Improving electronic structure methods to predict nano-optoelectronics and nano-catalyst functions.
- Massachusetts Institute of Technology
- University of New Mexico, Albuquerque, NM
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.
- Research Organization:
- Sandia National Laboratories
- Sponsoring Organization:
- USDOE
- DOE Contract Number:
- AC04-94AL85000
- OSTI ID:
- 1001019
- Report Number(s):
- SAND2009-6425
- Country of Publication:
- United States
- Language:
- English
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Related Subjects
10 SYNTHETIC FUELS
ACTINIDES
CARBON DIOXIDE
CARBON MONOXIDE
CHEMISTRY
DESIGN
ELECTROCHEMISTRY
ELECTRONIC STRUCTURE
ENERGY STORAGE
FREE ENERGY
HYDRATION
HYDROCARBONS
METHANE
METHANOL
NUCLEAR ENERGY
PRECURSOR
REACTION INTERMEDIATES
REDOX POTENTIAL
SIMULATION
SYNTHESIS
TRANSITION ELEMENTS
WATER