Abstract Solution‐processed graphene is a promising material for numerous high‐volume applications including structural composites, batteries, sensors, and printed electronics. However, the polydisperse nature of graphene dispersions following liquid‐phase exfoliation poses major manufacturing challenges, as incompletely exfoliated graphite flakes must be removed to achieve optimal properties and downstream performance. Incumbent separation schemes rely on centrifugation, which is highly energy‐intensive and limits scalable manufacturing. Here, cross‐flow filtration (CFF) is introduced as a centrifuge‐free processing method that improves the throughput of graphene separation by two orders of magnitude. By tuning membrane pore sizes between microfiltration and ultrafiltration length scales, CFF can also be used for efficient recovery of solvents and stabilizing polymers. In this manner, life cycle assessment and techno‐economic analysis reveal that CFF reduces greenhouse gas emissions, fossil energy usage, water consumption, and specific production costs of graphene manufacturing by 57%, 56%, 63%, and 72%, respectively. To confirm that CFF produces electronic‐grade graphene, CFF‐processed graphene nanosheets are formulated into printable inks, leading to state‐of‐the‐art thin‐film conductivities exceeding 104S m−1. This CFF methodology can likely be generalized to other van der Waals layered solids, thus enabling sustainable manufacturing of the diverse set of applications currently being pursued for 2D materials.
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Noble Metal Ion‐Directed Assembly of 2D Materials for Heterostructured Catalysts and Metallic Micro‐Texturing
Assembling 2D-material (2DM) nanosheets into micro- and macro-architectures with augmented functionalities requires effective strategies to overcome nanosheet restacking. Conventional assembly approaches involve external binders and/or functionalization, which inevitably sacrifice 2DM's nanoscale properties. Noble metal ions (NMI) are promising ionic crosslinkers, which can simultaneously assemble 2DM nanosheets and induce synergistic properties. Herein, a collection of NMI–2DM complexes are screened and categorized into two sub-groups. Based on the zeta potentials, two assembly approaches are developed to obtain 1) NMI-crosslinked 2DM hydrogels/aerogels for heterostructured catalysts and 2) NMI–2DM inks for templated synthesis. First, tetraammineplatinum(II) nitrate (TPtN) serves as an efficient ionic crosslinker to agglomerate various 2DM dispersions. By utilizing micro-textured assembly platforms, various TPtN–2DM hydrogels are fabricated in a scalable fashion. Afterward, these hydrogels are lyophilized and thermally reduced to synthesize Pt-decorated 2DM aerogels (Pt@2DM). The Pt@2DM heterostructures demonstrate high, substrate-dependent catalytic activities and promote different reaction pathways in the hydrogenation of 3-nitrostyrene. Second, PtCl4 can be incorporated into 2DM dispersions at high NMI molarities to prepare a series of PtCl4–2DM inks with high colloidal stability. By adopting the PtCl4–graphene oxide ink, various Pt micro-structures with replicated topographies are synthesized with accurate control of grain sizes and porosities.
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- Award ID(s):
- 2045258
- PAR ID:
- 10433133
- Date Published:
- Journal Name:
- Advanced Functional Materials
- ISSN:
- 1616-301X
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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