Molecular Dynamics of Catalyst-Free Edge Elongation of Boron Nitride Nanotubes Coaxially Grown on Single-Walled Carbon Nanotubes.

Recent advances in low-dimensional materials have enabled the synthesis of single-walled carbon nanotubes encapsulated in hexagonal boron nitride (BN) nanotubes (SWCNT@BNNT), creating one-dimensional van der Waals (vdW) heterostructures. However, controlling the quality and crystallinity of BNNT on the surface of SWCNTs using chemical vapor deposition (CVD) remains a challenge. To better understand the growth mechanism of the BNNT in SWCNT@BNNT, we conducted molecular dynamics (MD) simulations using empirical potentials.

Nondestructive flash cathode recycling.

Effective recycling of end-of-life Li-ion batteries (LIBs) is essential due to continuous accumulation of battery waste and gradual depletion of battery metal resources. The present closed-loop solutions include destructive conversion to metal compounds, by destroying the entire three-dimensional morphology of the cathode through continuous thermal treatment or harsh wet extraction methods, and direct regeneration by lithium replenishment. Here, we report a solvent- and water-free flash Joule heating (FJH) method combined with magnetic separation to restore fresh cathodes from waste cathodes, followed by solid-state relithiation.

Synthesis Landscapes for Ammonia Borane Chemical Vapor Deposition of -BN and BNNT: Unraveling Reactions and Intermediates from First-Principles.

Planar hexagonal boron nitride (-BN) and tubular BN nanotube (BNNT), known for their superior mechanical and thermal properties, as well as wide electronic band gap, hold great potential for nanoelectronic and optoelectronic devices. Chemical vapor deposition has demonstrated the best way to scalable synthesis of high-quality BN nanomaterials. Yet, the atomistic understanding of reactions from precursors to product-material remains elusive, posing challenges for experimental design.

Battery metal recycling by flash Joule heating.

The staggering accumulation of end-of-life lithium-ion batteries (LIBs) and the growing scarcity of battery metal sources have triggered an urgent call for an effective recycling strategy. However, it is challenging to reclaim these metals with both high efficiency and low environmental footprint. We use here a pulsed dc flash Joule heating (FJH) strategy that heats the black mass, the combined anode and cathode, to >2100 kelvin within seconds, leading to ~1000-fold increase in subsequent leaching kinetics.

Synthesis of Clean Hydrogen Gas from Waste Plastic at Zero Net Cost.

Hydrogen gas (H ) is the primary storable fuel for pollution-free energy production, with over 90 million tonnes used globally per year. More than 95% of H is synthesized through metal-catalyzed steam methane reforming that produces 11 tonnes of carbon dioxide (CO ) per tonne H . "Green H " from water electrolysis using renewable energy evolves no CO , but costs 2-3× more, making it presently economically unviable.

Floating Fe Catalyst Formation and Effects of Hydrogen Environment in the Growth of Carbon Nanotubes.

Hydrocarbon conversion to advanced carbon nanomaterials with concurrent hydrogen production holds promise for clean energy technologies. This has been largely enabled by the floating catalyst chemical vapor deposition (FCCVD) growth of carbon nanotubes (CNTs), where commonly catalytic iron nanoparticles are formed from ferrocene decomposition. However, the catalyst formation mechanism and the effect of the chemical environment, especially hydrogen, remain elusive.

Upcycling of Waste Plastic into Hybrid Carbon Nanomaterials.

Graphitic 1D and hybrid nanomaterials represent a powerful solution in composite and electronic applications due to exceptional properties, but large-scale synthesis of hybrid materials has yet to be realized. Here, a rapid, scalable method to produce graphitic 1D materials from polymers using flash Joule heating (FJH) is reported. This avoids lengthy chemical vapor deposition and uses no solvent or water.

Single-chirality nanotube synthesis by guided evolutionary selection.

Bringing to fruition the tantalizing properties, foreseen since the discovery of carbon nanotubes, has been hindered by the challenge to produce a desired helical symmetry type, single chirality. Despite progress in postsynthesis separation or somewhat sporadic success in selective growth, obtaining one chiral type at will remains elusive. The kinetics analysis here shows how a local yet moving reaction zone (the gas feedstock or elevated temperature) can entice the tubes to follow, so that, remotely akin to proverbial Lamarck giraffes, only the fastest survive.

Salt-Assisted MoS Growth: Molecular Mechanisms from the First Principles.

Two-dimensional transition metal dichalcogenides (TMD), such as molybdenum disulfide (MoS), have aroused substantial research interest in recent years, motivating the quest for new synthetic strategies. Recently, halide salts have been reported to promote the chemical vapor deposition (CVD) growth of a wide range of TMD. Nevertheless, the underlying promoting mechanisms and reactions are largely unknown.

Nickel particle-enabled width-controlled growth of bilayer molybdenum disulfide nanoribbons.

Transition metal dichalcogenides exhibit a variety of electronic behaviors depending on the number of layers and width. Therefore, developing facile methods for their controllable synthesis is of central importance. We found that nickel nanoparticles promote both heterogeneous nucleation of the first layer of molybdenum disulfide and simultaneously catalyzes homoepitaxial tip growth of a second layer via a vapor-liquid-solid (VLS) mechanism, resulting in bilayer nanoribbons with width controlled by the nanoparticle diameter.

Step-Edge Epitaxy for Borophene Growth on Insulators.

