Solid‐Phase Synthesis of Molecularly Imprinted Polymer Nanoparticles with a Reusable Template–“Plastic Antibodies”

Molecularly imprinted polymers (MIPs) are generic alternatives to antibodies in sensors, diagnostics, and separations. To displace biomolecules without radical changes in infrastructure in device manufacture, MIPs should share their characteristics (solubility, size, specificity and affinity, localized binding domain) whilst maintaining the advantages of MIPs (low‐cost, short development time, and high stability) hence the interest in MIP nanoparticles. Herein, a reusable solid‐phase template approach is reported (fully compatible with automation) for the synthesis of MIP nanoparticles and their precise manufacture using a prototype automated UV photochemical reactor. Batches of nanoparticles (30–400 nm) with narrow size distributions imprinted with: melamine (d = 60 nm, K_d = 6.3 × 10^?8 M ), vancomycin (d = 250 nm, K_d = 3.4 × 10^?9 M ), a peptide (d = 350 nm, K_d = 4.8 × 10^?8 M ) and proteins have been produced. The instrument uses a column packed with glass beads, bearing the template. Process parameters are under computer control, requiring minimal manual intervention. For the first time, the reliable re‐use of molecular templates is demonstrated in the synthesis of MIPs (≥30 batches of nanoMIPs without loss of performance). NanoMIPs are produced template‐free and the solid‐phase acts both as template and affinity separation medium.     

High‐Performance [001]c‐Textured PNN‐PZT Relaxor Ferroelectric Ceramics for Electromechanical Coupling Devices

[001]_C‐Textured 0.55Pb(Ni_1/3Nb_2/3)O₃–0.15PbZrO₃–0.3PbTiO₃ (PNN‐PZT) ceramics are prepared by the templated grain‐growth method using BaTiO₃ (BT) platelet templates. Samples with different template contents are fabricated and compared in terms of texture fraction, microstructure, and piezoelectric, ferroelectric and dielectric properties. High piezoelectric performance (d₃₃ = 1210 pC N^?1, d₃₃* = 1773 pm V^?1 at 5 kV cm^?1) and high figure of merit g₃₃?d₃₃ (21.92 × 10^?12 m² N^?1) are achieved in the [001]_C‐textured PNN‐PZT ceramic with 2 vol% BaTiO₃ template, for which the texture fraction is 82%. In addition, domain structures of textured PNN‐PZT ceramics are observed and analyzed, which provide clues to the origin of the giant piezoelectric and electromechanical coupling properties of PNN‐PZT ceramics.     

Integrated Approaches Toward High‐Affinity Artificial Protein Binders Obtained via Computationally Simulated Epitopes for Protein Recognition

Widely used diagnostic tools make use of antibodies recognizing targeted molecules, but additional techniques are required in order to alleviate the disadvantages of antibodies. Herein, molecular dynamic calculations are performed for the design of high affinity artificial protein binding surfaces for the recognition of neuron specific enolase (NSE), a known cancer biomarker. Computational simulations are employed to identify particularly stabile secondary structure elements. These epitopes are used for the subsequent molecular imprinting, where surface imprinting approach is applied. The molecular imprints generated with the calculated epitopes of greater stability (Cys‐Ep1) show better binding properties than those of lower stability (Cys‐Ep5). The average binding strength of imprints created with stabile epitopes is found to be around twofold and fourfold higher for the NSE derived peptide and NSE protein, respectively. The recognition of NSE is investigated in a wide concentration range, where high sensitivity (limit of detection (LOD) = 0.5 ng mL^?1) and affinity (dissociation constant (K_d) = 5.3 × 10^?11m ) are achieved using Cys‐Ep1 imprints reflecting the stable structure of the template molecules. This integrated approach employing stability calculations for the identification of stabile epitopes is expected to have a major impact on the future development of high affinity protein capturing binders.     

