SiO2 Phase Research Articles

Direct Conversion of Desiliconization Slag to a CaO-Mesoporous Silica Composite for CO<sub>2</sub> Capture: Effect of Acid Dissolution Agent

Calcium looping (CaL) utilizing CaO-based adsorbent has been studied to reduce carbon dioxide emissions (CO2). Synthesis of the CaO-based adsorbents from waste slags has captured the interest of the iron and steel industry, which is dealing with intensive amounts of waste slag produced. The drawback of using CaO-based adsorbents is their low regenerative ability during cyclic CO2 adsorption. In this study, aiming to synthesize a CaO-based adsorbent with better cyclic stability, we used desiliconization slag as a raw material, which is produced during the steel purification process by minimizing the silicon concentration. We synthesized a CaO and mesoporous silica (CaO-MS) composite from desiliconization slag using P123 as an organic template and several organic acids, including formic acid (FA), acetic acid (AA), and citric acid (CA) as dissolution agents. The structure and performance of the adsorbents were investigated using X-ray diffraction analysis (XRD), N2 adsorption-desorption, transmission electron microscopy (TEM), scanning transmission electron microscopy (STEM), and thermogravimetric analysis (TG). Compared to the samples synthesized with other organic acids, the slag-derived adsorbent synthesized with acetic acid (DSslag-CaO-MS(AA)) displayed the optimum CO2 adsorption capacity with 21.0 wt% per mass of adsorbent and the highest stability. The findings demonstrated that the mesoporous structure enhanced the CO2 adsorption and acetic acid is the best dissolution agent in synthesizing CaO-MS adsorbent by separating the crystalline CaO phase and SiO2 phase. Environmentally benign and economically viable CaO-based adsorbents synthesized from desiliconization slag can be used for CO2 capture, particularly in the iron and steel industry.

Investigation of the Effect of PbO Doping on Telluride Glass Ceramics as a Potential Material for Gamma Radiation Shielding.

The purpose of this paper is to study the effect of PbO doping of multicomponent composite glass-like ceramics based on TeO2, WO3, Bi2O3, MoO3, and SiO2, which are one of the promising materials for gamma radiation shielding. According to X-ray diffraction data, it was found that the PbO dopant concentration increase from 0.10 to 0.20-0.25 mol results in the initialization of the phase transformation and structural ordering processes, which are expressed in the formation of SiO2 and PbWO4 phases, and the crystallinity degree growth. An analysis of the optical properties showed that a change in the ratio of the contributions of the amorphous and ordered fractions leads to the optical density increase and the band gap alteration, as well as a variation in the optical characteristics. During the study of the strength and mechanical properties of the synthesized ceramics, depending on the dopant concentration, it was found that when inclusions in the form of PbWO4 are formed in the structure, the strength characteristics increase by 70-80% compared to the initial data, which indicates the doping efficiency and a rise in the mechanical strength of ceramics to external influences. During evaluation of the shielding protective characteristics of the synthesized ceramics, it was revealed that the formation of PbWO4 in the structure results in a rise in the high-energy gamma ray absorption efficiency.

Liquid–Crystal Structure Inheritance in Machine Learning Potentials for Network-Forming Systems

It has been studied whether machine learning interatomic potentials parameterized with only disordered configurations corresponding to liquid can describe the properties of crystalline phases and predict their structure. The study has been performed for a network-forming system SiO2, which has numerous polymorphic phases significantly different in structure and density. Using only high-temperature disordered configurations, a machine learning interatomic potential based on artificial neural networks (DeePMD model) has been parameterized. The potential reproduces well ab initio dependences of the energy on the volume and the vibrational density of states for all considered tetra- and octahedral crystalline phases of SiO2. Furthermore, the combination of the evolutionary algorithm and the developed DeePMD potential has made it possible to reproduce the really observed crystalline structures of SiO2. Such a good liquid–crystal portability of the machine learning interatomic potential opens prospects for the simulation of the structure and properties of new systems for which experimental information on crystalline phases is absent.

Physical, Thermal, and Chemical Properties of Fly Ash Cenospheres Obtained from Different Sources.

