Hydrogenation-Assisted Graphene Origami and Its Application in Programmable Molecular Mass Uptake, Storage, and Release

Abstract

The malleable nature of atomically thin graphene makes it a potential candidate material for nanoscale origami, a promising bottom-up nanomanufacturing approach to fabricating nanobuilding blocks of desirable shapes. The success of graphene origami hinges upon precise and facile control of graphene morphology, which still remains as a significant challenge. Inspired by recent progresses on functionalization and patterning of graphene, we demonstrate hydrogenation-assisted graphene origami (HAGO), a feasible and robust approach to enabling the formation of unconventional carbon nanostructures, through systematic molecular dynamics simulations. A unique and desirable feature of HAGO-enabled nanostructures is the programmable tunability of their morphology via an external electric field. In particular, we demonstrate reversible opening and closing of a HAGO-enabled graphene nanocage, a mechanism that is crucial to achieve molecular mass uptake, storage, and release. HAGO holds promise to enable an array of carbon nanostructures of desirable functionalities by design. As an example, we demonstrate HAGO-enabled high-density hydrogen storage with a weighted percentage exceeding the ultimate goal of US Department of Energy.

An assessment of strategies for the development of solid-state adsorbents for vehicular hydrogen storage

“…232 Over the last few decades, synthetic research has led to development of new graphene-inspired building blocks and several new carbonbased H 2 adsorbents designed to enhance binding enthalpies, such as graphene oxide, graphene origami, and others. [233][234][235] For example, various oxygenated functional moieties, including carboxyl and hydroxyl groups, can be introduced to graphene to form graphene oxide (Fig. 11); subsequent crosslinking of this scaffold with organic ligands can be carried out to prepare three-dimensional H 2 adsorbents.…”

“…233 Using MD simulations, the authors showed that a origami nanocage-which can be converted between open or closed configurations via an external electric field-could obtain a gravimetric capacity up to 9.7 wt%. Such a concept, although interesting, has yet to be experimentally verified.…”

Reconfigurable systems for multifunctional electronics

“…For example, with designed hydrogenated edges, a graphene origami can form 3D structures through hydrogenation by a trigger in the electric field for potential hydrogen storage. 47 In another example, a four-legged walking robot that is based on single graphene oxide film with asymmetric surfaces can move forward even on smooth glass substrate step by step, by alternating the infrared light on and off. 48 Structural instabilities (e.g., buckling, ripples, and wrinkles) of 2D nanomaterials lead to change in electronic structures.…”

Tailoring physical properties of graphene: Effects of hydrogenation, oxidation, and grain boundaries by atomistic simulations

“…Hydrogenation of graphene has attracted great interests owing to two issues: tuning band gap for graphene used in semiconductor-based electronic devices and possible devotions to hydrogen storage [18,[43][44][45]. There are two kinds of typical free-standing HG structures with distinctive properties: H atoms adsorbed graphene (with only one or two H atoms), and graphane, a fully HG.…”