Yolk-shell Architecture Research Articles

Construction of Hierarchical Yolk-Shell Co/N-Dope C@void@C@MoS2 Composites with Multiple Heterogeneous Interfaces toward Broadband Electromagnetic Wave Absorption.

The synthesis of materials with a multicomponent hierarchical structure is an essential strategy for achieving high-performance electromagnetic wave (EMW) absorption. However, conventional design strategies face challenges in terms of the rational construction of specific architecture. In this study, we employ a combined space-restricted and hierarchical construction strategy to surface-plant MoS2 nanosheets on yolk-shell structural carbon-modified Co-based composites, leading to the development of high-performance Co/NC@void@C@MoS2 absorbers with advanced architecture. The surface-planted MoS2 nanosheets, the Co/NC magnetic yolk, and the dielectric carbon shell work together to enhance the impedance matching characteristics and synergistic loss capabilities in the composites. Experimental results indicate that Co/NC@void@C-700@MoS2 exhibited the best absorption performance with an effective absorption bandwidth of 7.54 GHz (at 2.05 mm) and a minimum reflection loss of -60.88 dB (at 1.85 mm). Furthermore, radar cross-section simulation results demonstrate that Co/NC@void@C-700@MoS2 effectively suppresses the scattering and transmission of EMWs on perfect electric conductor substrates, implying its superior practical application value. This study provides inspiration and experimental basis for designing and optimizing EMW absorption materials with hierarchical yolk-shell architecture.

Universal and facile sol-gel approach for fabrication of multitudinous yolk-shell architectures

Universal and facile sol-gel approach for fabrication of multitudinous yolk-shell architectures

A general strategy for direct growth of yolk-shell MOF-on-MOF hybrids

Construction of metal–organic framework (MOF) hybrids with yolk-shell nanostructures via MOF-on-MOF growth is significant for MOF design toward elaborate properties and enhanced performances, while remains challenging. Here, we report the direct growth of yolk-shell MOF-on-MOF hybrids via an interfacial growth-reorganization strategy. The synthesis relies on the precise growth of guest CoZn-ZIF (ZIF = zeolite imidazole framework) with appropriate crystal diameter and arrangement on host MOFs, inducing an in-situ transformation of core–shell intermediate into yolk-shell product. This strategy can be generally applied to the growth of CoZn-ZIF onto various host MOFs with different shapes, crystal structures and compositions including rod-like and octahedral Fe-based NH2-MIL-88B (MIL = Material Institute Lavoisier) and cake-like Ti-based NH2-MIL-125 toward three kinds of yolk-shell MOF-on-MOF hybrids. Moreover, functional carbon materials with bridged yolk-shell architecture can be prepared by pyrolysis of MOF-on-MOF hybrids as precursors, exhibiting enhanced oxygen reduction reaction performance than their monomeric counterparts. Our work paves the way for the design and application of MOF based yolk-shell nanostructures.

Architecture and active motif engineering of N–CoS2@C yolk–shell nanoreactor for boosted tetracycline removal via peroxymonosulfate activation: Performance, mechanism and destruction pathways

Rational construction of yolk-shell architecture with regulated binding configuration is crucially important but challengeable for antibiotic degradation via peroxymonosulfate (PMS) activation. In this study, we report the utilization of yolk-shell hollow architecture consisted of nitrogen-doped cobalt pyrite integrated carbon spheres (N–CoS2@C) as PMS activator to boost tetracycline hydrochloride (TCH) degradation. The creation of yolk-shell hollow structure and nitrogen-regulated active site engineering of CoS2 endow the resulted N–CoS2@C nanoreactor with high activity for PMS activating toward TCH degradation. Intriguingly, the N–CoS2@C nanoreactor exhibits an optimal degradation performance with a rate constant of 0.194 min−1 toward TCH via PMS activation. The 1O2 and SO4•− species are demonstrated as the dominant active substances for TCH degradation through quenching experiments and electron spin resonance characterization. The possible degradation mechanism, intermediates and degradation pathways for TCH removal over the N–CoS2@C/PMS nanoreactor are unveiled. Graphitic N, sp2−hybrid carbon, oxygenated group (C–OH) and Co species are verified as the possible catalytic sites of N–CoS2@C for PMS activation toward TCH removal. This study offers a unique strategy to engineer sulfides as highly efficient and promising PMS activators for antibiotic degradation.

