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Two-dimensional (2D) amorphous nanosheets with ultrathin thicknesses have properties that differ from their crystalline counterparts. However, conventional methods for growing 2D materials often produce either crystalline flakes or amorphous nanosheets with an uncontrollable thickness. Here, we report that ultrathin amorphous metal-oxide nanosheets featuring superior flatness can be realized through the molecularly confined topochemical transformation of MXene. Using MXene Ti2CTxas an example, we show that surface modification of Ti2CTxnanosheets with molecular ligands, such as oleylamine (OAm) and oleic acid (OA), not only imparts notable colloidal dispersity to Ti2CTxnanosheets in nonpolar organic solvents but also confines their subsequent oxidation to in-plane configurations. We demonstrate that unlike the drastic oxidation conventionally observed for pristine MXene, hydrophobizing MXene with OAm and OA ligands enables individual Ti2CTxnanosheets to undergo independent oxidation in a nondestructive manner, resulting in amorphous titanium oxide (am-TiO2) nanosheets that faithfully retain the dimension and flatness of pristine MXene. These am-TiO2nanosheets exhibit exceptional activity as substrates for surface-enhanced Raman scattering. Importantly, this molecular confinement strategy can be extended to other MXene materials, providing a versatile approach for synthesizing ultrathin amorphous metal-oxide nanosheets with tailored compositions and functionalities.

On-skin patches that record biopotential and biomechanical signals are essential for wearable healthcare monitoring, clinical treatment, and human–machine interaction. To acquire wearing comfort and high-quality signals, patches with tissue-like softness, elastic recovery, damage tolerance, and robust bioelectronic interface are highly desired yet challenging to achieve. Here, we report a dry epidermal patch made from a supramolecular polymer (SESA) and an in situ transferred carbon nanotubes’ percolation network. The polymer possesses a hybrid structure of copolymerized permanent scaffold permeated by multiple dynamic interactions, which imparts a desired mechanical response transition from elastic recoil to energy dissipation with increased elongation. Such SESA-based patches are soft (Young’s modulus ∼0.1 MPa) and elastic within physiologically relevant strain levels (97% elastic recovery at 50% tensile strain), intrinsically mechanical-electrical damage-resilient (∼90% restoration from damage after 5 min), and interference-immune in dynamic signal acquisition (stretch, underwater, sweat). We demonstrate its versatile physiological sensing applications, including electrocardiogram recording under various disturbances, machine-learning-enabled hand-gesture recognition through electromyogram measurement, subtle radial artery pulse, and drastic knee kinematics sensing. This epidermal patch offers a promising noninvasive, long-duration, and ambulant bioelectronic interfacing with anti-interference robustness.

Hydrogels are promising starting materials for biomimetic soft robots as they are intrinsically soft and hold properties analogous to nature’s organic parts. However, the restrictive mold-casting and post-assembly fabrication alongside mechanical fragility impedes the development of hydrogel-based soft robots. Herein, we harness biocompatible alginate as a rheological modifier to manufacture 3D freeform architectures of both chemically and physically cross-linked hydrogels using the direct-ink-write (DIW) printing. The intrinsically hydrophilic polymer network of alginate allows the preservation of the targeted functions of the host hydrogels, accompanied by enhanced mechanical toughness. The integration of free structures and available functionalities from diversified hydrogel family renders an enriched design platform for bioinspired fluidic and stimulus-activated robotic prototypes from an artificial mobile tentacle, a bioengineered robotic heart with beating–transporting functions, and an artificial tendril with phototropic motion. The design strategy expands the capabilities of hydrogels in realizing geometrical versatility, mechanical tunability, and actuation complexity for biocompatible soft robots.

Scalable assembly of nanocrystals (NCs) into two-dimensional (2D) nanosheets has aroused great interest, yet it remains under-explored. This is because current 2D assembly methods rely mainly on the use of solid– or liquid–air interfaces, which are inherently difficult for upscaling and thus lack practicability. Here, with a microemulsion-based amphiphilic assembly technique, we achieve a fast and scalable preparation of free-standing nanosheets comprising few-layer, tightly packed NCs, namely, quasi-nanosheets (quasi-NSs). Acetic acid, acting as both solvent and surface-treatment agent, is used to render the initially hydrophobic NCs amphiphilic, while simultaneously inducing the interfacial instability right after the assembly of NCs at the emulsion interface to afford quasi-NSs. This amphiphilic assembly method is applicable to a variety of NCs, and multicomponent quasi-NSs are also attainable upon coassembly of different types of NCs. In addition, the structural advantages of quasi-NSs in catalysis are showcased by using NiFe2O4quasi-NSs as electrocatalysts for the oxygen evolution reaction. This work opens a new route for the scalable construction of 2D NC sheets with designated components and functions.

