Toward Ideal Metal–Organic Framework Thin-Film Growth via Automated Layer-by-Layer Deposition: Examples Based on Perylene Diimide Linkers

Goswami, Subhadip; Rimoldi, Martino; Anderson, Ryther; Lee, Changmin; Li, Xinlin; Li, Alice; Deria, Pravas; Chen, Lin X.; Schaller, Richard D.; Gómez-Gualdrón, Diego A.; Farha, Omar K.; Hupp, Joseph T.

doi:10.1021/acs.chemmater.2c01753

Toward Ideal Metal–Organic Framework Thin-Film Growth via Automated Layer-by-Layer Deposition: Examples Based on Perylene Diimide Linkers

Journal Article · Tue Oct 25 00:00:00 EDT 2022 · Chemistry of Materials

DOI:https://doi.org/10.1021/acs.chemmater.2c01753· OSTI ID:2217033

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Northwestern Univ., Evanston, IL (United States)
Colorado School of Mines, Golden, CO (United States)
Southern Illinois Univ., Carbondale, IL (United States)
Northwestern Univ., Evanston, IL (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)

Photoactive metal-organic framework (MOF) thin films offer an opportunity for translating the advantages of periodic, crystalline, and tailorable light-harvesting materials directly into devices such as those for photoelectrochemical solar energy conversion. In this study, we report the fabrication of light-absorbing perylene-diimide-containing pillared-paddlewheel MOF thin films using an automated layer-by-layer (LbL) deposition technique. Our focus here is on optimizing the growth of representative chromophoric MOFs as oriented films of uniform and predefined thickness. Growth was examined as a function of metal identity, pillaring ligand composition, and supporting-surface chemical functionality. Further, application of atomic force microscopy (AFM) and complementary techniques revealed that the surface-supported MOFs initially display island-type film growth (Volmer-Weber growth), resulting in comparatively rough films. Further growth is accompanied by the merging of islands, resulting in films that, depending on experimental details, can be remarkably smooth (i.e., roughness on the order of ±1 nm (one structural repeat unit in the pillaring direction)). These details include the use of 1,4-diazabicyclo[2.2.2]octane (DABCO) as a MOF pillar and ALD-grown zinc oxide as a film support (ALD = atomic layer deposition). Also helpful for mitigating island-type growth, at least in part, is the replacement of Zn²⁺ by Cu²⁺ as the metal component of the MOF. Notably, each of these adjustments entails replacing weaker chemical bonds with stronger ones.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB); National Science Foundation (NSF)

Grant/Contract Number:: AC02-06CH11357; FG02-87ER13808

OSTI ID:: 2217033

Journal Information:: Chemistry of Materials, Journal Name: Chemistry of Materials Journal Issue: 21 Vol. 34; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Toward Ideal Metal–Organic Framework Thin-Film Growth via Automated Layer-by-Layer Deposition: Examples Based on Perylene Diimide Linkers

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