Catalyst self-assembly accelerates bimetallic light-driven electrocatalytic H2 evolution in water
Hydrogen evolution is an important fuel-generating reaction that has been subject to mechanistic debate about the roles of monometallic and bimetallic pathways. The molecular iridium catalysts in this study undergo photoelectrochemical dihydrogen (H 2 ) evolution via a bimolecular mechanism, providi...
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| Published in | Nature chemistry Vol. 16; no. 5; pp. 709 - 716 |
|---|---|
| Main Authors | , , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
London
Nature Publishing Group UK
01.05.2024
Nature Publishing Group |
| Subjects | |
| Online Access | Get full text |
| ISSN | 1755-4330 1755-4349 1755-4349 |
| DOI | 10.1038/s41557-024-01483-3 |
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| Abstract | Hydrogen evolution is an important fuel-generating reaction that has been subject to mechanistic debate about the roles of monometallic and bimetallic pathways. The molecular iridium catalysts in this study undergo photoelectrochemical dihydrogen (H
2
) evolution via a bimolecular mechanism, providing an opportunity to understand the factors that promote bimetallic H–H coupling. Covalently tethered diiridium catalysts evolve H
2
from neutral water faster than monometallic catalysts, even at lower overpotential. The unexpected origin of this improvement is non-covalent supramolecular self-assembly into nanoscale aggregates that efficiently harvest light and form H–H bonds. Monometallic catalysts containing long-chain alkane substituents leverage the self-assembly to evolve H
2
from neutral water at low overpotential and with rates close to the expected maximum for this light-driven water splitting reaction. Design parameters for holding multiple catalytic sites in close proximity and tuning catalyst microenvironments emerge from this work.
Although the light-driven generation of hydrogen from water is a promising approach to renewable fuels, the H–H bond formation step represents a persistent mechanistic question. Now light-harvesting molecular catalysts have been shown to self-assemble into nanoscale aggregates that feature improved efficiency for photoelectrochemical H
2
evolution. |
|---|---|
| AbstractList | Hydrogen evolution is an important fuel-generating reaction that has been subject to mechanistic debate about the roles of monometallic and bimetallic pathways. The molecular iridium catalysts in this study undergo photoelectrochemical dihydrogen (H2) evolution via a bimolecular mechanism, providing an opportunity to understand the factors that promote bimetallic H-H coupling. Covalently tethered diiridium catalysts evolve H2 from neutral water faster than monometallic catalysts, even at lower overpotential. The unexpected origin of this improvement is non-covalent supramolecular self-assembly into nanoscale aggregates that efficiently harvest light and form H-H bonds. Monometallic catalysts containing long-chain alkane substituents leverage the self-assembly to evolve H2 from neutral water at low overpotential and with rates close to the expected maximum for this light-driven water splitting reaction. Design parameters for holding multiple catalytic sites in close proximity and tuning catalyst microenvironments emerge from this work.Hydrogen evolution is an important fuel-generating reaction that has been subject to mechanistic debate about the roles of monometallic and bimetallic pathways. The molecular iridium catalysts in this study undergo photoelectrochemical dihydrogen (H2) evolution via a bimolecular mechanism, providing an opportunity to understand the factors that promote bimetallic H-H coupling. Covalently tethered diiridium catalysts evolve H2 from neutral water faster than monometallic catalysts, even at lower overpotential. The unexpected origin of this improvement is non-covalent supramolecular self-assembly into nanoscale aggregates that efficiently harvest light and form H-H bonds. Monometallic catalysts containing long-chain alkane substituents leverage the self-assembly to evolve H2 from neutral water at low overpotential and with rates close to the expected maximum for this light-driven water splitting reaction. Design parameters for holding multiple catalytic sites in close proximity and tuning catalyst microenvironments emerge from this work. Not provided. Hydrogen evolution is an important fuel-generating reaction that has been subject to mechanistic debate about the roles of monometallic and bimetallic pathways. The molecular iridium catalysts in this study undergo photoelectrochemical dihydrogen (H2) evolution via a