Catalytic Supercritical Water Gasification of Sewage Sludge/Secondary Pulp/Paper-Mill Sludge for Hydrogen Production

dc.contributor.authorZhang, Linghongen
dc.contributor.departmentCivil Engineeringen
dc.contributor.supervisorChampagne, Pascaleen
dc.contributor.supervisorXu, Chunbao (Charles)en
dc.date2011-04-27 14:51:55.526
dc.date2011-04-27 17:20:49.193's University at Kingstonen
dc.descriptionThesis (Ph.D, Civil Engineering) -- Queen's University, 2011-04-27 17:20:49.193en
dc.description.abstractSupercritical water gasification (SCWG) is an innovative hydrothermal technique, employing supercritical water (SCW, T≥374oC, P≥22.1 MPa) as the reaction media, to convert wet biomass or aqueous organic waste directly into hydrogen (H2)-rich synthetic gas (syngas). In the first stage of this research, a secondary pulp/paper-mill sludge (SPP, provide by AbitibiBowater Thunder Bay Operations) was gasified at temperatures of 400-550oC for 20 to 120 min in a high-pressure batch reactor for H2 production. The highest H2 yield achieved was 14.5 mol H2/kg SPP (on a dry basis) at 550oC for 60 min. In addition, SPP exhibited higher H2-generation potential than sewage sludges, likely attributed to its higher pH and higher volatile matter and alkali salt contents. In the second stage, a novel two-step process for sludge treatment was established. The first step involved the co-liquefaction of SPP with waste newspaper in a batch reactor at varying mixing ratios, aimed at converting the organic carbons in the feedstocks into valuable bio-crude and water-soluble products. The highest heavy oil (HO) yield (26.9 wt%) was obtained at 300oC for 20 min with a SPP-to-newspaper ratio of 1:2. This co-liquefaction process transformed 39.1% of the carbon into HOs, where 16.3% of the carbon still remained in the aqueous waste. Next, an innovative Ru0.1Ni10/γ-Al2O3 catalyst (10 wt% Ni, Ru-to-Ni molar ratio=0.1), with long-term stability and high selectivity for H2 production, was developed for the SCWG of 50 g/L glucose, where no deactivation was observed after 33 h on stream at 700oC, 24 MPa and a WHSV (weight hourly space velocity) of 6 h-1. The H2 yield was maintained at ~50 mol/kg feedstock. The addition of small amounts of Ru to Ni10/γ-Al2O3 was found to be effective in enhancing Ni dispersion and increasing the reducibility of NiO. Finally, the Ru0.1Ni10/γ-Al2O3 catalyst together with an activated carbon (AC) supported catalyst (Ru0.1Ni10/AC) were utilized for treating the aqueous by-product from sludge-newspaper co-liquefaction using a continuous down-flow tubular reactor. More than 90% of the carbon in the waste was destroyed at 700oC with the highest H2 yield of 71.2 mol/kg carbon noted using Ru0.1Ni10/AC.en
dc.description.restricted-thesisChapters 2, 6, 7 and 8 as four separate manuscripts have been submitted to scientific journals and are currently under review. Specifically, Chapter 2 has been submitted to the journal of Biomass & Bioenergy, Elsevier. Chapter 6 has been submitted to the International Journal of Hydrogen Energy, Elsevier. Chapter 7 has been submitted to the journal of Applied Catalysis B: Environmental, Elsevier. And Chapter 8 has been submitted to the journal of Bioresource Technology, Elsevier.en
dc.relation.ispartofseriesCanadian thesesen
dc.rightsThis publication is made available by the authority of the copyright owner solely for the purpose of private study and research and may not be copied or reproduced except as permitted by the copyright laws without written authority from the copyright owner.en
dc.subjectSupercritical Water Gasificationen
dc.titleCatalytic Supercritical Water Gasification of Sewage Sludge/Secondary Pulp/Paper-Mill Sludge for Hydrogen Productionen
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