Simple preparation of yolk-shell ZnCr2O4 microspheres and their application to xylene gas sensor

Spinel-type oxides have attracted more and more attention due to their high thermodynamic stability, good catalytic characteristic and flexibly tunable features. Herein, we report the synthesis of yolk-shell ZnCr2O4 microspheres with superior xylene sensing properties by a one-step solvothermal approach. The gas sensing properties of the as-prepared ZnCr2O4 microspheres were investigated. The sensor based on yolk-shell ZnCr2O4 microspheres showed excellent selectivity to xylene having a high response value of 200.7–100 ppm xylene, which was almost 77 times than that of Cr2O3 microspheres at 225 °C. As for the detection limit, the response value of sensor to 0.5 ppm xylene was 1.2. In addition, after 22 days of measurement, it could still keep the response of nearly 200–100 ppm xylene, indicating good long-term stability. The excellent gas sensing performances of sensor to xylene can be ascribed to the yolk-shell architecture with a large specific surface area and the high surface adsorbed oxygen species concentration.

Yolk-shell Fe2O3@mesoporous hollow carbon sphere hybrid sub-micro reactors for effective degradation of organic contaminants

Carbon–metal oxide composites are important class of catalytic materials in persulfate (PS)/peroxymonosulfate (PMS) activation. But, their poor catalytic stability during oxidation limits its practical use. Herein, we demonstrate the yolk-shell architecture strategy for the fabrication of highly stable Fe2O3 mesoporous carbon hollow spheres (Fe2O3@MCHS) catalyst. The prepared material exhibits high PS activation ability for effective degradation of phenolics. The surface properties of hybrid Fe2O3@MCHS system were examined using FE-SEM, TEM, BET and VSM techniques. Physical characterization data confirmed that Fe2O3@MCHS sub-micro reactors possess a magnetic property, high specific surface area (SSA; >1200 m2 g−1), orderly arranged mesopores, and excellent degree of particle dispersion. Owing to the fact, the Fe2O3@MCHS catalyst exhibited highest reactivity for the degradation of 2,4-dichlorophenol and bisphenol-A by PS even with very low catalyst dosage (10 mg L−1). ESR and scavenging experiments exclude the role of reactive radicals and other reactive oxygen species (ROS) (1O2) during pollutant degradation. Open circuit potential (OCP) measurements further reveal that low pollutant degradation efficiencies in the presence of 1O2 scavengers (L-histidine and NaN3) were caused due to strong interaction between scavenging molecules and catalytic surfaces rather than ROS quenching. Electrochemical investigation also supports that degradation occurs through mediating electron transfer from pollutant to Fe2O3@MCHS. This study provides new understanding in PS activation and also in developing stable PS activating hybrid catalytic systems for pollutant degradation.

Sub-nanometric amorphous V–O clusters without grain boundaries bonded in yolk-shell carbon nanospheres for superior sodium-ion storage

The energy density of sodium-ion batteries (SIBs) reported so far is still low, which weakens their competitiveness in practical applications. Cluster engineering and sub-nanometric design are effective strategies for rapid and efficient storage of alkaline ions. Herein, a durable yolk-shell architecture is developed via a facile self-polymerization and calcination process, in which the sub-nanometric amorphous vanadium-oxide (V–O) clusters are bonded in N-doped carbon nanospheres (A-VOxC/N–C). As a SIB anode, the composite delivers a large reversible capacity (491.6 mAh g−1 at 0.05 A g−1), high-rate capability and ultra-long cyclic stability (246.4 mAh g−1 with 96.6% capacity retention after 30000 cycles at 20.0 A g−1). In addition, the full cell also exhibits great potential for practical applications. The detailed structural characterizations and density functional theory (DFT) calculations suggest that the amorphous clusters without grain boundaries are crucial for the creation of abundant active sites and highly isotropic channels, as well as the reduction of Na-intercalation stress. The yolk-shell N–C has the structural advantages of flexible cavity, strong bonding force and large spatial constraint, which can effectively alleviate volume changes and strengthen structural stability. In view of these, this study can provide guidance for the design of sub-nanometric clusters and their potential applications in alkaline ion batteries.

