Two dimensional inorganic electride-promoted electron transfer efficiency in transfer hydrogenation of alkynes and alkenes

Kim, Ye Ji; Kim, Sun Min; Cho, Eun Jin; Hosono, Hideo; Yang, Jung Woon

doi:10.1039/c5sc00933b

Cited by 56 publications

(42 citation statements)

References 26 publications

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“…The seminal example is the layered dicalcium nitride (Ca 2 N) with an Anti-CdCl 2 structure (R-3m), which can be taken as [Ca 2 N] + (e -). Remarkably, the excess electrons from counting oxidation numbers were confined in the space between the [Ca 2 N] + layers, forming dense twodimensional (2D) electron layer, 6,21 promising for electron dopant, [22][23][24][25][26] batteries, 27,28 and plasmonic device applications. [29][30][31] Meanwhile, monolayer Ca 2 N preserving its unique two-dimensional electron layers in interstitial space was predicted to be stable theoretically and subsequently was grown experimentally.…”

Section: Introductionmentioning

confidence: 99%

Discovery of Hidden Classes of Layered Electrides by Extensive High-Throughput Material Screening

et al. 2019

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Despite their extraordinary properties, electrides are still a relatively unexplored class of materials with only a few compounds grown experimentally. Especially for layered electrides, the current researches mainly focus on several isostructures of Ca 2 N with similar interlayer two-dimensional (2D) anionic electrons. An extensive screening for different layered electrides is still missing. Here, by screening materials with anionic electrons for the structures in Materials Project, we uncover 12 existing materials as new layered electrides. Remarkably, these layered electrides demonstrate completely different properties from Ca 2 N. For example, unusual fully spin-polarized zero-dimensional (0D) anionic electrons are shown in metal halides with MoS 2 -like structures; unique one-dimensional (1D) anionic electrons are confined within the tubes of the quasi-1D structures; a coexistence of magnetic and non-magnetic anionic electrons is found in ZrCl-like structures and a new ternary Ba 2 LiN with both 0D and 1D anionic electrons. These materials not only significantly increase the pool of experimentally synthesizable layered electrides but also are promising to be exfoliated into advanced 2D materials. ASSOCIATED CONTENT Supporting Information.This material is available free of charge via the Internet at http://pubs.acs.org." Basic structural, electronic and magnetic properties, as well as the distribution of anionic electrons of the 12 layered electrides

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Section: Introductionmentioning

confidence: 99%

Discovery of Hidden Classes of Layered Electrides by Extensive High-Throughput Material Screening

et al. 2019

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“…Dicalcium nitride (Ca2N) was recently proved to be a two-dimensional (2D) electride where anionic electrons are weakly localized in the 2D interspaces between two positively charged ionic [Ca2N] + layers 12 . Ca2N was then used as an efficient electron donating agent in the transfer hydrogenation of alkynes and alkenes 13 . Monolayer Ca2N encapsulated by graphene shows excellent predicted electron transport properties if compared to typical 2D electronic systems (e.g., GaAs-AlGaAs heterojunction, LaAlO3-SrTiO3 interface and graphene) 14 .…”

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confidence: 99%

Computer-Assisted Inverse Design of Inorganic Electrides

et al. 2017

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Electrides are ionic solids that consist of cationic frameworks and anionic electrons trapped in the voids of lattices. Organic electrides exist in a large abundance, but the thermal instability at room temperature and sensitivity to moisture are bottlenecks that limit their practical uses. Known inorganic electrides are rare but appear to have high thermal and chemical stability and exhibit promising applications as electron-emitting materials, superior catalysts and strong reducing agents. Here, we report a developed inverse-design method that can be used to search for a large variety of inorganic electrides. Our method utilizes the intrinsic property of interstitial electron localization of electrides as the global variable function being incorporated into the swarm-intelligence based structure searches. Through screening 99 binary ionic compounds, we have designed 89 new inorganic electrides that are classified into three-, two-, and zero-dimensional species according to the way that the interstitial electrons are localized and the conductive properties of the systems. Our work reveals the rich abundance of inorganic electrides by extending them into more general forms and provides new structure types for electrides that are not thought of as before.

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“…Electrides are important functional materials with exotic electronic properties and many potential applications, such as in optoelectrics 1 and catalysis [2][3][4] . The key feature of electride lies in its non-bound electrons serving as anions in the crystal 5,6 .…”

Section: Introductionmentioning

confidence: 99%

Computational design of flexible electrides with nontrivial band topology

Zhu

Wang

et al. 2019

Phys. Rev. Materials

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Electrides, with their excess electrons distributed in crystal cavities playing the role of anions, exhibit a variety of unique electronic and magnetic properties. In this work, we employ the first-principles crystal structure prediction to identify a new prototype of A3B electride in which both interlayer spacings and intralayer vacancies provide channels to accommodate the excess electrons in the crystal. This A3B type of structure is calculated to be thermodynamically stable for two alkaline metals oxides (Rb3O and K3O). Remarkably, the unique feature of multiple types of cavities makes the spatial arrangement of anionic electrons highly flexible via elastic strain engineering and chemical substitution, in contrast to the previously reported electrides characterized by a single topology of interstitial electrons. More importantly, our first-principles calculations reveal that Rb3O is a topological Dirac nodal line semimetal, which is induced by the Rb-s → O-p band inversion at the general electronic k momentums in the Brillouin zone associated with the intersitial electric charges. The discovery of flexible electride in combining with topological electronic properties opens an avenue for electride design and shows great promises in electronic device applications. arXiv:1811.11334v2 [cond-mat.mtrl-sci]

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Two dimensional inorganic electride-promoted electron transfer efficiency in transfer hydrogenation of alkynes and alkenes

Abstract: A simple and highly efficient transfer hydrogenation of alkynes and alkenes by using a two-dimensional electride, dicalcium nitride ([Ca2N]+·e–), as an electron transfer agent is disclosed.

Cited by 56 publications

References 26 publications

Discovery of Hidden Classes of Layered Electrides by Extensive High-Throughput Material Screening

Discovery of Hidden Classes of Layered Electrides by Extensive High-Throughput Material Screening

Computer-Assisted Inverse Design of Inorganic Electrides

Computational design of flexible electrides with nontrivial band topology

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