Interfacial-Bonding-Regulated CO Oxidation over Pt Atoms Immobilized on Gas-Exfoliated Hexagonal Boron Nitride

Liu, Xin; Zhu, Hongdan; Linguerri, Roberto; Han, Yu; Chambaud, Gilberte; Meng, Changgong

doi:10.1002/slct.201701663

Cited by 6 publications

(5 citation statements)

References 56 publications

(29 reference statements)

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“…4, right panel), suggesting the high reactivity of these supported clusters, similar to mono-dispersed Ir atoms, to approaching molecules for their activation and conversion. 30,32,54,55…”

Section: Discussionmentioning

confidence: 99%

Adsorption, diffusion and aggregation of Ir atoms on graphdiyne: a first-principles investigation

Liu

Han

et al. 2020

Phys. Chem. Chem. Phys.

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“…4, right panel), suggesting the high reactivity of these supported clusters, similar to mono-dispersed Ir atoms, to approaching molecules for their activation and conversion. 30,32,54,55…”

Section: Discussionmentioning

confidence: 99%

Adsorption, diffusion and aggregation of Ir atoms on graphdiyne: a first-principles investigation

Liu

Han

et al. 2020

Phys. Chem. Chem. Phys.

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“…We recently investigated CO oxidation over the defect-stabilized Fe and Pd SACs on graphene and demonstrated that the coadsorption of CO and O 2 would be more plausible on these SACs over van de Waals complexes and the coadsorption of 2 CO to initiate CO oxidation on ER type pathways. Thus, it would be a major reaction species with a population superior to those van de Waals complexes and is the active species to initiate CO oxidation [ 55 , 56 , 81 ]. The calculated thermodynamics stability of reaction species on AuBN ( Figure 1 j) also demonstrated such a trend that AuO 2 + CO is more plausible than AuO 2 + CO(g) and Au(CO) 2 , though AuCO is the most plausible species in reaction conditions.…”

Section: Resultsmentioning

confidence: 99%

Coadsorption Interfered CO Oxidation over Atomically Dispersed Au on h-BN

2022

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Similar to the metal centers in biocatalysis and homogeneous catalysis, the metal species in single atom catalysts (SACs) are charged, atomically dispersed and stabilized by support and substrate. The reaction condition dependent catalytic performance of SACs has long been realized, but seldom investigated before. We investigated CO oxidation pathways over SACs in reaction conditions using atomically dispersed Au on h-BN (AuBN) as a model with extensive first-principles-based calculations. We demonstrated that the adsorption of reactants, namely CO, O2 and CO2, and their coadsorption with reaction species on AuBN would be condition dependent, leading to various reaction species with different reactivity and impact the CO conversion. Specifically, the revised Langmuir–Hinshelwood pathway with the CO-mediated activation of O2 and dissociation of cyclic peroxide intermediate followed by the Eley–Rideal type reduction is dominant at high temperatures, while the coadsorbed CO-mediated dissociation of peroxide intermediate becomes plausible at low temperatures and high CO partial pressures. Carbonate species would also form in existence of CO2, react with coadsorbed CO and benefit the conversion. The findings highlight the origin of the condition-dependent CO oxidation performance of SACs in detailed conditions and may help to rationalize the current understanding of the superior catalytic performance of SACs.

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“…[160][161][162][163][164][165][166] Liu et al explicated the importance of the dangling bonds surrounding the B-and N-vacancies during the fabrication of Pt/h-BN SACs, noting that they led to the formation of strong interfacial bonds that maintained the dispersion of the Pt atoms on the support surface. [167] On a similar note, Li et al performed d) TEM images of ZIF-67, AC-FeCoNi, and Ru SAs/AC-FeCoNi. e,h) HRTEM images of Ru SAs/AC-FeCoNi.…”

