PdMo bimetallene for oxygen reduction catalysis.

The efficient interconversion of chemicals and electricity through electrocatalytic processes is central to many renewable-energy initiatives. The sluggish kinetics of the oxygen reduction reaction (ORR) and the oxygen evolution reaction (OER)1-4 has long posed one of the biggest challenges in this field, and electrocatalysts based on expensive platinum-group metals are often required to improve the activity and durability of these reactions. The use of alloying5-7, surface strain8-11 and optimized coordination environments12 has resulted in platinum-based nanocrystals that enable very high ORR activities in acidic media; however, improving the activity of this reaction in alkaline environments remains challenging because of the difficulty in achieving optimized oxygen binding strength on platinum-group metals in the presence of hydroxide. Here we show that PdMo bimetallene-a palladium-molybdenum alloy in the form of a highly curved and sub-nanometre-thick metal nanosheet-is an efficient and stable electrocatalyst for the ORR and the OER in alkaline electrolytes, and shows promising performance as a cathode in Zn-air and Li-air batteries. The thin-sheet structure of PdMo bimetallene enables a large electrochemically active surface area (138.7 square metres per gram of palladium) as well as high atomic utilization, resulting in a mass activity towards the ORR of 16.37 amperes per milligram of palladium at 0.9 volts versus the reversible hydrogen electrode in alkaline electrolytes. This mass activity is 78 times and 327 times higher than those of commercial Pt/C and Pd/C catalysts, respectively, and shows little decay after 30,000 potential cycles. Density functional theory calculations reveal that the alloying effect, the strain effect due to the curved geometry, and the quantum size effect due to the thinness of the sheets tune the electronic structure of the system for optimized oxygen binding. Given the properties and the structure-activity relationships of PdMo metallene, we suggest that other metallene materials could show great promise in energy electrocatalysis.

Multidimensional Integrated Chalcogenides Nanoarchitecture Achieves Highly Stable and Ultrafast Potassium-Ion Storage.

Potassium-ion batteries (KIBs) have come into the spotlight in large-scale energy storage systems because of cost-effective and abundant potassium resources. However, the poor rate performance and problematic cycle life of existing electrode materials are the main bottlenecks to future potential applications. Here, the first example of preparing 3D hierarchical nanoboxes multidimensionally assembled from interlayer-expanded nano-2D MoS2 @dot-like Co9 S8 embedded into a nitrogen and sulfur codoped porous carbon matrix (Co9 S8 /NSC@MoS2 @NSC) for greatly boosting the electrochemical properties of KIBs in terms of reversible capacity, rate capability, and cycling lifespan, is reported. Benefiting from the synergistic effects, Co9 S8 /NSC@MoS2 @NSC manifest a very high reversible capacity of 403 mAh g-1 at 100 mA g-1 after 100 cycles, an unprecedented rate capability of 141 mAh g-1 at 3000 mA g-1 over 800 cycles, and a negligible capacity decay of 0.02% cycle-1 , boosting promising applications in high-performance KIBs. Density functional theory calculations demonstrate that Co9 S8 /NSC@MoS2 @NSC nanoboxes have large adsorption energy and low diffusion barriers during K-ion storage reactions, implying fast K-ion diffusion capability. This work may enlighten the design and construction of advanced electrode materials combined with strong chemical bonding and integrated functional advantages for future large-scale stationary energy storage.

Enhanced interaction in TiO2/BiVO4 heterostructures via MXene Ti3C2-derived 2D-carbon for highly efficient visible-light photocatalysis.

Heterostructured photocatalysts play a significant role in the removal of contaminants by decreasing the recombination of the photo-induced charges. Herein, we presented novel TiO2/C/BiVO4 ternary hybrids employing a 2D layered Ti3C2 MXene precursor, overcoming the lattice mismatching of TiO2/BiVO4 binary heterostructures simultaneously. Raman and XPS analyses proved the strong coupling effects of TiO2, carbon and BiVO4 components, and the heterostructures were identified from high-resolution transmission electron microscopy results. Moreover, the ternary TiO2/C/BiVO4 composites exhibit excellent photocatalytic performance of Rhodamine B degradation, which is about four times higher than pure BiVO4 and twice that of binary TiO2/BiVO4 heterostructures, reaching a reaction constant of 13.7 × 10-3 min-1 under visible-light irradiation (λ > 420 nm). In addition, for the possible mechanism for dye elimination it was proposed that RhB molecule be directly oxidized by photo-induced holes (h+) on the BiVO4 components and superoxide radical ([Formula: see text]) generated from conduction band electrons of the heterostructures. This work will provide possibilities for developing visible-light responsive nanomaterials for efficient solar utilization.

