Improving electronic structure methods to predict nano-optoelectronics and nano-catalyst functions.

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This report focuses on quantum chemistry and ab initio molecular dynamics (AIMD) calculations applied to elucidate the mechanism of the multi-step, 2-electron, electrochemical reduction of the green house gas molecule carbon dioxide (CO{sub 2}) to carbon monoxide (CO) in aqueous media. When combined with H{sub 2} gas to form synthesis ('syn') gas, CO becomes a key precursor to methane, methanol, and other useful hydrocarbon products. To elucidate the mechanism of this reaction, we apply computational electrochemistry which is a fledgling, important area of basic science critical to energy storage. This report highlights several approaches, including the calculation of redox potentials, ... continued below

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51 p.

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Nielsen, Ida Marie B.; Marzari, Nicola (Massachusetts Institute of Technology); Shelnutt, John Allen; Kulik, Heather J. (Massachusetts Institute of Technology); Medforth, Craig John (University of New Mexico, Albuquerque, NM) & Leung, Kevin October 1, 2009.

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This report is part of the collection entitled: Office of Scientific & Technical Information Technical Reports and was provided by UNT Libraries Government Documents Department to Digital Library, a digital repository hosted by the UNT Libraries. It has been viewed 16 times . More information about this report can be viewed below.

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Description

This report focuses on quantum chemistry and ab initio molecular dynamics (AIMD) calculations applied to elucidate the mechanism of the multi-step, 2-electron, electrochemical reduction of the green house gas molecule carbon dioxide (CO{sub 2}) to carbon monoxide (CO) in aqueous media. When combined with H{sub 2} gas to form synthesis ('syn') gas, CO becomes a key precursor to methane, methanol, and other useful hydrocarbon products. To elucidate the mechanism of this reaction, we apply computational electrochemistry which is a fledgling, important area of basic science critical to energy storage. This report highlights several approaches, including the calculation of redox potentials, the explicit depiction of liquid water environments using AIMD, and free energy methods. While costly, these pioneering calculations reveal the key role of hydration- and protonation-stabilization of reaction intermediates, and may inform the design of CO{sub 2}-capture materials as well as its electrochemical reduction. In the course of this work, we have also dealt with the challenges of identifying and applying electronic structure methods which are sufficiently accurate to deal with transition metal ion complex-based catalyst. Such electronic structure methods are also pertinent to the accurate modeling of actinide materials and therefore to nuclear energy research. Our multi-pronged effort towards achieving this titular goal of the LDRD is discussed.

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51 p.

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  • Report No.: SAND2009-6425
  • Grant Number: AC04-94AL85000
  • DOI: 10.2172/1001019 | External Link
  • Office of Scientific & Technical Information Report Number: 1001019
  • Archival Resource Key: ark:/67531/metadc835460

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  • October 1, 2009

Added to The UNT Digital Library

  • May 19, 2016, 3:16 p.m.

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  • Dec. 5, 2016, 8:47 p.m.

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Nielsen, Ida Marie B.; Marzari, Nicola (Massachusetts Institute of Technology); Shelnutt, John Allen; Kulik, Heather J. (Massachusetts Institute of Technology); Medforth, Craig John (University of New Mexico, Albuquerque, NM) & Leung, Kevin. Improving electronic structure methods to predict nano-optoelectronics and nano-catalyst functions., report, October 1, 2009; United States. (digital.library.unt.edu/ark:/67531/metadc835460/: accessed September 21, 2017), University of North Texas Libraries, Digital Library, digital.library.unt.edu; crediting UNT Libraries Government Documents Department.