A5057820198- Electrocatalysts for Energy Conversion
- Electrochemical Analysis and Applications
- CO2 Reduction Techniques and Catalysts
- Radical Photochemical Reactions
- Crystallization and Solubility Studies
- X-ray Diffraction in Crystallography
- Electrochemical sensors and biosensors
- Semiconductor materials and devices
- Molecular Junctions and Nanostructures
- Fuel Cells and Related Materials
- Metalloenzymes and iron-sulfur proteins
- Microbial Fuel Cells and Bioremediation
- Crystallography and molecular interactions
- Conducting polymers and applications
- Ammonia Synthesis and Nitrogen Reduction
- Asymmetric Hydrogenation and Catalysis
- Axial and Atropisomeric Chirality Synthesis
- Advanced Photocatalysis Techniques
- Metal complexes synthesis and properties
- Electronic and Structural Properties of Oxides
- Piperaceae Chemical and Biological Studies
- Process Optimization and Integration
- Chemical Synthesis and Reactions
- Hybrid Renewable Energy Systems
- Machine Learning in Materials Science
University of Utah
2022-2024
The University of Texas at Austin
2018-2021
The first general enantioselective alkyl-Nozaki-Hiyama-Kishi (NHK) coupling reactions are disclosed herein by employing a Cr-electrocatalytic decarboxylative approach. Using easily accessible aliphatic carboxylic acids (via redox-active esters) as alkyl nucleophile synthons, in combination with aldehydes and enabling additives, chiral secondary alcohols produced good yield high enantioselectivity under mild reductive electrolysis. This reaction, which cannot be mimicked using stoichiometric...
The utility of transition metal hydride catalyzed hydrogen atom transfer (MHAT) has been widely demonstrated in organic transformations such as alkene isomerization and hydrofunctionalization reactions. However, the highly reactive nature radical intermediates hindered mechanistic insight into this pivotal reaction. Recent advances electrochemical MHAT have opened up possibility for new analytical approaches diagnosis. Here, we report a voltammetric interrogation Co-based reactivity,...
Electrosynthesis is a popular, environmentally friendly substitute for conventional organic methods. It involves using charge transfer to stimulate chemical reactions through the application of potential or current between two electrodes. In addition electrode materials and type reactor employed, strategies controlling have an impact on yields, product distribution, reaction mechanism. this Review, recent advances related electroanalysis applied in electrosynthesis were discussed. The first...
Biomass is an abundantly available, underutilized feedstock for the production of bulk and fine chemicals, polymers, sustainable biodegradable plastics that are traditionally sourced from petrochemicals. Among potential feedstocks, 2,5-furan dicarboxylic acid (FDCA) stands out its to be converted higher-value polymeric materials such as polyethylene furandicarboxylate (PEF), a bio-based plastic alternative. In this study, sustainable, electrocatalytic oxidation stable furan molecule...
Photoelectrochemical (PEC) device efficiency depends heavily on the energetics and band alignment of semiconductor|overlayer junction. Exerting energetic control over these junctions via molecular functionalization is an extremely attractive strategy. Herein we report a study structure–function relationship between chemically functionalized pSi(111) resulting solar fuels performance. Specifically, highlight interplay chemical structure electronic coupling attached molecule underlying...
This work provides insight into carrier dynamics in a model photoelectrochemical system comprised of semiconductor, metal oxide, and metal. To isolate from catalysis, common catalytic (Pt) is used concert with an outer-sphere redox couple. Silicon (111) substrates were surface-functionalized electronegative aryl moieties (p-nitrophenyl m-dinitrophenyl). A mixed monolayer using p-nitrophenyl/methyl exhibited high surface quality as determined by X-ray photoelectron spectroscopy (low SiOx...
Abstract Bioelectrocatalytic synthesis is the conversion of electrical energy into value‐added products using biocatalysts. These methods merge specificity and selectivity biocatalysis energy‐related electrocatalysis to address challenges in sustainable pharmaceuticals, commodity chemicals, fuels, feedstocks fertilizers. However, specialized experimental setups domain knowledge for bioelectrocatalysis pose a significant barrier adoption. This review introduces key concepts...
The utility of transition metal hydride catalyzed hydrogen atom transfer (MHAT) has been widely demonstrated in organic transformations such as alkene isomerization and hydrofunctionalization reactions. However, the highly reactive nature radical intermediates hindered mechanistic insight into this pivotal reaction. Recent advances electrochemical MHAT have opened possibility for new analytical approaches diagnosis. Here, we report a voltammetric interrogation Co-based reactivity, describing...
