First-principles study of peroxides effects on $lt;i$gt;β$lt;/i$gt;$lt;sub$gt;12$lt;/sub$gt;-borophene cathode for efficient lithium and sodium oxygen batteries

The shift to clean energy is crucial in mitigating the harmful effects of fossil fuels on the environment. Nevertheless, as we embrace clean energy sources, particularly solar and wind energies, high-energy-density storage devices like lithium and sodium-oxygen batteries are essential. However, challenges such as the irreversibility of lithium and sodium peroxides and their non-conductivity nature on the cathode electrode hinder practical use. 2D materials, particularly <inline-formula><math xmlns:mml="http://www.w3.org/1998/Math/MathML" altimg="c:\heptemp\HML50722833.png" baseline="-3.5" display="inline" id="mathml_M1" overflow="scroll"> <mml:mrow class="MJX-TeXAtom-ORD"><mml:msub><mml:mi>&#x03B2;</mml:mi><mml:mrow class="MJX-TeXAtom-ORD"><mml:mn>12</mml:mn></mml:mrow></mml:msub></mml:mrow></math></inline-formula>-borophene, show promise in addressing these challenges. In this study, we used density functional theory to thoroughly investigate the adsorption mechanisms of alkali-metal peroxides and their impact on the electronic properties of the <inline-formula><math xmlns:mml="http://www.w3.org/1998/Math/MathML" altimg="c:\heptemp\HML50722834.png" baseline="-3.5" display="inline" id="mathml_M2" overflow="scroll"> <mml:mrow class="MJX-TeXAtom-ORD"><mml:msub><mml:mi>&#x03B2;</mml:mi><mml:mrow class="MJX-TeXAtom-ORD"><mml:mn>12</mml:mn></mml:mrow></mml:msub></mml:mrow></math></inline-formula>-borophene. Our results revealed adsorption energies of &#x2212;3.71 and &#x2212;3.54 eV for <inline-formula><math xmlns:mml="http://www.w3.org/1998/Math/MathML" altimg="c:\heptemp\HML50722835.png" baseline="-3.5" display="inline" id="mathml_M3" overflow="scroll"> <mml:mrow class="MJX-TeXAtom-ORD"><mml:mrow class="MJX-TeXAtom-ORD"><mml:mi mathvariant="normal">L</mml:mi><mml:msub><mml:mi mathvariant="normal">i</mml:mi> <mml:mn>2</mml:mn></mml:msub><mml:msub><mml:mi mathvariant="normal">O</mml:mi><mml:mn>2</mml:mn></mml:msub></mml:mrow></mml:mrow></math></inline-formula> and <inline-formula><math xmlns:mml="http://www.w3.org/1998/Math/MathML" altimg="c:\heptemp\HML50722836.png" baseline="-3.5" display="inline" id="mathml_M4" overflow="scroll"><mml:mrow class="MJX-TeXAtom-ORD"> <mml:mrow class="MJX-TeXAtom-ORD"><mml:mi mathvariant="normal">N</mml:mi> <mml:msub><mml:mi mathvariant="normal">a</mml:mi><mml:mn>2</mml:mn></mml:msub> <mml:msub><mml:mi mathvariant="normal">O</mml:mi><mml:mn>2</mml:mn></mml:msub></mml:mrow></mml:mrow></math></inline-formula>, respectively, showing that the adsorbed peroxides are stable and unlikely to decompose into the electrolyte. The calculated Gibbs free energy changes that revealed low overpotentials of 1.03 V for <inline-formula><math xmlns:mml="http://www.w3.org/1998/Math/MathML" altimg="c:\heptemp\HML50722837.png" baseline="-3.5" display="inline" id="mathml_M5" overflow="scroll"> <mml:mrow class="MJX-TeXAtom-ORD"><mml:mrow class="MJX-TeXAtom-ORD"><mml:mi mathvariant="normal">L</mml:mi><mml:msub><mml:mi