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tissues could be organized into a helical assembly, [4][5][6] showing remarkable photonic properties and attractive structural anisotropy. The advantages of cellulosic sustainability and biocompatibility make it superior to other photonic materials to produce optical materials. Bioinspired cellulose's multiscale architecture has implemented a series of photonic building blocks, mainly including hydroxypropyl cellulose, [7] ethylcellulose, [8] and cellulose nanocrystal (CNC). [9,10] Among them, the self-assembly of CNCs into chiral photonic structures is the most representative. An artistic view (Figure 1a) shows a solid film formed by the selfassembly of CNCs, which is similar to the Bouligand structure of the beetle exoskeleton. [11,12] CNCs consist of each chain of β-(poly-1,4-D-glucose) stabilized via hydrogen bonds and hydrophobic interactions that provide mechanical stiffness to the solid film. [13] CNC-derived photonic materials have spawned a series of exciting applications in the fields of sensors, [14,15] optics, [16,17] electronics, [18] and engineering. [19,20] However, in many cases, the above materials rarely undergo elastic deformation but crack in bending, thus compromising their outstanding properties. In addition, the photonic structures of these materials are incompatible with humid and liquid environments because of their high hygroscopicity and water solubility.Cellulose nanocrystals (CNCs)-derived photonic materials have confirmed great potential in producing renewable optical and engineering areas. However, it remains challenging to simultaneously possess toughness, strength, and multi ple responses for developing high-performance sensors, intelligent coatings, flexible textiles, and multifunctional devices. Herein, the authors report a facile and robust strategy that poly(ethylene glycol) dimethacrylate (PEGDMA) can be converged into the chiral nematic structure of CNCs by ultraviolet-triggered free radical polymerization in an N,N-dimethylformamide solvent system. The resulting CNC-poly(PEGDMA) composite exhibits impressive strength (42 MPa), stretchability (104%), toughness (31 MJ m −3 ), and solvent resistance. Notably, it preserves vivid optical iridescence, displaying stretchable variation from red, yellow, to green responding to the applied mechanical stimuli. More interestingly, upon exposure to spraying moisture, it executes sensitive actuation (4.6° s −1 ) and multiple complex 3D deformation behaviors, accompanied by synergistic iridescent appearances. Due to its structural anisotropy of CNC with typical left-handedness, the actuation shows the capability to generate a high probability (63%) of right-handed helical shapes, mimicking a coiled tendril. The authors envision that this versatile system with sustainability, robustness, mechanochromism, and specific actuating ability will open a sustainable avenue in mechanical sensors, stretchable optics, intelligent actuators, and soft robots.The ORCID identification number(s) for the author(s) of this article can be found under https:/...

Cellulose nanocrystals (CNCs) are powerful photonic building blocks for the fabrication of biosourced colored films. A combination of the advantages of self-assembled CNCs and multiple templating agents offers access to the development of novel physicochemical sensors, structural coatings, and optic devices. However, due to the inherent brittleness and water instability of CNCderived materials, their further applications are widely questionable and restrictive. Here, a soft polymer of poly(vinyl alcohol) (PVA) was introduced into the rigid CNC system to balance molecular interactions, whereafter two hard/soft nanocomposites were fastened through a cross-linking reaction of glutaraldehyde (GA), resulting in a highly flexible, water-stable, and chiral nematic CNC composite film through an evaporation-induced self-assembly technique. For a 1.5 wt % GA-cross-linked 70 wt % CNC loading film, its treatment with harsh hydrophilic exposure (soaking in a strong acid, strong base, and seawater) and various organic solvents show exceptional solvent-resistant abilities. Furthermore, the film can even withstand a weight of 167 g cm −2 without failure, which is a highly stiff and durable character. Importantly, the film remains a highly ordered chiral nematic organization, being able to act as a highly transparent substrate for selective reflection of left-handed circularly polarized light, preparing fully covered and patterned full-color coatings on various substrates. Our work paves the way for applications in low-cost, durable, and photonic cellulosic coatings.

