3D Printing of Ultralow-Concentration 2D Nanomaterial Inks for Multifunctional Architectures.

The direct 3D printing of ultralight architectures with ultralow-concentration 2D nanomaterial inks is necessary yet challenging. Here, we describe an emulsion-based ink for direct printing using 2D nanomaterials, i.e., MXene and graphene oxide (GO). The electrostatic interactions between the ligands in the oil phase and the 2D nanomaterials in the aqueous phase help form sheet-like surfactants at the interface. The interactions between the anchored ligands among different droplets dictate the rheological characteristics of inks, enabling a gel-like behavior ideally suitable for 3D printing at ultralow concentrations of 2D nanomaterials. The 3D printed foams possess lightweight structures with densities of 2.8 mg cm-3 (GO-based) and 4.1 mg cm-3 (MXene-based), and the latter integrates outstanding electrical conductivity, electromagnetic shielding performance, and thermal insulation comparable to air. This work describes a general approach for direct-printing ultralight porous structures that take advantage of the inherent properties of 2D building blocks.

Constructing Dynamic Anode/Electrolyte Interfaces Coupled with Regulated Solvation Structures for Long-Term and Highly Reversible Zinc Metal Anodes.

Aqueous zinc ion batteries (AZIBs) show a great potential for next-generation energy storage due to their high safety and high energy density. However, the severe side reactions of zinc negative electrode largely hinder the further application of AZIBs. Herein, trace tris(hydroxymethyl)aminomethane (Tris) additive with rich lone-pair-electrons and zincophilic sites is firstly introduced to achieve long-term and highly reversible Zn plating/stripping. Specifically, Tris not only regulates the solvation structure of Zn2+, but is also adsorbed vertically on the Zn anode surface with a changed coordination intensity during the plating/stripping process of Zn to generate an in situ dynamic adsorption layer for the first time. The dynamic adsorption layer could successively attract the solvated Zn2+ and then promote the de-solvation of the solvated Zn2+ owing to the orientation polarization with regularly-changed applied electric field, the volume rejection effect, and strong intermolecular force towards H2O of the vertically-adsorbed Tris. Therefore, an improved Zn2+-transport kinetics as well as the inhibition of side reactions of Zn anode are successfully realized. Accordingly, the Zn||Zn symmetric cell provides an ultra-long cycle life of 2600 h. Furthermore, the Zn||MnO2 full cell with Tris could demonstrate a high capacity and structural stability for practical applications.

Scalable Production of Catecholamine-Densified MXene Coatings for Electromagnetic Shielding and Infrared Stealth.

Processing transition metal carbides/nitrides (MXenes) inks into large-area functional coatings expects promising potential for electromagnetic interference (EMI) shielding and infrared stealth. However, the coating performances, especially for scalable fabrication techniques, are greatly constrained by the flake size and stacking manner of MXene. Herein, the large-area production of highly densified and oriented MXene coatings is demonstrated by engineering interfacial interactions of small MXene flakes with catecholamine molecules. The catecholamine molecules can micro-crosslink MXene nanosheets, significantly improving the ink's rheological properties. It favors the shear-induced sheet arrangement and inhibition of structural defects in the blade coating process, making it possible to achieve high orientation and densification of MXene assembly by either large-area coating or patterned printing. Interestingly, the MXene/catecholamine coating exhibits high conductivity of up to 12 247 S cm-1 and ultrahigh specific EMI shielding effectiveness of 2.0 ×10 5  dB cm2 g-1 , obviously superior to most of the reported MXene materials. Furthermore, the regularly assembled structure also endows the MXene coatings with low infrared emissivities for infrared stealth applications. Therefore, MXene/catecholamine coatings with ultraefficient EMI shielding and low infrared emissivity prove the feasibility of applications in aerospace, military, and wearable devices.

In-Situ Constructing A Heterogeneous Layer on Lithium Metal Anodes for Dendrite-Free Lithium Deposition and High Li-ion Flux.

Constructing efficient artificial solid electrolyte interface (SEI) film is extremely vital for the practical application of lithium metal batteries. Herein, a dense artificial SEI film, in which lithiophilic Zn/Lix Zny are uniformly but nonconsecutively dispersed in the consecutive Li+ -conductors of Lix SiOy , Li2 O and LiOH, is constructed via the in situ reaction of layered zinc silicate nanosheets and Li. The consecutive Li+ -conductors can promote the desolvation process of solvated-Li+ and regulate the transfer of lithium ions. The nonconsecutive lithiophilic metals are polarized by the internal electric field to boost the transfer of lithium ions, and lower the nucleation barrier. Therefore, a low polarization of ≈50 mV for 750 h at 2.0 mA cm-2 in symmetric cells, and a high capacity retention of 99.2 % in full cells with a high lithium iron phosphate areal loading of ≈13 mg cm-2 are achieved. This work offers new sights to develop advanced alkali metal anodes for efficient energy storage.

