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

Abstract

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 themore » MOF. Notably, each of these adjustments entails replacing weaker chemical bonds with stronger ones.« less

Authors:
ORCiD logo [1]; ORCiD logo [1];  [2]; ORCiD logo [1]; ORCiD logo [3]; ORCiD logo [1]; ORCiD logo [3]; ORCiD logo [4]; ORCiD logo [4]; ORCiD logo [2]; ORCiD logo [1]; ORCiD logo [1]
+ Show Author Affiliations
  1. Northwestern Univ., Evanston, IL (United States)
  2. Colorado School of Mines, Golden, CO (United States)
  3. Southern Illinois Univ., Carbondale, IL (United States)
  4. Northwestern Univ., Evanston, IL (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)
Publication Date:
Research Org.:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB); National Science Foundation (NSF)
OSTI Identifier:
2217033
Grant/Contract Number:  
AC02-06CH11357; FG02-87ER13808; CHE-1944903
Resource Type:
Accepted Manuscript
Journal Name:
Chemistry of Materials
Additional Journal Information:
Journal Volume: 34; Journal Issue: 21; Journal ID: ISSN 0897-4756
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; atomic layer deposition; layer by layer deposition; metal organic frameworks; organic compounds; thin films

Citation Formats

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., and Hupp, Joseph T. Toward Ideal Metal–Organic Framework Thin-Film Growth via Automated Layer-by-Layer Deposition: Examples Based on Perylene Diimide Linkers. United States: N. p., 2022. Web. doi:10.1021/acs.chemmater.2c01753.
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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. Toward Ideal Metal–Organic Framework Thin-Film Growth via Automated Layer-by-Layer Deposition: Examples Based on Perylene Diimide Linkers. United States. https://doi.org/10.1021/acs.chemmater.2c01753
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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., and Hupp, Joseph T. Tue . "Toward Ideal Metal–Organic Framework Thin-Film Growth via Automated Layer-by-Layer Deposition: Examples Based on Perylene Diimide Linkers". United States. https://doi.org/10.1021/acs.chemmater.2c01753. https://www.osti.gov/servlets/purl/2217033.
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@article{osti_2217033,
title = {Toward Ideal Metal–Organic Framework Thin-Film Growth via Automated Layer-by-Layer Deposition: Examples Based on Perylene Diimide Linkers},
author = {Goswami, Subhadip and Rimoldi, Martino and Anderson, Ryther and Lee, Changmin and Li, Xinlin and Li, Alice and Deria, Pravas and Chen, Lin X. and Schaller, Richard D. and Gómez-Gualdrón, Diego A. and Farha, Omar K. and Hupp, Joseph T.},
abstractNote = {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.},
doi = {10.1021/acs.chemmater.2c01753},
journal = {Chemistry of Materials},
number = 21,
volume = 34,
place = {United States},
year = {Tue Oct 25 00:00:00 EDT 2022},
month = {Tue Oct 25 00:00:00 EDT 2022}
}
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