bimolecular mechanism, providing an opportunity to understand the factors that promote bimetallic H–H coupling. Covalently tethered diiridium catalysts evolve H2 from neutral water faster than monometallic catalysts, even at lower overpotential. The unexpected origin of this improvement is non-covalent supramolecular self-assembly into nanoscale aggregates that efficiently harvest light and form H–H bonds. Monometallic catalysts containing long-chain alkane substituents leverage the self-assembly to evolve H2 from neutral water at low overpotential and with rates close to the expected maximum for this light-driven water splitting reaction. Design parameters for holding multiple catalytic sites in close proximity and tuning catalyst microenvironments emerge from this work.Although the light-driven generation of hydrogen from water is a promising approach to renewable fuels, the H–H bond formation step represents a persistent mechanistic question. Now light-harvesting molecular catalysts have been shown to self-assemble into nanoscale aggregates that feature improved efficiency for photoelectrochemical H2 evolution. Hydrogen evolution is an important fuel-generating reaction that has been subject to mechanistic debate about the roles of monometallic and bimetallic pathways. The molecular iridium catalysts in this study undergo photoelectrochemical dihydrogen (H 2 ) evolution via a bimolecular mechanism, providing an opportunity to understand the factors that promote bimetallic H–H coupling. Covalently tethered diiridium catalysts evolve H 2 from neutral water faster than monometallic catalysts, even at lower overpotential. The unexpected origin of this improvement is non-covalent supramolecular self-assembly into nanoscale aggregates that efficiently harvest light and form H–H bonds. Monometallic catalysts containing long-chain alkane substituents leverage the self-assembly to evolve H 2 from neutral water at low overpotential and with rates close to the expected maximum for this light-driven water splitting reaction. Design parameters for holding multiple catalytic sites in close proximity and tuning catalyst microenvironments emerge from this work. Although the light-driven generation of hydrogen from water is a promising approach to renewable fuels, the H–H bond formation step represents a persistent mechanistic question. Now light-harvesting molecular catalysts have been shown to self-assemble into nanoscale aggregates that feature improved efficiency for photoelectrochemical H 2 evolution. |
| Author | Bonn, Annabell G. Jurado, Tamara Rose, Jamie Pitman, Catherine L. ter Horst, Marc A. Cloward, Isaac N. Miller, Alexander J. M. Liu, Tianfei Chambers, Matthew B. |
| Author_xml | – sequence: 1 givenname: Isaac N. surname: Cloward fullname: Cloward, Isaac N. organization: Department of Chemistry, University of North Carolina at Chapel Hill – sequence: 2 givenname: Tianfei orcidid: 0000-0002-9961-0137 surname: Liu fullname: Liu, Tianfei organization: Department of Chemistry, University of North Carolina at Chapel Hill, State Key Laboratory of Elemento-organic Chemistry, College of Chemistry, Nankai University – sequence: 3 givenname: Jamie surname: Rose fullname: Rose, Jamie organization: Department of Chemistry, University of North Carolina at Chapel Hill – sequence: 4 givenname: Tamara orcidid: 0009-0006-9574-4126 surname: Jurado fullname: Jurado, Tamara organization: Department of Chemistry, University of North Carolina at Chapel Hill – sequence: 5 givenname: Annabell G. surname: Bonn fullname: Bonn, Annabell G. organization: Department of Chemistry, University of North Carolina at Chapel Hill – sequence: 6 givenname: Matthew B. surname: Chambers fullname: Chambers, Matthew B. organization: Department of Chemistry, University of North Carolina at Chapel Hill – sequence: 7 givenname: Catherine L. surname: Pitman fullname: Pitman, Catherine L. organization: Department of Chemistry, University of North Carolina at Chapel Hill – sequence: 8 givenname: Marc A. surname: ter Horst fullname: ter Horst, Marc A. organization: Department of Chemistry, University of North Carolina at Chapel Hill – sequence: 9 givenname: Alexander J. M. orcidid: 0000-0001-9390-3951 surname: Miller fullname: Miller, Alexander J. M. email: ajmm@email.unc.edu organization: Department of Chemistry, University of North Carolina at Chapel Hill |
| BackLink | https://www.osti.gov/biblio/2578062$$D View this record in Osti.gov |
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| Title | Catalyst self-assembly accelerates bimetallic light-driven electrocatalytic H2 evolution in water |
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