Rational design of hierarchical yolk-double shell Fe@NCNs/MnO2 via thermal-induced phase separation toward wideband microwave absorption

Rational design of yolk-shell architectures with synergistic effect are vital for improving microwave attenuation ability, but still face challenges. In this work, we employ the thermal-induced phase separation engineering and redox strategy to fabricate hierarchical yolk-double shell Fe@NCNs/MnO2, in which magnetic Fe units are individually confined in N-doped carbon nanocubes (NCNs) cavity and hierarchical MnO2 nanosheets are intimately anchored on NCNs surface. It is found that the phase separation process between Prussian blue and poly-dopamine is significantly determined by the thermal-induced inward contraction owing to their different thermal stabilities and independent crystal structures. As results, the hierarchical composites exhibit matched impedance and wideband microwave absorption owing to the internal cavity architectures, multiple hetero-interfaces, dielectric-magnetic synergistic effect and hierarchical conformations. The minimum reflection loss reaches −46.7 dB with 3.3 mm thickness, and more importantly, the effective bandwidth (<-10 dB) achieves as strong as 10.8 GHz at 3.1 mm. This work opens up a novel and meaningful thinking for the construction of yolk-double shell architectures and the synthesized hierarchical composites can be used as promising candidates in addressing electromagnetic pollution.

Au@Cu2O Core–Shell and Au@Cu2Se Yolk–Shell Nanocrystals as Promising Photocatalysts in Photoelectrochemical Water Splitting and Photocatalytic Hydrogen Production

In this work, we demonstrated the practical use of Au@Cu2O core-shell and Au@Cu2Se yolk-shell nanocrystals as photocatalysts in photoelectrochemical (PEC) water splitting and photocatalytic hydrogen (H2) production. The samples were prepared by conducting a sequential ion-exchange reaction on a Au@Cu2O core-shell nanocrystal template. Au@Cu2O and Au@Cu2Se displayed enhanced charge separation as the Au core and yolk can attract photoexcited electrons from the Cu2O and Cu2Se shells. The localized surface plasmon resonance (LSPR) of Au, on the other hand, can facilitate additional charge carrier generation for Cu2O and Cu2Se. Finite-difference time-domain simulations were carried out to explore the amplification of the localized electromagnetic field induced by the LSPR of Au. The charge transfer dynamics and band alignment of the samples were examined with time-resolved photoluminescence and ultraviolet photoelectron spectroscopy. As a result of the improved interfacial charge transfer, Au@Cu2O and Au@Cu2Se exhibited a substantially larger photocurrent of water reduction and higher photocatalytic activity of H2 production than the corresponding pure counterpart samples. Incident photon-to-current efficiency measurements were conducted to evaluate the contribution of the plasmonic effect of Au to the enhanced photoactivity. Relative to Au@Cu2O, Au@Cu2Se was more suited for PEC water splitting and photocatalytic H2 production by virtue of the structural advantages of yolk-shell architectures. The demonstrations from the present work may shed light on the rational design of sophisticated metal-semiconductor yolk-shell nanocrystals, especially those comprising metal selenides, for superior photocatalytic applications.

Heterogeneous interface engineering for boosting electron transfer induced by MOF-derived Yolk-shell trimetallic phosphide nanospindles for robust water oxidation electrocatalysis

The heterogeneous interface engineering of nanocatalysts has been proved as an efficient strategy to promote the oxygen evolution reaction (OER) catalytic performance. Different from the conventional hollow structures, the yolk-shell construction could defend the distortion and dissolution during OER for stability improvement. However, it is still a great challenging to simultaneously construct heterogeneous interface and yolk-shell structure based on electrocatalysts with well-tuned composition and structure. Herein, we developed a facile synthetic method to prepare the yolk-shell trimetallic phosphide catalysts by starting with MIL-88A nanospindles templates. Benefitting from heterogeneous interface with fast electron transfer, yolk-shell architecture with rich channels for mass transportation, and active metal doping with electron structure modulation, the obtained CoNiFeP yolk-shell nanospindles (YSNSs) catalysts displayed superior OER catalytic properties with the overpotential of only 261 mV to deliver a current density of 10 mA cm−2 in alkaline media. Furthermore, the yolk-shell architecture endowed CoNiFeP with remarkable OER stability for 60 h. By coupling CoNiFeP with Pt/C electrodes to drive overall water splitting, an ultralow cell voltage of 1.56 V is required. The experimental and mechanistic studies indicated the optimized binding energy of *OOHad and *OHad intermediates by constructing robust phosphide interface.

