{"id":{"repo_id":"uiuc","oai_identifier":"oai:www.ideals.illinois.edu:2142/46901"},"canonical_url":"https://search.dev.ndltd.org/etd/uiuc/oai:www.ideals.illinois.edu:2142/46901","repository":{"repo_id":"uiuc","name":"University of Illinois - Urbana-Champaign","base_url":"https://www.ideals.illinois.edu/oai-pmh"},"display":{"title":"Development of a sustainable water treatment technology for oxyanions using palladium-based catalysts: catalyst design, reaction mechanisms, and life cycle assessment","abstract":"Perchlorate and nitrate are oxyanion contaminants found in many drinking water sources, causing human health risks when consumed even at low concentrations. These oxyanions are not removed via conventional drinking water treatment processes, and require specialized treatment. One emerging technology for destroying oxyanion water contaminants is catalytic reduction using supported Pd-based catalysts and an electron donor. While the technology is promising, several challenges need to be addressed before it is adapted by water treatment utilities. The overall goal of my thesis is to contribute to the development of catalytic treatment processes for removing oxyanion contaminants, specifically perchlorate and nitrate, from drinking water, either as a stand-alone system or in combination with ion exchange (IX), and to compare the overall costs and environmental sustainability of the technology with other available oxyanion treatment technologies. My thesis work specifically contributed to three areas of study: 1) elucidation of perchlorate reduction mechanisms using X-ray spectroscopic characterization to identify the chemical states and coordination of Re species in carbon supported Re-Pd catalysts (Re-Pd/C), 2) comparative assessment of environmental sustainability of the catalytic treatment technology with alternative perchlorate treatment technologies such as IX and biological reduction, and 3) evaluation of the applicability and environmental benefits of recycling spent IX brines via catalytic reduction using pelletized carbon supported Pd-In catalysts for removal of nitrate in drinking water. Results from the 1st study showed that Re in Re-Pd/C catalyst exists as ReVII species under oxic conditions and transforms to a mixture of two Re species under reducing solution conditions induced by H2 sparging. These Re species support a revised mechanism for catalytic reduction of perchlorate involving a series of oxygen atom transfer reactions between rhenium species and perchlorate. Results from the 2nd study showed catalytic treatment using Re- ii Pd/C catalyst has a higher (ca. 4,600 times) environmental impact than other perchlorate treatment technologies, but is within 0.9-30 times the impact of IX with a newly developed ligand-complexed Re-Pd catalyst suggesting catalytic reduction can be competitive with increased activity. Results from the 3rd study indicated the hybrid IX/catalyst system is more environmentally sustainable than the conventional IX for nitrate removal in drinking water, but the environmental impacts of the system are sensitive to brine conditions (e.g., presence of sulfate and bicarbonate) that influence catalyst activity. Overall, catalytic treatment technology showed the promise as an environmentally sustainable oxyanion treatment technology option for drinking water.","abstract_html":"Perchlorate and nitrate are oxyanion contaminants found in many drinking water sources, causing human health risks when consumed even at low concentrations. These oxyanions are not removed via conventional drinking water treatment processes, and require specialized treatment. One emerging technology for destroying oxyanion water contaminants is catalytic reduction using supported Pd-based catalysts and an electron donor. While the technology is promising, several challenges need to be addressed before it is adapted by water treatment utilities. The overall goal of my thesis is to contribute to the development of catalytic treatment processes for removing oxyanion contaminants, specifically perchlorate and nitrate, from drinking water, either as a stand-alone system or in combination with ion exchange (IX), and to compare the overall costs and environmental sustainability of the technology with other available oxyanion treatment technologies. My thesis work specifically contributed to three areas