THE OIL SANDS TAILINGS RESEARCH FACILITY Nicholas Beier and David Sego U of A Geotechnical Centre, Department of Civil and Environmental Engineering – University of Alberta, Edmonton, Alberta, Canada ABSTRACT The University of Alberta’s Oil Sands Tailings Research Facility (OSTRF), funded by government and industry, was created to facilitate innovative research and development of the next generation of environmentally superior tailings for Alberta’s oil sands industry. The OSTRF is equipped with specialized equipment to allow testing of a variety of processes and technologies, aimed at reducing the environmental impact of oil sand tailings disposal. The intent of this paper is to provide a background summary of the tailings issues facing the oil sands industry, detail the infrastructure and instrumentation at the OSTRF, and outline the OSTRF research program. RÉSUMÉ L'université de pétrole d'Alberta ponce le service de recherches de produits de queue (OSTRF), financé par gouvernement et l'industrie, a été créée pour faciliter la recherche et le développement innovateurs de la prochaine génération des produits de queue dans l'environnement supérieurs pour l'industrie des huile-sables d'Alberta. L'OSTRF est équipé de l'équipement spécialisé pour permettre l'essai d'une variété de processus et de technologies, destinée à réduire les incidences sur l'environnement de la disposition de produits de queue de sable d'huile. L'intention de cet article est de fournir un sommaire de fond des issues de produits de queue faisant face à l'industrie de sables d'huile, de détailler l'infrastructure et l'instrumentation à l'OSTRF, et décrire le programme de recherche d'OSTRF. 1 INTRODUCTION The Athabasca region of northern Alberta, Canada, is home to massive deposits of oil sands, estimated to contain approximately 300 billion barrels of recoverable bitumen (Figure 1). These oil sands are composed of bitumen (~12 wt%), sand, silts, clays (mineral content ~85 wt%) and water (3-6 wt%). The clay component is comprised of mainly kaolinite (50-60 %) and illite (30-50 %) with some montmorillonite (Chalaturnyk et al. 2002; FTFC, 1995). In the Fort McMurray area, there are currently three oil sands mining and extraction operations; Suncor Energy (Suncor), Syncrude Canada Ltd. (Syncrude) and Albian Sands (Albian), with several more mines under development. Production of the bitumen is based on open pit mining and oil sands processing using a hot water extraction process (FTFC 1995; Masliyah et al. 2004). The extraction process utilizes warm to hot water, steam, and process aides such as caustic (NaOH) to assist in extracting the bitumen from the sand matrix. Typical bitumen recoveries range from 88 to 95 % depending on oil sands grade and origin. Tailings include a mixture of water, sand, silt, clay and residual bitumen. This tailings slurry is approximately 55 wt% solids (82 wt% sand and 17 wt% fines < 44 µm). Historically, the tailings were pumped into large settling basins where the sand fraction settled out rapidly to form beaches. Some fines were trapped within the sand matrix of the

beaches. However, the remaining thin slurry of fines and water (8 wt%) flowed into the settling basin where the solids settled gradually to form a densified zone of fine tailings at depth. Released water was recycled back to the extraction plant. After a few years, the fines settled to 30 to 35 wt % and is referred to as mature fine tailings (MFT).

