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Activated carbon (AC)-based materials have shown promising performance in carbon capture, offering low cost and sustainable sourcing from abundant natural resources. Despite ACs growing as a new class of materials, theoretical guidelines for evaluating their viability in carbon capture are a crucial research gap. We address this gap by developing a hierarchical guideline, based on fundamental gas-solid interaction strength, that underpins the success and scalability of AC-based materials. The most critical performance indicator is the CO 2 adsorption energy, where an optimal range (-0.41 eV) ensures efficiency between adsorption and desorption. Additionally, we consider thermal stability and defect sensitivity to ensure consistent performance under varying conditions. Further, selectivity and capacity play significant roles due to external variables such as partial pressure of CO 2 and other ambient air gases (N 2 , H 2 O, O 2 ), bridging the gap between theory and reality. We provide actionable examples by narrowing our options to methylamine- and pyridine-grafted graphene.

Perfect graphene is believed to be one of the strongest materials, yet its resistance to fracture is much less impressive. The modest fracture toughness is thought to be related to the general brittle nature in the fracture process of graphene and its two-dimensional (2D) analogous. The brittleness also makes it extremely difficult to assess mechanical properties of 2D materials. The introduction of carbon nanotubes (CNTs) into bulk materials has proven to be a widely accepted method for toughening and strengthening materials. To date, such toughening effect of CNTs on 2D materials is largely unknown. A unique material, rebar graphene, has been synthesized that consists of CNTs embedded in graphene. In this study, by implementing a "dry" transfer technique, the freely suspended rebar graphene was systematically tested under uniaxial tension mode inside a scanning electron microscope. Our combined experiments and molecular dynamics simulations confirm that the embedded CNTs divert and bridge the propagating crack and provide a toughening mechanism for the material. Our work identifies a promising extrinsic toughening strategy for 2D materials and provides mechanistic insights into the fracture process of graphene hybrid material.

Vertically stacked van der Waals heterostructures composed of compositionally different two-dimensional atomic layers give rise to interesting properties due to substantial interactions between the layers. However, these interactions can be easily obscured by the twisting of atomic layers or cross-contamination introduced by transfer processes, rendering their experimental demonstration challenging. Here, we explore the electronic structure and its strain dependence of stacked MoSe2/WSe2 heterostructures directly synthesized by chemical vapor deposition, which unambiguously reveal strong electronic coupling between the atomic layers. The direct and indirect band gaps (1.48 and 1.28 eV) of the heterostructures are measured to be lower than the band gaps of individual MoSe2 (1.50 eV) and WSe2 (1.60 eV) layers. Photoluminescence measurements further show that both the direct and indirect band gaps undergo redshifts with applied tensile strain to the heterostructures, with the change of the indirect gap being particularly more sensitive to strain. This demonstration of strain engineering in van der Waals heterostructures opens a new route toward fabricating flexible electronics.

A solid-liquid self-adaptive composite (SAC) is synthesized using a simple mixing-evaporation protocol, with poly(dimethylsiloxane) (PDMS) and poly(vinylidene fluoride) (PVDF) as active constituents. SAC exists as a porous solid containing a near equivalent distribution of the solid (PVDF)-liquid (PDMS) phases, with the liquid encapsulated and stabilized within a continuous solid network percolating throughout the structure. The pores, liquid, and solid phases form a complex hierarchical structure, which offers both mechanical robustness and a significant structural adaptability under external forces. SAC exhibits attractive self-healing properties during tension, and demonstrates reversible self-stiffening properties under compression with a maximum of 7-fold increase seen in the storage modulus. In a comparison to existing self-healing and self-stiffening materials, SAC offers distinct advantages in the ease of fabrication, high achievable storage modulus, and reversibility. Such materials could provide a new class of adaptive materials system with multifunctionality, tunability, and scale-up potentials.

The practical recycling of carbon dioxide (CO2) by the electrochemical reduction route requires an active, stable, and affordable catalyst system. Although noble metals such as gold and silver have been demonstrated to reduce CO2 into carbon monoxide (CO) efficiently, they suffer from poor durability and scarcity. Here we report three-dimensional (3D) graphene foam incorporated with nitrogen defects as a metal-free catalyst for CO2 reduction. The nitrogen-doped 3D graphene foam requires negligible onset overpotential (-0.19 V) for CO formation, and it exhibits superior activity over Au and Ag, achieving similar maximum Faradaic efficiency for CO production (∼85%) at a lower overpotential (-0.47 V) and better stability for at least 5 h. The dependence of catalytic activity on N-defect structures is unraveled by systematic experimental investigations. Indeed, the density functional theory calculations confirm pyridinic N as the most active site for CO2 reduction, consistent with experimental results.

Large-scale suspended architectures of various two-dimensional (2D) materials (MoS2, MoSe2, WS2, and graphene) are demonstrated on nanoscale patterned substrates with different physical and chemical surface properties, such as flexible polymer substrates (polydimethylsiloxane), rigid Si substrates, and rigid metal substrates (Au/Ag). This transfer method represents a generic, fast, clean, and scalable technique to suspend 2D atomic layers. The underlying principle behind this approach, which employs a capillary-force-free wet-contact printing method, was studied by characterizing the nanoscale solid-liquid-vapor interface of 2D layers with respect to different substrates. As a proof-of-concept, a photodetector of suspended MoS2 has been demonstrated with significantly improved photosensitivity. This strategy could be extended to several other 2D material systems and open the pathway toward better optoelectronic and nanoelectromechnical systems.

Exfoliation of two-dimensional (2D) materials into mono- or few layers is of significance for both fundamental studies and potential applications. In this report, for the first time surface tension components were directly probed and matched to predict solvents with effective liquid phase exfoliation (LPE) capability for 2D materials such as graphene, h-BN, WS2, MoS2, MoSe2, Bi2Se3, TaS2, and SnS2. Exfoliation efficiency is enhanced when the ratios of the surface tension components of the applied solvent is close to that of the 2D material in question. We enlarged the library of low-toxic and common solvents for LPE. Our study provides distinctive insight into LPE and has pioneered a rational strategy for LPE of 2D materials with high yield.

The nitrogen-doped graphene (NG) with dominance of the pyridinic-N configuration is synthesized via a straightforward process including chemical vapor deposition (CVD) growth of graphene and postdoping with a solid nitrogen precursor of graphitic C3N4 at elevated temperature. The NG fabricated from CVD-grown graphene contains a high N content up to 6.5 at. % when postdoped at 800 °C but maintains high crystalline quality of graphene. The obtained NG exhibits high activity, long-standing stability, and outstanding crossover resistance for electrocatalysis of oxygen reduction reaction (ORR) in alkaline medium. The NG treated at 800 °C shows the best ORR performance. Further study of the dependence of ORR activity on different N functional groups in these metal-free NG electrodes provides deeper insights into the origin of ORR activity. Our results reveal that the pyridinic-N tends to be the most active N functional group to facilitate ORR at low overpotential via a four-electron pathway.

We report the observation of remarkable water molecule-induced stiffening in ZnO nanobelts using atomic force microscopy three-point bending test. It was found that the elastic modulus of ZnO nanobelts could increase significantly from 40 GPa under ambient condition up to 88 GPa at the relative humidity level of 80%. The physical mechanism for this phenomenon was explained in terms of increasing surface stress induced by water molecule adsorption on ZnO nanobelt surface. Our first-principles density functional theory calculations revealed that the water molecules adsorbed on the ZnO surface would attract surface Zn atoms to move outward and hence increase the value of surface stress of ZnO surface.