How molecular interactions tune the characteristic time of nanocomposite colloidal sensors

HypothesisMass transport critically controls the performance of colloidal metal-polymer sensors. We hypothesize that molecular-level pair interactions, such as electric, steric, and specific binding effects, govern the mass transport and, in return, the characteristic time of these sensors. TheoryHere we present a simple theory guided by experimental data to examine the sensing performance of two usually encountered archetypal metal-polymer sensors, namely (1) core-shell and (2) yolk-shell architectures. For this purpose, we use the static reactive density functional theory framework, determining how (i) charge, (ii) size, and (iii) non-covalent binding factors modulate the characteristic time. FindingsWe show how an interplay between diffusivity and partitioning governs the sensing time of the sensors, where an anti-correlation cancellation between them renders the time non-trivial. Our study demonstrates that the convoluted substrate-hydrogel shell interaction controls the characteristic time of these colloidal sensors, especially when the sensors are in a collapsed state. Notably, the substrates with a high dipole moment tend to equilibrate greatly, but undesirably, at the shell-solution interface. With this, we encourage the formation of a metastable sorption state.

Yolk-shell-type CaO-based sorbents for CO2 capture: assessing the role of nanostructuring for the stabilization of the cyclic CO2 uptake.

Improving the cyclic CO2 uptake stability of CaO-based solid sorbents can provide a means to lower CO2 capture costs. Here, we develop nanostructured yolk(CaO)-shell(ZrO2) sorbents with a high cyclic CO2 uptake stability which outperform benchmark CaO nanoparticles after 20 cycles (0.17 gCO2 gSorbent-1) by more than 250% (0.61 gCO2 gSorbent-1), even under harsh calcination conditions (i.e. 80 vol% CO2 at 900 °C). By comparing the yolk-shell sorbents to core-shell sorbents, i.e. structures with an intimate contact between the stabilizing phase and CaO, we are able to identify the main mechanisms behind the stabilization of the CO2 uptake. While a yolk-shell architecture stabilizes the morphology of single CaO nanoparticles over repeated cycling and minimizes the contact between the yolk and shell materials, core-shell architectures lead to the formation of a thick CaZrO3-shell around CaO particles, which limits CO2 transport to unreacted CaO. Hence, yolk-shell architectures effectively delay CaZrO3 formation which in turn increases the theoretically possible CO2 uptake since CaZrO3 is CO2-capture-inert. In addition, we observe that yolk-shell architectures also improved the carbonation kinetics in both the kinetic- and diffusion-controlled regimes leading to a significantly higher cyclic CO2 uptake for yolk-shell-type sorbents.

One-pot synthesis of MoS2/CoS2 yolk-shell nanospheres

In this work, MoS2/CoS2 yolk-shell nanospheres are synthesized by a one-pot hydrothermal reaction. Furthermore, the yolk-shell spherical morphologies are characterized and confirmed by SEM, TEM characterizations; and the components of CoS2 and MoS2 are investigated by XRD and XPS analysis. It is revealed that the Co precursor and thiourea result in the formation of hollow CoS2 nanospheres, while the Co precursor, Mo precursor and thiourea lead to the fabrication of MoS2/CoS2 yolk-shell nanostructure. The possible growth mechanism of MoS2/CoS2 yolk-shell nanospheres is suggested based on the comparative experiments and characterization of intermediate samples. This research provides a feasible and new strategy to prepare the MoS2/CoS2 hybrid material with yolk-shell architecture.

Ingeniously Designed Yolk-Shell-Structured FeSe2@NDC Nanoboxes as an Excellent Long-Life and High-Rate Anode for Half/Full Na-Ion Batteries.

