Adaptive nanotube networks enabling omnidirectionally deformable electro-driven liquid crystal elastomers towards artificial muscles.

Artificial muscles that can convert electrical energy into mechanical energy promise broad scientific and technological applications. However, existing electro-driven artificial muscles have been plagued with problems that hinder their practical applications: large electro-mechanical attenuation during deformation, high-driving voltages, small actuation strain, and low power density. Here, we design and create novel electro-thermal-driven artificial muscles rationally composited by hierarchically structured carbon nanotube (HS-CNT) networks and liquid crystal elastomers (LCEs), which possess adaptive sandwiched nanotube networks with angulated-scissor-like microstructures, thus effectively addressing above problems. These HS-CNT/LCE artificial muscles demonstrate not only large strain (>40%), but also remarkable conductive robustness (R/R0 < 1.03 under actuation), excellent Joule heating efficiency (≈ 233 °C at 4 V), and high load-bearing capacity (R/R0 < 1.15 at 4000 times its weight loaded). In addition, our artificial muscles exhibit real-muscle-like morphing intelligence that enables preventing mechanical damage in response to excessively heavyweight loading. These high-performance artificial muscles uniquely combining omnidirectional stretchability, robust electrothermal actuation, low driving voltage, and powerful mechanical output would exert significant technological impacts on engineering applications such as soft robotics and wearable flexible electronics.

Stabilizing Diluted Active Sites of Ultrasmall High-Entropy Intermetallics for Efficient Formic Acid Electrooxidation.

The poisoning of undesired intermediates or impurities greatly hinders the catalytic performances of noble metal-based catalysts. Herein, high-entropy intermetallics i-(PtPdIrRu)2FeCu (HEI) are constructed to inhibit the strongly adsorbed carbon monoxide intermediates (CO*) during the formic acid oxidation reaction. As probed by multiple-scaled structural characterizations, HEI nanoparticles are featured with partially negative Pt oxidation states, diluted Pt/Pd/Ir/Ru atomic sites and ultrasmall average size less than 2 nm. Benefiting from the optimized structures, HEI nanoparticles deliver more than 10 times promotion in intrinsic activity than that of pure Pt, and well-enhanced mass activity/durability than that of ternary i-Pt2FeCu intermetallics counterpart. In situ infrared spectroscopy manifests that both bridge and top CO* are favored on pure Pt but limited on HEI. Further theoretical elaboration indicates that HEI displayed a much weaker binding of CO* on Pt sites and sluggish diffusion of CO* among different sites, in contrast to pure Pt that CO* bound more strongly and was easy to diffuse on larger Pt atomic ensembles. This work verifies that HEIs are promising catalysts via integrating the merits of intermetallics and high-entropy alloys.

Improving Alkaline Hydrogen Oxidation through Dynamic Lattice Hydrogen Migration in Pd@Pt Core-Shell Electrocatalysts.

Tracking the trajectory of hydrogen intermediates during hydrogen electro-catalysis is beneficial for designing synergetic multi-component catalysts with division of chemical labor. Herein, we demonstrate a novel dynamic lattice hydrogen (LH) migration mechanism that leads to two orders of magnitude increase in the alkaline hydrogen oxidation reaction (HOR) activity on Pd@Pt over pure Pd, even ≈31.8 times mass activity enhancement than commercial Pt. Specifically, the polarization-driven electrochemical hydrogenation process from Pd@Pt to PdHx @Pt by incorporating LH allows more surface vacancy Pt sites to increase the surface H coverage. The inverse dehydrogenation process makes PdHx as an H reservoir, providing LH migrates to the surface of Pt and participates in the HOR. Meanwhile, the formation of PdHx induces electronic effect, lowering the energy barrier of rate-determining Volmer step, thus resulting in the HOR kinetics on Pd@Pt being proportional to the LH concentration in the in situ formed PdHx @Pt. Moreover, this dynamic catalysis mechanism would open up the catalysts scope for hydrogen electro-catalysis.

Cooperative Ni(Co)-Ru-P Sites Activate Dehydrogenation for Hydrazine Oxidation Assisting Self-powered H2 Production.

