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Self-sustained motions are widespread in biological systems by harvesting energy from surrounding environments, which inspire scientists to develop autonomous soft robots. However, most-existing soft robots require dynamic heterogeneous stimuli or complex fabrication with different components. Recently, control of topological geometry has been promising to afford soft robots with physical intelligence and thus life-like motions. Reported here are a series of closed twisted ribbon robots, which exhibit self-sustained flipping and rotation under constant light irradiation. Both Möbius strip and Seifert ribbon robots are devised for the first time by using an identical hydrogel, which responds to light irradiation on either side. Experiment and simulation results indicate that the self-regulated motions of the hydrogel robots are related to fast and reversible response of muscle-like gel, self-shadowing effect, and topology-facilitated refresh of light-exposed regions. The motion speeds and directions of the hydrogel robots can be tuned over a wide range. These closed twisted ribbon hydrogels are further applied to execute specific tasks in aqueous environments, such as collecting plastic balls, climbing a vertical rod, and transporting objects. This work presents new design principle for autonomous hydrogel robots by benefiting from material response and topology geometry, which may be inspirative for the robotics community., (© 2024 Wiley‐VCH GmbH.)

Creatures, such as Venus flytrap and hummingbirds, capable of rapid predation through snap-through transition, provide paradigms for the design of soft actuators and robots with fast actions. However, these artificial "snappers" usually need contact stimulations to trigger the flipping. Reported here is a constrained anisotropic poly(N-isopropylacrylamide) hydrogel showing fast snapping upon light stimulation. This hydrogel is prepared by flow-induced orientation of nanosheets (NSs) within a rectangular tube. The precursor containing gold nanoparticles is immediately exposed to UV light for photopolymerization to fix the ordered structure of NSs. Two ends of the slender gel are clamped to form a buckle with bistability nature, which snaps to the other side upon laser irradiation. Systematic experiments are conducted to investigate the influences of power intensity and irradiation angle of the laser, as well as thickness and buckle height of the gel, on the snapping behaviors. The fast snapping is further used to kick a plastic bead and control the switch state. Furthermore, synergetic or oscillated snapping of the gel with two buckles of opposite directions is realized by inclined irradiation of a laser or horizontal irradiation with two lasers, respectively. Such light-steered snapping of hydrogels should merit designing soft robots, energy harvests, etc., (© 2024 The Authors. Advanced Science published by Wiley‐VCH GmbH.)

Converting poly(ethylene terephthalate) (PET) into metal-organic frameworks (MOFs) has emerged as a promising innovation for upcycling of waste plastics. However, previous solvothermal methods suffer from toxic solvent consumption, long reaction time, high pressure, and high temperature. Herein, a mechanochemical milling strategy was reported to transform waste PET into a series of MOFs with high yields. This strategy had the merits of solvent-free conditions, ambient reaction temperature, short running time, and easy scale-up for large-scale production of MOFs. The as-prepared MOFs exhibited definite crystal structure and porous morphology composed of agglomerated nanoparticles. It was proven that, under mechanochemical milling, PET was firstly decomposed into 1,4-benzenedicarboxylate, which acted as linkers to coordinate with metal ions for forming fragments, followed by the gradual arrangement of fragments into MOFs. This work not only promotes high value-added conversion of waste polyesters but also offers a new opportunity to produce MOFs in a green and scalable manner., (© 2022 Wiley-VCH GmbH.)

Upcycling waste plastics into advanced semiconductor photocatalysts provides a new strategy to reasonably and economically solve the huge amount of waste plastics, which remains challenging. Herein, a carbon nitride-based donor-acceptor (D-A) conjugated copolymer by copolymerization of dicyandiamide and terephthalic acid from discarded polyethylene terephthalate (PET) using Zn(OH) 2 as catalyst and template at 360-440 °C is synthesized. The morphology and structure of the conjugated copolymer are well regulated by the calcination temperature. The resultant conjugated copolymer exhibits merits of high light absorption and low electron-hole recombination probability. Consequently, it works excellently in the persulfate-based advanced oxidation process for visible light-driven photocatalytic degradation of tetracycline. The kinetic constant (3.4 × 10 -2  min -1 ) is 40.5 and 2.3 times that of the conjugated copolymer system and persulfate system, respectively. Furthermore, the reactive species (including •OH, SO 4 •- , •O 2 - , 1 O 2 , and h + ) and degradation intermediates of tetracycline are analyzed to expound its degradation process. This work not only pioneers design guidelines on upcycling of waste plastics in a sustainable manner, but also provides a facile strategy to synthesize carbon nitride-based D-A conjugated copolymers for the efficient activation of persulfate-based advanced oxidation process in wastewater treatment., (© 2022 Wiley-VCH GmbH.)

Upcycling waste plastics (e.g., polyethylene (PE)) into value-added carbon products is regarded as a promising approach to address the increasingly serious waste plastic pollution and simultaneously achieve carbon neutrality. However, developing new carbonization technology routes to promote the oxidation of PE at low temperature and construct the stable cross-linking network remains challenging. Here, a facile carbon-grown-on-carbon strategy is proposed using carbon black (CB) to convert waste PE into core/shell carbon nanoparticles (CN) in high yields at low temperature. The yield of CN remarkably increases when the heating temperature decreases or the dosage of CB increases. The obtained CN displays turbostratic structure and closely aggregated granular morphology with a size of ≈80 nm. It is found that, prior to the oxidation and carbonization of PE, CB forms a 3D network architecture in the PE matrix. More importantly, CB not only catalyzes the partial oxidation of PE to form PE macromolecular radicals and introduce oxygen-containing groups at low temperature in the early stage, but also favors for the construction of a stable cross-linking network in the latter stage. This work offers a facile sustainable strategy for chemical upcycling of PE into value-added carbon products without post-treatments or usage of metallic catalysts., (© 2022 Wiley-VCH GmbH.)