Final Report: Sustainable Catalytic Treatment of Waste Ion Exchange Brines for Reuse During Oxyanion Treatment in Drinking Water

EPA Grant Number: R835174
Title: Sustainable Catalytic Treatment of Waste Ion Exchange Brines for Reuse During Oxyanion Treatment in Drinking Water
Investigators: Werth, Charles J , Strathmann, Timothy J.
Institution: University of Illinois at Urbana-Champaign
EPA Project Officer: Hiscock, Michael
Project Period: December 1, 2011 through November 30, 2014 (Extended to November 30, 2016)
Project Amount: $500,000
RFA: Research and Demonstration of Innovative Drinking Water Treatment Technologies in Small Systems (2011) RFA Text |  Recipients Lists
Research Category: Drinking Water , Water

Objective:

The objectives of this work were to 1) identify palladium (Pd) catalyst formulations with sufficient activity to reduce different target oxyanions in brine solutions, 2) determine if catalyst activity can be maintained for extended periods of operations, and 3) assess the economic and environmental life cycle costs of hybrid ion exchange/catalyst treatment systems.  

Summary/Accomplishments (Outputs/Outcomes):

Advancements were made in developing new catalysts and catalytic treatment processes for drinking water treatment of both nitrate and perchlorate.  Regarding nitrate treatment, we demonstrated that a hybrid ion exchange (IX) – catalytic treatment system for nitrate is technically feasible, and can have a lower environmental impact than IX alone, when sulfate and bicarbonate ion concentrations are <80 mg/L, and nitrate reduction activity is similar to that in batch reactors.  We determined this by first developing a hybrid IX–catalytic treatment model with separate treatment and regeneration cycles. We used this to evaluate treatment of 1 billion gallons of nitrate-contaminated source water at a 0.5 MGD water treatment plant. Switching from a conventional IX system with a two bed volume regeneration to a hybrid system with the same regeneration length and sequencing batch catalytic reactor for treatment would save 76% in salt cost.  We then extended this work by performing a life cycle assessment of the hybrid IX–catalyst system.  Environmental impacts of the hybrid IX–catalyst systems were evaluated for both sequencing-batch and continuous-flow packed-bed reactor designs based on laboratory results, and environmental impacts of the sequencing-batch hybrid system were found to be only 38-81% of those of conventional IX.  Unfortunately, the sequencing batch reactor is not a practically useful treatment approach at a water treatment plant, due to catalyst breakdown during mixing and poor catalyst recovery, and the environmental impacts of the hybrid system with a packed-bed reactor were far greater than IX alone.  Therefore, we focused on developing new packed-bed reactors with markedly higher rates of nitrate reduction, and focused specifically on developing trickle-bed reactors (TBR) for nitrate treatment in both waste brine and potable water. Gas and liquid flow rates in the TBRs were varied to optimize performance, as well as catalyst metal loadings and catalyst support sizes.  We obtained the highest rates of nitrate reduction ever reported in practically useful flow-through reactors.  However, based on economic analyses, improvements in reactor performance are still needed to make either hybrid ion exchange (IX)–catalytic treatment technology, or direct catalytic water treatment, cost competitive.  Specifically, improvements in TBR design are needed to overcome hydrogen mass transfer limitations from the gas to the liquid phase. Regarding perchlorate treatment, we developed a suite of bio-inspired complex-nanoparticle hybrid catalyst materials for aqueous phase perchlorate reduction, based on using a hydrogenation metal (e.g., Pd, platinum (Pt), rhodium (Rh)), coupled with a rhenium (Re) complex, all deposited on activated carbon (AC).  

Conclusions:

The primary achievements were (i) developing novel methodologies to selectively synthesize a number of rhenium complexes with controlled structure and activity, (ii) determining the surface reaction mechanisms that control catalyst activity and stability during water treatment, and (iii) using knowledge of these mechanisms to create more active and stable catalysts.  With respect to the third achievement, we determined that noble metal catalysts, which are more active for perchlorate reduction intermediates, result in a more stable catalyst during perchlorate treatment in drinking water.