Water electrolysis for H2 production is restricted by the sluggish oxygen evolution reaction (OER). Using the thermodynamically more favorable hydrazine oxidation reaction (HzOR) to replace OER has attracted ever-growing attention. Herein, we report a twisted NiCoP nanowire array immobilized with Ru single atoms (Ru1 -NiCoP) as superior bifunctional electrocatalyst toward both HzOR and hydrogen evolution reaction (HER), realizing an ultralow working potential of -60 mV and overpotential of 32 mV for a current density of 10 mA cm-2 , respectively. Inspiringly, two-electrode electrolyzer based on overall hydrazine splitting (OHzS) demonstrates outstanding activity with a record-high current density of 522 mA cm-2 at cell voltage of 0.3 V. DFT calculations elucidate the cooperative Ni(Co)-Ru-P sites in Ru1 -NiCoP optimize H* adsorption, and enhance adsorption of *N2 H2 to significantly lower the energy barrier for hydrazine dehydrogenation. Moreover, a self-powered H2 production system utilizing OHzS device driven by direct hydrazine fuel cell (DHzFC) achieve a satisfactory rate of 24.0 mol h-1 m-2 .

Pseudo-Pt Monolayer for Robust Hydrogen Oxidation.

Heteroepitaxial core-shell structure is conducive to combining the advantages of the epilayer and the substrate, creating a novel multifunctionality for catalysis application. Herein, we report a pseudomorphic-Pt atomic layer (PmPt) epitaxially growing on an IrPd-core matrix (PmPt@IrPd/C) as an efficient and stable catalyst for alkaline hydrogen oxidation reaction that exhibits ∼29.2 times more mass activity enhancement than that of benchmark Pt/C. The PmPt@IrPd/C catalyst also gives rise to ∼25.0 times more enhancement than Pt/C during a 50,000-cycle accelerated stability test. This robust stability originates from the resistance to carbon corrosion owing to the stronger H2O interaction instead of carbon oxide (COx) poison species, and the modulated hydroxyl (OH*) adsorption could inhibit the OH* species from shuffling the surface Pt atoms away from the substrate. Moreover, the anion-exchange membrane fuel cells assembled by PmPt@IrPd/C with an ultralow Pt loading of 0.009 mgPt cm-2 in the anode can deliver a power density of 1.27 W cm-2.

Photomorphogenesis of Diverse Autonomous Traveling Waves in a Monolithic Soft Artificial Muscle.

Biological organisms (e.g., batoid fish, etc.) possess the remarkable ability to morph their soft, sheet-like tissues into wavy morphologies and self-oscillate to make traveling waves, enabling myriad functionalities in propulsion, locomotion, and transportation. In contrast, current manmade soft robotic systems cannot adaptively make wavy morphologies and concurrently achieve wave propagation because the controllable actuation of desired 3D morphologies in entirely soft materials is a formidable challenge due to their continuously deformable bodies that own a large number of actuable degrees of freedom. Here, we report a bioinspired robotic system that not only allows photomorphogenesis of on-demand 3D wavy morphologies but also enables autonomous wave propagation in a monolithic soft artificial muscle (MSAM). This system employs a conceptually different design strategy based on a combination of two principles derived from plant morphogenesis and the undulatory motion of ray fish. The former offers a shaping principle based on differential growth that enables morphing MSAM into target wavy configurations, while the latter inspires a driving principle that induces autonomous propagation of shaped waves by rhythmic motor patterns. This waving system can be used as adaptive "soft engines/motors" that enable directional locomotion, intelligent transportation of cargo, and autonomous propulsion. It even produces programmable, complex artificial peristaltic waves. Our design allows controllable formation of 3D wavy morphologies and autonomous wave behaviors in the soft robotic system that would be useful for broad applications in adaptive, self-regulated mechanical systems for advanced robotics, soft machines, and energy harvest.

Reconfigurable Soft Actuators with Multiple-Stimuli Responses.

