Electrically responsive ionic soft actuators that can exhibit large bending strain under low electrical input power are promising candidates for future soft electronics and wearable devices. However, some drawbacks such as low blocking force, slow response time, and poor durability should be overcome for practical engineering applications. Herein, this study reports defectengineered 3D graphitic carbon nitride (GCN) and nitrogen-doped graphene (NG) hetero-nanostructure that were developed by one-pot hydrothermal method in order to design functionally antagonistic hybrid electrodes for superior ionic soft actuators. While NG facilitates rapid electron transfer in 3D networked nanoarchitectures, the enriched-nitrogen content in GCN provides good wettability and mechanical resiliency with poly(3,4 ethylenedioxythiophene) polystyrene sulfonate (PEDOT:PSS). The 3D hybrid nanostructures generate unimpeded ion channels and sufficient contact area with the electrolyte membrane to provide higher capacitance and mechanical integrity, which are critical prerequisites for high-performance actuation. The developed soft actuator based on the nitrogen-enriched 3D hetero-nanostructure is found to exhibit large bending strain (0.52%), wide frequency response, 5 h durability (93% retention), 2.4 times higher bending displacement, and twofold higher electromechanical efficiency compared to PEDOT:PSS under ±0.5 V input voltage. Such 3D functionally antagonistic hybrid electrodes offer hitherto unavailable opportunities in developing ultralow voltage-driven ionic actuators for the next-generation soft electronics.

More than the sum of the parts: The property of a supramolecular material can differ significantly from those of the constituent materials. Two organic components, which are nonconductive, nonphotochromic, and nonluminescent, were shown to self‐assemble by cation–π, π–π, and carboxylate–pyridinium interactions. An organic semiconductor is thus produced with significant charge mobility and photochromic and photoluminescence properties.

In this study, high-performance ionic soft actuators are developed for the first time using collectively exhaustive boron and sulfur co-doped porous carbon electrodes (BS-COF-Cs), derived from thiophene-based boronatelinked covalent organic framework (T-COF) as a template. The one-electron deficiency of boron compared to carbon leads to the generation of hole charge carriers, while sulfur, owing to its high electron density, creates electron carriers in BS-COF-C electrodes. This antagonistic functionality of BS-COF-C electrodes assists the charge-transfer rate, leading to fast charge separation in the developed ionic soft actuator under alternating current input signals. Furthermore, the hierarchical porosity, high surface area, and synergistic effect of co-doping of the BS-COF-Cs play crucial roles in offering effective interaction of BS-COF-Cs with poly(3,4-ethylenedioxythiophene) polystyrene sulfonate (PEDOT:PSS), leading to the generation of high electro-chemomechanical performance of the corresponding composite electrodes. Finally, the developed ionic soft actuator based on the BS-COF-C electrode exhibits large bending strain (0.62%), excellent durability (90% retention for 6 hours under operation), and 2.7 times higher bending displacement than PEDOT:PSS under extremely low harmonic input of 0.5 V. This study reveals that the antagonistic functionality of heteroatom co-doped electrodes plays a crucial role in accelerating the actuation performance of ionic artificial muscles.

A highly compressible, conductive nitrogen and sulfur co-doped holey graphene aerogel (NS-HGA) is developed for structurally resilient solid-state supercapacitors under high compressions.

Electroactive soft actuators and bioinspired artificial muscles have received burgeoning interest as essential components in future electronic devices such as soft haptic‐feedback systems, human‐friendly wearable electronics, and active biomedical devices. However, important challenging issues including fast response time, ultralow input power, robust operation in harsh environments, high‐resolution controllability, and cost‐effectiveness remain to be resolved for more practical applications. Here, an electroionic antagonistic artificial muscle is reported based on hierarchically porous nitrogen‐doped carbon (HPNC) electrodes derived from a microporous poly(triazine‐triptycene) organic framework (PtztpOF). The HPNC, which exhibits hierarchically micro‐ and mesoporous structures, high specific capacitance of 330 F g−1 in aqueous solution, large specific surface area of 830.46 m2 g−1, and graphitic nitrogen doping, offers high electrical conductivity of 0.073 MS m−1 and outstanding volumetric capacitance of 10.4 MF m−3. Furthermore, it is demonstrated that a novel electroionic antagonistic muscle based on HPNC electrodes successfully displays extremely reliable and large bending deformations and long‐term durability under ultralow input voltages. Therefore, microporous polymer or covalent organic frameworks can be applied to provide significant improvements in electroactive artificial muscles, which can play key roles as technological advances toward bioinspired actuating devices required for next‐generation soft and wearable electronics.

In this study, three novel luminescent nanofibrous metal-organic gels (MOGs) have been synthesized by the reaction of 1,3,5-tris(3-pyridylmethoxyl)benzene (L) with chloride salts of Cd(II), Hg(II), and Cu(II). The metal-ligand coordination, intermolecular π-π stacking and several other weak interactions found to play an important role in the formation of nanofibrous materials. The gel materials are characterized by rheology, diffuse reflectance spectra and various microscopic techniques such as TEM, FESEM, and AFM. The gels MOG-1 and MOG-2 were found to exhibit significant white photoluminescence, whereas the MOG-3 exhbits green emission upon excitation at 325 nm. Furthermore, the MOG-1 has shown its application as a chemosensor for the remarkable detection of nitroaromatics such as nitrobenzene (NB), 2,4-dinitrophenol (DNP). The significant quenching response for NB and DNP is attributed to the strong charge-transfer interactions between the electron-deficient aromatic ring of NB and the electron rich aromatic group of L in MOG-1. The crystal structure of Cd(II) complex of L reveals the formation one-dimensional network which contains strong π-π interactions within and between the networks and these strong π-π interactions generate the free charge carrier in all these nanofibrous gels.

To achieve large bending displacement and fast response time under ultralow input voltages, as well as improved durability, advanced high‐performance ionic actuators still face crucial design challenges that must be resolved. Here, hierarchically porous and unzipped graphitic nanoribbons anchored on graphene as an efficient electrode material for high‐performance electroionic artificial muscles are reported. Using controlled solvothermal and pyrolysis methods, nanoarchitectured carbon is derived from a self‐templated potassium‐based metal–organic frameworks–graphene hybrid. The newly designed ionic actuator demonstrates excellent actuation performance, including large bending displacement (17.4 mm) and a strain difference of 0.51% at 0.5 V AC input, very fast response time (700 ms) at 0.5 V DC input, wide frequency response (0.1–15 Hz), and excellent cycling stability (92%) after 25 000 cycles without any delamination of electrodes under continuous electrical operation. The breakthrough in actuation performance mainly stems from the unzipping of hollow nanorods to hierarchical porous graphitic nanoribbons anchored on graphene with the enlarged surface area, large pore volume, stronger mechanical integrity, and emerging charge storage and transport ability. Further, the electroionic actuator shows promise when applied in the demonstration of a biomimicking Venus flytrap.

The cocrystallization reactions of 2,2 0 ,6,6 0 -tetracarboxybiphenyl with bis(4-pyridyl) ethylene and 4,4 0 -bipyridine were studied, and it was found that molecular symmetry (pseudo-S 4 ) has been transferred into supramolecular symmetry to form an 8-fold interpenetrated diamondoid network only in the case of cocrystals but not in the case of salts.