mathvariant="normal">i</mml:mi> <mml:mrow class="MJX-TeXAtom-ORD"><mml:mn>2</mml:mn></mml:mrow></mml:msub><mml:msub> <mml:mi mathvariant="normal">O</mml:mi><mml:mrow class="MJX-TeXAtom-ORD"> <mml:mn>2</mml:mn></mml:mrow></mml:msub></mml:mrow></mml:mrow></math></inline-formula> and 1.61 V for <inline-formula><math xmlns:mml="http://www.w3.org/1998/Math/MathML" altimg="c:\heptemp\HML50722838.png" baseline="-3.5" display="inline" id="mathml_M6" overflow="scroll"><mml:mrow class="MJX-TeXAtom-ORD"> <mml:mrow class="MJX-TeXAtom-ORD"><mml:mi mathvariant="normal">N</mml:mi> <mml:msub><mml:mi mathvariant="normal">a</mml:mi><mml:mn>2</mml:mn></mml:msub> <mml:msub><mml:mi mathvariant="normal">O</mml:mi><mml:mn>2</mml:mn></mml:msub></mml:mrow></mml:mrow></math></inline-formula>. Moreover, even with increased concentrations of peroxides on the surface, <inline-formula><math xmlns:mml="http://www.w3.org/1998/Math/MathML" altimg="c:\heptemp\HML50722839.png" baseline="-3.5" display="inline" id="mathml_M7" overflow="scroll"> <mml:mrow class="MJX-TeXAtom-ORD"><mml:msub><mml:mi>&#x03B2;</mml:mi><mml:mrow class="MJX-TeXAtom-ORD"><mml:mn>12</mml:mn></mml:mrow></mml:msub></mml:mrow></math></inline-formula>-borophene retained its ability to adsorb additional peroxides, achieving theoretical voltages of 2.60 V for <inline-formula><math xmlns:mml="http://www.w3.org/1998/Math/MathML" altimg="c:\heptemp\HML50722840.png" baseline="-3.5" display="inline" id="mathml_M8" overflow="scroll"><mml:mrow class="MJX-TeXAtom-ORD"> <mml:mrow class="MJX-TeXAtom-ORD"><mml:mi mathvariant="normal">L</mml:mi> <mml:msub><mml:mi mathvariant="normal">i</mml:mi><mml:mrow class="MJX-TeXAtom-ORD"><mml:mn>2</mml:mn></mml:mrow></mml:msub><mml:msub><mml:mi mathvariant="normal">O</mml:mi><mml:mrow class="MJX-TeXAtom-ORD"><mml:mn>2</mml:mn></mml:mrow></mml:msub></mml:mrow></mml:mrow></math></inline-formula> and 2.04 V for <inline-formula><math xmlns:mml="http://www.w3.org/1998/Math/MathML" altimg="c:\heptemp\HML50722841.png" baseline="-3.5" display="inline" id="mathml_M9" overflow="scroll"><mml:mrow class="MJX-TeXAtom-ORD"> <mml:mrow class="MJX-TeXAtom-ORD"><mml:mi mathvariant="normal">N</mml:mi> <mml:msub><mml:mi mathvariant="normal">a</mml:mi><mml:mn>2</mml:mn></mml:msub> <mml:msub><mml:mi mathvariant="normal">O</mml:mi><mml:mn>2</mml:mn></mml:msub></mml:mrow></mml:mrow></math></inline-formula>. Notably, the metallic nature of <inline-formula><math xmlns:mml="http://www.w3.org/1998/Math/MathML" altimg="c:\heptemp\HML50722842.png" baseline="-3.5" display="inline" id="mathml_M10" overflow="scroll"><mml:mrow class="MJX-TeXAtom-ORD"> <mml:msub><mml:mi>&#x03B2;</mml:mi><mml:mrow class="MJX-TeXAtom-ORD"><mml:mn>12</mml:mn></mml:mrow></mml:msub></mml:mrow></math></inline-formula> remained stable despite the adsorption of peroxides, evidenced by an increase in electronic states around the Fermi level and the overlap of the valence and conduction bands. Furthermore, thermal stability analysis at 300 K confirmed that the structure of <inline-formula><math