Materials design by quantum‐chemical and other theoretical/computational means: Applications to energy storage and photoemissive materials

Németh, Károly

doi:10.1002/qua.24616

Cited by 11 publications

(4 citation statements)

References 27 publications

(42 reference statements)

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“…Density Functional Theory calculations were carried out using the Quantum Espresso program package [92,93], following the methodology in our former works [15,16,77,94]. A plane wave basis set with 50 Ry wave-function cut-off was used in conjunction with the PBEsol exchange-correlation functional [95,96] and the related ultrasoft pseudopotentials as provided by the software package.…”

Section: Computational Methodologymentioning

confidence: 99%

“…At this point, a reference will be made to our former works [13][14][15][16] in which we proposed to substitute GO with functionalized hexagonal boron nitride (h-BN) in order to cure the thermal stability problem of GO. In addition, we have predicted that the -OBF 3 functionalization of h-BN would be particularly advantageous for an efficient, h-BN-based battery.…”

Section: Introductionmentioning

confidence: 99%

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Radical anion functionalization of two-dimensional materials as a means of engineering simultaneously high electronic and ionic conductivity solids

Németh¹

2021

Nanotechnology

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A radical anion based functionalization of the basal plane of hexagonal boron nitride (h-BN) and other two-dimensional materials is proposed in the present study. The resulting materials can reversibly be oxidized without the detachment of the functional groups from the basal plane and can thus serve as surface-intercalation type cathode electroactive species and fast solid ion conductors at the same time. The functionalization of h-BN with [·OBX3]− radical anions (X=F, Cl) in the presence of Li, Na or Mg cations provides one example of such systems. This material can be realized in a proposed simple, two step synthesis. In the first step, a symmetric Lewis adduct of the corresponding Li, Na or Mg peroxides is formed with BX3. In the second step, the anion of the Lewis adduct is thermally split into two identical [·OBX3]− radical anions that covalently functionalize the B atoms of h-BN. In the maximum density surface packing functionalization, the product of the synthesis is A n [(BN)2OBX3] (A = Li, Na with n = 1 or A = Mg with n = 0.5). Its ionic conductivity is predicted to be in the order of 0.01-0.1 S cm-1 at room temperature, on the basis of Grotthus-like (or paddle-wheel) ion transport. In the highly oxidized states (0 ≤ n ≤ 1 for Li and Na and 0 ≤ n ≤ 0.5 for Mg), the electronic conductivity of this material is in the order of 1 S cm−1, similar to carbon black. In the fully reduced states (n = 2 for Li and Na and n = 1 for Mg), the material becomes an insulator, like h-BN. The tunability of the electronic properties of A n [(BN)2OBX3] via the cation concentration (n) allows for its application as multifunctional material in energy storage devices, simultaneously serving as cathode active species, solid electrolyte, electroconductive additive, separator, heat conductor and coating for metal anodes that enables dendrite-free plating. This multifunctionality reduces the number of phases needed in an all-solid-state battery or supercapacitor and thus reduces the interfacial impedance making energy storage devices more efficient. For example, Li[(BN)2OBF3] is predicted to have 5.6 V open circuit voltage versus Li metal anode, capacity of 191 mAh g− 1, specific energy of 1067 Wh kg− 1 and can store energy at a (materials only) cost of 24 USD kWh− 1.

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Section: Computational Methodologymentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Radical anion functionalization of two-dimensional materials as a means of engineering simultaneously high electronic and ionic conductivity solids

Németh¹

2021

Nanotechnology

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“…We have been working on the development of high-energy and high-power batteries based on functionalized 2D materials for about a decade [40][41][42][43][44][45]. We recently proposed the use of adducts of BF 3 with graphene oxide (GO) and oxidized hexagonal boron nitride (hBN) as cathode active species and solid electrolytes [42][43][44][45].…”

