Title: Assessing the quality of large-area monolayer graphene grown on liquid copper for size-selective ionic/molecular membrane separations

Abstract

Monolayer graphene growth on liquid copper (Cu) has attracted attention due to advantages of a flat/smooth catalytic growth surface, high synthesis temperature (>1080 °C) as well as the possibility of forming graphene domains that are mobile on the liquid Cu with potential to minimize grain boundary defects and self-assemble into a continuous monolayer film. However, the quality of monolayer graphene grown on liquid copper and its suitability for size-selective ionic/molecular membrane separations has not been evaluated/studied. Here, we probe the quality of monolayer graphene grown on liquid Cu (via a metallurgical process, HSMG^®) using Scanning Electron Microscope (SEM), High-resolution transmission electron microscope (HR-TEM), Raman spectroscopy and report on a facile approach to assess intrinsic sub-nanometer to nanometer-scale defects over centimeter-scale areas. We demonstrate high transfer yields of monolayer graphene (>93% coverage) from the growth substrate to polyimide track etched membrane (PITEM, pore diameter ~200 nm) supports to form centimeter-scale atomically thin membranes. Next, we use pressure-driven transport of ethanol to probe defects > 60 nm and diffusion-driven transport of analytes (KCl ~0.66 nm, L-Tryptophan ~0.7–0.9 nm, Vitamin B12 ~1–1.5 nm and Lysozyme ~3.8–4 nm) to probe nanoscale and sub-nanometer scale defects. Diffusive transport confirms the presence of intrinsic sub-nanometer tomore » nanometer scale defects in monolayer graphene grown on liquid Cu are no less than that in high-quality graphene synthesized via chemical vapor deposition (CVD) on solid Cu. Our work not only benchmarks quality of graphene grown on liquid copper for membrane applications but also provides fundamental insights into the origin of intrinsic defects in large-area graphene synthesized via bottom-up processes for membrane applications.« less

Authors:

Romaniak, Grzegorz  ^[1];

• Search DOE PAGES for author "Romaniak, Grzegorz"
• Search DOE PAGES for ORCID "0000-0001-7711-1540"

Cheng, Peifu  ^[2];

• Search DOE PAGES for author "Cheng, Peifu"
• Search DOE PAGES for ORCID "0000-0001-6010-6411"

Dybowski, Konrad  ^[1];

• Search DOE PAGES for author "Dybowski, Konrad"
• Search DOE PAGES for ORCID "0000-0003-4017-3830"

Kula, Piotr  ^[1];

• Search DOE PAGES for author "Kula, Piotr"
• Search DOE PAGES for ORCID "0000-0002-1796-9155"

Kidambi, Piran R.  ^[2]

• Search DOE PAGES for author "Kidambi, Piran R."
• Search DOE PAGES for ORCID "0000-0003-1546-5014"

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+ Show Author Affiliations

1. Lodz University of Technology (Poland)
2. Vanderbilt University, Nashville, TN (United States)

Publication Date:

Thu Oct 12 00:00:00 EDT 2023

Research Org.:

Vanderbilt Univ., Nashville, TN (United States)

Sponsoring Org.:

USDOE Office of Science (SC)

OSTI Identifier:

2324832

Grant/Contract Number:  

SC0022237

Resource Type:

Accepted Manuscript

Journal Name:

Materials Research Express (Online)

Additional Journal Information:

Journal Name: Materials Research Express (Online); Journal Volume: 10; Journal Issue: 10; Journal ID: ISSN 2053-1591

Publisher:

IOP Publishing

Country of Publication:

United States

Language:

English

Subject:

36 MATERIALS SCIENCE; atomically thin membranes; graphene; graphene membranes; molecular sieving; desalination; liquid copper growth; ionic/molecular separations