of study: 1) elucidation of perchlorate reduction mechanisms using X-ray spectroscopic characterization to identify the chemical states and coordination of Re species in carbon supported Re-Pd catalysts (Re-Pd/C), 2) comparative assessment of environmental sustainability of the catalytic treatment technology with alternative perchlorate treatment technologies such as IX and biological reduction, and 3) evaluation of the applicability and environmental benefits of recycling spent IX brines via catalytic reduction using pelletized carbon supported Pd-In catalysts for removal of nitrate in drinking water. Results from the 1st study showed that Re in Re-Pd/C catalyst exists as ReVII species under oxic conditions and transforms to a mixture of two Re species under reducing solution conditions induced by H2 sparging. These Re species support a revised mechanism for catalytic reduction of perchlorate involving a series of oxygen atom transfer reactions between rhenium species and perchlorate. Results from the 2nd study showed catalytic treatment using Re- ii Pd/C catalyst has a higher (ca. 4,600 times) environmental impact than other perchlorate treatment technologies, but is within 0.9-30 times the impact of IX with a newly developed ligand-complexed Re-Pd catalyst suggesting catalytic reduction can be competitive with increased activity. Results from the 3rd study indicated the hybrid IX/catalyst system is more environmentally sustainable than the conventional IX for nitrate removal in drinking water, but the environmental impacts of the system are sensitive to brine conditions (e.g., presence of sulfate and bicarbonate) that influence catalyst activity. Overall, catalytic treatment technology showed the promise as an environmentally sustainable oxyanion treatment technology option for drinking water.","abstract_has_math":false,"creators":["Choe, Jong Kwon"],"institution":"University of Illinois at Urbana-Champaign","degree_name":"Ph.D.","degree_level":"Dissertation","degree_discipline":"Environ Engr in Civil Engr","degree_department":null,"school":null,"contributors":["Werth, Charles J.","Strathmann, Timothy J.","Guest, Jeremy S.","Shapley, John R.","Kemner, Kenneth M."],"advisors":[],"committee_chairs":[],"committee_members":[],"year":2014,"date_issued":"2014-01-16T18:25:47Z","date_published":"2014-01-16T18:25:47Z","updated_at":"2026-07-22T22:25:38Z","subjects":["Perchlorate treatment","drinking water treatment technology","catalytic treatment","sustainability","life cycle assessment"],"languages":["en"],"rights":["Copyright 2013 Jong Kwon Choe"],"rights_urls":[],"identifier_entries":[]},"links":{"outbound_url":"http://hdl.handle.net/2142/46901","outbound_label":"Handle","outbound_source":"dc:identifier"},"metadata_groups":[{"id":"people","label":"People","entries":[{"key":"dc:contributor","label":"Contributor","values":["Werth, Charles J.","Strathmann, Timothy J.","Guest, Jeremy S.","Shapley, John R.","Kemner, Kenneth M."]},{"key":"dc:creator","label":"Author","values":["Choe, Jong Kwon"]}]},{"id":"academic_context","label":"Academic Context","entries":[{"key":"dc:date","label":"Dc Date","values":["2014-01-16T18:25:47Z","2016-01-16T11:02:27Z","2013-12"]},{"key":"dc:type","label":"Dc Type","values":["text"]},{"key":"thesis:degree_discipline","label":"Discipline","values":["Environ Engr in Civil Engr"]},{"key":"thesis:degree_level","label":"Degree Level","values":["Dissertation"]},{"key":"thesis:degree_name","label":"Degree Name","values":["Ph.D."]},{"key":"thesis:institution_name","label":"Thesis Institution Name","values":["University of Illinois at Urbana-Champaign"]}]},{"id":"subjects_keywords","label":"Subjects and Keywords","entries":[{"key":"dc:subject","label":"Dc Subject","values":["Perchlorate treatment","drinking water treatment technology","catalytic treatment","sustainability","life cycle assessment"]}]},{"id":"language_rights","label":"Language and Rights","entries":[{"key":"dc:language","label":"Dc Language","values":["en"]},{"key":"dc:rights","label":"Dc Rights","values":["Copyright 2013 Jong Kwon Choe"]}]},{"id":"identifiers","label":"Identifiers","entries":[{"key":"dc:identifier","label":"Identifier","values":["http://hdl.handle.net/2142/46901"]}]},{"id":"additional","label":"Additional Metadata","entries":[{"key":"dc:description","label":"Description","values":["Perchlorate and nitrate