Section: Others (Ldh 2d Mof H-bn)mentioning

confidence: 94%

“…explicated the importance of the dangling bonds surrounding the B‐ and N‐vacancies during the fabrication of Pt/h‐BN SACs, noting that they led to the formation of strong interfacial bonds that maintained the dispersion of the Pt atoms on the support surface. [ 167 ] On a similar note, Li et al. performed DFT calculations to confirm the feasibility of generating B‐ and N‐vacancies in h‐BN, which can provide active trap sites for capturing single Pd atoms.…”

Section: Enhancing Metal–support Interactions Via Surface Modificatio...mentioning

confidence: 99%

Modulating the Local Coordination Environment of Single‐Atom Catalysts for Enhanced Catalytic Performance in Hydrogen/Oxygen Evolution Reaction

Tomboc

Kim

Jung

et al. 2022

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source could provide an auspicious alternative for reducing humanity's dependency on fossil fuels, thus lowering their environmental impact. [1][2][3][4][5] Electrochemical water splitting technology is intended for the large-scale production of high-purity H 2 . The primary reaction in the electrochemical water splitting cell is divided into two half-reactions: the oxygen evolution reaction (OER), which takes place in the anode, and the hydrogen evolution reaction (HER), which takes place in the cathode. The overall chemical reaction is simplified as H 2 O → H 2 (cathode) + ½ O 2 (anode), which can theoretically proceed with a minimum energy input of ΔG = 237.1 kJ mol −1 at a thermodynamic potential of 1.23 V. Nevertheless, the large overpotentials required to overcome the high activation barriers of the OER severely hinder the mass production of H 2 via electrochemical water splitting. [2,[6][7][8][9][10] In this regard, noble metalbased catalysts, such as IrO 2 /RuO 2 and Pt/C, possess great catalytic performances towards OER and HER, respectively. [11,12] The high costs and limited resources of noble metals have mandated researchers to seek alternatives in various affordable, non-noble metal-based electrocatalysts, like transition metal oxides (hydroxides), sulfides, phosphides, nitrides and carbides, and functional metal-free carbon composites. [13][14][15][16][17][18][19][20][21][22] However, these alternatives offer acceptable OER and HER catalytic performances when used in alkaline and acidic solutions, respectively, thereby limiting their practical applications. Besides, these materials are susceptible to rapid particle agglomeration during electrochemical operation, leading to limited atomic utilization efficiency. Noble metals like Pt, Pd, Ir, Rh, and Ru are still considered benchmark electrocatalytic materials for both HER and OER; hence, the development of cost-effective noble metal-based electrocatalysts is highly demanded.Previous studies pointed out that the catalytic activity of HER and OER catalysts is highly dependent on the density and chemical nature of the active sites, which can be improved via downscaling of the particle size. Single-atom catalysts (SACs) are the smallest possible size for a catalyst and could expose a larger surface area and tailor the atomic configuration and electronic structure, leading to optimal HER and OER activities. Thus, the development of SACs has become at the forefront of both Single-atom catalysts (SACs) hold the promise of utilizing 100% of the participating atoms in a reaction as active catalytic sites, achieving a remarkable boost in catalytic efficiency. Thus, they present great potential for noble metal-based electrochemical application systems, such as water electrolyzers and fuel cells. However, their practical applications are severely hindered by intrinsic complications, namely atom agglomeration and relocation, originating from the uncontrollably high surface energy of isolated singleatoms (SAs) during postsynthetic treatment processes or catalytic ...

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Interfacial-Bonding-Regulated CO Oxidation over Pt Atoms Immobilized on Gas-Exfoliated Hexagonal Boron Nitride

Cited by 6 publications

References 56 publications

Adsorption, diffusion and aggregation of Ir atoms on graphdiyne: a first-principles investigation

Adsorption, diffusion and aggregation of Ir atoms on graphdiyne: a first-principles investigation

Coadsorption Interfered CO Oxidation over Atomically Dispersed Au on h-BN

Modulating the Local Coordination Environment of Single‐Atom Catalysts for Enhanced Catalytic Performance in Hydrogen/Oxygen Evolution Reaction

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