Hydrogenation of CuBTC Framework with the Introduction of a PtC Hydrogen Spillover Catalyst

Abstract

Hydrogen uptake of a microporous metal organic framework, CuBTC, is increased 3.5-fold at 298 K and 20 bar upon the addition of a hydrogen spillover catalyst, from 0.17 to 0.61 wt %. Structural integrity upon mixing with the catalyst is important to achieve this level of uptake. Increasing the adsorption temperature to 323 K significantly reduces the rate of uptake, but 0.55 wt % uptake is observed when the experimental equilibration time is extended. The slow, pressure-independent uptake at 323 K, along with the desorption behavior is suggestive of a hydrogenation process of the CuBTC substrate. PXRD analysis suggests the hydrogenated sample remains intact and FTIR demonstrates hydrogenation of the carboxylate group of the BTC ligand but finds no evidence for hydrogenation of the carbons of the BTC ligand. Although hydrogenation of the CuBTC does not lead to readily desorbable H2, the results shed light on a possible mechanism of the hydrogen spillover process.

Department(s)

Chemical and Biochemical Engineering

Sponsor(s)

United States. Department of Energy. Office of Basic Energy Sciences
United States. Department of Energy. Office of Energy Efficiency and Renewable Energy

Comments

The spectroscopic work in this paper was supported by the U.S. Department of Energy, Basic Energy Sciences Awards DE-FG02-09ER466556 and DE-SC0002157; material synthesis, diffraction, and isotherms were supported by the Energy Efficiency and Renewable Energy program, Award DE-FG36- 08GO18139

Keywords and Phrases

Adsorption temperature; Carboxylate groups; Desorption behavior; Equilibration time; FTIR; Hydrogen spillover; Hydrogen uptake; Hydrogenation process; Microporous metal organic frameworks; Adsorption; Carboxylation; Catalysts; Hydrogen; Ligands; Hydrogenation

International Standard Serial Number (ISSN)

1932-7447

Document Type

Article - Journal

Document Version

Citation

File Type

text

Language(s)

English

Rights

© 2012 American Chemical Society (ACS), All rights reserved.

Publication Date

01 Feb 2012

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