Influence of Magnetic Moment on Single Atom Catalytic Activation Energy Barriers

Ngo, H.; Li, Jie; Wang, Chen Santillan; Wu, Ruqian; Ragan, Regina

doi:10.1007/s10562-021-03737-y

Cited by 7 publications

(4 citation statements)

References 70 publications

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“…Previously studied N-doped ZGNRs edges were established as magnetic [26], different from our findings for FeN 4 -doped ZGNR edges. Other DFT studies have reported on the spin suppression of edge carbon sites in Ti-, Pt-, and Au-doped ZGNR edges [52][53][54]. The band structures depicted in Figure 4b also exhibited sensitivity to the FeN 4 location, which was especially noticeable in the spin-down channel (red curves in Figure 4b).…”

Section: Magnetic and Electronic Properties As A Function Of Fen4 Loc...mentioning

confidence: 74%

Section: Resultsmentioning

confidence: 99%

“…Furthermore, the spin-down dz 2 electrons in the at-edge FeN 4 -ZGNRs are practically localized at the Fermi level (see Figure 5 ), which would enhance their interaction with the spin-polarized πp* orbital of O 2 (the ground state of O 2 is a triplet spin state) or the doublet spin-state of OH*. The increase of spin asymmetry (the difference in the population of spin-up and spin-down states) in the band structure of MeN 4 -graphene catalysts was also suggested to improve the catalytic activity in the CO oxidation reaction [ 54 ]. Following the evolution of the band diagrams in Figure 4 b,d, we observed that moving FeN 4 from the in-plane to the edge resulted in increasing the differences between the populations of spin-down and spin-up channels close to the Fermi level, thus highlighting again the edge-doped FeN 4 graphene GNRs as potentially highly active catalysts.…”

Section: Resultsmentioning

confidence: 99%

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Exploring Spin Distribution and Electronic Properties in FeN4-Graphene Catalysts with Edge Terminations

Oguz,

Jaouen,

Mineva

2024

Molecules

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Understanding the spin distribution in FeN4-doped graphene nanoribbons with zigzag and armchair terminations is crucial for tuning the electronic properties of graphene-supported non-platinum catalysts. Since the spin-polarized carbon and iron electronic states may act together to change the electronic properties of the doped graphene, we provide in this work a systematic evaluation using a periodic density-functional theory-based method of the variation of spin-moment distribution and electronic properties with the position and orientation of the FeN4 defects, and the edge terminations of the graphene nanoribbons. Antiferromagnetic and ferromagnetic spin ordering of the zigzag edges were considered. We reveal that the electronic structures in both zigzag and armchair geometries are very sensitive to the location of FeN4 defects, changing from semi-conducting (in-plane defect location) to half-metallic (at-edge defect location). The introduction of FeN4 defects at edge positions cancels the known dependence of the magnetic and electronic proper-ties of undoped graphene nanoribbons on their edge geometries. The implications of the reported results for catalysis are also discussed in view of the presented electronic and magnetic properties.

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Section: Magnetic and Electronic Properties As A Function Of Fen4 Loc...mentioning

confidence: 74%

Section: Resultsmentioning

confidence: 99%

Section: Resultsmentioning

confidence: 99%

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Exploring Spin Distribution and Electronic Properties in FeN4-Graphene Catalysts with Edge Terminations

Oguz,

Jaouen,

Mineva

2024

Molecules

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“…The spin degrees of freedom have an important in uence on the catalytic performance of magnetic monatomic catalysts 47,48,49,50 . The spin density population of M 1 /PTA are presented in Fig.…”

Section: Screening M1/pta Catalysts For Ethyne Hydrogenation Reactionmentioning

confidence: 99%

Catalytic Performance of Single-Atom Catalysts M1/PW12O40 for Alkyne Hydrogenation

Talib

Jiang

et al. 2023

Preprint

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Single-atom catalysts (SACs) have provoked significant curiosity in heterogeneous catalysis due to the benefits of maximum metal atoms usage, robust metal-support interaction, single-metal-atom active sites, and high catalytic efficiency. Transition metal (M1) adatoms anchored on highly stable phosphotungstic acid (PTA) cluster (Scheme 1) provide an opportunity for altering their electronic, magnetic and catalytic characteristics. In this study, the electronic structures and catalytic mechanism of ethyne hydrogenation of SACs with the group-9 metal atoms M1 (M1= Co, Rh, Ir) anchored on PTA cluster have been explored by using first-principles quantum calculations. It is found that the catalytic activity of ethyne hydrogenation is determined by two critical parameters: the adsorption energies of the adsorbate (H2, C2H2) and the activation energy barrier of ethyne hydrogenation. We have shown that the reaction pathway of ethyne hydrogenation reaction on the experimentally characterized Rh1/PTA at room temperature consists of three steps: C2H2 and H2 coadsorption on Rh1/PTA, H2 attacking C2H2 to form C2H4, then C2H4 desorbing or further reacting with H2 to produce C2H6 and completing the catalytic cycle. The Rh1/PTA possesses fair catalytic activity with C2H4 desorption energy of 1.46 eV at the rate determining step and high selectivity for ethylene formation through the Langmuir−Hinshelwood mechanism. The potentially competitive mechanism for the formation of ethane is not kinetically favorable, with a 2.59 eV barrier for ethylene hydrogenation. Moreover, micro-kinetics analysis is also carried out to further understand the mechanism and catalytic performance. The work reveals that the PTA supported SACs can be a promising catalyst for alkyne hydrogenation.

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Non‐trivial Contribution of Carbon Hybridization in Carbon‐based Substrates to Electrocatalytic Activities in Li‐S Batteries

et al. 2022

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Appling an electrochemical catalyst is an efficient strategy for inhibiting the shuttle effect and enhancing the S utilization of Li-S batteries. Carbonbased materials are the most common conductive agents and catalyst supports used in Li-S batteries, but the correlation between the diversity of hybridizations and sulfur reduction reaction (SRR) catalytic activity remains unclear. Here, by establishing two forms of carbon models, i.e., graphitic carbon (GC) and amorphous carbon (AC), we observe that the nitrogen atom doped in the GC possesses a higher local charge density and a lower Gibbs free energy towards the formation of polysulfides than in the AC. And the GC-based electrode consistently inherits considerably enhanced SRR kinetics and superior cycling stability and rate capability in Li-S batteries. Therefore, the function of carbon in Li-S batteries is not only limited as conductive support but also plays an unignorable contribution to the electrocatalytic activities of SRR.

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Influence of Magnetic Moment on Single Atom Catalytic Activation Energy Barriers

Cited by 7 publications

References 70 publications

Exploring Spin Distribution and Electronic Properties in FeN4-Graphene Catalysts with Edge Terminations

Exploring Spin Distribution and Electronic Properties in FeN4-Graphene Catalysts with Edge Terminations

Catalytic Performance of Single-Atom Catalysts M1/PW12O40 for Alkyne Hydrogenation

Non‐trivial Contribution of Carbon Hybridization in Carbon‐based Substrates to Electrocatalytic Activities in Li‐S Batteries

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