Multiple-stimuli responsive soft actuators with tunable initial shapes would have substantial potential in broad technological applications, ranging from advanced sensors, smart robots to biomedical devices. However, existing soft actuators are often limited to single initial shape and are unable to reversibly reconfigure into desirable shapes, which severely restricts the multifunctions that can be integrated into one actuator. Here, a novel reconfigurable supramolecular polymer/polyethylene terephthalate (PET) bilayer actuator exhibiting multiple-stimuli responses is presented. In this bilayer actuator, the supramolecular polymer layer constructed of poly(5-Norbornene-2-carboxylic acid-1,3-cyclooctadiene) (PNCCO) and azopyridine derivative (PyAzoPy) via H-bonds provides multiple-stimuli responses: PyAzoPy offers light response and carboxylic groups in PNCCO endow the actuator with humidity response. Meanwhile thermoplastic PET layer enables the bilayer actuators to be reconfigured into various shapes by thermal stimuli. The rationally designed actuators exhibit versatile capabilities to reversibly reconfigure into a set of initial shapes and carry out multiple functions, such as photo-driven "foldback-clip" and Ω-shaped crawling robots. In addition, bio-inspired plants constructed by reconfiguration of such actuators demonstrate reversible multiple-stimuli responses. It is anticipated that these novel actuators with highly tunable geometries and actuation modes would be useful to develop multifunctional devices capable of performing diverse tasks.

Turning Waste into Treasure: Regulating the Oxygen Corrosion on Fe Foam for Efficient Electrocatalysis.

Iron corrosion causes a great damage to the economy due to the function attenuation of iron-based devices. However, the corrosion products can be used as active materials for some electrocatalytic reactions, such as oxygen evolution reaction (OER). Herein, the oxygen corrosion on Fe foams (FF) to synthesize effective self-supporting electrocatalysts for OER, leading to "turning waste into treasure," is regulated. A dual chloride aqueous system of "NaCl-NiCl2 " is employed to tailor the structures and OER properties of corrosion layers. The corrosion behaviors identify that Cl- anions serve as accelerators for oxygen corrosion, while Ni2+ cations guarantee the uniform growth of corrosion layers owing to the appeared chemical plating. The synergistic effect of "NaCl-NiCl2 " generates one of the highest OER activities that only an overpotential of 212 mV is required to achieve 100 mA cm-2 in 1.0 m KOH solution. The as-prepared catalyst also exhibits excellent durability over 168 h (one week) at 100 mA cm-2 and promising application for overall water splitting. Specially, a large self-supporting electrode (9 × 10 cm2 ) is successfully synthesized via this cost-effective and easily scale-up approach. By combining with corrosion science, this work provides a significant stepping stone in exploring high-performance OER electrocatalysts.

Hierarchical Bimetallic Ni-Co-P Microflowers with Ultrathin Nanosheet Arrays for Efficient Hydrogen Evolution Reaction over All pH Values.

Designing efficient nonprecious catalysts with pH-universal hydrogen evolution reaction (HER) performance is of importance for boosting water splitting. Herein, a self-template strategy based on Ni-Co-glycerates is developed to prepare bimetallic Ni-Co-P microflowers with ultrathin nanosheet arrays. The highly porous core-shell structure gives rise to affluent mass transfer channels and availably prevents the aggregation of nanosheets, while the ultrathin nanosheets are favorable for producing abundant active sites. Besides, the produced CoP/NiCoP heterostructure in the bimetallic Ni-Co-P catalyst has excellent HER performance in a wide pH range. The as-prepared catalyst shows low potentials of 90, 157, and 121 mV to deliver a current density of 10 mA cm-2 in 0.5 M H2SO4, 0.5 M PBS, and 1 M KOH solution, respectively. Meanwhile, negligible overpotential decay is achieved in the polarization curves after a long-term stability determination. This work supplies a promising strategy for developing pH-universal HER electrocatalysts based on solid-state metal alkoxides.

Optimizing PtFe intermetallics for oxygen reduction reaction: from DFT screening to in situ XAFS characterization.

Rational designing of catalysts to promote the sluggish kinetics of the cathode oxygen reduction reaction in proton exchange membrane fuel cells is still challenging, yet of crucial importance to its commercial application. In this work, on the basis of theoretical DFT calculations which suggest that order structured fct-phased PtFe (O-PtFe) with an atomic Pt shell exhibits superior electrocatalytic performance towards the ORR, the desired structure was prepared by using a scalable impregnation-reduction method. The as-prepared O-PtFe delivered enhanced activity (0.68 A mg-1Pt) and stability (73% activity retention after 10 000 potential cycles) compared with the corresponding disordered PtFe alloy (D-PtFe) and Pt. To confirm the excellent durability, in situ X-ray absorption fine structure spectroscopy was conducted to probe the local and electronic structure changes of O-PtFe during 10 000 cycle accelerated durability testing. We hope that this facile synthesis method and the in situ XAFS experiment could be readily adapted to other catalyst systems, facilitating the screening of highly efficient ORR catalysts for fuel cell application.

