Influence of Hydrogen Sulfide Exposure on the Transport and Structural Properties of the Metal–Organic Framework ZIF-8

doi:10.1021/acs.jpcc.8b00798

Title: Influence of Hydrogen Sulfide Exposure on the Transport and Structural Properties of the Metal–Organic Framework ZIF-8

Abstract

In this paper, the interaction between hydrogen sulfide and ZIF-8 was studied via structural characterizations and guest molecule diffusion measurements. It was found that hydrogen sulfide reacts with the ZIF-8 external particle surface to form a surface barrier that excludes the uptake of larger molecules (ethanol) and slows down the uptake of smaller molecules (carbon dioxide). Nonetheless, bulk transport properties were unaltered, as supported by pulsed field gradient nuclear magnetic resonance studies. Dispersion-corrected density functional theory calculations revealed that H ₂S is consumed by reactions occurring at the ZIF external surface. These reactions result in water and defect formation, both of which were found to be exothermic and independent of both crystallographic facets ({001} and {110}) and surface termination. Finally, we concluded that these surface reactions lead to structural and chemical changes to the ZIF-8 external surface that generate surface barriers to molecular transport.

Authors:

Dutta, Akshita ^[1];

^[2];

^[3]; Collins, James ^[4];

^[3];

^[2];

^[1]

Univ. of Florida, Gainesville, FL (United States). Dept. of Chemical Engineering
Univ. of Wisconsin, Madison, WI (United States). Theoretical Chemistry Inst. Dept. of Chemistry
Georgia Inst. of Technology, Atlanta, GA (United States). School of Chemical and Biomolecular Engineering
Univ. of Florida, Gainesville, FL (United States). National High Magnetic Field Lab.

Publication Date:: 2018-03-09

Research Org.:: Georgia Inst. of Technology, Atlanta, GA (United States); Univ. of Florida, Gainesville, FL (United States); Energy Frontier Research Centers (EFRC) (United States). Center for Understanding and Control of Acid Gas-induced Evolution of Materials for Energy (UNCAGE-ME)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Science Foundation (NSF)

OSTI Identifier:: 1428044

Grant/Contract Number:: SC0012577; ECCS-1542174; DMR-1157490

Resource Type:: Accepted Manuscript

Journal Name:: Journal of Physical Chemistry. C

Additional Journal Information:: Journal Volume: 122; Journal Issue: 13; Journal ID: ISSN 1932-7447

Publisher:: American Chemical Society

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats


                    Dutta, Akshita, Tymi?ska, Nina, Zhu, Guanghui, Collins, James, Lively, Ryan P., Schmidt, J. R., and Vasenkov, Sergey. Influence of Hydrogen Sulfide Exposure on the Transport and Structural Properties of the Metal–Organic Framework ZIF-8.  United States: N. p., 2018. 
        Web.  doi:10.1021/acs.jpcc.8b00798.

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                    Dutta, Akshita, Tymi?ska, Nina, Zhu, Guanghui, Collins, James, Lively, Ryan P., Schmidt, J. R., & Vasenkov, Sergey. Influence of Hydrogen Sulfide Exposure on the Transport and Structural Properties of the Metal–Organic Framework ZIF-8.  United States.  doi:10.1021/acs.jpcc.8b00798.

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                    Dutta, Akshita, Tymi?ska, Nina, Zhu, Guanghui, Collins, James, Lively, Ryan P., Schmidt, J. R., and Vasenkov, Sergey. Fri .  
        "Influence of Hydrogen Sulfide Exposure on the Transport and Structural Properties of the Metal–Organic Framework ZIF-8".  United States.  doi:10.1021/acs.jpcc.8b00798.  https://www.osti.gov/servlets/purl/1428044.

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@article{osti_1428044,

  title        = {Influence of Hydrogen Sulfide Exposure on the Transport and Structural Properties of the Metal–Organic Framework ZIF-8},

  author       = {Dutta, Akshita and Tymi?ska, Nina and Zhu, Guanghui and Collins, James and Lively, Ryan P. and Schmidt, J. R. and Vasenkov, Sergey},

  abstractNote = {In this paper, the interaction between hydrogen sulfide and ZIF-8 was studied via structural characterizations and guest molecule diffusion measurements. It was found that hydrogen sulfide reacts with the ZIF-8 external particle surface to form a surface barrier that excludes the uptake of larger molecules (ethanol) and slows down the uptake of smaller molecules (carbon dioxide). Nonetheless, bulk transport properties were unaltered, as supported by pulsed field gradient nuclear magnetic resonance studies. Dispersion-corrected density functional theory calculations revealed that H2S is consumed by reactions occurring at the ZIF external surface. These reactions result in water and defect formation, both of which were found to be exothermic and independent of both crystallographic facets ({001} and {110}) and surface termination. Finally, we concluded that these surface reactions lead to structural and chemical changes to the ZIF-8 external surface that generate surface barriers to molecular transport.},

  doi          = {10.1021/acs.jpcc.8b00798},

  journal      = {Journal of Physical Chemistry. C},

  number       = 13,

  volume       = 122,

  place        = {United States},

  year         = {2018},

  month        = {3}

}

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Journal Article:

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DOI: 10.1021/acs.jpcc.8b00798

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Cited by: 2 works

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Figures / Tables:

Table 1: Concentrations of Probe Molecules (Ethylene and Carbon Dioxide) in the As-Prepared and H₂S-Exposed ZIF-8 Samples at 298 K as Determined Using ¹³C NMR Signal Analysis

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