Biobased Inks Based on Cuttlefish Ink and Cellulose Nanofibers for Biodegradable Patterned Soft Actuators.

Soft actuators with stimuli-responsive and reversible deformations have shown great promise in soft robotics. However, some challenges remain in existing actuators, such as the materials involved derived from nonrenewable resources, complex and nonscalable preparation methods, and incapability of complex and programmable deformation. Here, a biobased ink based on cuttlefish ink nanoparticles (CINPs) and cellulose nanofibers (CNFs) was developed, allowing for the preparation of biodegradable patterned actuators by direct ink writing technology. The hybrid CNF/CINP ink displays good rheological properties, allowing it to be accurately printed on a variety of flexible substrates. A bilayer actuator was developed by printing an ink layer on a biodegradable poly(lactic acid) film using extrusion-based 3D printing technology, which exhibits reversible and large bending behavior under the stimuli of humidity and light. Furthermore, programmable and reversible folding and coiling deformations in response to stimuli have been achieved by adjusting the ink patterns. This work offers a fast, scalable, and cost-effective strategy for the development of biodegradable patterned actuators with programmable shape-morphing.

Multistimuli-Responsive Actuators Derived from Natural Materials for Entirely Biodegradable and Programmable Untethered Soft Robots.

Untethered soft robots have attracted growing attention due to their safe interaction with living organisms, good flexibility, and accurate remote control. However, the materials involved are often nonbiodegradable or are derived from nonrenewable resources, leading to serious environmental problems. Here, we report a biomass-based multistimuli-responsive actuator based on cuttlefish ink nanoparticles (CINPs), wood-derived cellulose nanofiber (CNF), and bioderived polylactic acid (PLA). Taking advantage of the good photothermal conversion performance and exceptionally hygroscopic sensitivity of the CINPs/CNF composite (CICC) layer and the opposite thermally induced deformation behavior between the CICC layer and PLA layer, the soft actuator exhibits reversible deformation behaviors under near-infrared (NIR) light, humidity, and temperature stimuli, respectively. By introducing patterned or alignment structures and combining them with a macroscopic reassembly strategy, diverse programmable shape-morphing from 2D to 3D such as letter-shape, coiling, self-folding, and more sophisticated 3D deformations have been demonstrated. All of these deformations can be successfully predicted by finite element analysis (FEA) . Furthermore, this actuator has been further applied as an untethered grasping robot, weightlifting robot, and climbing robot capable of climbing a vertical pole. Such actuators consisting entirely of biodegradable materials will offer a sustainable future for untethered soft robots.

Quantum Phase Transition in Magnetic Nanographenes on a Lead Superconductor.

Quantum spins, also known as spin operators that preserve SU(2) symmetry, lack a specific orientation in space and are hypothesized to display unique interactions with superconductivity. However, spin-orbit coupling and crystal field typically cause a significant magnetic anisotropy in d/f shell spins on surfaces. Here, we fabricate atomically precise S = 1/2 magnetic nanographenes on Pb(111) through engineering sublattice imbalance in the graphene honeycomb lattice. Through tuning the magnetic exchange strength between the unpaired spin and Cooper pairs, a quantum phase transition from the singlet to the doublet state has been observed, consistent with the quantum spin models. From our calculations, the particle-hole asymmetry is induced by the Coulomb scattering potential and gives a transition point about kBTk ≈ 1.6Δ. Our work demonstrates that delocalized π electron magnetism hosts highly tunable magnetic bound states, which can be further developed to study the Majorana bound states and other rich quantum phases of low-dimensional quantum spins on superconductors.

Dual Protective Porous Ti3 C2 Tx MXene/Polyimide Composite Film for Thermal Insulation and Electromagnetic Interference Shielding.

The thriving 5G communication technology leads to the high demand for EMI shielding materials and thermal management materials. Particularly, portable thermal-sensitive electronic devices have more stringent requirements for thermal insulation performances. In most cases, ultrathin EMI shielding materials integrated with ultralow thermal conductivity are not easy to be achieved. To overcome this obstacle, dual protective porous composite films based on Ti3 C2 Tx MXene and polyimide are fabricated by sacrificing polymethyl methacrylate (PMMA) templates. By optimizing the contact thermal resistance and Kapitza resistance, the composite film presents superior thermal insulation performances with a thermal conductivity of 0.0136 W m-1 K-1 . Moreover, the hybrid porous film maintains superior EMI shielding effectiveness of 63.0 dB and high SSE/t of 31651.2 dB cm2 g-1 . Nevertheless, the excellent active and passive heating ability based on Joule heating and photothermal conversion makes the composite film an ideal portable material for thermal management. This work sheds light on designing thermal management materials and EMI shielding materials for cutting-edge electronic devices.

Synthesis of Dendronized Polymers on the Au(111) Surface.