Figure 1. Alberta’s oil sands regions

Edmonton

Calgary

Athabasca Peace River

Wabasca

OOiill SSaannddss

DDeeppoossiittss

Fort McMurray

Cold Lake

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Figure 2. Conventional oil sands extraction and tailings disposal Further consolidation of the MFT is expected to take centuries (Chalaturnyk et al. 2002; FTFC, 1995). Figure 2 shows schematically a conventional oil sand extraction and tailings disposal system. On average, for every barrel of crude oil produced, approximately 1 m3 of sand and 0.25 m3 of MFT are produced (FTFC 1995; Mikula et al. 1996). Tailings management practises in the last four decades have resulted in massive inventories of MFT (650 millions m3) requiring long term storage within fluid containment structures (Dominski, 2007). Water management is also an issue for the mine sites in addition to managing large volumes of fluid fine tailings. The mines are operating under a zero-effluent discharge policy. Continual recycle of tailings and process water to the extraction plant has lead to a build up of dissolved ions within the recycle water. Elevated ion concentrations can lead to various operational issues including poor extraction recovery and scaling/fouling of piping and equipment. 1.1 State of the Industry – Tailings Management In an effort to deal with the massive inventory of MFT and provide a stable landscape in a timely manner, the industry has moved towards the use of non segregating tailings by implementing CT technology (Composite tailings – Syncrude, Consolidated tailings – Suncor). CT tailings are a mixture of coarse sand, gypsum (coagulant) and MFT at sand to fines ratios of approximately 4:1. To produce CT, total tailings from the extraction plant are passed through a hydrocyclone with the overflow (mainly fines) pumped to the settling basin to form MFT. The coarse underflow is then combined with MFT and gypsum to form the CT. The resulting mixture is pumped to the disposal area and should not segregate during transport, discharge, or deposition. CT provides an opportunity to consume the current inventories of MFT and also releases water rapidly for reuse (Matthews et al. 2002). When CT was initially implemented, it was anticipated that the deposits would reach a geotechnically stable state in a timely manner so reclamation activities could proceed. However, reduced dewatering rates were preventing the deposit from reaching the strength required to support reclamation. Also segregation of the

CT was occurring upon deposition. Variable clay content in the tailings stream due to heterogeneous oil sands and/or difficult to control tailings management and deposition techniques are factors that contribute to segregation of CT. To reduce long term liability of fluid containment the Industry wants to move from wet tailings towards a dry landscape – reduced use of settling basins and their elimination during reclamation. 2 OIL SANDS TAILINGS RESEARCH FACILITY Limited progress with respect to improved tailings management was recognized as an impediment to the future success of the oil sands industry. Members of the University of Alberta’s Geotechnical Centre understood that substantial fundamental tailings research at a pilot scale using tailings manufactured to a research specification held the key to sustainable and cost-effective utilization of the oil sands resources. Initially a meeting to discuss the need for a focussed effort related to tailings was held with H. Hamza, T. Lord and D. Sego in attendance. The next meeting brought together a broader group from industry and the concept of the Oil Sands Tailings Research Facility (OSTRF) was developed. They envisioned that the OSTRF would provide the innovative and novel research required to develop the next generation of environmentally superior tailings disposal options. This was also recognized by all stakeholders (Industry, Government, and University) who came together in late 2002 to support the OSTRF initiative. The OSTRF is owned by the University of Alberta and sponsored by Canadian Oil Sands Network for Research and Development (CONRAD). The OSTRF is located in Devon, Alberta, Canada, in a unique partnership using shared facilities with Alberta Research Council (ARC) and Natural Resources Canada’s CETC – Devon (Canadian Centre for Mineral and Energy Technology [CANMET]) (Figure 3). Funding for the OSTRF’s $2.3 million worth of capital infrastructure came from a Canada Foundation for Innovation grant (Federal Government), Natural Resources Canada, Alberta Science and Research Investment Program (Alberta Government) and Oil Sands industry partners (Syncrude., Suncor, Albian, and True North Energy). Canadian Natural Resources Limited [CNRL], Deer Creek Energy Limited (Total E&P Canada Ltd.), and FortHills Energy LP have subsequently

Sand Dykes

Sand Dykes

Sand Beach Sand Beach

Mature Fine Tailings

Reclaim Water

Extraction Water + Process aids

Oil Sands from Mine Bitumen to Upgrading

Extraction Tailings

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provided capital funds for the OSTRF. Yearly operational and research funding is provided by Oil Sands industry partners (Syncrude, Suncor, Albian, CNRL, Total, and FortHills) and Alberta Energy Research Institute (AERI) as well as in-kind support from CANMET and ARC. Locating the OSTRF adjacent to CANMET allows for closer collaboration with its 55 scientific personnel and permits access to $20 million in state of the art scientific research equipment and infrastructure. Students will be exposed to CANMET’s active tailings research program at the OSTRF and will have an opportunity to understand the oil sands industry from a number of different perspectives.