Constructing Atomic Fe and N Co-doped Hollow Carbon Nanospheres with a Polymer Encapsulation Strategy for High-Performance Lithium-Sulfur Batteries with Accelerated Polysulfide Conversion.

As competitive next-generation rechargeable batteries, lithium-sulfur batteries (LSBs) suffer from the shuttle effect and the sluggish kinetics of intermediate polysulfides during charge and discharge processes, adversely affecting their electrochemical performances and actual applications. Herein, we demonstrate a polymer encapsulation strategy to synthesize atomic Fe and N co-doped hollow carbon nanospheres (Fe-NHC) with Fe-Nx sites for modifying commercial PP separator of LSBs to suppress the shuttle effect and promote the kinetics of intermediate polysulfides. Benefiting from the excellent structural design, the doped-N with positive charges could effectively adsorb negatively charged soluble polysulfides, help attract the soluble polysulfides to the Fe atoms and boost the catalytic transformation of the soluble polysulfides. Additionally, such a thin carbon shell could provide a short mass diffusion pathway and hence promote the adsorption and the catalytic conversion. Therefore, the battery with the Fe-NHC/PP separator delivers outstanding cycling and rate performances. At the large current density of 1 C, the specific capacity is 1079 mA h g-1 and maintains a low loss of 0.076 % per cycle within 500 cycles. Even at a harsh current density of 4 C, a high capacity of 824 mA h g-1 is still achieved, indicating the advantage of the Fe-NHC/PP separator in LSBs.

Mesoporous Yolk-Shell Structured Organosulfur Nanotubes with Abundant Internal Joints for High-Performance Lithium-Sulfur Batteries by Kinetics Acceleration.

Although organosulfur compounds can protect lithium anodes, participate in the redox reaction, and suppress the shuttle effect, the sluggish electrochemical dynamics of their bulk structure and the notorious shuttle effect of covalent long-chain sulfurs largely impede their actual applications. Herein, sulfurized carbon nanotube@aminophenol-formaldehyde (SC@A) with covalently linked short-chain sulfurs is firstly synthesized by in situ polymerization of aminophenol-formaldehyde (AF) on the surface of carbon nanotubes (CNTs) followed by acetone etching and inverse sulfurization processes, forming mesoporous yolk-shell organosulfur nanotubes with abundant internal joints between the yolk of CNTs and the shell of sulfurized AF for the first time. In situ Raman spectra, in situ XRD patterns, and ex situ XPS spectra verify that the covalent short-chain sulfurs bring about a reversible solid-solid conversion process of sulfur, thoroughly avoiding the shuttle effect. The mesoporous yolk-shell structure with abundant internal joints can effectively accommodate the volume change, fully expose active sites and efficiently improve the transport of electrons and lithium ions, thus highly promoting the solid-solid electrochemical reaction kinetics. Therefore, the SC@A cathode exhibits a superior specific capacity of 841 mAh g-1 and a capacity decay of 0.06% per cycle within 500 cycles at a large current density of 5.0 C.

Cold-Resistant Nitrogen/Sulfur Dual-Doped Graphene Fiber Supercapacitors with Solar-Thermal Energy Conversion Effect.

Although graphene fiber-based supercapacitors are promising for wearable electronic devices, the low energy density of electrodes and poor cold resistance of aqueous electrolytes limit their wide application in cold environments. Herein, porous nitrogen/sulfur dual-doped graphene fibers (NS-GFs) are synthesized by hydrothermal self-assembly followed by thermal annealing, exhibiting an excellent capacitive performance of 401 F cm-3 at 400 mA cm-3 because of the synergistic effect of heteroatom dual-doping. The assembled symmetric all-solid-state supercapacitor with polyvinyl alcohol/H2 SO4 /graphene oxide gel electrolyte exhibits a high capacitance of 221 F cm-3 and a high energy density of 7.7 mWh cm-3 at 80 mA cm-3 . Interestingly, solar-thermal energy conversion of the electrolyte with 0.1 wt % graphene oxide extends the operating temperature range of the supercapacitor to 0 °C. Furthermore, the photocatalysis effect of the dual-doped heteroatoms increases the capacitance of NS-GFs. At an ambient temperature of 0 °C, the capacitance increases from 0 to 182 F cm-3 under 1 sun irradiation because of the excellent solar light absorption and efficient solar-thermal energy conversion of graphene oxide, preventing the aqueous electrolyte from freezing. The flexible supercapacitor exhibits a long cycle life, good bending resistance, reliable scalability, and ability to power visual electronics, showing great potential for outdoor electronics in cold environments.