Cenospheres are hollow particles in fly ash, a by-product of coal burning, and are widely used as a reinforcement when developing low-density composites called syntactic foams. This study has investigated the physical, chemical, and thermal properties of cenospheres obtained from three different sources, designated as CS1, CS2, and CS3, for the development of syntactic foams. Cenospheres with particle sizes ranging from 40 to 500 μm were studied. Different particle distribution by size was observed, and the most uniform distribution of CS particles was in the case of CS2: above 74% with dimensions from 100 to 150 μm. The CS bulk had a similar density for all samples and amounted to around 0.4 g·cm-3, with a particle shell material density of 2.1 g·cm-3. Post-heat-treatment samples showed the development of a SiO2 phase in the cenospheres, which was not present in the as-received product. CS3 had the highest quantity of Si compared to the other two, showing the difference in source quality. Energy-dispersive X-ray spectrometry and a chemical analysis of the CS revealed that the main components of the studied CS were SiO2 and Al2O3. In the case of CS1 and CS2, the sum of these components was on average from 93 to 95%. In the case of CS3, the sum of SiO2 and Al2O3 did not exceed 86%, and Fe2O3 and K2O were present in appreciable quantities in CS3. Cenospheres CS1 and CS2 did not sinter during heat treatment up to 1200 °C, while sample CS3 was already subjected to sintering at 1100 °C because of the presence of a quartz phase, Fe2O3 and K2O. For the application of a metallic layer and subsequent consolidation via spark plasma sintering, CS2 can be deemed the most physically, thermally, and chemically suitable.

Synthesis and Characterization of the Properties of (1-x)Si3N4-xAl2O3 Ceramics with Variation of the Components.

The aim of this paper is to study the effect of variation in the component ratio of (1-x)Si3N4-xAl2O3 ceramics on the phase composition, strength and thermal properties of ceramics. To obtain ceramics and their further study, the solid-phase synthesis method combined with thermal annealing of samples at a temperature of 1500 °C typical for the initialization of phase transformation processes was used. The relevance and novelty of this study lies in obtaining new data on the processes of phase transformations with a variation in the composition of ceramics, as well as determining the effect of the phase composition on the resistance of ceramics to external influences. According to X-ray phase analysis data, it was found that an increase in the Si3N4 concentration in the composition of ceramics leads to a partial displacement of the tetragonal phase of SiO2 and Al2(SiO4)O and an increase in the contribution of Si3N4. Evaluation of the optical properties of the synthesized ceramics depending on the ratio of the components showed that the formation of the Si3N4 phase leads to an increase in the band gap and the absorbing ability of the ceramics due to the formation of additional absorption bands from 3.7-3.8 eV. Analysis of the strength dependences showed that an increase in the contribution of the Si3N4 phase with subsequent displacement of the oxide phases leads to a strengthening of the ceramic by more than 15-20%. At the same time, it was found that a change in the phase ratio leads to the hardening of ceramics, as well as an increase in crack resistance.

Comparative X-Ray Diffraction (XRD) Study on the Synthesis of Natural Based Magnetic Silica Nanoparticles

The aim of this study was to compare the synthesis process of magnetic silica nanoparticles (Fe-SNP) through the analysis of X-ray Diffraction (XRD) results. Fe3O4 magnetic nanopowders was synthesized by ultrasonic assisted co-precipitation and Fe-SNP was synthesized by direct mixing method of sodium silicate (Na2SiO3) and magnetite (Fe3O4) and the sol-gel method. Silica sludge was used as a silica source from Indonesia geothermal power plant waste. The synthesized of Fe-SNP is the functionalization of Fe3O4 with silica. Variations concentration of Na2SiO3 is used for the direct mixing method and variations of Fe3O4 form is used for the sol-gel method. Particles formed and particle size were characterized by XRD. The XRD results showed that there is no SiO2 phase in the sample synthesized by direct mixing method while two phases of SiO2 and Fe3O4 were found in the sample synthesized by sol-gel method. The size of the Fe3O4 nanoparticles calculated with Scherer’s formula and it obtained 19.9 nm, while the Fe3O4 nanoparticles with the addition of 20 mL and 6 mL Na2SiO3 concentrations were 6,53 nm and 10,23 nm. For the sol-gel method the size of Fe3O4 nanoparticles obtained was 11,03 using Fe3O4 powders and 9,86 using Fe3O4 solutions.