Figure 3. NRCan-CETC Devon Facility and location of the Oil Sands Tailings Research Facility The OSTRF is a unique academic and industrial research facility dedicated to collaborative and multi-disciplinary tailings research. It provides crucial pilot scale infrastructure at the intermediate scale that was not previously available for university research in Canada. Until now research efforts have focussed on bench scale testing or larges scale field demonstrations. Activities at the OSTRF are intended to improve the multi-disciplinary aspects of tailings research, and to ensure that graduate student-focused research is industrially relevant, well planned and well conducted. The OSTRF will contribute to the training of significant pools of highly qualified personnel (graduate students) who will become the next generation of oil sands industry leaders or consultants. One of the mandates of the OSTRF is to be exceptional by international standards: ‘to facilitate world-class research’. It will have a major impact on tailings management practices and provide facilities for highly innovative research. The collaborative and multi-disciplinary activities will encourage new, integrated thinking and approaches to develop the critical mass of knowledge necessary for a paradigm shift to environmentally superior tailings management strategies.

3 EQUIPMENT AND INFRASTRUCTURE The OSTRF was designed to provide maximum research flexibility. The OSTRF is an intermediate scale continuous-flow-through facility capable of accommodating a number of interdisciplinary research projects concurrently. The infrastructure consists of three independent modules for delivery/production, treatment and deposition of tailings. Each module contains interchangeable units, skid-mounted with self-contained instrumentation. The modules are easily re-configured to access and/or bypass any piece of process equipment during a given set of experiments, with quick return of bypassed equipment into the test circuit. The OSTRF has been designed to process tailing slurries at 600 kg solids per hour and 2000 kg solids per hour. The 2000 kg/hr capability is to ensure upward scalability of the process data to full scale operations. The lower capacity is to reduce the material handling challenges as significant research and development studies are undertaken. Modular equipment skids can be arranged in several Process-Flow-configurations, allowing subsequent additions and/or exchange of process modules – as it may be required in the future. The OSTRF includes provisions for the delivery, handling, storage and processing of such materials as: tailing sand, MFT, total tailing slurries and tailings water. Several processing techniques are available to manufacture tailings to required specifications, including preparation of:

• High density CT from Beach Sand and MFT • Low density CT from Hydrocyclone U/flow and

MFT • Hydrocyclone-de-sanded Fine Tailings for

Flocculation Thickening • Engineered Tailings at specified Sand/Fines

ratios and % solids, from beach Sand, water and MFT

Upon installation of a pilot thickener (summer 2007), it will also be possible to test fine tailings flocculation-thickening processes and produce a variety of mixtures including thickener paste, beach sand and/or hydrocyclone underflow. In the future, other equipment such as vacuum belt filter and/or belt filter presses may also be tested. The plant has appropriate storage facilities such as: MFT storage tank, two tailings water tanks, agitated tailings tanks for feed tailings, fine tailings and composite tailings, as well as multi-purpose piping, progressive cavity slurry pumps, valves, instrumentation, comprehensive process controls and computer based data storage system. The processing equipment includes a precision weight-loss-hopper with belt-feeder, multi-purpose Rotary Mixer/Screen with paddle-mixer-pump-box, 2.5” DIA. hydrocyclone, weight-loss coagulant feeder and agitated flocculant tank. Processed tailings can be deposited in two large settling columns (813 mm ID x 4700 mm tall), each equipped with eighteen (18) surgical sampling points, or in re-configurable ‘flexi-flume’ deposition cell allowing several potential depositional configurations. A

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2 m long rheological section is also provided, to enable hydraulic-friction-loss measurements for tested mixtures. Critical slurry pipelines are equipped with Coriolis type mass flow meters, which provide simultaneous measurement of temperature, density and mass flow, as well as inferred measure of volumetric flow (Figures 4 and 5). The OSTRF is highly instrumented to allow fundamental understanding of the internal and external interactions between the fluid and mineral particles. Most equipment, piping and instrumentation have been designed to perform several functions, as per specific projects. For example, the Rotary Mixer/Screen can be used for a variety of operations including:

• Removal of oversize from tailings before pipelining

• Mixing beach sand with MFT to prepare higher density CT

• Mixing and screening a variety of tailings streams to prepare engineered tailing mixtures

• Mixing overburden clays with tailings streams The OSTRF’s equipment and infrastructure provide the opportunity for innovative research related to the challenging issues of oil sands tailings management. 4 RESEARCH 4.1 Research Themes The main purpose for the OSTRF is to facilitate research and development of new tailings processes and provide research support to the existing tailings management practices. The OSTRF will carry out fundamental research on the segregation and dewatering behaviour of oil sands tailings from bitumen separation to deposition and ultimately to restoration. A November, 2002 OSTRF Tailings Workshop brought together stakeholders to establish the following research themes:

• Tailings Production: MFT, CT, Paste, Separators and Thickeners

• Engineered Tailings: Deposition, Dewatering (Natural Processes), Rapid Progressive Reclamation and Sustainability

• Water: Recovery, Reuse and Release • Interdependency: Extraction- Tailings-

Environment • Energy: Recovery and Green house gas (GHG)

Reduction • Instrumentation: Tailings process, Disposal and

Reclamation • Regional Impacts: Stakeholders, Landscapes

and Certification • By-products

The workshop began with presentations from industry representatives who articulated their company’s vision for the future of tailings management.