Journal Articles on this Report : 14 Displayed | Download in RIS Format

Other project views: All 57 publications 15 publications in selected types All 15 journal articles
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Journal Article Bergquist AM, Choe JK, Strathmann TJ, Werth CJ. Evaluation of a hybrid ion exchange-catalyst treatment technology for nitrate removal from drinking water. Water Research 2016;96:177-187. R835174 (2014)
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  • Journal Article Bergquist AM, Bertoch M, Gildert G, Strathmann TJ, Werth CJ. Catalytic denitrification in a trickle bed reactor: ion exchange waste brine treatment. Journal of the American Water Works Association 2017;109(5):E129-E151. R835174 (Final)
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  • Journal Article Bertoch M, Bergquist AM, Gildert G, Strathmann TJ, Werth CJ. Catalytic nitrate removal in a trickle bed reactor: direct drinking water treatment. Journal of the American Water Works Association 2017;109(5):E144-E171. R835174 (Final)
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  • Journal Article Chen X, Huo X, Liu J, Wang Y, Werth CJ, Strathmann TJ. Exploring beyond palladium:catalytic reduction of aqueous oxyanion pollutants with alternative platinum group metals and new mechanistic implications. Chemical Engineering Journal 2017;313:745-752. R835174 (Final)
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  • Journal Article Choe JK, Mehnert MH, Guest JS, Strathmann TJ, Werth CJ. Comparative assessment of the environmental sustainability of existing and emerging perchlorate treatment technologies for drinking water. Environmental Science & Technology 2013;47(9):4644-4652. R835174 (2012)
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  • Journal Article Choe JK, Boyanov MI, Liu J, Kemner KM, Werth CJ, Strathmann TJ. X-ray spectroscopic characterization of immobilized rhenium species in hydrated rhenium–palladium bimetallic catalysts used for perchlorate water treatment. The Journal of Physical Chemistry C 2014;118(22):11666-11676. R835174 (2014)
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  • Journal Article Choe JK, Bergquist AM, Jeong S, Guest JS, Werth CJ, Strathmann TJ. Performance and life cycle environmental benefits of recycling spent ion exchange brines by catalytic treatment of nitrate. Water Research 2015;80:267-280. R835174 (2014)
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  • Journal Article Liu J, Choe JK, Sasnow Z, Werth CJ, Strathmann TJ. Application of a Re–Pd bimetallic catalyst for treatment of perchlorate in waste ion-exchange regenerant brine. Water Research 2013:47(1):91-101. R835174 (2012)
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  • Journal Article Liu J, Choe JK, Wang Y, Shapley JR, Werth CJ, Strathman TJ. Bioinspired complex-nanoparticle hybrid catalyst system for aqueous perchlorate reduction:rhenium speciation and its influence on catalyst activity. ACS Catalysis 2015;5(2):511-522. R835174 (2014)
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  • Journal Article Liu J, Chen X, Wang Y, Strathmann TJ, Werth CJ. Mechanism and mitigation of the decomposition of an oxorhenium complex-based heterogeneous catalyst for perchlorate reduction in water. Environmental Science & Technology 2015;49(21):12932-12940. R835174 (2014)
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  • Journal Article Liu J, Han M, Wu D, Chen X, Choe JK, Werth CJ, Strathmann TJ. A new bioinspired perchlorate reduction catalyst with significantly enhanced stability via rational tuning of rhenium coordination chemistry and heterogeneous reaction pathway. Environmental Science & Technology 2016;50(11):5874-5881. R835174 (Final)
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  • Journal Article Liu J, Wu D, Su X, Han M, Kimura SY, Gray DL, Shapley JR, Abu-Omar MM, Werth CJ, Strathmann TJ. Configuration control in the synthesis of homo- and heteroleptic bis(oxazolinylphenolato/thiazolinylphenolato) chelate ligand complexes of oxorhenium(V): isomer effect on ancillary ligand exchange dynamics and implications for perchlorate reduction catalysis. Inorganic Chemistry 2016;55(5):2597-2611. R835174 (Final)
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  • Journal Article Liu J, Su X, Han M, Wu D, Gray DL, Shapley JR, Werth CJ, Strathmann TJ. Ligand design for isomer-selective oxorhenium(V) complex synthesis. Inorganic Chemistry 2017;56(3):1757-1769. R835174 (Final)
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  • Journal Article Zhang R, Shuai D, Guy KA, Shapley JR, Strathmann TJ, Werth CJ. Elucidation of nitrate reduction mechanisms on a Pd-In bimetallic catalyst using isotope labeled nitrogen species. ChemCatChem 2013;5(1):313-321. R835174 (2012)
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  • Progress and Final Reports:

    Original Abstract
  • 2012 Progress Report
  • 2013 Progress Report
  • 2014 Progress Report
  • 2015 Progress Report