Theoretical Exploration of Peculiar Sandwich-Type Clusters Formed by the Coordination of E<sub>9</sub><sup>2–</sup> (E = Si, Ge, Sn) Zintl Clusters: Structural Properties, Active Sites, and Hydrogen Storage

Wang, Yue; Shi, Xin; Wu, Wenbin; Deng, Xianhong; Xin, Kai; Zhou, Ziqing; Tang, Lihong; Ning, Zhiyuan

doi:10.1021/acs.langmuir.2c02600

Cited by 3 publications

(3 citation statements)

References 75 publications

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“…Chemical bonding analysis was performed for each stoichiometry via AdNDP 2.0 algorithm, [60,61] which is an effective tool for deciphering bonding patterns with untrivial electron localization. This method is productive for investigating structures possessing multi-center bonds, [62][63][64][65] which is essential for Tl hydride structures. The algorithm is based on the concept that an electron pair is the main bonding elements.…”

Section: Computational Detailsmentioning

confidence: 99%

Global Minimum Search and Bonding Analysis of Tl₂H_x and Tl₃H_y (x=0–6; y=0–5) Series

et al. 2023

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A remarkable distinction between boron and carbon hydrides lies in their extremely different bonding patterns and chemical reactivity, resulting in diverse areas of application. Particularly, carbon, characterized by classical two‐center – two‐electron bonds, gives rise to organic chemistry. In contrast, boron forms numerous exotic and non‐intuitive compounds collectively called non‐classical structures. It is reasonable to anticipate that other elements of Group 13 exhibit their own unusual bonding patterns; however, our knowledge of the hydride chemistry for other elements in Group 13 is much more limited, especially for the heaviest stable element, thallium. In this work, we performed a conformational analysis of Tl2Hx and Tl3Hy (x=0–6, y=0–5) series via Coalescence Kick global minimum search algorithm, DFT, and ab initio quantum chemistry methods; we investigated the bonding pattern using the AdNDP algorithm, thermodynamic stability, and stability toward electron detachment. All found global minimum structures are classified as non‐classical structures featuring at least one multi‐center bond.

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Section: Computational Detailsmentioning

confidence: 99%

Global Minimum Search and Bonding Analysis of Tl₂H_x and Tl₃H_y (x=0–6; y=0–5) Series

et al. 2023

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“…AdNDP is effectively used to decipher the chemical bonding pattern of molecules, [24,25] solid materials, [28,29] and clusters, which is the most essential for the current work; more specifically, it was applied for describing and interpreting structure properties of Boron clusters, [30][31][32][33] Aluminum clusters, [34][35] Tin clusters, [36][37] Germanium [38][39][40] and many others. [41][42][43][44][45][46][47] This makes the approach adequate for bonding analysis of bismuth polycation clusters.…”

Section: Introductionmentioning

confidence: 99%

“…This method is capable of providing not only Lewis's bonding elements (1c–2e lone pairs and 2c–2e “classical” bonds) but also a non‐classic multi‐center representation of delocalized bonds (nc–2e bonds, where n≥3), which allows to introduce the concepts of aromaticity naturally. AdNDP is effectively used to decipher the chemical bonding pattern of molecules, [24,25] solid materials, [28,29] and clusters, which is the most essential for the current work; more specifically, it was applied for describing and interpreting structure properties of Boron clusters, [30–33] Aluminum clusters, [34–35] Tin clusters, [36–37] Germanium [38–40] and many others [41–47] . This makes the approach adequate for bonding analysis of bismuth polycation clusters.…”

Section: Introductionmentioning

confidence: 99%

Bismuth Infrared Star: Being at a Glance

Pozdeev

Rublev

Boldyrev

2023

Chemistry A European J

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Bismuth polycations have garnered significant attention from researchers due to their extraordinary and counter‐intuitive structures and stoichiometries. Despite extensive experimental and theoretical investigations, our understanding of the bonding in such clusters remains insufficient. In this study, we conducted an AdNDP bonding analysis to elucidate the bonding characteristics using both homoatomic and heteroatomic bismuth clusters with various stoichiometries. By analyzing the calculated nucleus‐independent chemical shift data, we confirmed the aromatic nature of these species. We identified some universal bonding patterns that can be applied to a range of homoatomic and heteroatomic bismuth clusters. Additionally, we performed calculations of absorbance and fluorescence spectra to gain insights into the near‐infrared emission and establish a potential correlation between absorbance and the identified bonding patterns.

