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Hybridization of low-dimensional components with diverse geometrical dimensions should offer an opportunity for the discovery of synergistic nanocomposite structures. In this regard, how to establish a reliable interfacial interaction is the key requirement for the successful integration of geometrically different components. Here, we present 1D/2D heterodimensional hybrids via dopant induced hybridization of 2D Ti3C2TxMXene with 1D nitrogen-doped graphene nanoribbon. Edge abundant nanoribbon structures allow a high level nitrogen doping (∼6.8 at%), desirable for the strong coordination interaction with Ti3C2TxMXene surface. For piezoresistive pressure sensor application, strong adhesion between the conductive layers and at the conductive layer/elastomer interface significantly diminishes the sensing hysteresis down to 1.33% and enhances the sensing stability up to 10 000 cycles at high pressure (100 kPa). Moreover, large-area pressure sensor array reveals a high potential for smart seat cushion-based posture monitoring application with high accuracy (>95%) by exploiting machine learning algorithm.

An effective pathway to build macroscopic scale functional architectures bearing diverse structural dimensions is one of the critical challenges in the two-dimensional (2D) MXene research area. Unfortunately, assembling MXene without adhesive binder is largely limited due to its innate brittle nature and the relatively weak inter-flake van der Waals contact, in contrast to other mechanically compliant 2D materials such as graphene. Herein, an electrochemical self-assembly of pure Ti3C2TxMXenes is presented for functional multidimensional MXene structures, effectively driven by layer-by-layer spontaneous interfacial reduction at metal template surfaces and subsequent defunctionalization. A three-dimensional open porous aerogel as well as 2D highly stacked thin film structures could be readily obtained in this approach, along with largely enhanced electrical properties induced by spontaneous removal of charge-trapping oxygen functional groups. Accordingly, supercapacitors and electromagnetic interference shielding films based on the multidimensional assembly demonstrate excellent performances.

Two-dimensional (2D) MXene has shown enormous potential in scientific fields, including energy storage and electromagnetic interference (EMI) shielding. Unfortunately, MXene-based material structures generally suffer from mechanical fragility and vulnerability to oxidation. Herein, mussel-inspired dopamine successfully addresses those weaknesses by improving interflake interaction and ordering in MXene assembled films. Dopamine undergoes in situpolymerization and binding at MXene flake surfaces by spontaneous interfacial charge transfer, yielding an ultrathin adhesive layer. Resultant nanocomposites with highly aligned tight layer structures achieve approximately seven times enhanced tensile strength with a simultaneous increase of elongation. Ambient stability of MXene films is also greatly improved by the effective screening of oxygen and moisture. Interestingly, angstrom thick polydopamine further promotes the innate high electrical conductivity and excellent EMI shielding properties of MXene films. This synergistic concurrent enhancement of physical properties proposes MXene/polydopamine hybrids as a general platform for MXene based reliable applications.

We report the geometric and electronic effects of amine (with one lone pair electron) and thiol (with two lone pair electrons) ligands on the structural transformation of Pt55nanoparticles (NPs) by first-principles calculation. Although a cuboctahedral (COh) structure is less stable than an icosahedral (Ih) structure by 1.36 eV for a bare Pt55NP, the activation barrier from the COh to the Ih structure is very high, by 1.97 eV, indicating that it would be difficult to observe the structural evolution of a COh structure to an Ih structure for a bare Pt55NP at ambient temperature. However, with the help of the adsorption of methylamine, the structural evolution from a COh structure to an Ih structure is accomplished by the Mackay transformation. This transformation is driven by a combination of both the external forces resulting from the adsorption of the ligand, which pull out the Pt atoms on the face sites of NPs in a radial direction, and the contraction forces in a tangential direction. As more methylamine is added, the Ih structure is observed to return to the original COh structure owing to the directional orbital hybridization that occurs between the Pt NPs and the methylamine. In contrast, such structural evolutions are not observed in the case of methylthiol because the sulfur (S) in the ligand has two lone pair electrons, leading to two Pt–S bonds. As a result, the radial-directed external force that the NPs experience because of the adsorption of methylthiols is much lower than that found in methylamine-ligated NPs. Furthermore, the adsorption of methylthiol leads to an expansion (not contraction) in the tangential direction, which does not qualify as a Mackay transformation. Thus, the Pt NPs ligated with methylthiol do not have a driving force strong enough to cause structural change. The methylthiol-stabilized Pt NPs retain their initial COh structure despite an abundance of ligand adsorption. From these results, we suggest that the NP structure can be controlled by varying the amount and species of ligands.