In Situ Growth of Hierarchical Ni-Mn-O Solid Solution on a Flexible and Porous Ni Electrode for High-Performance All-Solid-State Asymmetric Supercapacitors.

To endow all-solid-state asymmetric supercapacitors with high energy density, cycling stability, and flexibility, we design a binder-free supercapacitor electrode by in situ growth of well-distributed broccoli-like Ni0.75 Mn0.25 O/C solid solution arrays on a flexible and three-dimensional Ni current collector (3D-Ni). The electrode consists of a bottom layer of compressed but still porous Ni foam with excellent flexibility and high electrical conductivity, an intermediate layer of interconnected Ni nanoparticles providing a large specific surface area for loading of active substances, and a top layer of vertically aligned mesoporous nanosheets of a Ni0.75 Mn0.25 O/C solid solution. The resultant 3D-Ni/Ni0.75 Mn0.25 O/C cathode exhibits a specific capacitance of 1657.6 mF cm-2 at 1 mA cm-2 and shows no degradation of the capacitance after 10 000 cycles at 3 mA cm-2 . The assembled 3D-Ni/Ni0.75 Mn0.25 O/C//activated carbon asymmetric supercapacitor has a high specific capacitance of 797.7 mF cm-2 at 2 mA cm-2 and an excellent cycling stability with 85.3 % of capacitance retention after 10 000 cycles at a current density of 3 mA cm-2 . The energy density and power density of the asymmetric supercapacitor are up to 6.6 mW h cm-3 and 40.8 mW cm-3 , respectively, indicating a fairly promising future of the flexible 3D-Ni/Ni0.75 Mn0.25 O/C electrode for efficient energy storage applications.

Self-Assembly of MXene-Surfactants at Liquid-Liquid Interfaces: From Structured Liquids to 3D Aerogels.

2D transition metal carbides and nitrides (MXenes), a class of emerging nanomaterials with intriguing properties, have attracted significant attention in recent years. However, owing to the highly hydrophilic nature of MXene nanosheets, assembly strategies of MXene at liquid-liquid interfaces have been very limited and challenging. Herein, through the cooperative assembly of MXene and amine-functionalized polyhedral oligomeric silsesquioxane at the oil-water interface, we report the formation, assembly, and jamming of a new type MXene-based Janus-like nanoparticle surfactants, termed MXene-surfactants (MXSs), which can significantly enhance the interfacial activity of MXene nanosheets. More importantly, this simple assembly strategy opens a new platform for the fabrication of functional MXene assemblies from mesoscale (e.g., structured liquids) to macroscale (e.g., aerogels), that can be used for a range of applications, including nanocomposites, electronic devices, and all-liquid microfluidic devices.

Multifunctional, Superelastic, and Lightweight MXene/Polyimide Aerogels.

2D transition metal carbides and nitrides (MXenes) have gained extensive attention recently due to their versatile surface chemistry, layered structure, and intriguing properties. The assembly of MXene sheets into macroscopic architectures is an important approach to harness their extraordinary properties. However, it is difficult to construct a freestanding, mechanically flexible, and 3D framework of MXene sheets owing to their weak intersheet interactions. Herein, an interfacial enhancement strategy to construct multifunctional, superelastic, and lightweight 3D MXene architectures by bridging individual MXene sheets with polyimide macromolecules is developed. The resulting lightweight aerogel exhibits superelasticity with large reversible compressibility, excellent fatigue resistance (1000 cycles at 50% strain), 20% reversible stretchability, and high electrical conductivity of ≈4.0 S m-1 . The outstanding mechanical flexibility and electrical conductivity make the aerogel promising for damping, microwave absorption coating, and flexible strain sensor. More interestingly, an exceptional microwave absorption performance with a maximum reflection loss of -45.4 dB at 9.59 GHz and a wide effective absorption bandwidth of 5.1 GHz are achieved.