Chemical Blowing Approach for Ultramicroporous Carbon Nitride Frameworks and Their Applications in Gas and Energy Storage

A scalable, template‐free synthetic strategy is presented for the preparation of ultramicroporous carbon nitride frameworks (CNFs) through a chemical blowing approach by using ammonium chloride as blowing agent and hexamethylene tetraamine as the C and N precursor and a subsequent potassium hydroxide chemical activation is employed to obtain CNFs with surface areas up to 1730 m² g^?1 along with a high nitrogen content of 13.3 wt%. CNFs showed CO₂ uptake capacities up to 5.74 mmol g^?1 at 1 bar and 1.67 mmol g^?1 at 0.15 bar, 273 K along with a very high CO₂/N₂ selectivity. In addition, H₂ uptake capacity of 1.9 wt% and the isosteric heats of adsorption (Q _st) value of 9.0 kJ mol^?1 at zero coverage have been also observed. Moreover, the presence of nitrogen‐doped graphene walls in CNFs also facilitated their application as supercapacitors, with capacitance values up to ≈114 F g^?1 at 0.5 A g^?1, along with a good cyclability and capacitance retention. This approach effectively extends unique surface properties of carbon nitrides into the micropore regime for effective capture of small gases and energy storage applications. Importantly, textural properties of CNFs can be simply tuned by judicious choice of organic precursors and the blowing agent.     

A Controllable Synthesis of Rich Nitrogen‐Doped Ordered Mesoporous Carbon for CO2 Capture and Supercapacitors

A controllable one‐pot method to synthesize N‐doped ordered mesoporous carbons (NMC) with a high N content by using dicyandiamide as a nitrogen source via an evaporation‐induced self‐assembly process is reported. In this synthesis, resol molecules can bridge the Pluronic F127 template and dicyandiamide via hydrogen bonding and electrostatic interactions. During thermosetting at 100 °C for formation of rigid phenolic resin and subsequent pyrolysis at 600 °C for carbonization, dicyandiamide provides closed N species while resol can form a stable framework, thus ensuring the successful synthesis of ordered N‐doped mesoporous carbon. The obtained N‐doped ordered mesoporous carbons possess tunable mesostructures (p6m and Im m symmetry) and pore size (3.1–17.6 nm), high surface area (494–586 m² g^?1), and high N content (up to 13.1 wt%). Ascribed to the unique feature of large surface area and high N contents, NMC materials show high CO₂ capture of 2.8–3.2 mmol g^?1 at 298 K and 1.0 bar, and exhibit good performance as the supercapacitor electrode with specific capacitances of 262 F g^?1 (in 1 M H₂SO₄) and 227 F g^?1 (in 6 M KOH) at a current density of 0.2 A g^?1.     

Novel Insoluble Organic Cathodes for Advanced Organic K‐Ion Batteries

Organic redox‐active molecules are inborn electrodes to store large‐radius potassium (K) ion. High‐performance organic cathodes are important for practical usage of organic potassium‐ion batteries (OPIBs). However, small‐molecule organic cathodes face serious dissolution problems against liquid electrolytes. A novel insoluble small‐molecule organic cathode [N,N′‐bis(2‐anthraquinone)]‐perylene‐3,4,9,10‐tetracarboxydiimide (PTCDI‐DAQ, 200 mAh g^?1) is initially designed for OPIBs. In half cells (1–3.8 V vs K⁺/K) using 1 m KPF₆ in dimethoxyethane (DME), PTCDI‐DAQ delivers a highly stable specific capacity of 216 mAh g^?1 and still holds the value of 133 mAh g^?1 at an ultrahigh current density of 20 A g^?1 (100 C). Using reduced potassium terephthalate (K₄TP) as the organic anode, the resulting K₄TP||PTCDI‐DAQ OPIBs with the electrolyte 1 m KPF₆ in DME realize a high energy density of maximum 295 Wh kg^?1_cathode (213 mAh g^?1_cathode × 1.38 V) and power density of 13 800 W Kg^?1_cathode (94 mAh g^?1 × 1.38 V @ 10 A g^?1) during the working voltage of 0.2–3.2 V. Meanwhile, K₄TP||PTCDI‐DAQ OPIBs fulfill the superlong lifespan with a stable discharge capacity of 62 mAh g^?1_cathode after 10 000 cycles and 40 mAh g^?1_cathode after 30 000 cycles (3 A g^?1). The integrated performance of PTCDI‐DAQ can currently defeat any cathode reported in K‐ion half/full cells.     