Two-Dimensional Water-Coupled Metallic MoS2 with Nanochannels for Ultrafast Supercapacitors.

MoS2 is a promising electrode material for energy storage. However, the intrinsic multilayer pure metallic MoS2 (M-MoS2) has not been investigated for use in supercapacitors. Here, an ultrafast rate supercapacitor with extraordinary capacitance using a multilayer M-MoS2-H2O system is first investigated. Intrinsic M-MoS2 with a monolayer of water molecules covering both sides of nanosheets is obtained through a hydrothermal method with water as solvent. The super electrical conductivity of the as-prepared pure M-MoS2 is beneficial to electron transport for high power supercapacitor. Meanwhile, nanochannels between the layers of M-MoS2-H2O with a distance of ∼1.18 nm are favorable for increasing the specific space for ion diffusion and enlarging the surface area for ion adsorption. By virtue of this, M-MoS2-H2O reaches a high capacitance of 380 F/g at a scan rate of 5 mV/s and still maintains 105 F/g at scan rate of 10 V/s. Furthermore, the specific capacitance of the symmetric supercapacitor based on M-MoS2-H2O electrodes retain a value as high as 249 F/g under 50 mV/s. These findings suggest that multilayered M-MoS2-H2O system with ion accessible large nanochannels and efficient charge transport provide an efficient energy storage strategy for ultrafast supercapacitors.

Spectroscopic Identification of the Au-C Bond Formation upon Electroreduction of an Aryl Diazonium Salt on Gold.

Electroreduction of aryl diazonium salts on gold can produce organic films that are more robust than their analogous self-assembled monolayers formed from chemical adsorption of organic thiols on gold. However, whether the enhanced stability is due to the Au-C bond formation remains debated. In this work, we report the electroreduction of an aryl diazonium salt of 4,4'-disulfanediyldibenzenediazonium on gold forming a multilayer of Au-(Ar-S-S-Ar)n, which can be further degraded to a monolayer of Au-Ar-S- by electrochemical cleavage of the S-S moieties within the multilayer. By conducting an in situ surface-enhanced Raman spectroscopic study of both the multilayer formation/degradation and the monolayer reduction/oxidation processes, coupled to density functional theory calculations, we provide compelling evidence that an Au-C bond does form upon electroreduction of aryl diazonium salts on gold and that the enhanced stability of the electrografted organic films is due to the Au-C bond being intrinsically stronger than the Au-S bond for a given phenylthiolate compound by ca. 0.4 eV.

Reversibility of Noble Metal-Catalyzed Aprotic Li-O2 Batteries.

The aprotic Li-O2 battery has attracted a great deal of interest because, theoretically, it can store far more energy than today's batteries. Toward unlocking the energy capabilities of this neotype energy storage system, noble metal-catalyzed high surface area carbon materials have been widely used as the O2 cathodes, and some of them exhibit excellent electrochemical performances in terms of round-trip efficiency and cycle life. However, whether these outstanding electrochemical performances are backed by the reversible formation/decomposition of Li2O2, i.e., the desired Li-O2 electrochemistry, remains unclear due to a lack of quantitative assays for the Li-O2 cells. Here, noble metal (Ru and Pd)-catalyzed carbon nanotube (CNT) fabrics, prepared by magnetron sputtering, have been used as the O2 cathode in aprotic Li-O2 batteries. The catalyzed Li-O2 cells exhibited considerably high round-trip efficiency and prolonged cycle life, which could match or even surpass some of the best literature results. However, a combined analysis using differential electrochemical mass spectrometry and Fourier transform infrared spectroscopy, revealed that these catalyzed Li-O2 cells (particularly those based on Pd-CNT cathodes) did not work according to the desired Li-O2 electrochemistry. Instead the presence of noble metal catalysts impaired the cells' reversibility, as evidenced by the decreased O2 recovery efficiency (the ratio of the amount of O2 evolved during recharge/that consumed in the preceding discharge) coupled with increased CO2 evolution during charging. The results reported here provide new insights into the O2 electrochemistry in the aprotic Li-O2 batteries containing noble metal catalysts and exemplified the importance of the quantitative assays for the Li-O2 reactions in the course of pursuing truly rechargeable Li-O2 batteries.