The linear assembly of nanocrystals (NCs) with orientational order presents a significant challenge in the field of colloidal assembly. This study presents an efficient strategy for assembling oleic acid (OAH)-capped, faceted rare earth NCs─such as nanorods, nanoplates, and nanodumbbells─into flexible chain-like superstructures. Remarkably, these NC chains exhibit a high degree of particle orientation even with an interparticle distance reaching up to 15 nm. Central to this oriented assembly method is the facet-selective adsorption of low-molecular-weight polyethylene glycol (PEG), such as PEG-400 (Mn= 400), onto specific facets of NCs. This regioselectivity is achieved by exploiting the lower binding affinity of OAH ligands on the (100) facets of rare earth NCs, enabling facet-specific ligand displacement and subsequent PEG attachment. By adjusting the solvent polarity, the linear assembly of NCs is induced by the solvophobic effect, which simultaneously promotes the formation of hydrogen-bonded PEG supramolecular bridges. These supramolecular bridges effectively connect NCs and exhibit sufficient robustness to maintain the structural integrity of the chains, despite the large interparticle spacing. Notably, even when coassembling different types of NCs, the resulting multicomponent chains still feature highly selective facet-to-facet connections. This work not only introduces a versatile method for fabricating well-aligned linear superstructures but also provides valuable insights into the fundamental principles governing the facet-selective assembly of NCs in solution.

Self-assembled binary nanocrystal superlattices (BNSLs) represent an important class of solid-state materials with potentially designed properties. In pursuit of widening the range of applications for binary superlattice materials, it is desirable to develop scalable assembly methods that enable high-quality BNSLs with tailored compositions, structures, and morphologies. Here, we report the gram-scale assembly of crystalline binary nanocrystal superparticles with high phase purity through an emulsion-based process. The structure of the resulting BNSL colloids can be tuned in a wide range (AB13, AlB2, MgZn2, NaCl, and CaCu5) by varying the size and/or number ratios of the two nanocrystal components. Access to large-scale, phase-pure BNSL colloids offers vast opportunities for investigating their physiochemical properties, as exemplified by AB13-type CoFe2O4–Fe3O4binary superparticles. Our results show that CoFe2O4–Fe3O4binary superparticles not only display enhanced magnetic coupling but also exhibit superior lithium-storage properties. The nonclosed-packed NC packing arrangements of AB13-type binary superparticles are found to play a key role in facilitating lithiation/delithiation kinetics and maintaining structural integrity during repeated cycling. Our work establishes the scalable assembly of high-quality BNSL colloids, which is beneficial for accelerating the exploration of multicomponent nanocrystal superlattices toward various applications.

Despite the recent boom in moisture-enabled electricity generation (MEG), it suffers from fabrication intricacy and materials inadequacy for water and energy harvesting purposes. Moreover, conventional MEGs face challenges in restricted operating humidity, inertness to subtle humidity fluctuations and inability to sustain long-lasting power output under high humidity due to limitations in hydrophilicity and hydration. Here, we exploit a unique oppositely-charged hydrogel heterojunction for electricity and fresh water harvesting from atmospheric air without trade-offs in process simplicity and humidity limits. This anion-cation heterostructure engages two oppositely polarized ions and features a self-regulating ionic gradient for MEG in a dynamically fluctuating ambient, making it not only capable of responding to sluggish and subtle humidity fluctuations but delivering undisrupted power even under extremely wet conditions. Different from other MEGs, moisture can be captured and largely stored in the hydrogel and then released as fresh water. This moisture absorption/desorption, interestingly, is accompanied by electricity generation, indicating a two-in-one strategy to address the water-energy nexus. In such a hydrogel heterojunction, multiple environmental elements like moisture, light, temperature, wind, etc., are feasibly mobilized for energy harvesting. This work provides a promising autonomous and continuous operation of an energy-water system for sustainable and decentralized purposes.

This contribution describes the self-assembly of colloidal nanodumbbells (NDs) with tunable shapes within cylindrical channels. We present that the intrinsic concave geometry of NDs endows them with peculiar packing and interlocking behaviors, which, in conjunction with the adjustable confinement constraint, leads to a variety of superstructures such as tilted-ladder chains and crossed-chain superlattices. A mechanistic investigation, corroborated by geometric calculations, reveals that the phase behavior of NDs under strong confinement can be rationalized by the entropy-driven maximization of the packing efficiency. Based on the experimental results, an empirical phase diagram is generated, which could provide general guidance in the design of intended superstructures from NDs. This study provides essential insight into how the interplay between the particle shape and confinement conditions can be exploited to direct the orientationally ordered assembly of concave nanoparticles into unusual superlattices.