xmlns:mml="http://www.w3.org/1998/Math/MathML" altimg="c:\heptemp\HML50722843.png" baseline="-3.5" display="inline" id="mathml_M11" overflow="scroll"> <mml:mrow class="MJX-TeXAtom-ORD"><mml:msub><mml:mi>&#x03B2;</mml:mi><mml:mrow class="MJX-TeXAtom-ORD"><mml:mn>12</mml:mn></mml:mrow></mml:msub></mml:mrow></math></inline-formula>-borophene remained intact, reinforcing its suitability as a cathode at standard temperature of the battery. The low diffusion energy barriers of 1.04 and 0.92 eV were obtained for <inline-formula><math xmlns:mml="http://www.w3.org/1998/Math/MathML" altimg="c:\heptemp\HML50722844.png" baseline="-3.5" display="inline" id="mathml_M12" overflow="scroll"><mml:mrow class="MJX-TeXAtom-ORD"> <mml:mrow class="MJX-TeXAtom-ORD"><mml:mi mathvariant="normal">L</mml:mi> <mml:msub><mml:mi mathvariant="normal">i</mml:mi><mml:mn>2</mml:mn></mml:msub> <mml:msub><mml:mi mathvariant="normal">O</mml:mi><mml:mn>2</mml:mn></mml:msub></mml:mrow></mml:mrow></math></inline-formula> and <inline-formula><math xmlns:mml="http://www.w3.org/1998/Math/MathML" altimg="c:\heptemp\HML50722845.png" baseline="-3.5" display="inline" id="mathml_M13" overflow="scroll"> <mml:mrow class="MJX-TeXAtom-ORD"><mml:mrow class="MJX-TeXAtom-ORD"><mml:mi mathvariant="normal">N</mml:mi><mml:msub><mml:mi mathvariant="normal">a</mml:mi> <mml:mn>2</mml:mn></mml:msub><mml:msub><mml:mi mathvariant="normal">O</mml:mi><mml:mn>2</mml:mn></mml:msub></mml:mrow></mml:mrow></math></inline-formula>, respectively, suggesting a high rate of peroxides migration on the substrate surface. The dissociation energy barriers for <inline-formula><math xmlns:mml="http://www.w3.org/1998/Math/MathML" altimg="c:\heptemp\HML50722846.png" baseline="-3.5" display="inline" id="mathml_M14" overflow="scroll"><mml:mrow class="MJX-TeXAtom-ORD"> <mml:mrow class="MJX-TeXAtom-ORD"><mml:mi mathvariant="normal">L</mml:mi> <mml:msub><mml:mi mathvariant="normal">i</mml:mi><mml:mn>2</mml:mn></mml:msub> <mml:msub><mml:mi mathvariant="normal">O</mml:mi><mml:mn>2</mml:mn></mml:msub></mml:mrow></mml:mrow></math></inline-formula> and <inline-formula><math xmlns:mml="http://www.w3.org/1998/Math/MathML" altimg="c:\heptemp\HML50722847.png" baseline="-3.5" display="inline" id="mathml_M15" overflow="scroll"> <mml:mrow class="MJX-TeXAtom-ORD"><mml:mrow class="MJX-TeXAtom-ORD"><mml:mi mathvariant="normal">N</mml:mi><mml:msub><mml:mi mathvariant="normal">a</mml:mi> <mml:mn>2</mml:mn></mml:msub><mml:msub><mml:mi mathvariant="normal">O</mml:mi><mml:mn>2</mml:mn></mml:msub></mml:mrow></mml:mrow></math></inline-formula> were found to be minimal at 1.86 and 1.69 eV, respectively, indicating the catalytic effects and enhancing electrochemical processes. Our findings suggest that <inline-formula><math xmlns:mml="http://www.w3.org/1998/Math/MathML" altimg="c:\heptemp\HML50722848.png" baseline="-3.5" display="inline" id="mathml_M16" overflow="scroll"><mml:mrow class="MJX-TeXAtom-ORD"> <mml:msub><mml:mi>&#x03B2;</mml:mi><mml:mrow class="MJX-TeXAtom-ORD"><mml:mn>12</mml:mn></mml:mrow></mml:msub></mml:mrow></math></inline-formula>-borophene can be a potential cathode electrode for the next-generation lithium and sodium-oxygen batteries.