are oxyanion contaminants found in many drinking water sources, causing human health risks when consumed even at low concentrations. These oxyanions are not removed via conventional drinking water treatment processes, and require specialized treatment. One emerging technology for destroying oxyanion water contaminants is catalytic reduction using supported Pd-based catalysts and an electron donor. While the technology is promising, several challenges need to be addressed before it is adapted by water treatment utilities. The overall goal of my thesis is to contribute to the development of catalytic treatment processes for removing oxyanion contaminants, specifically perchlorate and nitrate, from drinking water, either as a stand-alone system or in combination with ion exchange (IX), and to compare the overall costs and environmental sustainability of the technology with other available oxyanion treatment technologies. My thesis work specifically contributed to three areas of study: 1) elucidation of perchlorate reduction mechanisms using X-ray spectroscopic characterization to identify the chemical states and coordination of Re species in carbon supported Re-Pd catalysts (Re-Pd/C), 2) comparative assessment of environmental sustainability of the catalytic treatment technology with alternative perchlorate treatment technologies such as IX and biological reduction, and 3) evaluation of the applicability and environmental benefits of recycling spent IX brines via catalytic reduction using pelletized carbon supported Pd-In catalysts for removal of nitrate in drinking water. Results from the 1st study showed that Re in Re-Pd/C catalyst exists as ReVII species under oxic conditions and transforms to a mixture of two Re species under reducing solution conditions induced by H2 sparging. These Re species support a revised mechanism for catalytic reduction of perchlorate involving a series of oxygen atom transfer reactions between rhenium species and perchlorate. Results from the 2nd study showed catalytic treatment using Re- ii Pd/C catalyst has a higher (ca. 4,600 times) environmental impact than other perchlorate treatment technologies, but is within 0.9-30 times the impact of IX with a newly developed ligand-complexed Re-Pd catalyst suggesting catalytic reduction can be competitive with increased activity. Results from the 3rd study indicated the hybrid IX/catalyst system is more environmentally sustainable than the conventional IX for nitrate removal in drinking water, but the environmental impacts of the system are sensitive to brine conditions (e.g., presence of sulfate and bicarbonate) that influence catalyst activity. Overall, catalytic treatment technology showed the promise as an environmentally sustainable oxyanion treatment technology option for drinking water.","Item withdrawn by Laura Spradlin (lspradl2@illinois.edu) on 2013-11-04T15:03:21Z Item was in collections: University of Illinois Theses & Dissertations (ID: 1) No. of bitstreams: 1 Choe_Jong Kwon.pdf: 4774855 bytes, checksum: e35e48fec9ff1fd2c5077fff2fb5a086 (MD5)","Made available in DSpace on 2014-01-16T18:25:47Z (GMT). No. of bitstreams: 2 Jong Kwon_Choe.pdf: 5758594 bytes, checksum: 72818a6ca6c58d1b14405afb477d44c1 (MD5) license.txt: 4061 bytes, checksum: fbc03b298defa3f1d5a7f9353efcbe41 (MD5)","Item marked as restricted to the 'Administrator' Group (id=1) by Seth Robbins (robbins.sd@gmail.com) on 2014-01-16T18:27:33Z Item is restricted until 2016-01-16T18:27:27Z","Restriction data tranferred 2014-07-01T11:36:45-05:00 Original Data Group with Access Administrator Release Date: 2016-01-16 12:27:27 UTC Reason: Author requested closed access (OA after 2yrs) in Vireo ETD system","Limited Restriction Lifted for Item 46920 on 2016-01-16T11:02:27Z."]