Dual-Carbon-Confined Fe7 S8 Anodes with Enhanced Electrochemical Catalytic Conversion Process for Ultralong Lithium Storage.

Although the electrochemical catalytic conversion process is effective in increasing the reversible capacity of lithium-ion batteries, the low contact efficiency between metal catalyst and substrate and pulverization of the solid electrolyte interface (SEI) film without protection are not beneficial for the electrochemical reactions. Herein, Fe7 S8 nanoparticles are confined by both reduced graphene oxide (RGO) and in-situ-formed amorphous carbon (C) to form dual-carbon-confined Fe7 S8 as a lithium-ion anode. The dual-carbon-confined structure provides a confined space to prevent pulverization of the SEI film and increases the local concentration of intermediate phases, which could be electrocatalytically decomposed by Fe nanoparticles formed in situ to increase the reversibility of the electrochemical reactions and gain high reversible capacity. In addition, the dual-carbon-confined structure ensures fast transfer of electrons and boosts transport of lithium ions due to the highly conductive dual-carbon shell. Thus, the Fe7 S8 /C/RGO anode delivers an excellent rate performance and long cycling stability. At current densities of 2000 and 5000 mA g-1 , the reversible capacities are 520 mA h g-1 over 1500 cycles and 294 mA h g-1 over 2000 cycles, respectively.

K2 Mn4 O8 /Reduced Graphene Oxide Nanocomposites for Excellent Lithium Storage and Adsorption of Lead Ions.

Ion diffusion efficiency at the solid-liquid interface is an important factor for energy storage and adsorption from aqueous solution. Although K2 Mn4 O8 (KMO) exhibits efficient ion diffusion and ion-exchange capacities, due to its high interlayer space of 0.70 nm, how to enhance its mass transfer performance is still an issue. Herein, novel layered KMO/reduced graphene oxide (RGO) nanocomposites are fabricated through the anchoring of KMO nanoplates on RGO with a mild solution process. The face-to-face structure facilitates fast transfer of lithium and lead ions; thus leading to excellent lithium storage and lead ion adsorption. The anchoring of KMO on RGO not only increases electrical conductivity of the layered nanocomposites, but also effectively prevents aggregation of KMO nanoplates. The KMO/RGO nanocomposite with an optimal RGO content exhibits a first cycle charge capacity of 739 mA h g-1 , which is much higher than that of KMO (326 mA h g-1 ). After 100 charge-discharge cycles, it still retains a charge capacity of 664 mA h g-1 . For the adsorption of lead ions, the KMO/RGO nanocomposite exhibits a capacity of 341 mg g-1 , which is higher than those of KMO (305 mg g-1 ) and RGO (63 mg g-1 ) alone.

Anisotropic MXene/Poly(vinyl alcohol) Composite Hydrogels with Vertically Oriented Channels and Modulated Surface Topography for Efficient Solar-Driven Water Evaporation and Purification.

Hierarchical structure and surface topography play pivotal roles in developing high-performance solar-driven evaporators for clean water production; however, there exists a notable gap in research addressing simultaneous modulation of internal microstructure and surface topography in hydrogels to enhance both solar steam generation performance and desalination efficiency. Herein, anisotropic poly(vinyl alcohol)/MXene composite hydrogels for efficient solar-driven water evaporation and wastewater purification are fabricated using a template-assisted directional freezing approach followed by precise surface wettability modulation. The resultant composite hydrogels exhibit vertically oriented channels that ensure fast water supply during evaporation, and their poly(vinyl alcohol) skeletons can reduce the vaporization enthalpy of the water in the hydrogels. The incorporation of MXene sheets enables efficient solar light absorption and solar-thermal conversion while providing structural reinforcement to the hydrogels. More importantly, the as-created undulating solar-thermal surface, featuring modulated hydrophilic troughs and hydrophobic crests, significantly enhances solar-thermal conversion efficiency, thereby boosting solar evaporation performances. As a result, the fabricated hydrogel-based evaporator exhibits an impressive evaporation rate of 2.55 kg m-2 h-1 under 1 sun irradiation, coupled with long-term durability and desalination stability. Notably, the outstanding mechanical robustness of the hydrogel further enables high portability through a readily achievable process of reversible dehydration/hydration.

Well-designed lamellar reduced graphene oxide-based foam for high-performance solar-driven water purification.