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Publication Details

Journal
Frontiers of Physics
Published
2025-01-01
DOI
https://doi.org/10.15302/frontphys.2025.064201
Primary Topic
Advancements in Battery Materials
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article

First-principles study of peroxides effects on $lt;i$gt;&#x03B2;$lt;/i$gt;$lt;sub$gt;12$lt;/sub$gt;-borophene cathode for efficient lithium and sodium oxygen batteries

Frontiers of Physics
Advancements in Battery Materials
article

First-principles study of peroxides effects on $lt;i$gt;&#x03B2;$lt;/i$gt;$lt;sub$gt;12$lt;/sub$gt;-borophene cathode for efficient lithium and sodium oxygen batteries

article en

Abstract

The shift to clean energy is crucial in mitigating the harmful effects of fossil fuels on the environment. Nevertheless, as we embrace clean energy sources, particularly solar and wind energies, high-energy-density storage devices like lithium and sodium-oxygen batteries are essential. However, challenges such as the irreversibility of lithium and sodium peroxides and their non-conductivity nature on the cathode electrode hinder practical use. 2D materials, particularly <inline-formula><math xmlns:mml="http://www.w3.org/1998/Math/MathML" altimg="c:\heptemp\HML50722833.png" baseline="-3.5" display="inline" id="mathml_M1" overflow="scroll"> <mml:mrow class="MJX-TeXAtom-ORD"><mml:msub><mml:mi>&#x03B2;</mml:mi><mml:mrow class="MJX-TeXAtom-ORD"><mml:mn>12</mml:mn></mml:mrow></mml:msub></mml:mrow></math></inline-formula>-borophene, show promise in addressing these challenges. In this study, we used density functional theory to thoroughly investigate the adsorption mechanisms of alkali-metal peroxides and their impact on the electronic properties of the <inline-formula><math xmlns:mml="http://www.w3.org/1998/Math/MathML" altimg="c:\heptemp\HML50722834.png" baseline="-3.5" display="inline" id="mathml_M2" overflow="scroll"> <mml:mrow class="MJX-TeXAtom-ORD"><mml:msub><mml:mi>&#x03B2;</mml:mi><mml:mrow class="MJX-TeXAtom-ORD"><mml:mn>12</mml:mn></mml:mrow></mml:msub></mml:mrow></math></inline-formula>-borophene. Our results revealed adsorption energies of &#x2212;3.71 and &#x2212;3.54 eV for <inline-formula><math xmlns:mml="http://www.w3.org/1998/Math/MathML" altimg="c:\heptemp\HML50722835.png" baseline="-3.5" display="inline" id="mathml_M3" overflow="scroll"> <mml:mrow class="MJX-TeXAtom-ORD"><mml:mrow class="MJX-TeXAtom-ORD"><mml:mi mathvariant="normal">L</mml:mi><mml:msub><mml:mi mathvariant="normal">i</mml:mi> <mml:mn>2</mml:mn></mml:msub><mml:msub><mml:mi mathvariant="normal">O</mml:mi><mml:mn>2</mml:mn></mml:msub></mml:mrow></mml:mrow></math></inline-formula> and <inline-formula><math xmlns:mml="http://www.w3.org/1998/Math/MathML" altimg="c:\heptemp\HML50722836.png" baseline="-3.5" display="inline" id="mathml_M4" overflow="scroll"><mml:mrow class="MJX-TeXAtom-ORD"> <mml:mrow class="MJX-TeXAtom-ORD"><mml:mi mathvariant="normal">N</mml:mi> <mml:msub><mml:mi mathvariant="normal">a</mml:mi><mml:mn>2</mml:mn></mml:msub> <mml:msub><mml:mi mathvariant="normal">O</mml:mi><mml:mn>2</mml:mn></mml:msub></mml:mrow></mml:mrow></math></inline-formula>, respectively, showing that the adsorbed peroxides are stable and unlikely to decompose into the electrolyte. The calculated Gibbs free energy changes that revealed low overpotentials of 1.03 V for <inline-formula><math xmlns:mml="http://www.w3.org/1998/Math/MathML" altimg="c:\heptemp\HML50722837.png" baseline="-3.5" display="inline" id="mathml_M5" overflow="scroll"> <mml:mrow class="MJX-TeXAtom-ORD"><mml:mrow class="MJX-TeXAtom-ORD"><mml:mi mathvariant="normal">L</mml:mi><mml:msub><mml:mi mathvariant="normal">i</mml:mi> <mml:mrow class="MJX-TeXAtom-ORD"><mml:mn>2</mml:mn></mml:mrow></mml:msub><mml:msub> <mml:mi mathvariant="normal">O</mml:mi><mml:mrow class="MJX-TeXAtom-ORD"> <mml:mn>2</mml:mn></mml:mrow></mml:msub></mml:mrow></mml:mrow></math></inline-formula> and 1.61 V for <inline-formula><math xmlns:mml="http://www.w3.org/1998/Math/MathML" altimg="c:\heptemp\HML50722838.png" baseline="-3.5" display="inline" id="mathml_M6" overflow="scroll"><mml:mrow class="MJX-TeXAtom-ORD"> <mml:mrow class="MJX-TeXAtom-ORD"><mml:mi mathvariant="normal">N</mml:mi> <mml:msub><mml:mi mathvariant="normal">a</mml:mi><mml:mn>2</mml:mn></mml:msub> <mml:msub><mml:mi mathvariant="normal">O</mml:mi><mml:mn>2</mml:mn></mml:msub></mml:mrow></mml:mrow></math></inline-formula>. Moreover, even with increased concentrations of peroxides on the surface, <inline-formula><math xmlns:mml="http://www.w3.org/1998/Math/MathML" altimg="c:\heptemp\HML50722839.png" baseline="-3.5" display="inline" id="mathml_M7" overflow="scroll"> <mml:mrow class="MJX-TeXAtom-ORD"><mml:msub><mml:mi>&#x03B2;</mml:mi><mml:mrow class="MJX-TeXAtom-ORD"><mml:mn>12</mml:mn></mml:mrow></mml:msub></mml:mrow></math></inline-formula>-borophene retained its ability to adsorb additional peroxides, achieving theoretical voltages of 2.60 V for <inline-formula><math xmlns:mml="http://www.w3.org/1998/Math/MathML" altimg="c:\heptemp\HML50722840.png" baseline="-3.5" display="inline" id="mathml_M8" overflow="scroll"><mml:mrow class="MJX-TeXAtom-ORD"> <mml:mrow class="MJX-TeXAtom-ORD"><mml:mi mathvariant="normal">L</mml:mi> <mml:msub><mml:mi mathvariant="normal">i</mml:mi><mml:mrow class="MJX-TeXAtom-ORD"><mml:mn>2</mml:mn></mml:mrow></mml:msub><mml:msub><mml:mi mathvariant="normal">O</mml:mi><mml:mrow class="MJX-TeXAtom-ORD"><mml:mn>2</mml:mn></mml:mrow></mml:msub></mml:mrow></mml:mrow></math></inline-formula> and 2.04 V for <inline-formula><math xmlns:mml="http://www.w3.org/1998/Math/MathML" altimg="c:\heptemp\HML50722841.png" baseline="-3.5" display="inline" id="mathml_M9" overflow="scroll"><mml:mrow class="MJX-TeXAtom-ORD"> <mml:mrow class="MJX-TeXAtom-ORD"><mml:mi mathvariant="normal">N</mml:mi> <mml:msub><mml:mi mathvariant="normal">a</mml:mi><mml:mn>2</mml:mn></mml:msub> <mml:msub><mml:mi mathvariant="normal">O</mml:mi><mml:mn>2</mml:mn></mml:msub></mml:mrow></mml:mrow></math></inline-formula>. Notably, the metallic nature of <inline-formula><math xmlns:mml="http://www.w3.org/1998/Math/MathML" altimg="c:\heptemp\HML50722842.png" baseline="-3.5" display="inline" id="mathml_M10" overflow="scroll"><mml:mrow class="MJX-TeXAtom-ORD"> <mml:msub><mml:mi>&#x03B2;</mml:mi><mml:mrow class="MJX-TeXAtom-ORD"><mml:mn>12</mml:mn></mml:mrow></mml:msub></mml:mrow></math></inline-formula> remained stable despite the adsorption of peroxides, evidenced by an increase in electronic states around the Fermi level and the overlap of the valence and conduction bands. Furthermore, thermal stability analysis at 300 K confirmed that the structure of <inline-formula><math