Section: Introductionmentioning

confidence: 99%

High-Energy and High-Power Primary Li-CFx Batteries Enabled by the Combined Effects of the Binder and the Electrolyte

et al. 2023

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Several effective methods have been developed recently to demonstrate simultaneous high energy and high power density in Lithium - carbon fluoride (Li-CFx) batteries. These methods can achieve as high as a 1000 Wh/kg energy density at a 60–70 kW/kg power density (40–50 C rate) in coin cells and a 750 Wh/kg energy density at a 12.5 kW/kg power density (20 C rate) in pouch cells. This performance is made possible by an ingenious nano-architecture design, controlled porosity, boron doping, and electrolyte additives. In the present study, we show that a similarly great performance, a 931 Wh/kg energy density at a 59 kW/kg power density, can be achieved by using a polyacrylonitrile binder and a LiBF4 electrolyte in Li-graphite fluoride coin cells. We also demonstrate that the observed effect is the result of the right combination of the binder and the electrolyte. We propose that the mechanistic origin of the observed phenomena is an electro-catalytic effect of the polyacrylonitrile binder. While our proposed method has a competitive performance, it also offers a simple implementation and a scalable production of high-energy and high-power primary Li-CFx cells.

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“…Control of the surface reactivity of two-dimensional materials by the selection of an appropriate substrate has attracted much attention presently and enabled further progress in the field of nanotechnology, such as electronics, catalysis, and energy storage. − For electrochemical energy storage development, batteries should have high gravimetric and volumetric energy and power densities, the safety of operation, economic composition, rechargeability, and long cycle life . The above properties have been successfully achieved by light elements, such as derivatives of graphene (G) or hexagonal boron nitride (h-BN). − Boron nitride (BN) compounds have displayed great potential as anode materials for lithium-ion batteries due to their unique structural, mechanical, and electrical properties . Although non-carbon-based materials are widely used in ion batteries, nowadays researchers are focused on lighter nanoelements such as B and N, due to their high chemical stability, excellent mechanical properties, and high thermal conductivities, , which is the reason for their implementation in various nanodevices. ,− Many previously reported works have described that the addition of nanocoating of boron nitride makes lithium batteries longer lasting. − …”

Section: Introductionmentioning

confidence: 99%

Inquisitive Geometric Sites in h-BN Monolayer for Alkali Earth Metal Ion Batteries

et al. 2019

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Electrochemical energy storage has been at the center of interest over the past years due to the ever-faster technological development and the need for high-capacity batteries with high voltages and energy densities. Alkali batteries show the greatest potential for improving current characteristics, and this work examines several hexagonal boron nitride configurations as electrodes for ion batteries. First-principles calculations based on density functional theory have been used to study structural, electronic, and electrochemical properties of a graphenelike hexagonal boron nitride (h-BN) monolayer for various point defects. The maximum theoretical capacities for alkali earth metal ions adsorbed on the h-B9N8 monolayer are 762.264, 571.698, and 127.044 mAh/g, and average electrode potentials are 0.188, 0.009, and 5.735 V for the adsorption of Li+, Na+, and K+, respectively. Studied structures have been explored for the use as anode materials to hold alkali metal ions, namely, Li+, K+, and Na+, and we have found that for some cases, the alkali metal–h-BN structure shows metallic character, which leads to good electrical conductivity, without the change of structural geometry. Our results show that studied materials have characteristics suitable for the electrode-based ion batteries.

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Materials design by quantum‐chemical and other theoretical/computational means: Applications to energy storage and photoemissive materials

Cited by 11 publications

References 27 publications

Radical anion functionalization of two-dimensional materials as a means of engineering simultaneously high electronic and ionic conductivity solids

Radical anion functionalization of two-dimensional materials as a means of engineering simultaneously high electronic and ionic conductivity solids

High-Energy and High-Power Primary Li-CFx Batteries Enabled by the Combined Effects of the Binder and the Electrolyte

Inquisitive Geometric Sites in h-BN Monolayer for Alkali Earth Metal Ion Batteries

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