Two-stage Catalytic Reduction of NOx with Hydrocarbons
A two-stage system for the catalytic reduction of NO from lean-burn natural gas reciprocating engine exhaust is investigated. Each of the two stages uses a distinct catalyst. The first stage is oxidation of NO to NO{sub 2} and the second stage is reduction of NO{sub 2} to N{sub 2} with a hydrocarbon. The central idea is that since NO{sub 2} is a more easily reduced species than NO, it should be better able to compete with oxygen for the combustion reaction of hydrocarbon, which is a challenge in lean conditions. Early work focused on demonstrating that the N{sub 2} yield obtained when NO{sub 2} was reduced was greater than when NO was reduced. NO{sub 2} reduction catalysts were designed and silver supported on alumina (Ag/Al{sub 2}O{sub 3}) was found to be quite active, able to achieve 95% N{sub 2} yield in 10% O{sub 2} using propane as the reducing agent. The design of a catalyst for NO oxidation was also investigated, and a Co/TiO{sub 2} catalyst prepared by sol-gel was shown to have high activity for the reaction, able to reach equilibrium conversion of 80% at 300 C at GHSV of 50,000h{sup -1}. After it was shown that NO{sub 2} could be more easily reduced to N{sub 2} than NO, the focus shifted on developing a catalyst that could use methane as the reducing agent. The Ag/Al{sub 2}O{sub 3} catalyst was tested and found to be inactive for NOx reduction with methane. Through iterative catalyst design, a palladium-based catalyst on a sulfated-zirconia support (Pd/SZ) was synthesized and shown to be able to selectively reduce NO{sub 2} in lean conditions using methane. Development of catalysts for the oxidation reaction also continued and higher activity, as well as stability in 10% water, was observed on a Co/ZrO{sub 2} catalyst, which reached equilibrium conversion of 94% at 250 C at the same GHSV. The Co/ZrO{sub 2} catalyst was also found to be extremely active for oxidation of CO, ethane, and propane, which could potential eliminate the need for any separate oxidation catalyst. At every stage, catalyst synthesis was guided by the insights gained through detailed characterization of the catalysts using many surface and bulk analysis techniques such as X-ray diffraction, X-ray photoelectron spectroscopy, Temperature-programmed Reduction, Temperature programmed Desorption, and Diffuse Reflectance InfraRed Fourier Transform Spectroscopy as well as steady state reaction experiments. Once active catalysts for each stage had been developed, a physical mixture of the two catalysts was tested for the reduction of NO with methane in lean conditions. These experiments using a mixture of the catalysts produced N2 yields as high as 90%. In the presence of 10% water, the catalyst mixture produced 75% N{sub 2} yield, without any optimization. The dual catalyst system developed has the potential to be implemented in lean-burn natural gas engines for reducing NOx in lean exhaust as well as eliminating CO and unburned hydrocarbons without any fuel penalty or any system modifications. If funding continues, future work will focus on improving the hydrothermal stability of the system to bring the technology closer to application.
- Research Organization:
- The Ohio State Univ., Columbus, OH (United States)
- Sponsoring Organization:
- USDOE
- DOE Contract Number:
- FC26-02NT41610
- OSTI ID:
- 876786
- Country of Publication:
- United States
- Language:
- English
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