Facile self-template fabrication of hierarchical nickel-cobalt phosphide hollow nanoflowers with enhanced hydrogen generation performance.

Developing facile methods to construct hierarchical-structured transition metal phosphides is beneficial for achieving high-efficiency hydrogen evolution catalysts. Herein, a self-template strategy of hydrothermal treatment of solid Ni-Co glycerate nanospheres followed by phosphorization is delivered to synthesize hierarchical NiCoP hollow nanoflowers with ultrathin nanosheet assembly. The microstructure of NiCoP can be availably tailored by adjusting the hydrothermal treatment temperature through affecting the hydrolysis process of Ni-Co glycerate nanospheres and the occurred Kirkendall effect. Benefitting from the promoted exposure of active sites and affluent mass diffusion routes, the HER performance of the NiCoP hollow nanoflowers has been obviously enhanced in contrast with the solid NiCoP nanospheres. The fabricated NiCoP hollow nanoflowers yield the current density of 10 mA cm-2 at small overpotentials of 95 and 127 mV in 0.5 mol L-1 H2SO4 and 1.0 mol L-1 KOH solution, respectively. Moreover, the two-electrode alkaline cell assembled with the NiCoP and Ir/C catalysts exhibits sustainable stability for overall water splitting. The work provides a simple but efficient method to regulate the microstructure of transition metal phosphides, which is helpful for achieving high-performance hydrogen evolution catalysts based on solid-state metal alkoxides.

Restricting Growth of Ni3Fe Nanoparticles on Heteroatom-Doped Carbon Nanotube/Graphene Nanosheets as Air-Electrode Electrocatalyst for Zn-Air Battery.

Exploring bifunctional oxygen electrode catalysts with efficient and stable oxygen reduction reaction (ORR)/oxygen evolution reaction (OER) performance is one of the limitations for high-performance zinc-air battery. In this work, Ni3Fe alloy nanoparticles incorporated in three-dimensional (3D) carbon nanotube (CNT)/graphene nanosheet composites with N and S codoping (Ni3Fe/N-S-CNTs) as bifunctional oxygen electrode electrocatalysts for zinc-air battery. The main particle size of Ni3Fe nanoparticles could be well restricted because of the unique 3D structure of carbon nanotube/graphene nanosheet composites (N-S-CNTs). The large specific area of N-S-CNTs is conducive to the uniform dispersion of Ni3Fe nanoparticles. On the basis of the synergistic effect of Ni3Fe nanoparticles with N-S-CNTs, and the sufficient exposure of reactive sites, the synthesized Ni3Fe/N-S-CNTs catalyst exhibits excellent OER performance with a low overpotential of 215 mV at 10 mA cm-2, and efficient ORR activity with a half-wave potential of 0.877 V. When used as an electrocatalyst in zinc-air battery, the device exhibits a power density of 180.0 mW cm-2 and long term durability for 500 h.

A novel method of predicting protein disordered regions based on sequence features.

With a large number of disordered proteins and their important functions discovered, it is highly desired to develop effective methods to computationally predict protein disordered regions. In this study, based on Random Forest (RF), Maximum Relevancy Minimum Redundancy (mRMR), and Incremental Feature Selection (IFS), we developed a new method to predict disordered regions in proteins. The mRMR criterion was used to rank the importance of all candidate features. Finally, top 128 features were selected from the ranked feature list to build the optimal model, including 92 Position Specific Scoring Matrix (PSSM) conservation score features and 36 secondary structure features. As a result, Matthews correlation coefficient (MCC) of 0.3895 was achieved on the training set by 10-fold cross-validation. On the basis of predicting results for each query sequence by using the method, we used the scanning and modification strategy to improve the performance. The accuracy (ACC) and MCC were increased by 4% and almost 0.2%, respectively, compared with other three popular predictors: DISOPRED, DISOclust, and OnD-CRF. The selected features may shed some light on the understanding of the formation mechanism of disordered structures, providing guidelines for experimental validation.