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The structural and electronic split: Boron vs aluminum hydrides

Pozdeev,

Popov

2024

Chemical Physics Reviews

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We systematically investigated the structural evolution of boron (B) and aluminum (Al) hydrides using various DFT and ab initio methods, aiming to reveal the similarities and differences in their geometric and electronic structures. While B hydrides have been extensively studied both experimentally and theoretically, less is known about its group 13 heavier congener, Al. Extensive global minimum searches of the B2Hx (Al2Hx) and B3Hy (Al3Hy) hydrides (x = [0–6], y = [0–9]) were performed to identify the most stable geometric structures for each stoichiometry. In most of the series, B and Al hydrides exhibit qualitatively different structures, except for the most saturated X2H5 and X2H6 stoichiometries. Chemical bonding analyses employing adaptive natural density partitioning and electron localization function methods identified notable differences between B and Al hydrides in most of the compositions. B hydrides predominantly possess two-center (2c) and three-center (3c) bonding elements, suggesting a relatively balanced electron distribution. On the contrary, Al hydrides tend to retain unpaired electrons or lone pairs on Al atoms, forming a large number of closely lying isomers with various combinations of 1c, 2c, 3c, and 4c bonding elements. Thermodynamic stability analyses revealed that all studied clusters demonstrated stability toward various H/H2 dissociation pathways, with Al hydrides being less stable than B counterparts.

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Theoretical Exploration of Peculiar Sandwich-Type Clusters Formed by the Coordination of E₉^2– (E = Si, Ge, Sn) Zintl Clusters: Structural Properties, Active Sites, and Hydrogen Storage

Abstract: A peculiar heterogeneous metal sandwich fragment {(Ge 9 ) 2 [η 6 -Ge(PdPPh 3 ) 3 ]} 4− anion cluster was synthesized for the first time by Xu et al.

Cited by 3 publications

References 75 publications

Global Minimum Search and Bonding Analysis of Tl₂H_x and Tl₃H_y (x=0–6; y=0–5) Series

Global Minimum Search and Bonding Analysis of Tl₂H_x and Tl₃H_y (x=0–6; y=0–5) Series

Bismuth Infrared Star: Being at a Glance

The structural and electronic split: Boron vs aluminum hydrides

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Theoretical Exploration of Peculiar Sandwich-Type Clusters Formed by the Coordination of E92– (E = Si, Ge, Sn) Zintl Clusters: Structural Properties, Active Sites, and Hydrogen Storage

Abstract: A peculiar heterogeneous metal sandwich fragment {(Ge 9 ) 2 [η 6 -Ge(PdPPh 3 ) 3 ]} 4− anion cluster was synthesized for the first time by Xu et al.

Cited by 3 publications

References 75 publications

Global Minimum Search and Bonding Analysis of Tl2Hx and Tl3Hy (x=0–6; y=0–5) Series

Global Minimum Search and Bonding Analysis of Tl2Hx and Tl3Hy (x=0–6; y=0–5) Series

Bismuth Infrared Star: Being at a Glance

The structural and electronic split: Boron vs aluminum hydrides

Contact Info

Product

Resources

About

Theoretical Exploration of Peculiar Sandwich-Type Clusters Formed by the Coordination of E₉^2– (E = Si, Ge, Sn) Zintl Clusters: Structural Properties, Active Sites, and Hydrogen Storage

Global Minimum Search and Bonding Analysis of Tl₂H_x and Tl₃H_y (x=0–6; y=0–5) Series

Global Minimum Search and Bonding Analysis of Tl₂H_x and Tl₃H_y (x=0–6; y=0–5) Series