Presentations of these visions were made by :

• R. Birkholz from Albian Sands • A. Hyndman from True North Energy • D. Kennedy from Suncor • W. Mckee from Syncrude • J. Romero from CNRL

4.2 Proposed Research The research themes will be satisfied by focusing on the development of a fundamental understanding of the impact of changing the handling of the extraction tailings. These tailings have a propensity to segregate into a coarse and fine fraction; the fine tailings requiring extremely long-term containment. The implementation of the use of CT attempts to addresses this issue. It also permits incorporation of the present inventory of MFT into a non-segregating mixture. The proposed next generation of tailings management involves separation of sand and fines water mixture immediately after bitumen separation. Then rapid separation of the fines from the process water prior to disposal of both the fines and sand. The proposed research will focus on improving the understanding of these separation processes and the end products. This understanding will assist ultimate safe disposal of the sand and fine tailings, and the recycling of the released water. The research will focus on three separate aspects of post extraction tailings management to fulfill the research themes. First is primary solids separation by particle size and the impact of different extraction processes on this physical separation. The second will be studying the dynamic and chemical interaction associated with the separation of water from the fine particle-water suspension. The third phase will be the study of the deposition and the disposal characteristics of separate sand and fine tailings streams, as well as the recombined but dewatered total tailings stream. It will also examine the quality of release water from both the second phase fines-water separation along with the water release during and after tailings deposition. Additional details of potential research associated with each phase follows. 4.2.1 Sand – Fines Separation Sand–fines separation will be examined in the first phase using predominantly hydrocyclones and various other separators. The impact of pre-chemical treatment on the separation will also be examined. The important effect of natural variability of particle size on this separation will also be studied. The mass balance of the mineral, fluid and chemical phase will be ascertained using pre- and post-device instrumentation. Overflow would then pass to the fines-fluid separator and the underflow will pass to the depositional module (Phase 3). The solids content, sand-to-fines ratio and chemical analyses of both the inflow and outflow of each phase will be measured continuously to evaluate the influence of any variation on the extraction process tailings.

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Figure 4. Various infrastructure and equipment at the Oil Sands Tailings Research Facility 4.2.2 Fines-Fluid Separation The second phase will examine the important aspects of fines-fluid separation. This is challenging because of its critical impact on extraction and thus production. The desire for rapid recycle is mainly to benefit from higher temperatures, however ionic concentration build up could be detrimental to extraction. The processes affecting the release water chemistry and its influence on bitumen extraction are therefore of critical importance through the research. The research program will evaluate the important influence of oil sand variability, in-situ fluid chemistry, bitumen content and fines content on water separation from fines. The importance of changing the bitumen extraction process and chemical amendments will also be studied to include the above variability in the oil sands. These variables will be evaluated using the same fines-fluid configuration (pilot thickener after installation) to establish baseline data for mass balance of fluid chemistry and solids. In addition, this baseline data will be used for comparison with data using different configurations or separators.

4.2.3 Deposition, Disposal Characteristics and Long Term Dewatering via Natural Processes

The third phase will study the post-fluid separation pumping, deposition, dewatering and natural processes to stabilize the surface of the deposit to allow restoration processes to proceed. Different tailings streams will be studied, namely; the sand and fines streams individually or as a combined tailings stream. Each will be varied with respect to solids content, sand-to-fines ratio and water chemistry (little influence is expected from the sand stream alone). The fundamental tailings stream characteristics related to pumpability will be measured. Different pump type and configurations along with the characteristics of material being pumped will be evaluated. This will allow for evaluation of the technical and economic feasibility of using different pumping systems. This work will be carried out in collaboration and using technical advice provided by CANMET and the Saskatchewan Research Council’s recognized experts in pumping of high-solids-content slurries. The tailings streams will be sampled and tested to establish their basic physical and chemical characteristics.