xmlns:mml="http://www.w3.org/1998/Math/MathML" altimg="c:\heptemp\HML50722843.png" baseline="-3.5" display="inline" id="mathml_M11" overflow="scroll"> <mml:mrow class="MJX-TeXAtom-ORD"><mml:msub><mml:mi>&#x03B2;</mml:mi><mml:mrow class="MJX-TeXAtom-ORD"><mml:mn>12</mml:mn></mml:mrow></mml:msub></mml:mrow></math></inline-formula>-borophene remained intact, reinforcing its suitability as a cathode at standard temperature of the battery. The low diffusion energy barriers of 1.04 and 0.92 eV were obtained for <inline-formula><math xmlns:mml="http://www.w3.org/1998/Math/MathML" altimg="c:\heptemp\HML50722844.png" baseline="-3.5" display="inline" id="mathml_M12" overflow="scroll"><mml:mrow class="MJX-TeXAtom-ORD"> <mml:mrow class="MJX-TeXAtom-ORD"><mml:mi mathvariant="normal">L</mml:mi> <mml:msub><mml:mi mathvariant="normal">i</mml:mi><mml:mn>2</mml:mn></mml:msub> <mml:msub><mml:mi mathvariant="normal">O</mml:mi><mml:mn>2</mml:mn></mml:msub></mml:mrow></mml:mrow></math></inline-formula> and <inline-formula><math xmlns:mml="http://www.w3.org/1998/Math/MathML" altimg="c:\heptemp\HML50722845.png" baseline="-3.5" display="inline" id="mathml_M13" overflow="scroll"> <mml:mrow class="MJX-TeXAtom-ORD"><mml:mrow class="MJX-TeXAtom-ORD"><mml:mi mathvariant="normal">N</mml:mi><mml:msub><mml:mi mathvariant="normal">a</mml:mi> <mml:mn>2</mml:mn></mml:msub><mml:msub><mml:mi mathvariant="normal">O</mml:mi><mml:mn>2</mml:mn></mml:msub></mml:mrow></mml:mrow></math></inline-formula>, respectively, suggesting a high rate of peroxides migration on the substrate surface. The dissociation energy barriers for <inline-formula><math xmlns:mml="http://www.w3.org/1998/Math/MathML" altimg="c:\heptemp\HML50722846.png" baseline="-3.5" display="inline" id="mathml_M14" overflow="scroll"><mml:mrow class="MJX-TeXAtom-ORD"> <mml:mrow class="MJX-TeXAtom-ORD"><mml:mi mathvariant="normal">L</mml:mi> <mml:msub><mml:mi mathvariant="normal">i</mml:mi><mml:mn>2</mml:mn></mml:msub> <mml:msub><mml:mi mathvariant="normal">O</mml:mi><mml:mn>2</mml:mn></mml:msub></mml:mrow></mml:mrow></math></inline-formula> and <inline-formula><math xmlns:mml="http://www.w3.org/1998/Math/MathML" altimg="c:\heptemp\HML50722847.png" baseline="-3.5" display="inline" id="mathml_M15" overflow="scroll"> <mml:mrow class="MJX-TeXAtom-ORD"><mml:mrow class="MJX-TeXAtom-ORD"><mml:mi mathvariant="normal">N</mml:mi><mml:msub><mml:mi mathvariant="normal">a</mml:mi> <mml:mn>2</mml:mn></mml:msub><mml:msub><mml:mi mathvariant="normal">O</mml:mi><mml:mn>2</mml:mn></mml:msub></mml:mrow></mml:mrow></math></inline-formula> were found to be minimal at 1.86 and 1.69 eV, respectively, indicating the catalytic effects and enhancing electrochemical processes. Our findings suggest that <inline-formula><math xmlns:mml="http://www.w3.org/1998/Math/MathML" altimg="c:\heptemp\HML50722848.png" baseline="-3.5" display="inline" id="mathml_M16" overflow="scroll"><mml:mrow class="MJX-TeXAtom-ORD"> <mml:msub><mml:mi>&#x03B2;</mml:mi><mml:mrow class="MJX-TeXAtom-ORD"><mml:mn>12</mml:mn></mml:mrow></mml:msub></mml:mrow></math></inline-formula>-borophene can be a potential cathode electrode for the next-generation lithium and sodium-oxygen batteries.

Frontiers of PhysicsVol. 20(6)
Ulyanovsk State University (RU), Copperbelt University (ZM), University of Pretoria (ZA)
Openalex Percentile: Top 91%
Advancements in Battery Materials
DOISourceOpenAlex
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