Constructing two-dimensional holey graphyne with unusual annulative π-extension

Liu, Xinghui; Cho, Soo Min; Lin, Shiru; Chen, Zhongfang; Choi, Wooseon; Kim, Young‐Min; Yun, Eunbhin; Baek, Eun Hee; Ryu, Do Hyun; Lee, Hyoyoung

doi:10.1016/j.matt.2022.04.033

Cited by 44 publications

(49 citation statements)

References 39 publications

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“…The HGY is a novel 2D carbon allotrope that has a space group of P6/mmm with a hexagonal lattice structure. The structure of HGY comprises six vertex and eight vertex rings linked via sp and sp 2 carbon bonds 60 . The optimized structure of the HGY with optimized C–C bond lengths of 1.461, 1.396, 1.413, and 1.226 Å is illustrated in Figure 1A.…”

Section: Resultsmentioning

confidence: 99%

“…Although there have been a lot of studies on the hydrogen storage performance of metal decorated carbon nanomaterials, the study is very limited for the systems beyond graphene having a large number of pores. The holey graphyne (HGY) is one of the novel two‐dimensional porous carbon allotropes, recently synthesized through the Castro‐Stephen coupling reaction from 1,3,5‐tribromo‐2,4,6‐triethynylbenzene 60 . The structure of HGY follows the pattern of six vertex and highly strained, eight vertex carbon rings with an equal percentage of sp 2 and sp hybridized carbon bonds.…”

Section: Introductionmentioning

confidence: 99%

“…The structure of HGY follows the pattern of six vertex and highly strained, eight vertex carbon rings with an equal percentage of sp 2 and sp hybridized carbon bonds. The p‐type semiconducting character and presence of uniformly distributed pores make HGY a promising material for energy storage applications 60 . The H 2 storage behavior of the Li‐decorated HGY and Sc‐decorated HGY system has already been investigated theoretically.…”

Section: Introductionmentioning

confidence: 99%

“…The holey graphyne (HGY) is one of the novel twodimensional porous carbon allotropes, recently synthesized through the Castro-Stephen coupling reaction from 1,3,5-tribromo-2,4,6-triethynylbenzene. 60 The structure of HGY follows the pattern of six vertex and highly strained, eight vertex carbon rings with an equal percentage of sp 2 and sp hybridized carbon bonds. The p-type semiconducting character and presence of uniformly distributed pores make HGY a promising material for energy storage applications.…”

Section: Introductionmentioning

confidence: 99%

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Reversible hydrogen adsorption in Ti‐functionalized porous holey graphyne: Insights from first‐principles calculation

et al. 2022

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By performing the density functional theory simulations, we have studied the H2 adsorption and desorption properties of the Ti‐functionalized holey graphyne system. The simulation results revealed that the Ti atom is bonded strongly to the holey graphyne sheet with a binding energy of −4.16 eV through the Dewar interaction. The Ti‐functionalized holey graphyne can capture 7H2 molecules with an average H2 adsorption energy of −0.38 eV/H2, leading to a hydrogen gravimetric density of 10.52 wt%. The average desorption temperature is computed by the Van't Hoff relation and obtained to be 486 K, optimum for practical applications. The adsorbed H2 molecules are attached with the Ti‐functionalized holey graphyne via the Kubas interactions involving charge donation and back donation between Ti‐3d orbitals and H‐1 s orbital. Subsequently, the ab initio molecular dynamics simulations have been conducted to verify the structural constancy of the storage media. We have found a sufficiently high energy barrier of 2.3 eV that prevents the system from metal‐metal clustering. Therefore, the Ti‐functionalized holey graphyne can be utilized as a promising high‐capacity reversible hydrogen storage medium.

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Section: Resultsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Reversible hydrogen adsorption in Ti‐functionalized porous holey graphyne: Insights from first‐principles calculation

et al. 2022

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“…Experimentally discovered perfect planar hexagonal and triangular lattices of graphene [9], h-BN [101], graphane [102], graphdiynes [103,104], gamma- [105] and holey-graphynes [106], g-C 3 N 4 [107], and g-C 4 N 3 [108] perfectly satisfy mandatory requirements of TCT since the structural fragments of low-dimensional crystals perfectly fill in the planar 2D space. It is necessary to note that hypothetic free-standing one-side hydrogenated graphan, so-called graphone [109], does not satisfy TCT mandatory requirements due to strong structural anisotropy.…”

Section: Phc(00) (R 57 Haeckelite) Latticementioning

confidence: 99%

Topological and quantum stability of low-dimensional crystalline lattices with multiple nonequivalent sublattices*

Avramov

Kuklin

2022

New J. Phys.