Difference in Structure and Electronic Properties of Oxygen Vacancies in α-Quartz and α-Cristobalite Phases of SiO2

α-cristobalite (α-C) is a polymorph of silica, mainly found in space exploration and geochemistry research. Due to similar densities, α-C is often used as a proxy for amorphous SiO2, particularly in computer simulations of SiO2 surfaces and interfaces. However, little is known about the properties of α-C and its basic oxygen defects. Using density functional theory (DFT) simulations we provide a comprehensive report on the properties of perfect structure and oxygen vacancies in α-C. The calculated properties of α-C are compared with those of the better-characterized α-quartz (α-Q). Our results demonstrated that the positively charged O vacancy in α-C is most stable in the dimer configuration, in contrast to α-Q, which favors the puckered configuration. A back-projected configuration was also predicted in both polymorphs. We calculated the optical transition energies and isotropic hyperfine constants for O vacancies in both α-Q and α-C, and compared our findings with the results of previous studies and experiments. This work, thus, offers one of the first in-depth investigations of the properties of oxygen vacancies in α-C.

Growth characteristics of scanning micro-arc oxidation coating on Ti6Al4V alloy

ABSTRACT In this study, the ceramic coating was prepared on Ti6Al4V alloy by scanning micro-arc oxidation (SMAO). The growth features of SMAO coating were investigated by combining the voltage and discharge variation. The result shows that a higher working voltage is obtained during SMAO treatment owing to additional resistance from the electrolyte column. As the SMAO goes on, the discharge region moves to the electrolyte column edge, exhibiting an annular shape. The current density with Gaussian distribution is observed between the stainless-steel tube (cathode) and titanium substrate (anode), which causes the SMAO coating to show a higher thickness in the middle and lower on both sides. Similar to traditional MAO, the SMAO coating has an enhancement in the thickness, pore size and Si content with increasing oxidation time, but coating degradation occurs in the later stage of SMAO. The SMAO coating mainly consists of amorphous SiO2, rutile and anatase phases.

Rosa Damascena mediated ZnO-Red Ochre nanocomposite for the electrochemical determination of 5-Fluorouracil

In this study, ZnO-Red Ochre nanocomposite was green synthesized by Rosa Damascena (RD) extract (RDZRONCs). Proton Induced X-ray Emission microanalysis (Micro-PIXE) and X-ray diffraction (XRD) pattern confirmed the presence of hematite (Fe2O3), and quartz (SiO2) mineral phases in the Red Ochre (RO) nanoclay. In addition, the XRD pattern shows the ZnO, ZnFe2O4, SiO2, Fe2O3, and Si phases in the RDZRONCs that were green synthesized with natural RD extract and RO. The RDZRONCs were used to modify the carbon paste electrode (CPE) for the electrochemical determination of the anticancer drug 5-fluorouracil (5-FU). Cyclic voltammetry (CV) and electrochemical impedance spectroscopy (EIS) techniques were employed to investigate the surface behavior of modified CPE (RDZRONCs/CPE). The electrochemical behavior of 5-FU at the RDZRONCs/CPE was exanimated by CV, differential pulse voltammetry (DPV), chronoamperometry (CA), and chronocoulometry (CC). Based on the DPV technique, a linear relationship between peak current and concentration of 5-FU was obtained in the dynamic range of 0.05–140.0 μM and with a detection limit equal to 0.0016 μM. The selectivity of RDZRONCs/CPE for 5-FU was studied in the presence of different inorganic and organic species. Also, the content of 5-FU was measured in real samples by RDZRONCs/CPE.

Thermal and Dielectric Behaviour of Polymer-Based Nanocomposites Flexible Sheets as Highly Stable Dielectric Materials

The silica zinc oxide nanoparticles filled poly-vinylidene-fluoride (PVDF)-based nanocomposite flexible sheets (NC FSs) are synthesized by co-precipitation method. The X-ray diffraction patterns reveal the development of various diffraction planes related to zinc oxide (ZnO) and SiO2 phases. The crystallinity of ZnO phase is decreased with increasing weight percent (wt.%) of silica nanofillers (NFs). The scanning electron microscope microstructure of synthesized PVDF-based NCs FSs is changed with increasing wt.% of silica NFs. The energy-dispersive X-ray spectroscopy and Fourier-transform infrared spectroscopy analyses confirm the presence of different elements and the formation of chemical bonding between them. In high temperature region, the weight-loss of synthesized PVDF-based NCs FSs is decreased from 89.90% to 49.26% with increasing wt.% of silica NFs. The values of dielectric permittivity, loss-factor, impedance, and AC-conductivity of PVDF-based NC FSs synthesized for maximum amount of silica NFs are found to be 13.7, 0.03, 0.16 MΩ, and 19.9 × 10 − 6 S/m, respectively. Results show that the synthesized PVDF-based NC FSs are the potential candidates of light emitting diodes and energy storage devices.