Borophene─a monatomic layer of boron atoms─stands out among two-dimensional (2D) materials, with its versatile properties tantalizing for physics exploration and next-generation devices. Yet its phases are all synthesized on and stay bound to metal substrates, hampering both characterization and use. Borophene growth on an inert insulator would allow postsynthesis exfoliation, but the weak adhesion to such a substrate results in a high 2D nucleation barrier, preventing clean borophene growth.

Kinetically Determined Shapes of Grain Boundaries in Graphene.

A large-scale chemical synthesis of graphene produces a polycrystalline material with grain boundaries (GBs) that disturb the lattice structure and drastically affect material properties. An uncontrollable formation of GB can be detrimental, yet precise GB engineering can impart added functionalities onto graphene-and its noncarbon two-dimensional "cousins." While the importance of growth kinetics in shaping single-crystalline graphene islands has lately been appreciated, kinetics' role in determining a GB structure remains unaddressed.

Millisecond Conversion of Metastable 2D Materials by Flash Joule Heating.

Controllable phase engineering is vital for precisely tailoring material properties since different phase structures have various electronic states and atomic arrangements. Rapid synthesis of thermodynamically metastable materials, especially two-dimensional metastable materials, with high efficiency and low cost remains a large challenge. Here we report flash Joule heating (FJH) as an electrothermal method to achieve the bulk conversion of transition metal dichalcogenides, MoS and WS, from 2H phases to 1T phases in milliseconds.

Flash Graphene Morphologies.

Flash Joule heating (FJH) can convert almost any carbon-based precursor into bulk quantities of graphene. This work explores the morphologies and properties of flash graphene (FG) generated from carbon black. It is shown that FG is partially comprised of sheets of turbostratic FG (tFG) that have a rotational mismatch between neighboring layers.

Zeolite Nanosheets Stabilize Catalyst Particles to Promote the Growth of Thermodynamically Unfavorable, Small-Diameter Carbon Nanotubes.

A challenge in the synthesis of single-wall carbon nanotubes (SWCNTs) is the lack of control over the formation and evolution of catalyst nanoparticles and the lack of control over their size or chirality. Here, zeolite MFI nanosheets (MFI-Ns) are used to keep cobalt (Co) nanoparticles stable during prolonged annealing conditions. Environmental transmission electron microscopy (ETEM) shows that the MFI-Ns can influence the size and shape of nanoparticles via particle/support registry, which leads to the preferential docking of nanoparticles to four or fewer pores and to the regulation of the SWCNT synthesis products.

Gram-scale bottom-up flash graphene synthesis.

Most bulk-scale graphene is produced by a top-down approach, exfoliating graphite, which often requires large amounts of solvent with high-energy mixing, shearing, sonication or electrochemical treatment. Although chemical oxidation of graphite to graphene oxide promotes exfoliation, it requires harsh oxidants and leaves the graphene with a defective perforated structure after the subsequent reduction step. Bottom-up synthesis of high-quality graphene is often restricted to ultrasmall amounts if performed by chemical vapour deposition or advanced synthetic organic methods, or it provides a defect-ridden structure if carried out in bulk solution.

Janus Segregation at the Carbon Nanotube-Catalyst Interface.

The contact between a carbon nanotube (CNT) edge and a catalyst is a curvilinear interface of fundamental and practical importance. Here, the first-principles evidence shows that on a rigid/solid catalyst the faceted CNT edge is significantly lower in energy compared to the minimal-length circle, with the interface energy difference decreasing on more compliant surfaces. This universal trend, found for typical monometallic (Ni, Co), bimetallic (CoW), and metal carbide (WC) catalysts, results in a peculiar edge segregation into one-dimensional Janus (armchair-zigzag) interface.

How the Complementarity at Vicinal Steps Enables Growth of 2D Monocrystals.

Large 2D monocrystals are highly sought after yet hard to achieve; unlike graphene, most dichalcogenides and h-BN possess low symmetry, which allows for nucleation of mutually inverted pieces, merging into polycrystals replete with grain boundaries. On vicinal substrate surfaces such growing pieces were observed to orient alike, and very recently this effect apparently enabled the growth of large single crystal h-BN. Addressing the compelling questions of how such a growth process can operate and what the key mechanisms are is crucial in guiding the substrate selection for optimal synthesis of perhaps many materials.

Transient Kinetic Selectivity in Nanotubes Growth on Solid Co-W Catalyst.

Solid Co-W catalysts have been shown to yield single-walled carbon nanotubes (CNT) with high selectivity, simplistically attributed to CNT-catalyst symmetry match for certain chiral indices ( n, m). Here, based on large-scale first-principles calculations combined with kinetic Monte Carlo simulations, we show instead that such selectivity arises from a complex kinetics of growth. The solid CoW catalyst strongly favors a restructured, asymmetric CNT edge which entails preferential nucleation of tubes with 2 m < n but much faster growth of chiral tubes with n ⩽ 2 m.

Evolutionary selection growth of two-dimensional materials on polycrystalline substrates.

There is a demand for the manufacture of two-dimensional (2D) materials with high-quality single crystals of large size. Usually, epitaxial growth is considered the method of choice in preparing single-crystalline thin films, but it requires single-crystal substrates for deposition. Here we present a different approach and report the synthesis of single-crystal-like monolayer graphene films on polycrystalline substrates.