Thanks to their high conductivity and theoretical capacity, transition metal selenides have demanded significant research attention as prospective anodes for sodium-ion batteries. Nevertheless, their practical applications are hindered by finite cycle life and inferior rate performance because of large volume expansion, polyselenide dissolution, and sluggish dynamics. Herein, the nitrogen-doped carbon (NC)-coated FeSe2 nanoparticles encapsulated in NC nanoboxes (termed FeSe2@NDC NBs) are fabricated through the facile thermal selenization of polydopamine-wrapped Prussian blue precursors. In this composite, the existing nitrogen-doped dual carbon layer improves the intrinsic conductivity and structural integrity, while the unique porous yolk-shell architecture significantly mitigates the volume swelling during the sodium/desodium process. Moreover, the derived Fe-N-C bonds can effectively capture polyselenide, as well as promote Na+ transportation and good reversible conversion reaction. As expected, the FeSe2@NDC NBs deliver remarkable rate performance (374.9 mA h g-1 at 10.0 A g-1) and long-cycling stability (403.3 mA h g-1 over 2000 loops at 5.0 A g-1). When further coupled with a self-made Na3V2(PO4)3@C cathode in sodium-ion full cells, FeSe2@NDC NBs also exhibit considerably high and stable sodium-storage performance.

Stress-release design for high-capacity and long-time lifespan aqueous zinc-ion batteries

Mn-based cathodes are promising candidates for aqueous zinc-ion batteries (ZIBs) owing to the merits of low toxicity, high energy density, and safety. However, due to the strong electrostatic resistance of Zn2+, ZIBs usually suffer from huge mechanical stress during cycling and result in serious volume fluctuation and structural instability. Correspondingly, it is still significant to explore an effective stress-release strategy for achieving a long-time cycle lifespan with high available capacity. Herein, we report an urchin-like hierarchical porous Mn2O3 yolk-shell microspheres (HP–Mn2O3-YSMSs). As a proof of concept, the designed hierarchical porous yolk-shell architecture effectively releases the internal stresses from both radial and tangential directions via the internal void space and porous shell. Specifically, the HP-Mn2O3-YSMSs manifest high reversible capacity (311 mAh/g at 0.1 A/g) and long cycle life (81.3% retention at 2.0 A/g after 4000 cycles). This effective stress-release design opens a new direction for the development of the structural stable electrodes for practical energy applications.

Yolk-Shell-Structured Nanospheres with Goat Pupil-Like S-Doped SnSe Yolk and Hollow Carbon-Shell Configuration as Anode Material for Sodium-Ion Storage.

Rationally nanostructured electrode materials exhibit excellent sodium-ion storage performance. In particular, yolk-shell configurations of metal chalcogenide@void@C are introduced in various synthetic strategies for use as superior anode materials. Herein, yolk-shell-structured nanospheres, with goat pupil-like configuration of S-doped SnSe yolks and hollow carbon shells, are synthesized by salt-infiltration and a simple post-treatment procedure. Impressively, the co-infiltration of thiourea and selenium oxide enables the doping of sulfur into SnSe (SnSeS) and carbon shells, as well as the formation of a goat pupil-like yolk-shell architecture. High-reactivity thiourea-derived H2 S gas forms nanocrystals inside the carbon nanospheres. The nanocrystals act as seeds for the crystal growth of SnSeS through Ostwald ripening. The unique yolk-shell structure and composition with a heterointerface provide not only structural stability but also fast electrode reaction kinetics during repeated cycling. The SnSeS@C electrode shows an excellent cycle life (186mA h g-1 for 1000 cycles at 0.5 A g-1 ) and rate capability (112mA h g-1 at 5.0 A g-1 ).

Synthesis of yolk‐shell‐structured iron monosulfide‐carbon microspheres and understanding of their conversion reaction for potassium‐ion storage

Nanostructured transition metal chalcogenides (TMCs) have attracted attention as potential anode materials owing to the anticipation of next-generation battery systems, particularly potassium-ion batteries (PIBs). In this study, the electrochemical reaction mechanism of iron monosulfide (FeS) with potassium ions was systemically investigated for the first time. To enhance the electrochemical properties by improving the structural stability and electrical conductivity during cycling, rational strategies of introducing a yolk-shell architecture via an aerosol process and pitch solution infiltration were applied, resulting in the formation of yolk-shell-structured FeS/pitch-derived carbon composite microspheres (Y-FeS@C). From in situ and ex situ investigations of electrodes in fully discharged and charged states, the following reaction mechanism was determined from the second cycle onward: 4Fe + 4K2S ↔ KxFe2S3 + FeS + Fe + (8 − x)K+ + (8 − x)e−. The inhibition of substantial FeS crystal growth thanks to the pitch-derived carbon encapsulation as well as the formation of metallic Fe after the initial conversion reaction contributed to the excellent electrochemical kinetic properties of Y-FeS@C. Y-FeS@C showed stable cycle performance (256.5 mA h g−1 for the 100th cycle at 0.5 A g−1) and high rate capability (113.8 mA h g−1 at 5.0 A g−1) as an anode material for PIBs.