Mechanical grinding activation of modified magnesium slag and its use as backfilling cementitious material

The utilization of industrial solid waste with potential cementitious activity to prepare low carbon, economic and environmental backfilling cementitious materials is an urgent issue in cemented paste backfill (CPB). In this work, the mechanical grinding activation of modified magnesium slag (MMS), including grinding kinetics, crystallinity, and the influences on backfilling paste characteristics, have been investigated systematically. The indexes of particle size distribution (PSD), fineness, and sieve residue indicate that the grinding efficiency of MMS is high when grinding time ranges [20,80] min. The particle coarsening appears when the grinding time increases to 120 min from 100 min. A fitted grinding kinetics function of MMS has been established based on the measured PSDs with six grinding time. The XRD shows that the diffraction peak intensities of CaSO4 and SiO2 phases decreases with the increasing of grinding time, indicating the increasing of lattice defects and amorphization degree. Both of grinding dispersion refinement and amorphization increase of MMS contribute to the activation of cementitious reactivity. Grinding time has a great influence on the properties of modified magnesium slag-based (MMS-based) backfilling pastes. The fresh backfilling pastes conformed to both of the H-B model and revised Bingham model well. The critical shear rate, critical apparent viscosity, and extended degree increase with the increasing of grinding time, indicating that the fluidity decreases. The TG-DTG, SEM tests show that hydration rate of the MMS-based backfilling pastes is slow and there are many interconnected micropores when the grinding time is below 60 min. Besides, the uniaxial compressive strengths (UCS) of MMS-based backfilling mortar samples also show a similar pattern. All tests showed that grinding for 60 min could stimulate most of the potential cementitious reactivity of MMS. Meanwhile, the corresponding backfilling paste behaves good working condition. Taken together, 60 min is suggested as the optimal grinding time for MMS in consideration of energy consumed and technical benefits, and the corresponding specific surface area (SSA) and 45 µm sieve residue (SR) are 503 m2/kg and 3.83 %, respectively.

High-entropy Fe-Cr-Ni-Co-(Cu) coatings produced by vacuum electro-spark deposition for marine and coastal applications

High-entropy coatings (HECs) are of a great interest for the protection of structural steels and alloys used in the costal and offshore areas. Here, thick, dense, and uniform Fe-Cr-Ni-Co-(Cu) coatings with a crack-free surface have been successfully deposited on AISI 420S steel by vacuum electro-spark deposition using CrNiCo and CrNiCoCu electrodes. The coatings consist of columnar grains (approximately 300 nm in diameter) and subgrains (10–50 nm thick) of an fcc phase and spherical inclusions of mixed SiO2 + (Cr,Ti)2O3 oxide, 30–50 nm in size. Although Cu is an element prone to segregation, the experimental results show that Cu does not form its own phase and is in the metal solid solution. Molecular dynamics simulation shows that Cu has a slight tendency to self-clustering and form Cu-rich clusters in FeCrNiCo-Cu HECs. However, several regions enriched in Cu are observed in the FeCrNiCo-Cu samples. FeCrNiCo coatings tested in artificial seawater and the Black Sea exhibited enhanced corrosion resistance. In tribocorrosion tests, FeCrNiCo-(Cu) coatings performed better than steel substrate due to faster recovery of a passive film. The addition of Cu has a positive effect on the antibacterial activity of FeCrNiCo coatings against Gram-positive B. cereus Arc30 and B. cereus F strains.

Experimental phase equilibria study and thermodynamic modelling of the “CuO0.5”-AlO1.5-SiO2 ternary system in equilibrium with metallic copper

Phase equilibria studies were undertaken on the “CuO0.5”-AlO1.5-SiO2 system in equilibrium with metallic copper using equilibration and quenching technique followed by the electron probe X-ray microanalysis (EPMA). The liquidus of the “CuO0.5”-AlO1.5-SiO2 system, including the two 2-liquid miscibility gaps in the system as well as the cuprite (Cu2O), corundum (Al2O3), delafossite (CuAlO2), tridymite and cristobalite (Si1-x(CuAl)xO2), and mullite (Al6+2xSi2-2xO13-x) primary phase fields has been characterized. New experimental results together with phase equilibria and thermodynamic literature data were used to obtain a self-consistent set of parameters of the thermodynamic model for all phases. The liquidus projection of the “CuO0.5”-AlO1.5-SiO2 system was presented for the first time in the full range of temperatures and compositions. It was found that the simultaneous dissolution of a small amount of alumina and copper oxide (CuAlO2) in SiO2 phases stabilize cristobalite over tridymite at low temperatures.