MFT Tank Total Tailings

Tank

CT Tank

Fine Tailings Tank

Rotary Mixer

Settling Columns

Water Tanks Flexi-Flume Deposition Cell

Hydrocyclone

Long Flume

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Deposition Cells

Flocculant

Tank

Hot Water

Uses

Heater

Water

Tanker

Water

Tanks

External

Process

Modules

Settling

Columns

Rheology Section

Hydrocyclones

Coagulant

Fine Tailings

Tank

MFT

Tanker

Beach SandMixer

Screen

CT Tank

MFT

Tank

Total

Tailingss

Tank

Wet Tailings

Bench Test

Area

Exchangeable

Thickener

Modules

Figure 5. Simplified process flow diagram The tailings streams’ basic time rate of deformation (consolidation) and gain-in-strength behaviour also will be examined. The sand to fines ratio and the water chemistry will be studied to examine the influence of the fines-fluid separation phase on the basic characteristics of the tailings. This data will provide a baseline parameter for comparison to similar data obtained on the waste stream following discharge, flow within the disposal area and self-weight consolidation and natural dewatering mechanisms. The tailings deposited in the shallow disposal area will be subjected to the following natural dewatering mechanisms: surface evaporation, evapotranspiration using plants and freeze thaw. Limits on the depth of the disposal areas preclude higher self-weight stress at a large-scale (consolidation) of the deposit. Therefore, laboratory large-strain consolidation tests will be undertaken along with centrifuge tests to simulate 25-50 m deep deposits. The centrifuge tests will simulate the high stresses from the thick deposit by carrying out the tests under different imposed gravity forces through changing the rotational speed of the centrifuge. The research has the potential to reduce emissions of greenhouse gases through lower energy required for heating of water due to improved recycle of heated water and pumping of the larger volume of tailings for disposal. The improved dewatering will also reduce the size of the

disposal areas required and dewatered tailings will be available for restoration activities sooner. 4.3 Current Research Since 2002, fifteen student projects have been funded by the OSTRF. In addition, three projects were grandfathered by sponsoring companies. During construction of the OSTRF, the initial research projects were conducted at other locations such as the U of A geotechnical laboratories or at the oil sands sponsor sites. The research projects stem from several disciplines including geotechnical, geoenvironmental, chemical, environmental and water resources engineering, biological sciences and renewable resources. A summary of the completed and current research projects is included in Table 1. With the successful commissioning of the OSTRF, research projects will now be conducted there for the most part. Of the eighteen projects funded, to date nine students have completed and are currently employed by industry or went on to pursue doctoral degrees following their Master’s program.

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Table 1. Summary of Oil Sands Tailings Research Facility projects

Research project Degree Status Date Complete Discipline

Response of Dense Beach Above Water Tailings to Cyclic Equipment Loading at Syncrude’s Southwest Sand Storage Facility– Renata Wood

MSc Complete Fall 2003 Geotechnical Engineering

Compression Beahviour of Thixotropic Oil Sands Tailings – Silawat Jeevaripoolvam MSc Complete Spring 2005 Geotechnical

Engineering

Freeze Separation of Saline Oil Sands Mine Waste Water – Nicholas Beier MSc Complete Spring 2006 Geoenvironmental

Engineering

The Use of CPT and SPT in Loose Sands – Eric Niven MSc Complete Spring 2006 Geotechnical

Engineering

Freeze-Thaw Dewatering of Oil Sands Tailings as Part of a Natural Remediation Strategy – Bryan Bales

MSc Complete Spring 2007 Geotechnical Engineering

CFD Modeling of Oil Sands Sluries – Juwen Yang PhD Thesis

Written Awaiting examination

Geotechnical Engineering

Fundamentals of Segregation – Yetimega Mihiretu PhD Thesis

Written Awaiting examination

Geotechnical Engineering

Rapid Densification of MFT – Chengmai Guo PhD Thesis Written

Awaiting examination

Geotechnical Engineering

Recovery of Commercial Grade Kaolin from Oil Sands Fine Tailings – Michelle Chang MSc Thesis

Written Expected in 2007

Chemical Engineering

Tailings Processes using Natural Processes: Field Experiment of Biological Dewatering. – Shihong Wu MSc Ongoing Expected in

