- Metal-Catalyzed Oxygenation Mechanisms
- Extraction and Separation Processes
- Catalytic C–H Functionalization Methods
- Advancements in Battery Materials
- Recycling and Waste Management Techniques
- Synthesis and Catalytic Reactions
- Porphyrin and Phthalocyanine Chemistry
- Radical Photochemical Reactions
- Metal complexes synthesis and properties
- Water Systems and Optimization
- Asymmetric Hydrogenation and Catalysis
- Environmental Education and Sustainability
- IoT-based Smart Home Systems
- Photosynthetic Processes and Mechanisms
- Metalloenzymes and iron-sulfur proteins
- Crystallization and Solubility Studies
- Water Quality Monitoring Technologies
- Energy and Environment Impacts
- Social Acceptance of Renewable Energy
- CO2 Reduction Techniques and Catalysts
- Sulfur-Based Synthesis Techniques
- X-ray Diffraction in Crystallography
Duke University
2024
Yale University
2015-2020
Worcester Polytechnic Institute
2014-2017
ConspectusProton-coupled electron transfer (PCET) covers a wide range of reactions involving the transfer(s) electrons and protons. The best-known PCET reaction, hydrogen atom (HAT), has been studied in detail for more than century. HAT is generally described as concerted (H• ≡ H+ + e–) from one group to another, Y H–X → Y–H X, but strict definition difficult establish. Distinctions are challenging when "H•" involves e– that to/from spatially distinct sites or even completely separate...
A new reaction for carbon: Separating the electron and proton allows C–H bonds to be cleaved formed with mild reagents.
The selective transformation of C–H bonds is a longstanding challenge in modern chemistry. A recent report details oxidation via multiple-site concerted proton–electron transfer (MS-CPET), where the proton and electron bond are transferred to separate sites. Reactivity at specific was achieved by appropriate positioning an internal benzoate base. Here, we extend that reactions series molecules with differently substituted fluorenyl-benzoates varying outer-sphere oxidants. These results probe...
In order to facilitate the development of recycling technologies for rare earth magnets from postconsumer products, we present herein an analysis neodymium (Nd) content in shredder scrap. This waste stream has been chosen on basis current business practices steel, aluminum, and copper cars household appliances, which contain significant amounts magnets. Using approximations based literature data, have calculated average Nd ferrous product be between 0.13 0.29 kg per ton A value considering...
Abstract Biological [Fe‐S] clusters are increasingly recognized to undergo proton‐coupled electron transfer (PCET), but the site of protonation, mechanism, and role for PCET remains largely unknown. Here we explore this reactivity with synthetic model clusters. Protonation arylthiolate‐ligated [4Fe‐4S] cluster [Fe 4 S (SAr) ] 2− ( 1 , SAr=S‐2,4‐6‐( i Pr) 3 C 6 H 2 ) leads thiol dissociation, reversibly forming L] 1− ArSH (L=solvent, and/or conjugate base). Solutions +ArSH react nitroxyl...
Abstract Analysis of slag from steel mini‐mills reveals that substantial amounts the rare earth element neodymium (Nd, an average 0.032 wt % in tested samples) are present this waste product. This provides insight into a currently unknown part lifecycle after end‐of‐life for magnet motors. Furthermore, reprocess scrap is therefore important potential source Nd especially countries without established mining operations or direct access to ores.
Photoredox catalysis using proton-coupled electron transfer (PCET) has emerged as a powerful method for bond transformations. We previously employed traditional chemical oxidants to achieve multiple-site concerted proton–electron (MS-CPET) activation of C–H in proof-of-concept fluorenyl-benzoate substrate. As described here, photoredox oxidation the follows same rate constant vs driving force trend determined thermal MS-CPET. Analogous enables and H/D exchange number additional substrates...
This work demonstrates the use of hydroxylamine-based amination reagents RSO2NH-OAc for nondirected, Cu-catalyzed benzylic C-H bonds. The can be prepared on a gram scale, are benchtop stable, and provide products with up to 86% yield. Mechanistic studies established reactivity toluene as substrate reveal ligand-promoted, mechanism proceeding through Ph-CH2(NTsOAc) major intermediate. Stoichiometric produce Ph-CH2-NHTs suggests two-cycle, radical pathway amination, in which decomposition...
Patients' report of bowel movement consistency is unreliable. We demonstrate the feasibility long-term automated stool image data collection using a novel Smart Toilet and evaluate deterministic computer-vision analytic approach to assess form according Bristol Stool Form Scale (BSFS).