Rapid and Scalable Synthesis of Mo‐Based Binary and Ternary Oxides for Electrochemical Applications

Mo‐based binary oxides (MBOs) and Mo‐based ternary oxides (MTOs) are a research focus because of their widespread applications. The traditional synthesis routes for MBOs and MTOs require high temperature and are time intense. Here, a rapid, facile, and scalable strategy to efficiently fabricate MBOs and MTOs with various morphologies and crystal structures is reported. Only 1 min is required for the whole process and the yield is above 90%. This strategy is the simplest and the fastest method reported and exhibits large potential for application. Furthermore, the as‐synthesized H_x MoO₃ nanobelts and NiMoO₄·x H₂O nanowires display a specific capacitance of 660.3 F g^?1 at 2 mV s^?1 and a specific capacity of 549 C g^?1 at 1 A g^?1. In addition, to assemble the H_x MoO₃ and NiMoO₄·x H₂O electrodes together, the solid state hybrid electrolyte is employed to take advantage of MBOs and MTOs. The obtained NiMoO₄·x H₂O//H_x MoO₃ device delivers a specific capacitance of 156 F g^?1 at 0.8 A g^?1 and an energy density of 55.6 Wh kg^?1 at a power density of 640 W kg^?1, making it attractive for application as an energy storage material.     

Designing Defective Crystalline Carbon Nitride to Enable Selective CO2 Photoreduction in the Gas Phase

Polymeric carbon nitrides are promising photocatalysts for CO₂ photoreduction, but still show lower activity and selectivity. Herein, the synthesis of an ordered crystalline carbon nitride is reported which is simultaneously rich in special defects, accomplished via the co‐condensation of guanidine hydrochloride and dicyandiamide under acetonitrile‐promoted solvothermal conditions. The high crystallinity boosts charge migration, and the structural terminations with cyano and carboxyl groups result in the improvement of optical absorption, the ability to store charges at the surface, and CO₂ binding. The crystalline carbon nitride with surface defect design enables the effective gas‐phase CO₂ photoreduction into hydrocarbon fuels while oxidizing water to oxygen, at a rate of 12.07 µmol h^?1 g^?1 and a selectivity of 91.5%, both values of which are remarkably higher than those of most previous carbon nitride photocatalysts. This study highlights the preparation of defective crystalline carbon nitride using a low‐temperature solvothermal synthesis, as well as a resultant good selectivity toward hydrocarbons in the application of gas‐phase CO₂ photoreduction in the absence of any cocatalyst or sacrificial agent.     

Solution‐Processed Small‐Molecule Bulk Heterojunction Ambipolar Transistors

Solution‐processed small‐molecule bulk heterojunction (BHJ) ambipolar organic thin‐film transistors are fabricated based on a combination of [2‐phenylbenzo[d,d']thieno[3,2‐b;4,5‐b']dithiophene (P‐BTDT) : 2‐(4‐n‐octylphenyl)benzo[d,d ']thieno[3,2‐b;4,5‐b']dithiophene (OP‐BTDT)] and C₆₀. Treating high electrical performance vacuum‐deposited P‐BTDT organic semiconductors with a newly developed solution‐processed organic semiconductor material, OP‐BTDT, in an optimized ratio yields a solution‐processed p‐channel organic semiconductor blend with carrier mobility as high as 0.65 cm² V^?1 s^?1. An optimized blending of P‐BTDT:OP‐BTDT with the n‐channel semiconductor, C₆₀, results in a BHJ ambipolar transistor with balanced carrier mobilities for holes and electrons of 0.03 and 0.02 cm² V^?1 s^?1, respectively. Furthermore, a complementary‐like inverter composed of two ambipolar thin‐film transistors is demonstrated, which achieves a gain of 115.     

Metal Ion‐Terpyridine‐Functionalized L‐Tyrosinamide Aptamers: Nucleoapzymes for Oxygen Insertion into C?H Bonds and the Transformation of L‐Tyrosinamide into Amidodopachrome

A series of metal ion‐terpyridine‐modified L‐tyrosinamide aptamers (M^{n +} = Cu²⁺ or Fe³⁺) act as enzyme‐mimicking catalysts (nucleoapzymes) for oxygen‐insertion into C? H bonds and the transformation of L‐tyrosinamide into amidodopachrome. The reaction proceeds in the presence of H₂O₂ and coadded L‐ascorbic acid. In one series of experiments, the catalyzed oxidation of L‐tyrosinamide to amidodopachrome by a set of nucleoapzymes consisting of Fe³⁺‐ or Cu²⁺‐terpyridine complexes tethered directly or through a 4 × thymidine (4 × T) bridge, to the 5′‐ or 3′‐end of the 49‐mer L‐tyrosinamide aptamer or to a shorter 23‐mer L‐tyrosinamide aptamer is examined. All nucleoapzymes reveal catalytic Michaelis–Menten enzyme‐like activities and the separated Fe³⁺‐ or Cu²⁺‐terpyridine and L‐tyrosinamide aptamer units show only minute catalytic properties. The catalytic activities of the nucleoapzymes are attributed to the concentration of the L‐tyrosinamide substrate by the aptamer units in proximity to the catalytic sites (K_d = (14 ± 0.1) × 10^?6 m for all 49‐mer catalysts and K_d = (2.5 ± 0.1) × 10^?6 m and K_d = (0.8 ± 0.04) × 10^?6 m for the 23‐mer catalysts). Electron spin resonance experiments reveal that ?OH radicals and ascorbate radicals participate in the transformation of tyrosine derivatives to catechol products. An autocatalytic feedback mechanism for the amplified generation of the two radicals is suggested.     

