| NSF Org: |
CHE Division Of Chemistry |
| Recipient: |
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| Initial Amendment Date: | December 18, 2014 |
| Latest Amendment Date: | February 11, 2016 |
| Award Number: | 1454747 |
| Award Instrument: | Continuing Grant |
| Program Manager: |
Robin McCarley
CHE Division Of Chemistry MPS Directorate for Mathematical and Physical Sciences |
| Start Date: | February 1, 2015 |
| End Date: | January 31, 2021 (Estimated) |
| Total Intended Award Amount: | $650,000.00 |
| Total Awarded Amount to Date: | $650,000.00 |
| Funds Obligated to Date: |
FY 2016 = $130,000.00 |
| History of Investigator: |
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| Recipient Sponsored Research Office: |
1776 E 13TH AVE EUGENE OR US 97403-1905 (541)346-5131 |
| Sponsor Congressional District: |
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| Primary Place of Performance: |
1253 University of Oregon Eugene OR US 97403-1253 |
| Primary Place of
Performance Congressional District: |
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| Unique Entity Identifier (UEI): |
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| Parent UEI: |
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| NSF Program(s): | Chemistry of Life Processes |
| Primary Program Source: |
01001617DB NSF RESEARCH & RELATED ACTIVIT |
| Program Reference Code(s): |
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| Program Element Code(s): |
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| Award Agency Code: | 4900 |
| Fund Agency Code: | 4900 |
| Assistance Listing Number(s): | 47.049 |
ABSTRACT
Hydrogen sulfide (H2S) is historically recognized for its malodorous rotten-egg smell, but is now accepted to be involved in diverse and important biological signaling processes. The fundamental chemistry by which H2S exerts this biological action, however, remains unclear. This project focuses on using synthetic model complexes to study H2S reactivity, with the goal of providing a greater understanding of how H2S reacts with important biological targets. Specific goals include understanding how H2S reacts with metal-containing biomolecules and how sulfur-rich compounds react in relation to H2S release and storage. The educational component of this project focuses on providing hands-on laboratory-based experiments for local middle and high school students while also providing career-development mentoring opportunities for college and graduate students.
With this CAREER Award, the Chemistry of Life Processes Program in the Chemistry Division is funding Professor Michael Pluth from the University of Oregon to investigate the mechanisms by which H2S interacts with bioinorganic and bioorganic targets. Synthetic small-molecule model complexes will be used to investigate the mechanisms by which H2S reacts with transition-metal containing biomolecules. Parallel investigations will focus on establishing new methods of preparing small-molecule persulfides and understanding how these compounds react with biologically-relevant small molecules. Both foci share the goal of providing greater insight into the fundamental chemistry associated with H2S-mediated biological signaling. This CAREER award also supports the expansion of an outreach program co-developed by Professor Pluth that addresses reduced lab-based science education for local students due to state budget cuts. This program brings local middle and high school students to the University of Oregon to participate in STEM-based outreach activities and provides leadership and mentoring opportunities for high school, undergraduate, and graduate students.
PUBLICATIONS PRODUCED AS A RESULT OF THIS RESEARCH
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PROJECT OUTCOMES REPORT
Disclaimer
This Project Outcomes Report for the General Public is displayed verbatim as submitted by the Principal Investigator (PI) for this award. Any opinions, findings, and conclusions or recommendations expressed in this Report are those of the PI and do not necessarily reflect the views of the National Science Foundation; NSF has not approved or endorsed its content.
Research activities from this grant have focused on advancing the fundamental chemistry of small molecule reactive sulfur species, including hydrogen sulfide (H2S). H2S is an important small molecule signaling agent in biology that plays important functions in different physiological processes and disease states. The chemical mechanisms by which H2S and related small molecules react with biologically-relevant metal-containing species or other reactive sulfur species remain underdeveloped.
The intellectual merit resulting from this grant includes the (1) development and investigation of simple tri- and tetra-sulfides as H2S donors; (2) new insights into the reaction of H2S with transition metal complexes; (3) development and application of synthetic small molecules receptors that can bind hydrosulfide (HS-) reversibly; and (4) chemical platforms for the binding and/or delivery of hydrogen selenide (H2Se) / hydroselenide (HSe-). Tetrasulfides were found to be efficient H2S donors, and the H2S release upon reaction with biologically-relevant thiols was examined in vitro and in live cells. Reactions of H2S/HS- with different transition metal porphyrin species further clarified binding and/or reduction reactions mediated by H2S/HS- at different metal centers. Experiments with pyridine-diimine zinc complexes established that complementary hydrogen bond accepting groups on the ligand could enable reversible HS- binding. These results were further expanded to demonstrate that synthetic anion binding receptors could be used to bind HS- reversibly. This work established that HS- may be a previously overlooked target for anion recognition and binding. Further expansion of this work led to the first examples of reversible HSe- binding to synthetic receptors. Related investigations into small molecule selenium species provided an early example of a well-characterized H2Se releasing donor system that results in H2Se upon donor hydrolysis.
The broader impacts resulting from this grant include (1) an outreach program in which local middle school students come to the University of Oregon to participate in hands-on science education; (2) training of graduate students and postdoctoral researchers who have gone on to STEM careers; and (3) training of undergraduate students through participation in research.
Last Modified: 03/24/2021
Modified by: Michael D Pluth
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