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Directional transport of liquid droplets is crucial for various applications including water harvesting, anti-icing, and condensation heat transfer. Here, bouncing of water droplets with patterned superhydrophobic surfaces composed of circular equidistant grooves was studied. The directional transport of droplets toward the pole of the grooves was observed. The impact of the Weber number, initial polar distance r, and geometrical parameters of the surface on the directional droplet bouncing was experimentally explored. The nature of bouncing was switched when the Weber numbers exceeded We ≅ 20−25. The rebouncing height was slightly dependent on the initial polar coordinate of the impact point for a fixed We, whereas it grew for We > 20. The weak dependence of the droplet spreading time on the Weber number was close to the dependence predicted by the Hertz bouncing, thus evidencing the negligible influence of viscosity in the process. Change in the scaling exponent describing the dependence of the normalized spreading time on the Weber number was registered for We ≅ 25. The universal dependence of the offset distance ΔL of the droplets on the Weber number ΔL/D 0 ∼ We 1.5 was established. The normalized offset distance decreased with the normalized initial polar distance as ΔL/D 0 ∼ (r/S) −1 , where D 0 and S are the droplet diameter and groove width, respectively. This research may yield more insights into droplet bouncing on patterned surfaces and offer more options in directed droplet transportation.

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The reactivity of a ceria-rich Ce0.85Zr0.15O2 solid solution towards the thermochemical water splitting process (TWS) was studied over repeated H2/H2O redox cycles. The structural and surface modifications after treatment at high temperature under air or N2 atmospheres were characterized by High-Resolution Transmission Electron Microscopy (HRTEM), X-ray diffraction (XRD), Raman spectroscopy, X-ray Photoemission Spectroscopy (XPS) and Positron Annihilation Lifetime Spectroscopy (PALS). Samples treated under nitrogen resulted more active due to phase segregation with formation of a zirconyl oxynitride phase in catalytic amount. Insertion of N 3into the structure contributes to increase the numbers of oxygen vacancies that preferably arrange in large clusters, and to stabilize Ce 3+ centers on the surface. In comparison, treatment under air resulted in a different arrangement of defects with less Ce 3+ and smaller and more numerous vacancy clusters. This affects charge transfer and H-coupling processes, that play an important role in boosting the rate of H2 production. The behavior is found to be only slightly dependent on the starting ceria-zirconia composition and it is related to the development of a similar surface hetero-structure configuration, characterized by the presence of at least a ceria-rich solid solution and a (cerium-doped) zirconyl oxynitride phase, which is supposed to act as a promoter for TWS reaction. The above findings confirm the importance of a multi-phase structure in the design of ceria-zirconia oxides for water splitting reaction and allow a step forward to find an optimal composition. Moreover, the results indicate that doping with nitrogen might be a novel approach for the design of robust, thermally resistant and redox active materials. All these findings suggest new approaches for the development and design of ceria based materials for the two-step water splitting reaction and highlight the importance of engineering the surface defect structure/configuration of the material to obtain an efficient catalyst. In this regard, the role and the impact of nitridation process need to be further investigated.

Designing intelligent slippery surfaces for droplet manipulation is critical for many applications from drug delivery to bio‐analysis, while is of great challenging in sustainability for inescapable wastage of lubricant layer. Herein, an ultrafast lubricant self‐mediating (self‐replenishing/‐absorbing) photothermal slippery surface is designed that achieves sustainable transport of droplet under the irradiation of near infrared light (NIL) even if the lubricant layer is wiped clean completely, as well as at other man‐made extreme conditions. The ultrafast lubricant self‐mediating performance is caused by synergistic effects of interconnection of porous structure and photothermal expansion of the material. When lubricant on surface is lost, photothermal expansion of material can quickly squeeze the lubricant inside the base to flow into and out of the interconnected porous structure to generate a fresh lubricant layer. Attractively, when the NIL is turned off, the rebuilt lubricant layer can be swiftly self‐absorbed into the porous to inhibit unnecessary wastage. Moreover, an arbitrary split of droplet in desired configurations can be achieved by controlling the NIL irradiating route. This sustainable droplet manipulation induced by ultrafast lubricant self‐mediating can be extensively applied in microfluidics and micro‐reactor settings.