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The terms of topological and quantum stabilities of low-dimensional crystalline carbon lattices with multiple non-equivalent sublattices are coined using theoretical analysis, multilevel simulations, and available experimental structural data. It is demonstrated that complex low-dimensional lattices are prone to periodicity breakdown caused by structural deformations generated by linear periodic boundary conditions (PBC). To impose PBC mandatory limitations for complex low-dimensional lattices, the Topology Conservation Theorem (TCT) is introduced, formulated and proved. It is shown that the lack of perfect filling of planar 2D crystalline space by structural units may cause the formation of i) Structure waves of either variable or constant wavelength; ii) Nanotubes or rolls; iii) Saddle structures; iv) Aperiodic ensembles of irregular asymmetric atomic clusters; v) Stabilization of 2D lattices by aromatic resonance, correlation effects, or van-der-Waals interactions. The effect of quantum instability and periodicity breakdown of infinite structural waves is studied using quasiparticle approach. It is found that both perfect finite-sized, or stabilized structural waves can exist and can be synthesized. It is shown that for low-dimensional lattices prone to breakdown the translation invariance (TI), complete active space of normal coordinates cannot be reduced to a subspace of TI normal coordinates. As a result, constrained TI subspace structural minimization may artificially return a regular point at the potential energy surface as either a global/local minimum/maximum. It is proved that for such lattices, phonon dispersion cannot be used as solid and final proof of either their stability or metastability. It is shown that ab initio molecular dynamics (MD) PBC Nosé-Hoover thermostat algorithm constrains the linear dimensions of the periodic slabs in MD box preventing their thermostated equilibration. Based on rigorous TCT analysis, a flowchart algorithm for structural analysis of low-dimensional crystals is proposed and proved to be a powerful tool for theoretical design of advanced complex nanomaterials.

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Design of Graphdiyne and Holey Graphyne‐Based Single Atom Catalysts for CO₂ Reduction With Interpretable Machine Learning

Ren

Guo

Zhang

et al. 2023

Adv Funct Materials

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Using electrochemical CO2 reduction reaction (CO2RR) to synthesize value‐added hydrocarbons provides a useful solution for environmental issues and energy crisis. However, this process is impeded by the low activity and selectivity of electrocatalysts toward targeted products. Employing density functional theory computations, the graphdiyne and holey graphyne supported single‐atom catalysts (SACs, M/GDY and M/HGY) are demonstrated to be the promising candidates for the CO2RR. By taking full elemental diversity of metal sites across the periodic table, 25 catalysts are found to effectively activate CO2 and inhibit competitive hydrogen evolution, and 8 of them show higher activity for CH4 production than Cu(211). Remarkably, changing supports are found to greatly affect limiting potentials and reaction pathways, even leading to an “inert‐active” transition for some metal centers. The resulting SACs, including Mn/GDY, Co/HGY, Ru/GDY, and Os/GDY, can achieve high activity with low limiting potentials of ≈ −0.22 to −0.58 V. Machine learning enables to identify the critical role of the polarized charge and magnetic moment of metal atoms in affecting the activity. The built machine learning model also shows an interpretable capability to predict the activity of the other types of SACs, offering a great promise to quick screening of high‐performance SACs.

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Constructing two-dimensional holey graphyne with unusual annulative π-extension

Cited by 44 publications

References 39 publications

Reversible hydrogen adsorption in Ti‐functionalized porous holey graphyne: Insights from first‐principles calculation

Reversible hydrogen adsorption in Ti‐functionalized porous holey graphyne: Insights from first‐principles calculation

Topological and quantum stability of low-dimensional crystalline lattices with multiple nonequivalent sublattices*

Design of Graphdiyne and Holey Graphyne‐Based Single Atom Catalysts for CO₂ Reduction With Interpretable Machine Learning

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Constructing two-dimensional holey graphyne with unusual annulative π-extension

Cited by 44 publications

References 39 publications

Reversible hydrogen adsorption in Ti‐functionalized porous holey graphyne: Insights from first‐principles calculation

Reversible hydrogen adsorption in Ti‐functionalized porous holey graphyne: Insights from first‐principles calculation

Topological and quantum stability of low-dimensional crystalline lattices with multiple nonequivalent sublattices*

Design of Graphdiyne and Holey Graphyne‐Based Single Atom Catalysts for CO2 Reduction With Interpretable Machine Learning

Contact Info

Product

Resources

About

Design of Graphdiyne and Holey Graphyne‐Based Single Atom Catalysts for CO₂ Reduction With Interpretable Machine Learning