Pt Nanoparticles Sensitized Ordered Mesoporous WO3 Semiconductor: Gas Sensing Performance and Mechanism Study

In this study, a straightforward coassembly strategy is demonstrated to synthesize Pt sensitized mesoporous WO₃ with crystalline framework through the simultaneous coassembly of amphiphilic poly(ethylene oxide)‐b‐polystyrene, hydrophobic platinum precursors, and hydrophilic tungsten precursors. The obtained WO₃/Pt nanocomposites possess large pore size (≈13 nm), high surface area (128 m² g^?1), large pore volume (0.32 cm³ g^?1), and Pt nanoparticles (≈4 nm) in situ homogeneously distributed in mesopores, and they exhibit excellent catalytic sensing response to CO of low concentration at low working temperature with good sensitivity, ultrashort response‐recovery time (16 s/1 s), and high selectivity. In‐depth study reveals that besides the contribution from the fast diffusion of gaseous molecules and rich interfaces in mesoporous WO₃/Pt nanocomposites, the partially oxidized Pt nanoparticles that chemically and electronically sensitize the crystalline WO₃ matrix, dramatically enhance the sensitivity and selectivity.     

RGD‐Conjugated Nanoscale Coordination Polymers for Targeted T1‐ and T2‐weighted Magnetic Resonance Imaging of Tumors in Vivo

Development of multifunctional nanoscale coordination polymers (NCPs) allowing for T₁‐ and T₂‐weighted targeted magnetic resonance (MR) imaging of tumors could significantly improve the diagnosis accuracy. In this study, nanoscale coordination polymers (NCPs) with a diameter of ≈80 nm are obtained with 1,1′‐dicarboxyl ferrocene (Fc) as building blocks and magnetic gadolinium(III) ions as metallic nodes using a nanoprecipitation method, then further aminated through silanization. The amine‐functionalized Fc‐Gd@SiO₂ NCPs enable the covalent conjugation of a fluorescent rhodamine dye (RBITC) and an arginine‐glycine‐aspartic acid (RGD) peptide as a targeting ligand onto their surface. The formed water‐dispersible Fc‐Gd@SiO₂(RBITC)–RGD NCPs exhibit a low cytotoxicity, as confirmed by MTT assay. They have a longitudinal relaxivity (r₁) of 5.1 mM^?1 s^?1 and transversal relaxivity (r₂) of 21.7 mM^?1 s^?1, suggesting their possible use as both T₁‐positive and T₂‐negative contrast agents. In vivo MR imaging experiments show that the signal of tumor over‐expressing high affinity α_vβ₃ integrin from T₁‐weighted MR imaging is positively enhanced 47±5%, and negatively decreased 33±5% from T₂‐weighted MR imaging after intravenous injection of Fc‐Gd@SiO₂(RBITC)–RGD NCPs.     

A New Material for High‐Temperature Lead‐Free Actuators

Unimorph cantilevers are made from 0.5BaTiO₃‐0.5Sm₂O₃ (BTO‐SmO) self‐assembled vertical heteroepitaxial nanocomposite thin films, grown by PLD on (001) SrTiO₃ single crystal substrates. The films remain piezoelectric up to at least 250 °C without losing any actuation. The longitudinal piezoelectric coefficient, d₃₃, is ≈45 to 50 pm V^?1 measured from room temperature to 250 °C. The transverse piezoelectric coefficient, d₃₁, a key parameter of actuator performance, exceeds PZT (Pb_1–xZr_xTiO₃) films at >200 pm V^?1. Since the d₃₁ coefficient was found to be positive, this opens up exciting new applications opportunities. The possible reasons for d₃₁ > 0 are discussed in the light of 3D strain control in the nanocomposites.     

