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Published on: July 27, 2018
Spectral observation of conversion between ionized vs. non-ionized proton-coupled electron transfer interfaces
Elizabeth R Young1, Joel Rosenthal, Daniel G Nocera
1Department of Chemistry, Massachusetts Institute of Technology, Cambridge, MA 02139-4307, USA.
Modular assembly of proton-coupled electron transfer (PCET) networks is achieved using two-point hydrogen bonding. The proton configuration within the interface can be determined by knowing the conjugate acid pK(a) values.
Area of Science:
- Supramolecular Chemistry
- Chemical Physics
Background:
- Two-point hydrogen bonding offers a modular approach for constructing complex molecular assemblies.
- Proton-coupled electron transfer (PCET) networks are crucial for various chemical and biological processes.
Purpose of the Study:
- To present a system for the modular assembly of PCET networks using specific hydrogen bonding interactions.
- To demonstrate a method for determining the proton configuration within these PCET interfaces.
Main Methods:
- Utilizing two-point hydrogen bonding between acid and base functionalities, specifically an amidinium and a two-point anionic partner.
- Employing the pK(a) values of conjugate acids to predict and determine proton configurations.
Main Results:
- Successfully assembled PCET networks with a defined interface.
- Established a correlation between pK(a) values and the resulting proton configuration within the interface.
Conclusions:
- Two-point hydrogen bonding provides a versatile and predictable strategy for designing PCET networks.
- The pK(a) values of conjugate acids are key parameters for controlling and understanding proton positioning in these systems.
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