Identifying Reactive Sites and Transport Limitations of Oxygen Reactions in Aprotic Lithium-O2 Batteries at the Stage of Sudden Death.

Discharging of the aprotic Li-O2 battery relies on the O2 reduction reaction (ORR) forming solid Li2 O2 in the positive electrode, which is often characterized by a sharp voltage drop (that is, sudden death) at the end of discharge, delivering a capacity far below its theoretical promise. Toward unlocking the energy capabilities of Li-O2 batteries, it is crucial to have a fundamental understanding of the origin of sudden death in terms of reactive sites and transport limitations. Herein, a mechanistic study is presented on a model system of Au|Li2 O2 |Li(+) electrolyte, in which the Au electrode was passivated with a thin Li2 O2 film by discharging to the state of sudden death. Direct conductivity measurement of the Li2 O2 film and in situ spectroscopic study of ORR using (18) O2 for passivation and (16) O2 for further discharging provide compelling evidence that ORR (and O2 evolution reaction as well) occurs at the buried interface of Au|Li2 O2 and is limited by electron instead of Li(+) and O2 transport.

Amorphous Li2 O2 : Chemical Synthesis and Electrochemical Properties.

When aprotic Li-O2 batteries discharge, the product phase formed in the cathode often contains two different morphologies, that is, crystalline and amorphous Li2 O2 . The morphology of Li2 O2 impacts strongly on the electrochemical performance of Li-O2 cells in terms of energy efficiency and rate capability. Crystalline Li2 O2 is readily available and its properties have been studied in depth for Li-O2 batteries. However, little is known about the amorphous Li2 O2 because of its rarity in high purity. Herein, amorphous Li2 O2 has been synthesized by a rapid reaction of tetramethylammonium superoxide and LiClO4 in solution, and its amorphous nature has been confirmed by a range of techniques. Compared with its crystalline siblings, amorphous Li2 O2 demonstrates enhanced charge-transport properties and increased electro-oxidation kinetics, manifesting itself a desirable discharge phase for high-performance Li-O2 batteries.

Unlocking the critical roles of N, P Co-Doping in MXene for Lithium-Oxygen Batteries: Elevated d-Band center and expanded interlayer spacing.

The design and fabrication of bifunctional catalysts with high electrocatalytic activity and stability are critical for developing highly reversible Li-O2 batteries (LOBs). Herein, the N, P co-doped MXene (NP-MXene) is prepared by one-step annealing method and evaluated as bifunctional catalyst for LOBs. The results suggest that the P doping plays a crucial role in increasing interlayer distance of MXene, thereby effectively providing more active sites, fast mass transfer, and ample space for the deposition/decomposition of Li2O2. Moreover, the N doping can significantly elevate the d-band center of Ti, thereby remarkably improving the adsorption of reaction intermediates and accelerating the deposition/decomposition of Li2O2 films. Consequently, the MXene-based LOBs deliver an ultrahigh specific capacity of 13,995 mAh/g at 500 mA g-1, a discharge/charge voltage gap of 0.89 V, and a cycle life up to 523 cycles with a limited capacity of 1000 mAh/g at 500 mA g-1. Impressively, the as-fabricated flexible LOBs with NP-MXene cathode display excellent cycling stability and ability to continuously power LEDs even after bending. Our findings pave the road of heteroatom doped MXenes as next-generation electrodes for high-performance energy storage and conversion systems.

A High-Rate and Ultrastable Re2Te5/MXene Anode for Potassium Storage Enabled by Amorphous/Crystalline Heterointerface Engineering.

The pursuit of anode materials capable of rapid and reversible potassium storage performance is a challenging yet fascinating target. Herein, a heterointerface engineering strategy is proposed to prepare a novel superstructure composed of amorphous/crystalline Re2Te5 anchored on MXene substrate (A/C-Re2Te5/MXene) as an advanced anode for potassium-ion batteries (KIBs). The A/C-Re2Te5/MXene anode exhibits outstanding reversible capacity (350.4 mAh g-1 after 200 cycles at 0.2 A g-1), excellent rate capability (162.5 mAh g-1 at 20 A g-1), remarkable long-term cycling capability (186.1 mAh g-1 at 5 A g-1 over 5000 cycles), and reliable operation in flexible full KIBs, outperforming state-of-the-art metal chalcogenides-based devices. Experimental and theoretical investigations attribute this high performance to the synergistic effect of the A/C-Re2Te5 with a built-in electric field and the elastic MXene, enabling improved pseudocapacitive contribution, accelerated charge transfer behavior, and high K+ ion adsorption/diffusion ability. Meanwhile, a combination of intercalation and conversion reactions mechanism is observed within A/C-Re2Te5/MXene. This work offers a new approach for developing metal tellurides- and MXene-based anodes for achieving stable cyclability and fast-charging KIBs.