Synergistic effects of yolk-shell and nanopore architectures on the microwave absorption performance of Co@void@C nanocomposites

Due to deficiencies of poor dielectric loss and narrow absorption bandwidth, how to improve the performance of cobalt-based absorbers remains a challenge in the field of microwave absorption materials. In this work, a convenient and efficient strategy combining hydrogen plasma-metal reaction (HPMR) and chemical dealloying has been developed for the fabrication of nanoporous Co@void@C nanocomposites (NCs). The performance exhibits apparent enhancement owing to the synergistic effects of yolk-shell and nanopore architectures. The minimum reflection loss (RLmin) value reaches −19.5 dB at the thickness of 1.6 mm and the effective absorption bandwidth (EAB, RL ≤ −10 dB) goes up to 6.8 GHz at the thickness of 1.9 mm. For comparison, the porous Co@C NCs with only nanopore architecture have a narrow EAB of 2.6 GHz and Co@void@C NCs with only yolk-shell architecture cannot effectively absorb the incident microwave (RL > −10 dB) within 2–18 GHz. The novel Co-based absorber with yolk-shell and nanopore architectures possesses great potential for the application in microwave absorption field.

Optimizing inner voids in yolk-shell TiO2 nanostructure for high-performance and ultralong-life lithium-sulfur batteries

The TiO 2 nanosheets constructed yolk-shell sulfur-TiO 2 (S@void@TiO 2 ) architecture with optimized inner voids demonstrates high-performance and ultralong-life for Li-S battery. • Designing TiO 2 nanosheets constructed yolk-shell TiO 2 (S@void@TiO 2 ) nanostructure for Li-S battery. • Verifying intense chemical interaction via the hybridization of Li 1 s, S 2p and O 2p orbitals in S@void@TiO 2. • Optimizing the inner voids for volume expansion to guarantee the cathode integrity. • Improving the electrolyte wettability and Li + kinetics in S@void@TiO 2. • Realizing high capacity and long cycle with a small capacity decay for Li-S battery. A TiO 2 nanosheets constructed yolk-shell architecture with tunable inner voids is designed and prepared as sulfur host for high-performance and ultralong-life Li-S battery. With the integration of TiO 2 nanosheets to form yolk-shell sulfur-TiO 2 (S@void@TiO 2 ) architecture with controllable inner voids, the S@void@TiO 2 composite with optimized inner voids provides sufficient contacting sites to improve the utilization of insulating sulfur and allows sulfur to freely expand without destroying the electrode. In particular, the density functional theory (DFT) calculations from molecular level reveal that the hybridization of Li 1s, S 2p and O 2p orbitals ensures the effective chemisorption between polysulfides and TiO 2 with long-term cycling stability. Consequently, the optimized S@void@TiO 2 electrode maintains a capacity of 766 mAhg −1 after 1000 cycles at 0.2C. Even at 2C for 400 cycles, the capacity still retains at 511 mAhg −1 , representing the best results of TiO 2 -based nanostructures for Li-S batteries. This work illustrates that carefully design novel yolk-shell structure is important to address the shortages of sulfur-based cathodes for advanced Li-S battery.

Dual confinement of carbon/TiO2 hollow shells enables improved lithium storage of Si nanoparticles

Silicon is regarded as one of the most promising anode materials for next generation lithium-ion batteries (LIBs). However, the severe volume changes during lithiation/delithiation, leading to fast capacity decay and reduced cycling life, remains an obstacle to its practical application. In this work, we propose the design of a yolk-shell structure of carbon@TiO2@Si (CTS) by template process based on sol-gel chemistry. The Si nanoparticles are confined in the carbon/TiO2 double shells with abundant void space between the Si core and carbon/TiO2 shells. The yolk-shell architecture with concentric double shells substantially improves the structure stability of the electrodes. Consequently, the CTS delivers a high capacity of 747 mA h g−1 at a current density of 100 mA g−1, which is far superior to that (356 mA h g−1) of C@Si (CS) with only a single carbon shell. The double-shelled confinement strategy proposed in this work sheds some light on the development of improved Si-based anode for next-generation LIBs.