Although solar steam generation is promising for seawater desalination, it is less effective in purifying wastewater with both salt/heavy metal ions and organic contaminants. It is thus imperative to develop multifunctional integrated solar-driven water purification systems with high solar-thermal evaporation and photocatalytic degradation efficiencies. Herein, a lamellar reduced graphene oxide (L-RGO) foam with the vertical lamellar structure is fabricated by bidirectional-freezing, lyophilization, and slight chemical reduction for water purification. The unique vertical lamellar structure not only accelerates upward transport of water for facilitating water evaporation but also endows the L-RGO foam with superb high elasticity for tuning the interlayer distance and varying interactions between the oxygen-containing groups and water molecules to adjust water energy state. As a result, the L-RGO foam achieves a superb water evaporation rate of 2.40 kg m-2 h-1 along with an energy efficiency of 95.3 % under the compressive strain of 44.7 % under 1-sun irradiation. Equally importantly, the decoration of L-RGO foam with polypyrrole is capable of efficiently degrading organic pollutants while retaining high solar steam generation performances, exhibiting great potential in the comprehensive treatment of various water sources for relieving freshwater crisis.

Highly Aligned Graphene Aerogels for Multifunctional Composites.

Stemming from the unique in-plane honeycomb lattice structure and the sp2 hybridized carbon atoms bonded by exceptionally strong carbon-carbon bonds, graphene exhibits remarkable anisotropic electrical, mechanical, and thermal properties. To maximize the utilization of graphene's in-plane properties, pre-constructed and aligned structures, such as oriented aerogels, films, and fibers, have been designed. The unique combination of aligned structure, high surface area, excellent electrical conductivity, mechanical stability, thermal conductivity, and porous nature of highly aligned graphene aerogels allows for tailored and enhanced performance in specific directions, enabling advancements in diverse fields. This review provides a comprehensive overview of recent advances in highly aligned graphene aerogels and their composites. It highlights the fabrication methods of aligned graphene aerogels and the optimization of alignment which can be estimated both qualitatively and quantitatively. The oriented scaffolds endow graphene aerogels and their composites with anisotropic properties, showing enhanced electrical, mechanical, and thermal properties along the alignment at the sacrifice of the perpendicular direction. This review showcases remarkable properties and applications of aligned graphene aerogels and their composites, such as their suitability for electronics, environmental applications, thermal management, and energy storage. Challenges and potential opportunities are proposed to offer new insights into prospects of this material.

Self-Powered and Self-Healable Extraocular-Muscle-Like Actuator Based on Dielectric Elastomer Actuator and Triboelectric Nanogenerator.

Although dielectric elastomer actuators (DEAs) are promising artificial muscles for use as visual prostheses in patients with oculomotor nerve palsy (ONP), high driving voltage coupled with vulnerable compliant electrodes limits their safe long-term service. Herein, a self-healable polydimethylsiloxane compliant electrode based on reversible imine bonds and hydrogen bonds is prepared and coated on an acrylic ester film to develop a self-healable DEA (SDEA), followed by actuation with a high-output triboelectric nanogenerator (TENG) to construct a self-powered DEA (TENG-SDEA). Under 135.9 kV mm-1 , the SDEA exhibits an elevated actuated strain of 50.6%, comparable to the actuation under DC power. Moreover, the mechanically damaged TENG-SDEA displays a self-healing efficiency of over 90% for 10 cycles. The TENG ensures the safe using of TENG-SDEAs and an extraocular-muscle-like actuator with oriented motion ability integrated by several TENG-SDEAs is constructed. Additionally, the SDEA is directly used as a flexible capacitive sensor for real-time monitoring of the patient's muscle movement. Accordingly, a medical aid system based on a conjunction of the extraocular-muscle-like actuator and a flexible capacitive sensor is manufactured to help the patients suffering from ONP with physical rehabilitation and treatment.

Multistimuli-Responsive Shape-Memory Composites with a Water-Assisted Self-Healing Function Based on Sodium Carboxymethyl Cellulose/Poly(vinyl alcohol)/MXene.