Dendronized polymers (DPs) consist of a linear polymeric backbone with dendritic side chains. Fine-tuning of the functional groups in the side chains enriches the structural versatility of the DPs and imparts a variety of novel physical properties. Herein, the first on-surface synthesis of DPs is achieved via the postfunctionalization of polymers on Au(111), in which the surface-confinement-induced planar conformation and chiral configurations were unambiguously characterized. While the dendronized monomer was synthesized in situ on Au(111), the subsequent polymerization afforded only short, cross-linked DP chains owing to multiple side reactions. The postfunctionalization approach selectively produced brominated polyphenylene backbone moieties by the deiodination polymerization of 4-bromo-4″-iodo-5'-(4-iodophenyl)-1,1':3',1″-terphenyl on Au(111), which smoothly underwent divergent cross-coupling reactions with two different isocyanides to form two types of DPs as individual long chains.

On-Surface Synthesis of [3]Radialenes via [1+1+1] Cycloaddition.

[3]Radialenes are the smallest carbocyclic structures with unusual topologies and cross-conjugated π-electronic structures. Here, we report a novel [1+1+1] cycloaddition reaction for the synthesis of aza[3]radialenes on the Ag(111) surface, where the steric hindrance of the chlorine substituents guides the selective and orientational assembling of the isocyanide precursors. By combining scanning tunneling microscopy, non-contact atomic force microscopy, and time-of-flight secondary ion mass spectrometry, we determined the atomic structure of the produced aza[3]radialenes. Furthermore, two reaction pathways including synergistic and stepwise are proposed based on density functional theory calculations, which reveal the role of the chlorine substituents in the activation of the isocyano groups via electrostatic interaction.

An ultra-broad-range pressure sensor based on a gradient stiffness design.

The question of how to make artificial intelligence robots perceive the power of "light as a feather" and "heavy as a mountain" at the same time has always been a goal that people are striving to achieve. However, pressure sensors, the key components of electronic equipment, are often unable to incorporate high sensitivity and wide range performance. Here, we proposed a "gradient stiffness design" strategy to prepare a kind of carbon nanotube sponge with a stiffness difference of up to 254 times between different layers, but still maintaining an integral conductive network without delamination. This gradient stiffness structure sponge shows prominent sensing properties with ultra-broad range (from 0.0022 MPa to 5.47 MPa) and high sensitivity. The low stiffness layer can detect low stress (0.0022 MPa) with high sensitivity of 0.765 MPa-1, and the high stiffness layer can greatly extend the sensing range to an unprecedentedly high value (5.47 MPa). It can concisely detect various motions with different stress, from slight clamping of fragile fries by the robot fingers to heavily stomping motions by a 90 kg person. Moreover, a series of human movements from small-scale to large-scale can be also monitored, revealing the great potential of this gradient stiffness structure in future sensing research.

Flame-retardant MXene/polyimide film with outstanding thermal and mechanical properties based on the secondary orientation strategy.

With the development of multifunction and miniaturization in modern electronics, polymeric films with strong mechanical performance and high thermal conductivity are urgently needed. Two-dimensional transition metal carbides and nitrides (MXenes) have attracted extensive attention due to their tunable surface chemistry, layered structure and charming properties. However, there are few studies on using MXenes as fillers to enhance polymer properties. In this paper, we fabricate a three-dimensional foam by the freeze-drying method to enhance the interfacial interaction between adjacent MXene sheets and polyimide (PI) macromolecules, and then a composite film with a dense and well-ordered layer-by-layer structure is produced by the hot-pressing process. Based on the secondary orientation strategy, the resultant MXene/PI film exhibits an enhanced thermal conductivity of 5.12 ± 0.37 W m-1 K-1 and tensile strength of 102 ± 3 MPa. Moreover, the composite film has good flexibility and flame retardancy owing to the synergistic effect of MXene sheets and PI chains. Hence, the MXene/PI composite film with the properties of flexibility, flame-retardancy, high mechanical strength and efficient heat transmission is expected to be used as the next thermal management material in a variety of applications.

Artificial muscle with reversible and controllable deformation based on stiffness-variable carbon nanotube spring-like nanocomposite yarn.

Carbon nanotube yarn actuators are in great demand for flexible devices or intelligent applications. Artificial muscles based on carbon nanotube yarn have achieved great progress over past decades. However, uncontrollable, small deformations and relatively slow deformation recovery are still great challenges for carbon nanotube yarn artificial muscles. Here we propose an artificial muscle based on a stiffness-variable carbon nanotube spring-like nanocomposite yarn. This nanocomposite yarn can be fabricated as artificial muscles by directly inflating epoxy resin on spring-like carbon nanotube yarn, and it shows a rapid response, and reversible and controllable deformation. The driving mechanism of the nanocomposite yarn artificial muscle is based on the change in the resin modulus controlled by Joule heat. This novel nanocomposite yarn artificial muscle can work at low voltages (≤0.8 V), and the whole reversible driving process is completed within 5 seconds (the deformation recovery process is about 2 seconds). The strain of the nanocomposite yarn artificial muscle is controlled by applied voltages, and the maximum strain can reach more than 12%. The novel nanocomposite yarn artificial muscle can produce output forces more than 20 times higher than human skeletal muscle. This CNT nanocomposite yarn artificial muscle with a spiral structure shows potential applications for actuators, sensors and micro robots.