Enhancing humidity resistance of nickel-rich layered cathode materials by low water-soluble CaF2 coating.

A low water-solubility but hydrophilic coating of CaF2 is demonstrated to be effective in mitigating the susceptibility of nickel-rich cathodes to moisture and even water. The ability of the cathode to resist water erosion is not inherently linked to either hydrophobicity or hydrophilicity, but lies in robust chemical bonding within the protective layer exhibiting low water solubility.

In-Situ growing tungsten Sulfide/Carbon nanosheets on sodium titanate nanorods to stabilize Surface-Structure for enhanced Sodium-ion storage.

Sodium-ions hybrid capacitors (SIHCs) have been recognized as one of the most potential energy storage devices, which can deliver high power and energy densities simultaneously. However, the sluggish kinetics of electrode materials severely restricts the performance of SIHCs. Herein, N, P-codoped carbon and WS2 nanosheets coating on sodium titanate nanorods (NTO@WS2/N, PC) were first designed by in-situ growing process and sulfuration treatment for boosting sodium-ion storage. Specifically, NTO@WS2/N, PC electrodes displayed a satisfactory specific capacity of 274.7 mAh g-1 at 3.0 A g-1 after 1200 cycles. Furthermore, as-assembled SIHCs delivered high-energy density of 112.1 Wh kg-1 and high-power density of 4334.4 W kg-1. Besides, long-term cycling test revealed that a remarkable capacity retention rate of 89.7% was obtained at 8.0 A g-1 after 2000 cycles. The excellent cycling stability and rate property could be ascribed to following aspects. On the one hand, N, P-codoped carbon could enhance the electrical conductivity and strengthen the structural integrality of the composites. On the other hand, ultrathin WS2 nanosheets and one-dimensional (1D) NTO nanorods structure were conducive to the rapid diffusion of Na+. This work provides a convenient technique to stabilize the structure of electrode materials, which can promote the practical application of SIHCs.

Dynamic Intercalation-Conversion Site Supported Ultrathin 2D Mesoporous SnO2/SnSe2 Hybrid as Bifunctional Polysulfide Immobilizer and Lithium Regulator for Lithium-Sulfur Chemistry.

The practical application of lithium-sulfur batteries is impeded by the polysulfide shuttling and interfacial instability of the metallic lithium anode. In this work, a twinborn ultrathin two-dimensional graphene-based mesoporous SnO2/SnSe2 hybrid (denoted as G-mSnO2/SnSe2) is constructed as a polysulfide immobilizer and lithium regulator for Li-S chemistry. The as-designed G-mSnO2/SnSe2 hybrid possesses high conductivity, strong chemical affinity (SnO2), and a dynamic intercalation-conversion site (LixSnSe2), inhibits shuttle behavior, provides rapid Li-intercalative transport kinetics, accelerates LiPS conversion, and decreases the decomposition energy barrier for Li2S, which is evidenced by the ex situ XAS spectra, in situ Raman, in situ XRD, and DFT calculations. Moreover, the mesoporous G-mSnO2/SnSe2 with lithiophilic characteristics enables homogeneous Li-ion deposition and inhibits Li dendrite growth. Therefore, Li-S batteries with a G-mSnO2/SnSe2 separator achieve a favorable electrochemical performance, including high sulfur utilization (1544 mAh g-1 at 0.2 C), high-rate capability (794 mAh g-1 at 8 C), and long cycle life (extremely low attenuation rate of 0.0144% each cycle at 5 C over 2000 cycles). Encouragingly, a 1.6 g S/Ah-level pouch cell realizes a high energy density of up to 359 Wh kg-1 under a lean E/S usage of 3.0 µL mg-1. This work sheds light on the design roadmap for tackling S-cathode and Li-anode challenges simultaneously toward long-durability Li-S chemistry.

Co0.7Fe0.3 NPs confined in yolk-shell N-doped carbon: engineering multi-beaded fibers as an efficient bifunctional electrocatalyst for Zn-air batteries.