In this work, we report the effects of NNS-thiolate ligands and nuclearity (monomer, dimer) on stability iron complexes related to active site monoiron hydrogenase (Hmd). A thermally stable iron(II) dicarbonyl motif is core feature site, but coordination features that lead property have not been independently evaluated for their contributions {Fe(CO)2}2+ stability. As such, non-bulky bulky benzothiazoline (thiolate precursors) were synthesized characterized. The use thiolate low-temperature...
Shahid Rasul opened the discussion of introductory Spiers Memorial Lecture by Toshio Fuchigmai: From your overview (https://doi.org/10.1039/d3fd00129f), which top three electrochemical reactions for electrosynthesis are most suitable commercialization, considering significant challenge scaling in e
The area of organic electrocatalysis has been growing in importance as many new transformations have developed and previously known are adapted to be accomplished electrochemically. As the field synthetic electrochemistry emerges, it is becoming ever more important study mechanisms these electrocatalytic reactions. Understanding mechanics chemical processes how they coupled electrode critical for continuing expand utility electrocatalysis. Radical based hydrofunctionalization alkenes through...
Electrochemical organic synthesis shows promise for the sustainable of agrochemical and pharmaceutically relevant molecules. However, complexity integrating electrochemical methods often leads to overlooked reaction parameters. For example, electrolyte salts are used decrease resistivity cell traditionally viewed as benign species in systems. electroorganic literature is filled with examples which changing identity impacts selectivity significantly, implying that these ‘benign’ molecules...
Bioelectrocatalysis involves the use of biomaterials to catalyze redox reactions at an electrode. Biocatalysis offers improved selectivity and typically milder reaction conditions, while electrocatalysis can involve renewable energy as electron source. Cobalamin (B 12 ) dependent enzymes C-C C-N bond forming via radical mechanisms through formation a Co(III)-alkyl intermediate. Homolysis Co(III)-C leads coupling with various substrates form product. However, these alkyl radicals react...
Automated electrochemistry platforms provide a pathway for speeding up the discovery and optimization of electrochemical systems, especially when broad range molecules reaction conditions must be explored. 1-3 Additionally, incorporation machine learning enables closed-loop campaigns, where obtained experimental data guides selection next set parameters to test. This type autonomous exploration is ideally suited study enzyme electrocatalysis, as combinatorics different enzymes, substrates,...
Abstract Photoelectrochemical solar energy conversion to chemical products is a promising avenue towards renewable fuels, and TiO 2 deposition on semiconductor photocathodes widespread surface protection strategy. However, the electronic, thermodynamic, kinetic effects of layers interfacial energetics remains poorly understood. Here, electrochemical data (photocurrent onset flatband potentials) p ‐Si(111)|TiO |Pt collected in contact with an outer‐sphere redox couple. We find that potentials...
We explore the often neglected impact of supporting electrolyte on homogeneous electrocatalytic mechanisms using catalytic reduction benzyl chlorides via Co and Fe tetraphenylporphyrins as a model reaction.
The first general enantioselective alkyl-Nozaki-Hiyama-Kishi (NHK) coupling reactions are disclosed herein by em-ploying a Cr-electrocatalytic decarboxylative approach. Using easily accessible aliphatic carboxylic acids (via redox-active esters) as alkyl nucleophile synthons, in combination with aldehydes and enabling additives, chiral secondary alcohols produced good yield high enantioselectivity under mild reductive electrolysis. This reaction, which cannot be mimicked using stoichiometric...
Robert Francke opened a general discussion of the paper by Bernardo Antonio Frontana-Uribe: The plot ionic conductivity vs. supporting electrolyte concentration in your (https://doi.org/10.1039/d3fd00064h), appears to follow discontinuous function cyrene–EtOH (1 : 1). How can this unusual be
Mickaël Avanthay opened discussion of the paper by Lutz Ackermann: Compared to direct, non-photochemical methods, do you see a higher conversion or more selectivity? Ackermann replied: We primarily observed better conversions. Belen Batanero enquired: Even when this is mediated process and considering that
Shelley D. Minteer opened discussion of the paper by T. Leo Liu: Based on your results, it seems imperative that in field electrosynthesis we need to focus more situ and operando techniques fundamentally understand our systems. What do you think are best for studyin
Dylan G. Boucher opened the discussion of paper by Talal Ashraf: What does surface termination look like after electrolysis? BDD chemistry can change quite substantially during process. Ashraf responded: Since we are using boron-doped diamond with a high concentration boron (2000–5000