Economical construction of spin coater for the fabrication of dielectric reflectors

Spin-coating is a versatile technique that utilizes only a few drops of the synthesized gel as an empirical method to fabricate the appropriate thin films. However, the economical design of a spin coater is always ground-breaking research. This paper reports the development of a spin coater using low-cost components such as SMPS, a brushless D.C. motor, and a proximity sensor. All of these components were contained in a stainless-steel unit and the entire equipment cost only 63 dollars, making it significantly less expensive than a standard one. The constructed spin coater was tested by fabricating three-and-five multilayer structures of TiO2/SiO2 with their respective sol–gel synthesized gels, and an X-ray diffraction (XRD) studies on the structures revealed a broad peak at 25°, confirming the existence of anatase TiO2 (titania) phase and non-crystalline amorphous phase of SiO2 (silica). Fourier transform infrared (FT-IR) spectroscopy endorsed the presence of titania and silica functional linkages by revealing vibrational bonds at 736 and 612 cm−1, respectively. Field emission scanning electron microscopy (FESEM) in cross-sectional mode on the three- and five-multilayer titania and silica structures evidenced the presence of titania and silica layers with intense (bright) and gloomy (dark) nature respectively. Finally, the reflectance study of the multilayer structures utilising ultraviolet–visible and near-infrared (UV–vis-NIR) spectroscopic showed 68 % and 100 % reflectance in the near-infrared region respectively, and demonstrated to be a dielectric reflector.

Mechanochemical remediation of the chlorinated compounds contaminated soil depending on the minerals inside-the most reasonable approach

This study explored a possible destruction of hexachlorobenzene (HCB) as example of persistent organic pollutants (POPs) as well as the dechlorination mechanism by directly using minerals in the soil, such as antigorite, talc and olivine. Compared with a stable quartz phase of SiO2, all three Mg silicate minerals demonstrated certain degrading capacity for HCB with different efficiency order as: antigorite > talc > olivine > SiO2 at 2 h of milling time. Interestingly, olivine exhibited a better performance than antigorite at 4 h of milling time, giving destruction percentage of 92.7% over 89.0% even at high concentrated HCB up to 5% added. Raman and ESR characterizations of the ball milled sample with olivine indicated the formation of amorphous carbon and graphitic carbon, and the occurrence of free radicals was observed to play an important role in dechlorination and carbonization of HCB. The first identified effectiveness of directly using Mg silicate minerals, allowed no addition of active chemicals during the ball milling, therefore avoided the concern over extrinsic contaminations on the soil. Olivine was further utilized to deal with actual contaminated soil and showed unique advantages on application prospects.

Dense hydrous silica carrying water to the deep Earth and promotion of oxygen fugacity heterogeneity

Water has remarkable effects on the properties of mantle rocks, but, owing to the high temperatures in the mantle, uncertainties remain about how and how much water is transported into the deep Earth. Recent studies have shown that stishovite and post-stishovites as high-pressure phases of SiO2 have the potential to carry weight percent levels of water into the Earth’s interior along the geotherm of the subducting oceanic crust. As slabs are subducted to the deepest mantle, dehydration of these dense hydrous silica phases has the potential to change the physicochemical properties of the mantle by reducing melting points, forming new high-pressure phases, and enhancing the oxygen fugacity heterogeneity of the lower mantle.

Effect of the Silica-Magnetite Nanocomposite Coating Functionalization on the Doxorubicin Sorption/Desorption.

A series of new composite materials based on Fe3O4 magnetic nanoparticles coated with SiO2 (or aminated SiO2) were synthesized. It has been shown that the use of N-(phosphonomethyl)iminodiacetic acid (PMIDA) to stabilize nanoparticles before silanization ensures the increased content of a SiO2 phase in the Fe3O4@SiO2 nanocomposites (NCs) in comparison with materials obtained under similar conditions, but without PMIDA. It has been demonstrated for the first time that the presence of PMIDA on the surface of NCs increases the level of Dox loading due to specific binding, while surface modification with 3-aminopropylsilane, on the contrary, significantly reduces the sorption capacity of materials. These regularities were in accordance with the results of quantum chemical calculations. It has been shown that the energies of Dox binding to the functional groups of NCs are in good agreement with the experimental data on the Dox sorption on these NCs. The mechanisms of Dox binding to the surface of NCs were proposed: simultaneous coordination of Dox on the PMIDA molecule and silanol groups at the NC surface leads to a synergistic effect in Dox binding. The synthesized NCs exhibited pH-dependent Dox release, as well as dose-dependent cytotoxicity in in vitro experiments. The cytotoxic effects of the studied materials correspond to their calculated IC50 values. NCs with a SiO2 shell obtained using PMIDA exhibited the highest effect. At the same time, the presence of PMIDA in NCs makes it possible to increase the Dox loading, as well as to reduce its desorption rate, which may be useful in the design of drug delivery vehicles with a prolonged action. We believe that the data obtained can be further used to develop stimuli-responsive materials for targeted cancer chemotherapy.