In Vivo Imaging of MMP‐13 Activity Using a Specific Polymer‐FRET Peptide Conjugate Detects Early Osteoarthritis and Inhibitor Efficacy

Imaging early molecular changes in osteoarthritic (OA) joints is instrumental for the development of disease‐modifying drugs. To this end, a fluorescent resonance energy transfer‐based peptide probe that is cleavable by matrix metalloproteinase 13 (MMP‐13) has been developed. This protease degrades type II collagen, a major matrix component of cartilage. The probe exhibits high catalytic efficiency (k_cat/K_M = 6.5 × 10⁵m ^?1 s^?1) and high selectivity for MMP‐13 over a set of nine MMPs. To achieve optimal in vivo pharmacokinetics and tissue penetration, the probe has been further conjugated to a linear l ‐polyglutamate chain of 30 kDa. The conjugate detects early biochemical events that occur in a surgically induced murine model of OA before major histological changes. The nanometric probe is suitable for the monitoring of in vivo efficacy of an orally bioavailable MMP‐13 inhibitor, which effectively blocks cartilage degradation during the development of OA. This new polymer‐probe can therefore be a useful tool in detecting early OA, disease progression, and in developing MMP‐13‐based disease‐modifying drugs for OA.     

Giant Piezoelectricity of Ternary Perovskite Ceramics at High Temperatures

Here, novel ferroelectric ceramics of (0.95 ? x)BiScO₃‐xPbTiO₃‐0.05Pb(Sn_1/3Nb_2/3)O₃ (BS‐xPT‐PSN) of complex perovskite structure are reported with compositions near the morphotropic phase boundary (MPB), and which exhibit a piezoelectric coefficient d₃₃ = 555 pC N^?1, a large‐signal coefficient $d_{33}^{?}$ ≈ 1200 pm V^?1 at room temperature, and a high Curie temperature T_C of 408 °C. More interestingly, this ternary system exhibits a giant and stable piezoelectric response at 200 °C with a large‐signal $d_{33}^{?}$ ≈ 2500 pm V^?1, matching that of the costly relaxor‐based piezoelectric single crystals at room temperature. The mechanisms of such giant piezoelectricity and its characteristic temperature dependence are attributed to the spontaneous polarization rotation and extension under an electric field and the MPB‐related phase transition. The findings reveal that the BS‐xPT‐PSN ceramics constitute a new family of high‐performance piezoelectric materials suitable for electromechanical transducers that can be operated at high temperatures (at 200 °C, or higher).     

Oxygen‐Deficient Homo‐Interface toward Exciting Boost of Pseudocapacitance

Pseudocapacitors hold great promise as charge storage systems that combine battery‐level energy density and capacitor‐level power density. The utilization of pseudocapacitive material, however, is usually restricted to the surface due to poor electrode kinetics, leading to less accessible charge storage sites and limited capacitance. Here, tin oxide is successfully endowed with outstanding pseudocapacitance and fast electrode kinetics in a negative potential window by engineering oxygen‐deficient homo‐interfaces. The as‐prepared SnO_2?x@SnO_2?x electrode yields a specific capacitance of 376.6 F g^?1 at the current density of 2.5 A g^?1 and retains 327 F g^?1 at a high current density of 80 A g^?1. The theoretical calculation reveals that the oxygen defects are more favorable at homo‐interfaces than at the surface due to the lower defect formation energy. Meanwhile, as compared with the surface, the homo‐interface possesses more stable Li⁺ storage sites that are readily accessed by Li⁺ due to the occurrence of oxygen vacancies, enabling outstanding pseudocapacitance as well as high rate capability. This oxygen‐deficient homo‐interface design opens up new opportunities to develop high‐energy and power pseudocapacitors.     

Domain Engineering of Lead‐Free Li‐Modified (K,Na)NbO3 Polycrystals with Highly Enhanced Piezoelectricity

Aging and re‐poling induced enhancement of piezoelectricity are found in (K,Na)NbO₃ (KNN)‐based lead‐free piezoelectric ceramics. For a compositionally optimized Li‐doped composition, its piezoelectric coefficient d₃₃ can be increased up to 324 pC N^?1 even from a considerably high value (190 pC N^?1) by means of a re‐poling treatment after room‐temperature aging. Such a high d₃₃ value is only reachable in KNN ceramics with complicated modifications using Ta and Sb dopants. High‐angle X‐ray diffraction analysis reveals apparent changes in the crystallographic orientations related to a 90° domain switching before and after the aging and re‐poling process. A possible mechanism considering both defect migration and rotation of spontaneous polarization explains the experimental results. The present study provides a general approach towards piezoelectric response enhancement in KNN‐based piezoelectric ceramics.     

