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Pyridinium-Catalyzed Electrochemical and Photoelectrochemical Conversion of Carbon Dioxide to Fuels.: (English)

Pyridinium-Catalyzed Electrochemical and Photoelectrochemical Conversion of Carbon Dioxide to Fuels.: (English)

          
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About the Book

Although various electrochemical and photoelectrochemical schemes for the reduction of CO2 to storable fuels have been developed over the past few decades, all approaches have produced systems having excessive overpotentials, limited stability, and low product yields. Previous work in the Bocarsly lab has demonstrated that CO2 can be converted into methanol, a useful bulk chemical and potential fuel, at ∼ 25% faradaic efficiency using a hydrogenated palladium electrode. In contrast to prior work in this area, a homogenous pyridinium-based catalyst was employed to reduce CO2 at minimal overpotential. This work expands upon this electrochemical system by employing a photoelectrode capable of using light energy to effect the reduction of CO2 to methanol. The new photoelectrochemical system using a p-GaP photocathode and the same homogeneous pyridinium catalyst, is the first reported instance of a system able to produce methanol at near 100% faradaic yield at an underpotential. Thus, the process offers the prospect of a pure solar energy conversion system requiring no input of electrical energy. Furthermore, the mechanism of pyridinium-catalyzed CO2 reduction in our electrochemical and photoelectrochemical systems has been studied, with a proposed mechanism reported. Various electrochemical and computational methods were employed to understand the complete 6 e- reduction of CO2 to methanol. Intermediates such as formic acid and formaldehyde were observed along the route to methanol. Surprisingly, this single pyridinium catalyst is capable of reducing a variety of different species through various coordinative interactions. This works also extends the knowledge of pyridinium-based catalysts by examining various analogues and their observed CO2 reduction products. Surprisingly, even higher order products such as 2-propanol were obtained using specific pyridine derivatives. Few reduction schemes exist in the literature for the production of such highly reduced species. The reduction of CO 2 to 2-propanol in both electrochemical and photoelectrochemical systems is described, along with key mechanistic information.


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Product Details
  • ISBN-13: 9781243643575
  • Publisher: Proquest, Umi Dissertation Publishing
  • Publisher Imprint: Proquest, Umi Dissertation Publishing
  • Height: 254 mm
  • No of Pages: 144
  • Series Title: English
  • Weight: 299 gr
  • ISBN-10: 1243643579
  • Publisher Date: 06 Sep 2011
  • Binding: Paperback
  • Language: English
  • Returnable: N
  • Spine Width: 9 mm
  • Width: 203 mm


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Pyridinium-Catalyzed Electrochemical and Photoelectrochemical Conversion of Carbon Dioxide to Fuels.: (English)
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