The development of bifunctional catalysts with a delicate structure, high efficiency, and good durability for the oxygen evolution reaction (ORR) and oxygen evolution reaction (OER) is crucial to renewable Zn-air batteries. In this work, Co0.7Fe0.3 alloy nanoparticles (NPs) confined in N-doped carbon with a yolk-shell structure in multi-beaded fibers were prepared as a bifunctional electrocatalyst. The confinement structure was composed of an N-doped graphitized carbon shell and a core formed by numerous Co0.7Fe0.3 NPs, and was evenly threaded into a one-dimensional fiber. Moreover, this distinctive hierarchical structure featured abundant mesopores, a high BET surface area of 743.8 m2 g-1, good electronic conductivity, and uniformly distributed Co0.7Fe0.3/Co(Fe)-Nx coupling active sites. Therefore, the experimentally optimized Co0.7Fe0.3@NC2:1-800 showed excellent OER performance (overpotential reached 314 mV at 10 mA cm-2) that far exceeded RuO2 (353 mV), and good ORR catalytic performance (half-wave potential of 0.827 V) comparable to Pt/C (0.818 V). Impressively, the Co0.7Fe0.3@NC2:1-800 Zn-air battery delivered a higher open circuit voltage of 1.449 V, large power density of 85.7 mW cm-2, and outstanding charge-discharge cycling stability compared with the commercial RuO2 + 20 wt% Pt/C catalyst. This work provides new ideas for the structural design of electrocatalysts and energy conversion systems.

Orthorhombic Cobalt Ditelluride with Te Vacancy Defects Anchoring on Elastic MXene Enables Efficient Potassium-Ion Storage.

The fast and reversible potassiation/depotassiation of anode materials remains an elusive yet intriguing goal. Herein, a class of the P-doping-induced orthorhombic CoTe2 nanowires with Te vacancy defects supported on MXene (o-P-CoTe2 /MXene) is designed and prepared, taking advantage of the synergistic effects of the conductive o-P-CoTe2 arrays with rich Te vacancy defects and the elastic MXene sheets with self-autoadjustable function. Consequently, the o-P-CoTe2 /MXene superstructure exhibits boosted potassium-storage performance, in terms of high reversible capacity (373.7 mAh g-1 at 0.2 A g-1 after 200 cycles), remarkable rate capability (168.2 mAh g-1 at 20 A g-1 ), and outstanding long-term cyclability (0.011% capacity decay per cycle over 2000 cycles at 2 A g-1 ), representing the best performance in transition-metal-dichalcogenides-based anodes to date. Impressively, the flexible full battery with o-P-CoTe2 /MXene anode achieves a satisfying energy density of 275 Wh kg-1 and high bending stability. The kinetics analysis and first-principles calculations reveal superior pseudocapacitive property, high electronic conductivity, and favorable K+ ion adsorption and diffusion capability, corroborating fast K+ ion storage. Especially, ex situ characterizations confirm o-P-CoTe2 /MXene undergoes reversible evolutions of initially proceeding with the K+ ion insertion, followed by the conversion reaction mechanism.

SnS2 Nanosheets Anchored on Nitrogen and Sulfur Co-Doped MXene Sheets for High-Performance Potassium-Ion Batteries.

Potassium-ion batteries (KIBs) are emerging as the prospective alternatives to lithium-ion batteries in energy storage systems owing to the sufficient resources and relatively low cost of K-related materials. However, serious volume expansion and low specific capacity are found in most materials systems resulting from the large intrinsic radius of K+. Herein, SnS2 nanosheets anchored on nitrogen and sulfur co-doped MXene (SnS2 NSs/MXene) are creatively designed as advanced anode materials for KIBs. SnS2 NSs/MXene with a unique hierarchical structure can not only provide fast transmission channels for K+ but also avoid the accumulation of K+ and volume expansion. These novel features make SnS2 NSs/MXene electrodes exhibit a superior reversible specific capacity of 342.4 mA h g-1 under 50 mA g-1. Also, they maintain 206.1 mA h g-1 at an even higher current density of 0.5 A g-1 over 800 cycles almost without capacity decay. Moreover, the multistep alloying reaction mechanism of SnS2 NSs/MXene composites and K+ is revealed by the ex situ X-ray diffraction measurement. In addition, the density functional theory calculations confirm the existence of Ti-S bonds between SnS2 nanosheets and MXene, which significantly enhance the structural stability and cycling electrochemical performance of SnS2 NSs/MXene composites.

In-situ construction of Bi/defective Bi4NbO8Cl for non-noble metal based Mott-Schottky photocatalysts towards organic pollutants removal.

