatile applicability spans various sectors including industry, power generation, and transportation. However, the commercialization of hydrogen necessitates further technological innovations. Notably, high-pressure compression for hydrogen storage presents safety challenges and inherent limitations in storage capacity about 30%–50% lost production of hydrogen. Consequently, substantial research endeavors are underway in the domain of material-based chemical hydrogen storage that reactions to occur at temperatures below 200 ℃. This approach enables the utilization of existing infrastructure, such as fossil fuels and natural gas, while offering comparatively elevated hydrogen storage capacities. This study aims to introduce recent investigations concerning the synthesis and decomposition mechanisms of chemical hydrogen storage materials, including methanol, ammonia, and Liquid Organic Hydrogen Carrier (LOHC).

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“…Seriani et al 21 have reported the formation of a metastable carbide that corresponds to 13–14% of C concentration in which hydrogen diffusion is hindered as compared to pristine Pd. This Pd 6 C metastable carbide formation has been further investigated through experimental 22 and theoretical methods. 23 In the recent study of He et al , C diffusion into the Pd(100) and Pd(111) surface models show zigzag trajectories for the migration pathways and a non-uniform distribution in the slab.…”

Section: Introductionmentioning

confidence: 99%

Atomistic simulations on the carbidisation processes in Pd nanoparticles

et al. 2023

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Metastability of palladium carbide nanoparticles during hydrogen release from liquid organic hydrogen carriers

Abstract: The metastability of the Pd6C phase results from the thermodynamically favorable growth of graphene.

Cited by 6 publications

References 53 publications

Computational Insights into Ru, Pd and Pt fcc Nano-Catalysts from Density Functional Theory Calculations: The Influence of Long-Range Dispersion Corrections

Computational Insights into Ru, Pd and Pt fcc Nano-Catalysts from Density Functional Theory Calculations: The Influence of Long-Range Dispersion Corrections

Chemical material as a hydrogen energy carrier: A review

Atomistic simulations on the carbidisation processes in Pd nanoparticles

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