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Title: Effect of Spin State on the Dihydrogen Binding Strength to Transition Metal Centers in Metal-Organic Frameworks

Abstract

In several recent experimental studies, it has been found that exposed transition metal (TM) sites in metal-organic frameworks (MOFs) yield the largest binding to H2 by about 10 kJ/mol. However, this binding is significantly smaller than what has been observed in the so-called Kubas molecules, also with exposed metal sites. Our ab initio calculations quantitatively account for the experimental findings and further show that the splitting and occupation of the spin orbitals in the MOF systems are the reasons for their unexpected small binding energies. We predict that the binding energy to H2 in the MOF systems can be tuned between 10 and 50 kJ/mol by using early TM elements, namely, Sc, Ti, V, Cr, and Mn.

Authors:
; ;
Publication Date:
Research Org.:
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
981975
DOE Contract Number:
AC36-08GO28308
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of the American Chemical Society; Journal Volume: 129; Journal Issue: 2007
Country of Publication:
United States
Language:
English
Subject:
08 HYDROGEN; 36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; ALKYL BENZENESULFONATES; BINDING ENERGY; ELEMENTS; METALS; MOLECULES; OCCUPATIONS; SPIN; TRANSITION ELEMENTS; YIELDS; Materials Science and Semiconductors

Citation Formats

Sun, Y. Y., Kim, Y. H., and Zhang, S. B. Effect of Spin State on the Dihydrogen Binding Strength to Transition Metal Centers in Metal-Organic Frameworks. United States: N. p., 2007. Web. doi:10.1021/ja0740061.
Sun, Y. Y., Kim, Y. H., & Zhang, S. B. Effect of Spin State on the Dihydrogen Binding Strength to Transition Metal Centers in Metal-Organic Frameworks. United States. doi:10.1021/ja0740061.
Sun, Y. Y., Kim, Y. H., and Zhang, S. B. Mon . "Effect of Spin State on the Dihydrogen Binding Strength to Transition Metal Centers in Metal-Organic Frameworks". United States. doi:10.1021/ja0740061.
@article{osti_981975,
title = {Effect of Spin State on the Dihydrogen Binding Strength to Transition Metal Centers in Metal-Organic Frameworks},
author = {Sun, Y. Y. and Kim, Y. H. and Zhang, S. B.},
abstractNote = {In several recent experimental studies, it has been found that exposed transition metal (TM) sites in metal-organic frameworks (MOFs) yield the largest binding to H2 by about 10 kJ/mol. However, this binding is significantly smaller than what has been observed in the so-called Kubas molecules, also with exposed metal sites. Our ab initio calculations quantitatively account for the experimental findings and further show that the splitting and occupation of the spin orbitals in the MOF systems are the reasons for their unexpected small binding energies. We predict that the binding energy to H2 in the MOF systems can be tuned between 10 and 50 kJ/mol by using early TM elements, namely, Sc, Ti, V, Cr, and Mn.},
doi = {10.1021/ja0740061},
journal = {Journal of the American Chemical Society},
number = 2007,
volume = 129,
place = {United States},
year = {Mon Jan 01 00:00:00 EST 2007},
month = {Mon Jan 01 00:00:00 EST 2007}
}