2008

Geotechnical Engineering and Renewable Resources

Impact of Clay Mineral-Water-Bitumen Geochemistry on Oil Sand Tailings Behavior and Recycled Water Quality – Nafisul Islam

MSc Ongoing Expected in 2008

Geoenvironmental Engineering

Mineralogy of Oil Sand Solids Using High Resolution Transmission Electron Microscopy – Heather Kaminsky

PhD Ongoing Expected in 2008

Chemical Engineering

Physical Laboratory Study of Oil Sands Tailings Slurries I - Neil Hall MSc Ongoing Expected in

2008 Water Resources Engineering

Dewatering Non-Segregating Mixtures of Oil Sands Tailings – Reza Moussavi Nik PhD Ongoing Expected in

2008 Geotechnical Engineering

The Potential Role of Aliphatic Diluent in Biogenic Methane Production and Accelerated Densification of Tailings at Albian Sands

MSc Start in 2007 Biological Sciences

Water Treatment Options and Their Applicability to Oil Sands Operations for Recycle and Safe Discharge

PhD Start in 2007 Environmental

Engineering

Physical Laboratory Study of Oil Sands Tailings Slurries II MSc Start in

2007 Water Resources Engineering

Thickening of Oil Sands Tailings using Longitudinal, Inclined Vibrating Plate Thickener Awaiting

Student Geotechnical Engineering

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5 CONCLUSIONS The research carried out at the OSTRF with the support of industry on new tailings management technologies promises to change the oil sands industry by reducing the dependence on and need for construction of large fluid containment structures. The research to achieve rapid settling and consolidation of the fines would allow for the rapid establishment of stable deposits, rapid recycling of water, and reclaim the disturbed land more quickly. This has the potential for substantial economic savings to the industry. The research will ensure that current oil sands plants and future developments are environmentally responsible and sustainable. Canada now has a unique student based research facility that can manufacture tailings to specification and test at a continuous 2000 kg/hr pilot scale. The current OSTRF research program is for oil sands tailings with the expectation that through focussed research innovative and sustainable tailings management techniques will be developed. ACKNOWLEDGEMENTS The writers would like to acknowledge the contribution of a number of individuals to the OSTRF. The input of these colleagues greatly assisted with formulating the concept of OSTRF initiative, the application for capital funding, the design, construction and ongoing operations of OSTRF: R. Birkholz, B. Bjornson, R. Chow, G. Cymmerman, T. Dereniwski, G. Foulds, H. Hamza, K. Hashmi, A. Hyndman, D. Kennedy, K. Manzer, T. Lord, R. Mikula, N. Morgenstern, J. Romero, D. Sheeran, and B. Temple. Special thanks to Syncrude Canada Ltd. For their commitment to OSTRF by making available G. Cymmerman to oversee the design and construction of OSTRF and the ongoing involvement of T. Lord. Special thanks to H. Hamza and T. Lord for their steadfast commitment to the vision of OSTRF and to making OSTRF an ongoing success. REFERENCES Chalaturnyk, R.J., Scott, D., and Ozum, B. 2002

Management of oil sands tailings. Petroleum Science and Technology, 20(9&10):1025-1046.

Dominski, M. 2007. Personal communication, Alberta Energy and Utilities Board, March 23, 2007.

FTFC (Fine Tailings Fundamentals Consortium), 1995. Advances in oil sands tailings research, Alberta Department of Energy, Oil Sands and Research Division, Edmonton, Alberta, Canada.

Masliyah, J., Zhou, Z., Xu, Z., Czarnecki, J. and Hamza, H. 2004. Understanding water-based bitumen extraction from Athabasca oil sands. The Canadian Journal of Chemical Engineering, 82: 628-654.

Matthews, J.G., Shaw, W.H., MacKinnon, M.D., and Cuddy, R.G. 2002. Development of composite tailings technology at Syncrude. International Journal of Surface Mining, Reclamation, and Environment, 16(1): 24-39.

Mikula R.J., Kasperski, K.L., Burns, R.D., and MacKinnon, M.D. 1996. Nature and fate of oil sands fine tailings. Suspensions: Fundamentals and Applications in the Petroleum Industry. Edited by Laurier L. Schramm. Advances in Chemistry Series 251. American Chemical Society, Washington, DC, USA.

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