The strategy to improve the photocatalytic performance is still a challenge for the novel Sillen-Aurivillius perovskite type Bi4NbO8Cl. Herein, heterostructured Bi/Bi4NbO8Cl was fabricated via in-situ solvothermal method, without the additional introduction of Bi-sources. Simultaneously, the amount of oxygen vacancies (OVs) were increased, as the [Bi2O2] blocks released in the solvothermal process to serve as precursors for Bi particles. Due to the large work function of Bi, a Schottky barrier formed at the Bi/Bi4NbO8Cl interface, promoting photo-induced charge separation generated in the Bi4NbO8Cl semiconductor, supplying more holes for the organic compounds decomposition, which could be widely applied in water decontamination. Furthermore, the OVs facilitate the consumption of photo-induced electrons by assisting oxygen activation to produce superoxide radicals (·O2-), leaving more holes in the valence band of Bi4NbO8Cl, and thus result in the enhancement of Rhodamine B (RhB) degradation by 1.82 times over Bi/Bi4NbO8Cl photocatalysts. Through the synergistic effect of Bi and OVs, the Bi/Bi4NbO8Cl also exhibits enhanced photocatalytic performance towards various organic water-contaminants, such as methyl orange, acid orange 7, p-nitrophenol and tetracycline hydrochloride.

A High-Performance Carbonate-Free Lithium|Garnet Interface Enabled by a Trace Amount of Sodium.

Garnet-type solid-state electrolytes (SSEs) are promising for the realization of next-generation high-energy-density Li metal batteries. However, a critical issue associated with the garnet electrolytes is the poor physical contact between the Li anode and the garnet SSE and the resultant high interfacial resistance. Here, it is reported that the Li|garnet interface challenge can be addressed by using Li metal doped with 0.5 wt% Na (denoted as Li*) and melt-casting the Li* onto the garnet SSE surface. A mechanistic study, using Li6.4 La3 Zr1.4 Ta0.6 O12 (LLZTO) as a model SSE, reveals that Li2 CO3 resides within the grain boundaries of newly polished LLZTO pellet, which is difficult to remove and hinders the wetting process. The Li* melt can phase-transfer the Li2 CO3 from the LLZTO grain boundary to the Li*'s top surface, and therefore facilitates the wetting process. The obtained Li*|LLZTO demonstrates a low interfacial resistance, high rate capability, and long cycle life, and can find applications in future all-solid-state batteries (e.g., Li*|LLZTO|LiFePO4 ).

Strongly coupled ultrasmall-Fe7C3/N-doped porous carbon hybrids for highly efficient Zn-air batteries.

This report presents a simple method to produce an ultrasmall-Fe7C3/N-doped porous carbon hybrid (u-Fe7C3@NC) as an excellent oxygen reduction reaction (ORR) electrocatalyst. A zinc-air battery assembled with u-Fe7C3@NC performs at a higher open potential (1.486 V) and at a lower discharge overpotential compared with the commercial Pt/C catalyst.

MXene/Si@SiO x@C Layer-by-Layer Superstructure with Autoadjustable Function for Superior Stable Lithium Storage.

Despite its very high capacity (4200 mAh g-1), the widespread application of the silicon anode is still hampered by severe volume changes (up to 300%) during cycling, which results in electrical contact loss and thus dramatic capacity fading with poor cycle life. To address this challenge, 3D advanced Mxene/Si-based superstructures including MXene matrix, silicon, SiO x layer, and nitrogen-doped carbon (MXene/Si@SiO x@C) in a layer-by-layer manner were rationally designed and fabricated for boosting lithium-ion batteries (LIBs). The MXene/Si@SiO x@C anode takes the advantages of high Li+ ion capacity offered by Si, mechanical stability by the synergistic effect of SiO x, MXene, and N-doped carbon coating, and excellent structural stability by forming a strong Ti-N bond among the layers. Such an interesting superstructure boosts the lithium storage performance (390 mAh g-1 with 99.9% Coulombic efficiency and 76.4% capacity retention after 1000 cycles at 10 C) and effectively suppresses electrode swelling only to 12% with no noticeable fracture or pulverization after long-term cycling. Furthermore, a soft package full LIB with MXene/Si@SiO x@C anode and Li[Ni0.6Co0.2Mn0.2]O2 (NCM622) cathode was demonstrated, which delivers a stable capacity of 171 mAh g-1 at 0.2 C, a promising energy density of 485 Wh kg-1 based on positive active material, as well as good cycling stability for 200 cycles even after bending. The present MXene/Si@SiO x@C becomes among the best Si-based anode materials for LIBs.