},{"key":"dc:title","label":"Title","values":["Development of a sustainable water treatment technology for oxyanions using palladium-based catalysts: catalyst design, reaction mechanisms, and life cycle assessment"]}]}],"canonical_facts":{"dc:contributor":["Werth, Charles J.","Strathmann, Timothy J.","Guest, Jeremy S.","Shapley, John R.","Kemner, Kenneth M."],"dc:creator":["Choe, Jong Kwon"],"dc:date":["2014-01-16T18:25:47Z","2016-01-16T11:02:27Z","2013-12"],"dc:description":["Perchlorate and nitrate are oxyanion contaminants found in many drinking water sources, causing human health risks when consumed even at low concentrations. These oxyanions are not removed via conventional drinking water treatment processes, and require specialized treatment. One emerging technology for destroying oxyanion water contaminants is catalytic reduction using supported Pd-based catalysts and an electron donor. While the technology is promising, several challenges need to be addressed before it is adapted by water treatment utilities. The overall goal of my thesis is to contribute to the development of catalytic treatment processes for removing oxyanion contaminants, specifically perchlorate and nitrate, from drinking water, either as a stand-alone system or in combination with ion exchange (IX), and to compare the overall costs and environmental sustainability of the technology with other available oxyanion treatment technologies. My thesis work specifically contributed to three areas of study: 1) elucidation of perchlorate reduction mechanisms using X-ray spectroscopic characterization to identify the chemical states and coordination of Re species in carbon supported Re-Pd catalysts (Re-Pd/C), 2) comparative assessment of environmental sustainability of the catalytic treatment technology with alternative perchlorate treatment technologies such as IX and biological reduction, and 3) evaluation of the applicability and environmental benefits of recycling spent IX brines via catalytic reduction using pelletized carbon supported Pd-In catalysts for removal of nitrate in drinking water. Results from the 1st study showed that Re in Re-Pd/C catalyst exists as ReVII species under oxic conditions and transforms to a mixture of two Re species under reducing solution conditions induced by H2 sparging. These Re species support a revised mechanism for catalytic reduction of perchlorate involving a series of oxygen atom transfer reactions between rhenium species and perchlorate. Results from the 2nd study showed catalytic treatment using Re- ii Pd/C catalyst has a higher (ca. 4,600 times) environmental impact than other perchlorate treatment technologies, but is within 0.9-30 times the impact of IX with a newly developed ligand-complexed Re-Pd catalyst suggesting catalytic reduction can be competitive with increased activity. Results from the 3rd study indicated the hybrid IX/catalyst system is more environmentally sustainable than the conventional IX for nitrate removal in drinking water, but the environmental impacts of the system are sensitive to brine conditions (e.g., presence of sulfate and bicarbonate) that influence catalyst activity. Overall, catalytic treatment technology showed the promise as an environmentally sustainable oxyanion treatment technology option for drinking water.","Item withdrawn by Laura Spradlin (lspradl2@illinois.edu) on 2013-11-04T15:03:21Z Item was in collections: University of Illinois Theses & Dissertations (ID: 1) No. of bitstreams: 1 Choe_Jong Kwon.pdf: 4774855 bytes, checksum: e35e48fec9ff1fd2c5077fff2fb5a086 (MD5)","Made available in DSpace on 2014-01-16T18:25:47Z (GMT). No. of bitstreams: 2 Jong Kwon_Choe.pdf: 5758594 bytes, checksum: 72818a6ca6c58d1b14405afb477d44c1 (MD5) license.txt: 4061 bytes, checksum: fbc03b298defa3f1d5a7f9353efcbe41 (MD5)","Item marked as restricted to the 'Administrator' Group (id=1) by Seth Robbins (robbins.sd@gmail.com) on 2014-01-16T18:27:33Z Item is restricted until 2016-01-16T18:27:27Z","Restriction data tranferred 2014-07-01T11:36:45-05:00 Original Data Group with Access Administrator Release Date: 2016-01-16 12:27:27 UTC Reason: Author requested closed access (OA after 2yrs) in Vireo ETD system","Limited Restriction Lifted for Item 46920 on 2016-01-16T11:02:27Z."],"dc:identifier":["http://hdl.handle.net/2142/46901"],"dc:language":["en"],"dc:rights":["Copyright 2013 Jong Kwon Choe"],"dc:subject":["Perchlorate treatment","drinking water treatment technology","catalytic treatment","sustainability","life cycle assessment"],"dc:title":["Development of a sustainable water treatment technology for oxyanions using palladium-based catalysts: catalyst design, reaction mechanisms, and life cycle assessment"],"dc:type":["text"],"thesis:degree_discipline":["Environ Engr in Civil Engr"],"thesis:degree_level":["Dissertation"],"thesis:degree_name":["Ph.D."],"thesis:institution_name":["University of Illinois at Urbana-Champaign"]},"updated_at":"2026-07-22T22:25:38Z"}