Hydrogen gas formation from the photolysis of rhenium hydrides - mechanistic and computational studies
The photolysis of 4,4′-disubstituted, 2,2′-bipyridine fac -Re(bpy)(CO) 3 H derivatives produces stoichiometric H 2 gas. The rate of production varies greatly depending on the electronic nature of the disubstituted bipyridine (bpy) with halogenated substituents increasing the rate. Isotope labeling s...
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| Published in | Dalton transactions : an international journal of inorganic chemistry Vol. 48; no. 43; pp. 16148 - 16152 |
|---|---|
| Main Authors | , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
Cambridge
Royal Society of Chemistry
21.11.2019
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| Subjects | |
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| Abstract | The photolysis of 4,4′-disubstituted, 2,2′-bipyridine
fac
-Re(bpy)(CO)
3
H derivatives produces stoichiometric H
2
gas. The rate of production varies greatly depending on the electronic nature of the disubstituted bipyridine (bpy) with halogenated substituents increasing the rate. Isotope labeling studies along with B3LYP geometry optimization DFT modeling studies indicate a mechanism involving a Re-H-Re bridging complex that leads to a dimeric Re-Re(η
2
-H
2
) state prior to dissociating H
2
gas.
The photolysis of
fac
-Re(bpy)(CO)
3
H derivatives produce stoichiometric H
2
gas. Isotope labeling and computational studies indicate a mechanism involving a Re-H-Re bridging complex that leads to a dimeric Re-Re(η
2
-H
2
) state prior to dissociating H
2
. |
|---|---|
| AbstractList | The photolysis of 4,4′-disubstituted, 2,2′-bipyridine
fac
-Re(bpy)(CO)
3
H derivatives produces stoichiometric H
2
gas. The rate of production varies greatly depending on the electronic nature of the disubstituted bipyridine (bpy) with halogenated substituents increasing the rate. Isotope labeling studies along with B3LYP geometry optimization DFT modeling studies indicate a mechanism involving a Re–H–Re bridging complex that leads to a dimeric Re–Re(η
2
-H
2
) state prior to dissociating H
2
gas. The photolysis of 4,4′-disubstituted, 2,2′-bipyridine fac -Re(bpy)(CO) 3 H derivatives produces stoichiometric H 2 gas. The rate of production varies greatly depending on the electronic nature of the disubstituted bipyridine (bpy) with halogenated substituents increasing the rate. Isotope labeling studies along with B3LYP geometry optimization DFT modeling studies indicate a mechanism involving a Re-H-Re bridging complex that leads to a dimeric Re-Re(η 2 -H 2 ) state prior to dissociating H 2 gas. The photolysis of fac -Re(bpy)(CO) 3 H derivatives produce stoichiometric H 2 gas. Isotope labeling and computational studies indicate a mechanism involving a Re-H-Re bridging complex that leads to a dimeric Re-Re(η 2 -H 2 ) state prior to dissociating H 2 . The photolysis of 4,4′-disubstituted, 2,2′-bipyridine fac-Re(bpy)(CO)3H derivatives produces stoichiometric H2 gas. The rate of production varies greatly depending on the electronic nature of the disubstituted bipyridine (bpy) with halogenated substituents increasing the rate. Isotope labeling studies along with B3LYP geometry optimization DFT modeling studies indicate a mechanism involving a Re–H–Re bridging complex that leads to a dimeric Re–Re(η2-H2) state prior to dissociating H2 gas. |
| Author | Webster, Alyssa A Huo, Jianqiang Milliken, Jenna Hoberg, John O Kubelka, Jan Sullivan, Pat |
| AuthorAffiliation | Department of Chemistry University of Wyoming Department of Petroleum Engineering |
| AuthorAffiliation_xml | – name: Department of Petroleum Engineering – name: University of Wyoming – name: Department of Chemistry |
| Author_xml | – sequence: 1 givenname: Alyssa A surname: Webster fullname: Webster, Alyssa A – sequence: 2 givenname: Jianqiang surname: Huo fullname: Huo, Jianqiang – sequence: 3 givenname: Jenna surname: Milliken fullname: Milliken, Jenna – sequence: 4 givenname: Pat surname: Sullivan fullname: Sullivan, Pat – sequence: 5 givenname: Jan surname: Kubelka fullname: Kubelka, Jan – sequence: 6 givenname: John O surname: Hoberg fullname: Hoberg, John O |
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| Cites_doi | 10.1039/C7CP07770J 10.1002/1521-3765(20020315)8:6<1361::AID-CHEM1361>3.0.CO;2-E 10.1016/j.jorganchem.2005.08.014 10.1021/ic048910v 10.1246/cl.1989.765 10.1063/1.3382344 10.1021/ic0206894 10.1039/a801230j 10.1021/ja982284h 10.1021/ic00101a033 10.1021/ja00040a028 10.1002/ejic.200600166 10.1021/ic701458h 10.1557/mrs2007.168 10.1002/(SICI)1521-3765(19991105)5:11<3341::AID-CHEM3341>3.0.CO;2-F 10.1021/j100338a009 10.1007/3418_2009_2 10.1021/ja00178a077 10.1021/jp305461z 10.1021/ja035960a 10.1073/pnas.0603395103 10.1021/ja00301a029 10.1039/f29868202401 10.1021/jp810292n 10.1021/om960044+ 10.1021/ic00032a029 10.1021/ic102317u 10.1039/C39830000536 10.1002/ejic.200700860 10.1002/hlca.19860690824 10.1021/om00007a022 10.1021/jp102860m 10.1021/acs.chemrev.6b00204 10.1021/ic050901e 10.1021/ic00099a022 10.1021/om00138a035 |
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| Notes | 10.1039/C9DT03364E In memory of Pat Sullivan. Electronic supplementary information (ESI) available. See DOI ObjectType-Article-1 SourceType-Scholarly Journals-1 ObjectType-Feature-2 content type line 23 |
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| Snippet | The photolysis of 4,4′-disubstituted, 2,2′-bipyridine
fac
-Re(bpy)(CO)
3
H derivatives produces stoichiometric H
2
gas. The rate of production varies greatly... The photolysis of 4,4′-disubstituted, 2,2′-bipyridine fac-Re(bpy)(CO)3H derivatives produces stoichiometric H2 gas. The rate of production varies greatly... |
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| SubjectTerms | Gas formation Hydrogen storage Optimization Photolysis Rhenium |
| Title | Hydrogen gas formation from the photolysis of rhenium hydrides - mechanistic and computational studies |
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