Nanostructured Li2MnSiO4/C Cathodes with Hierarchical Macro‐/Mesoporosity for Lithium‐Ion Batteries

Li₂MnSiO₄/C nanocomposite with hierarchical macroporosity is prepared with poly(methyl methacrylate) (PMMA) colloidal crystals as a sacrificial hard‐template and water‐soluble phenol‐formaldehyde (PF) resin as the carbon source. Scanning electron microscopy (SEM) and transmission electron microscopy (TEM) analyses confirm that the periodic macropores are ≈400 nm in diameter with 20–40 nm walls comprising Li₂MnSiO₄/C nanocrystals that produce additional large mesopores (< 30 nm) between the nanocrystals. The nanostructured Li₂MnSiO₄/C cathode exhibits a high reversible discharge capacity of 200 mAh g^?1 at C/10 (16 mA g^?1) rate at 1.5–4.8 V at 45 °C. Although the discharge capacity can be further increased on operating at 55 °C, the sample exhibits a relatively fast capacity fade at 55 °C, which can be partially solved by simply narrowing the voltage window to avoid side reactions of the electrolyte. The good performance of the Li₂MnSiO₄/C cathodes is attributed to the unique macro‐/mesostructure of the silicate coupled with uniform carbon coating.     

H2xMnxSn3‐xS6 (x = 0.11–0.25): A Novel Reusable Sorbent for Highly Specific Mercury Capture Under Extreme pH Conditions

The H_2xMn_xSn_3‐xS₆ (x = 0.11–0.25) is a new solid acid with a layered hydrogen metal sulfide (LHMS). It derives from K_2xMn_xSn_3–xS₆ (x = 0.5–0.95) (KMS‐1) upon treating it with highly acidic solutions. We demonstrate that LHMS‐1 has enormous affinity for the very soft metal ions such as Hg²⁺ and Ag⁺ which occurs via a rapid ion exchange process. The tremendous affinity of LHMS‐1 for Hg²⁺ is reflected in very high distribution coefficient K_d^Hg values (>10⁶ mL g^?1). The large affinity and selectivity of LHMS‐1 for Hg²⁺ persists in a very wide pH range (from less than zero to nine) and even in the presence of highly concentrated HCl and HNO₃ acids. LHMS‐1 is significantly more selective for Hg²⁺ and Ag⁺ than for the less soft cations Pb²⁺ and Cd²⁺. The Hg²⁺ ions are immobilized in octahedral sites between the sulfide layers of the materials via Hg–S bonds as suggested by pair distribution function (PDF) analysis. LHMS‐1 could decrease trace concentrations of Hg²⁺ (e.g. <100 ppb) to well below the acceptable limits for the drinking water in less than two min. Hg‐laden LHMS‐1 shows a remarkable hydrothermal stability and resistance in 6 M HCl solutions. LHMS‐1 could be regenerated by treating Hg‐loaded samples with 12 M HCl and re‐used without loss of its initial exchange capacity.     

Watermelon‐Like Structured SiOx–TiO2@C Nanocomposite as a High‐Performance Lithium‐Ion Battery Anode

A unique watermelon‐like structured SiO_x–TiO₂@C nanocomposite is synthesized by a scalable sol–gel method combined with carbon coating process. Ultrafine TiO₂ nanocrystals are uniformly embedded inside SiO_x particles, forming SiO_x–TiO₂ dual‐phase cores, which are coated with outer carbon shells. The incorporation of TiO₂ component can effectively enhance the electronic and lithium ionic conductivities inside the SiO_x particles, release the structure stress caused by alloying/dealloying of Si component and maximize the capacity utilization by modifying the Si–O bond feature and decreasing the O/Si ratio (x‐value). The synergetic combination of these advantages enables the synthesized SiO_x–TiO₂@C nanocomposite to have excellent electrochemical performances, including high specific capacity, excellent rate capability, and stable long‐term cycleability. A stable specific capacity of ≈910 mAh g^?1 is achieved after 200 cycles at the current density of 0.1 A g^?1 and ≈700 mAh g^?1 at 1 A g^?1 for over 600 cycles. These results suggest a great promise of the proposed particle architecture, which may have potential applications in the improvement of various energy storage materials.