Recent advancements in artificial intelligence have propelled the development of shape-memory polymers (SMPs) with sophisticated, environment-sensitive capabilities. Despite the progress, most of the existing SMPs are limited to responding to a single stimulus and show poor functionality, which has severely hindered their future applications. Herein, we report a high-performance multistimuli-responsive shape-memory and self-healing composite film fabricated by embedding MXene nanosheets into a conventional shape-memory sodium carboxymethyl cellulose (CMC) and poly(vinyl alcohol) (PVA) matrix. The incorporation of photothermal MXene nanosheets not only enhances the composite films' mechanical strength but also provides efficient solar-thermal conversion and robust light-actuated shape-memory properties. The resultant composite films exhibit an exceptional shape-memory response to various stimuli including heat, light, and water. Meanwhile, the interfacial interactions can be modulated by adjusting the MXene content, thereby enabling precise manipulation of the shape-memory performance. Moreover, thanks to the intrinsic hydrophilicity of the components and the unique physically cross-linked network, the composite films also demonstrate an effective water-assisted self-healing capability with an impressive healing efficiency of 85.7%. This work offers insights into the development of multifunctional, multistimuli-responsive shape-memory composites, opening up new possibilities for future applications in smart technologies.

Antifreezing, Antidrying, and Conductive Hydrogels for Electronic Skin Applications at Ultralow Temperatures.

Although conductive hydrogel-based flexible electronic devices have superb flexibility and high conductivities, they tend to malfunction in dry or frigid areas. Herein, an ultralow-temperature tolerant, antidrying, and conductive composite hydrogel is designed for electronic skin applications on the basis of the synergy of double-cross-linked polymer networks, Hofmeister effect, and electrostatic interaction and fabricated by in situ free radical polymerization of 2-acrylamido-2-methyl-1-propanesulfonic acid and acrylic acid in the presence of poly(vinyl alcohol) and conductive MXene sheets, followed by impregnation with LiCl. Thanks to the synergy of LiCl and the charged polar terminal groups of the synthesized polymers, the composite hydrogel can not only bear an ultralow temperature of -80 °C without freezing but also maintain its original mass. Meanwhile, the resultant hydrogel possesses satisfactory self-regeneration ability benefiting from the moisturizing effect of LiCl. The conductive network of MXene sheets greatly improves the ionic conductivity of the hydrogel at low temperatures, exhibiting an ionic conductivity of 1.4 S m-1 at -80 °C. Furthermore, the electronic skin assembled by the multifunctional hydrogel is efficient in monitoring human motions at -80 °C. The antifreezing and antidrying features along with favorable ionic conductivity, high tensile strength, and outstanding flexibility make the composite hydrogel promising for applications in frigid and dry regions.

Biphasic GaIn Alloy Constructed Stable Percolation Network in Polymer Composites over Ultrabroad Temperature Region.

Flexible and adaptable polymer composites with high-performance reliability over wide temperature range are imperative for various applications. However, the distinct filler-matrix thermomechanical behaviors often cause severe structure damage and performance degradation upon large thermal shock. To address this issue, a general strategy is proposed to construct leakage-free, self-adaptive, stable percolation networks in polymer composites over wide temperature (77-473 K) with biphasic Ga35In65 alloy. The in situ micro-CT technology, for the first time, reveals the conformable phase transitions of Ga35In65 alloys in the polymer matrix that help repair the disruptive conductive networks over large temperature variations. The cryo-expanded Ga compensates the disruptive carbon networks at low temperatures, and flowable Ga and melted In at high temperatures conformably fill and repair the deboned interfaces and yielded crevices. As a proof-of-concept, this temperature-resistant composite demonstrates superb electrical conductivity and electromagnetic interference shielding properties and stability even after a large temperature shock (ΔT = 396 K). Furthermore, the superiority of the construction of temperature self-adaptive networks within the composite enables them for additive manufacturing of application-oriented components. This work offers helpful inspiration for developing high-performance polymer composites for extreme-temperature applications.

High-Precision Printing of Flexible MXene Patterns for Dynamically Tunable Electromagnetic Interference Shielding Performance.

Smart electromagnetic interference (EMI) shielding materials are of great significance in coping with the dynamic performance demands of cutting-edge electronic devices. However, smart EMI shielding materials are still in their infancy and face a variety of challenges (e.g., large thickness, limited tunable range, poor reversibility, and unclear mechanisms). Here, we report a method for controllable shielding electromagnetic (EM) waves through subwavelength structure changes regulated by the customized structure via a direct printing route. The highly conductive MXene ink is regulated with metal ions (Al3+ ions), giving superb metallic conductivity (∼5000 S cm-1) for the printed lines without an annealing treatment. The reversible tunability of EMI shielding effectiveness (SE) ranging from 8.2 dB ("off" state) to 34 dB ("on" state) is realized through the controllable modulation of subwavelength structure driven by stress. This work provides a feasible strategy to develop intelligent shielding materials and EM devices.