2022
DOI: 10.1021/acs.nanolett.2c02829
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High Utilization of Composite Magnesium Metal Anodes Enabled by a Magnesiophilic Coating

Abstract: Metallic magnesium is a promising high-capacity anode material for energy storage technologies beyond lithium-ion batteries. However, most reported Mg metal anodes are only cyclable under shallow cycling (≤1 mAh cm −2 ) and thus poor Mg utilization (<3%) conditions, significantly compromising their energy-dense characteristic. Herein, composite Mg metal anodes with high capacity utilization of 75% are achieved by coating magnesiophilic gold nanoparticles on copper foils for the first time. Benefiting from homo… Show more

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Cited by 28 publications
(22 citation statements)
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“…In addition, we also probe the influence of the InCl 3 additive on the electrochemical reaction kinetics. Generally, in the voltage–time curve of Mg plating, the initial peak voltage represents the nucleation overpotential (μ n ), which is related to the energy barrier of the heterogeneous nucleation process. , As reflected in Figure a, at a current density of 0.5 mA cm –2 , a low μ n of 0.23 V is achieved in the Mg­(OTf) 2 + InCl 3 electrolyte. This value is much smaller than that of Mg­(OTf) 2 + MgCl 2 (0.98 V) and pure Mg­(OTf) 2 (1.60 V), verifying the reduced energy barrier for Mg nucleation with In/MgIn sites, which are consistent with the DFT calculation results.…”
mentioning
confidence: 55%
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“…In addition, we also probe the influence of the InCl 3 additive on the electrochemical reaction kinetics. Generally, in the voltage–time curve of Mg plating, the initial peak voltage represents the nucleation overpotential (μ n ), which is related to the energy barrier of the heterogeneous nucleation process. , As reflected in Figure a, at a current density of 0.5 mA cm –2 , a low μ n of 0.23 V is achieved in the Mg­(OTf) 2 + InCl 3 electrolyte. This value is much smaller than that of Mg­(OTf) 2 + MgCl 2 (0.98 V) and pure Mg­(OTf) 2 (1.60 V), verifying the reduced energy barrier for Mg nucleation with In/MgIn sites, which are consistent with the DFT calculation results.…”
mentioning
confidence: 55%
“…To understand the dynamic behavior of Mg electrode during deposition in different electrolytes, the finite element method (FEM) was used to investigate the Mg 2+ concentration and electrical field distributions at the electrode–electrolyte interphase by COMSOL simulation (Figures S20 and S21). 2D geometric models (Figure S22 and Figure S24) were built based on the SEM results in Figure . As depicted in Figure a and Figure S23a, at a current density of 0.5 mA cm –2 , due to the protruding Mg deposits in pure Mg(OTf) 2 , the Mg-ion flux and electric field tend to concentrate around the sharp edges, indicating that further Mg deposition will preferentially occur on the protuberance sites, ultimately leading to short circuiting with the continuous growth of Mg protrusions (consistent with the cycling performance of pure Mg(OTf) 2 in Figure c).…”
mentioning
confidence: 99%
“…The binding energies of Mg‐Sb (−3.54 eV) and Mg‐ Mg 3 Sb 2 (−2.97 eV) are much more negative than that of Mg‐MgCl 2 (−0.20 eV), revealing that Sb metal and Mg 3 Sb 2 alloy are the more magnesiophilic components in the artificial hybrid interphase. The calculated adsorption energy values of Mg on Sb and Mg 3 Sb 2 are also much larger in magnitude than those on metallic Mg (−0.75 eV) and many other metals (e.g., −0.83 eV for Au, [ 13 ] −1.61 eV for Cu, [ 6b ] and −1.46 eV for Bi [ 19c ] ). Thus, the introduction of magnesiophilic Sb‐Mg composites into the artificial hybrid interphase can preferentially adsorb Mg 2+ ions in the electrolyte and effectively reduce the energy barriers of Mg 2+ desolvation and its subsequent nucleation on the electrode surface.…”
Section: Resultsmentioning
confidence: 98%
“…[ 12 ] Meanwhile, the electrode volume variation would be exacerbated at an industrial‐level areal capacity (≥ 3 mAh cm −2 ), resulting in more severe electrode instability and even the collapse of the battery system. [ 6b,13 ] Therefore, despite its great challenge, it is highly desirable to simultaneously resolve these problems of sluggish ion‐transfer kinetics and thermodynamic instability, while achieving long cyclability of Mg metal anodes under these practical working conditions.…”
Section: Introductionmentioning
confidence: 99%
“…Increasing demand for lithium-ion batteries (LIBs), spurred by the rapid adoption of electric vehicles, has exposed significant shortcomings of LIBs, which include safety concerns and lithium supply chain issues. The development of safer alternative metal-ion batteries with higher material abundance, higher energy density, and longer cycling stability can alleviate such shortcomings. A potential alternative to LIBs is rechargeable magnesium-ion batteries (MIBs), which stand out due to their relatively low cost, safety at ambient temperatures, high volumetric capacity (Mg: 3837 mA h cm –3 , vs Li: 2062 mA h cm –3 , Na: 1136 mA h cm –3 ), and suitable reduction potential (−2.4 V vs standard hydrogen electrode). However, industrial adoption of MIBs is impeded by the sluggish electrochemical kinetics of Mg 2+ caused by electrostatic force and the incompatibility between the electrolyte and electrode. …”
mentioning
confidence: 99%