Energy Efficient Catalytic Activation of Hydrogen peroxide for Green Chemical Processes: Final Report
A new, highly energy efficient approach for using catalytic oxidation chemistry in multiple fields of technology has been pursued. The new catalysts, called TAML® activators, catalyze the reactions of hydrogen peroxide and other oxidants for the exceptionally rapid decontamination of noninfectious simulants (B. atrophaeus) of anthrax spores, for the energy efficient decontamination of thiophosphate pesticides, for the facile, low temperature removal of color and organochlorines from pulp and paper mill effluent, for the bleaching of dyes from textile mill effluents, and for the removal of recalcitrant dibenzothiophene compounds from diesel and gasoline fuels. Highlights include the following: 1) A 7-log kill of Bacillus atrophaeus spores has been achieved unambiguously in water under ambient conditions within 15 minutes. 2) The rapid total degradation under ambient conditions of four thiophosphate pesticides and phosphonate degradation intermediates has been achieved on treatment with TAML/peroxide, opening up potential applications of the decontamination system for phosphonate structured chemical warfare agents, for inexpensive, easy to perform degradation of stored and aged pesticide stocks (especially in Africa and Asia), for remediation of polluted sites and water bodies, and for the destruction of chemical warfare agent stockpiles. 3) A mill trial conducted in a Pennsylvanian bleached kraft pulp mill has established that TAML catalyst injected into an alkaline peroxide bleach tower can significantly lower color from the effluent stream promising a new, more cost effective, energy-saving approach for color remediation adding further evidence of the value and diverse engineering capacity of the approach to other field trials conducted on effluent streams as they exit the bleach plant. 4) Dibenzothiophenes (DBTs), including 4,6-dimethyldibenzothiophene, the most recalcitrant sulfur compounds in diesel and gasoline, can be completely removed from model gasoline (octane or decane) at low temperature and ambient pressure via treatment with a TAML activator and hydrogen peroxide in a two-phase system consisting of the fuel as the first phase and a water/tertiary butanol second phase. The DBTs are oxidized to sulphones (or sulfoxides), which then completely extract into the water/t-butanol phase. Treatment of commercial diesel spiked with DBT under the same conditions results in compete DBT oxidation. In contrast with the octane and decane experiments, removal to the water/t-butanol phase is not yet complete and is being further optimized. Analysis by the sulfur specific GC-FPD technique suggests that >70% sulfur compounds are removed from unspiked diesel after one treatment. Further treatments are being investigated. The GC-FPD results will be checked by total sulfur analysis methodology.
- Research Organization:
- Carnegie Mellon University, Pittsburgh, PA
- Sponsoring Organization:
- USDOE Office of Science (SC)
- DOE Contract Number:
- FG02-03ER63587
- OSTI ID:
- 834329
- Report Number(s):
- A001793- Final Report; DE-FG02-03ER63587-DOE-COLLINS
- Country of Publication:
- United States
- Language:
- English
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catalysis
energy efficiency
hydrogen peroxide
energy efficient pulp and paper effluent treatment
energy efficient textiles industry effluent treatment
diesel desulfurization
gasoline desulfurization
chemical warfare and terrorism agent decontamination
biological warfare and terrorism agent decontamination
energy efficient pesticide decontamination