Preparation and water-vapour corrosion behaviour of BSAS environmental barrier coatings fabricated on ceramic matrix composites

Environmental barrier coatings (EBCs) are commonly utilized to protect ceramic matrix composite components from water vapour attacks in commercial gas turbine engines. In this work, Si/3Al2O3·2SiO2 (Mullite)/BaO-SrO-Al2O3-SiO2 (BSAS) tri-layered EBCs were fabricated on SiC-based ceramic matrix composites (CMC) substrate via atmospheric plasma spraying technique. The phase composition, microstructure, and bond strength of the environmental barrier coatings were studied by scanning electron microscope, energy dispersive spectrometer, X-ray diffraction analyzer, and mechanical test machine. The water vapour resistance of the BSAS coating and CMC was evaluated with a self-assembled water-vapour corrosion test device. The results indicate that the as-sprayed BSAS coating with a porosity of (5.9 ± 0.8) % mainly comprises the monoclinic celsian BSAS phase, hexacelsian BSAS phase, and SiO2 phase. The consumption velocity of the BSAS coating is about 12 % that of the naked CMC material in a 1300 °C water vapour environment. After corrosion for 300 h, the average flexural strength of naked samples was (481 ± 9) MPa, which was about 64 % of the coated ones. In addition, the bond strength of the as-sprayed coating is (18.7 ± 1.6) MPa. Even after 300 h of water vapour corrosion, the bond strength of the coating does not decay. Evidently, BSAS coating can protect CMC materials from water vapour corrosion at 1300 °C.

Study the Stable Diatomite-supported Catalyst for Biodiesel Production

The stable of natural diatomite supported by potassium hydroxide (KOH) as catalysts were synthesized for biodiesel production. A heterogeneous base catalyst prepared by impregnating KOH onto diatomite was also used to synthesize biodiesel from palm oil. All samples have been thoroughly characterized by Wavelength Dispersive X-ray Fluorescence (WDXRF), X-ray diffraction (XRD), N2 adsorption/desorption, Scanning electron microscopy (SEM), Energy dispersive spectrometer (EDS), and Temperature-programmed desorption of carbon dioxide (CO2-TPD). The XRD, XRF, and SEM results confi rm that adding KOH to diatomite results in structural change. The SiO2 and K2O phases form in the diatomite structural matrix during impregnation and the total basicity amount of this compound promotes the transesterifi cation process. A maximum fatty acid methyl ester (FAME) content of 84.56% was obtained. The reaction conditions were as follows: molar ratio of oil to methanol 1:9, catalyst loading 5 wt%, reaction time 2 h, and reaction temperature 75 °C. This work provides a possible new method for converting KOH from a homogeneous to a heterogeneous catalyst (Diatomite/KOH) that may show stable reusability, avoiding the separation and pollution problems in the environment.

Endothermic Dehydrogenation-Driven Preventive Magnesiation of SiO for High-Performance Lithium Storage Materials.

Silicon monoxide (SiO)-based materials have gained much attention as high-capacity lithium storage materials based on their high capacity and stable capacity retention. However, low initial Coulombic efficiency associated with the irreversible electrochemical reaction of the amorphous SiO2 phase in SiO inhibits the wide usage of SiO-based anode materials for lithium-ion batteries. Magnesiation of SiO is one of the most promising solutions to improve the initial efficiency of SiO-based anode materials. Herein, we demonstrate that endothermic dehydrogenation-driven magnesiation of SiO employing MgH2 enhanced the initial Coulombic efficiency of 89.5% with much improved long-term cycle performance over 300 cycles compared to the homologue prepared by magnesiation of SiO with Mg and pristine SiO. High-resolution transmission electron microscopy with thermogravimetry-differential scanning calorimetry revealed that the endothermic dehydrogenation of MgH2 suppressed the sudden temperature rise during magnesiation of SiO, thereby inhibiting the coarsening of the active Si phase in the resulting Si/Mg2SiO4 nanocomposite.