Annual report Foundation for Fundamental Research on Matter FOM
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1 FOM Annual report 2015 FOM programme nr. i40 'Rock-on-a-Chip: Salt-controlled wettability alteration in oil-watersolid systems for applications in enhanced oil recovery' Foundation for Fundamental Research on Matter Surface profile (left) and surface charge map (right) of a Gibbsite nanoparticle adsorbed on silica. The image was obtained in 10mM aqueous NaCl solution at ph 9. Red color indicates negative surface charge, blue color positive surface charge. The charge map demonstrates that topographic steps (compare left image) display more negative local surface charge than flat terraces. (Image size: 50x50µm2). May 2016
2 Content 1. Scientific results Added value of the programme Personnel Publications Valorisation and outreach Vacancies... 4 Fact sheet as of 1 January Historical overview of input eand output... 7 PhD defences... 7 Patents (new/changes)... 7 Overview of projects and personnel... 8 Workgroup FOM-N Workgroup FOM-T Workgroup FOM-U
3 1. Scientific results 2015 The project was formally granted in April The search for suitable candidates started immediately. By December 2016 all PhD but one projects started and by February 2016 most students completed most of their initial training. First contacts between students were established at various occasions (see below) and a few first experimental results are coming up. Specific results have so far emerged in two sub-projects: M. Haagh (UT) (started earlier) and B. Werkhoven (UU). Haagh studied the effect of the salt content and ph on the wettability of aqueous drops on mica immersed in ambient decane containing a dissolved surface-active fatty acid. The experiments were directly motivated by empirical observations of BP and other oil companies regarding the influence of both divalent cations and the total salinity of the aqueous phase on competitive oil-water-rock interactions. The experiments confirmed that the removal of divalent cations from the aqueous phase is crucial to improve the water wettability (which facilitates oil removal). The results further demonstrate a strong preferential adsorption of Ca 2+ ions as compared to Na + on mica even at a bulk excess of Na + of almost fifty times, as commonly observed in sea water. Additional experiments with K + and Mg 2+ ions suggest strong specific ions effects beyond simply valency. Numerical calculations by Werkhoven demonstrate the charge regulation-induced adsorption and desorption of ions to interfaces upon approaching two solid surfaces in an ambient electrolyte solution. The results obtained so far match well with earlier calculations in a simple parallel plate geometry but are currently being extended to the three-dimensional geometry of an AFM tip approaching a sample surface. The simulation programme also allows for the implementation of laterally varying chemical properties on the surface, as encountered in the AFM experiments by S. van Lin imaging nanoparticles of Montmorillonite and other clays adsorbed onto mica or silica (see image on cover page). Regarding the AFM work, experimental protocols were established and van Lin was trained to perform AFM spectroscopy measurements of the local charge density of solid-electrolyte interfaces and to image such surfaces at atomic resolution. E. Mazzi started only in December He is following his start-up training in confocal Raman microscopy to image micrometer-sized clay particles first in air and subsequently inside liquid-filled microfluidic channels. S. Pintea developed a measurement cell and thin films of Al 2O 3 as model substrates for upcoming X-ray absorption spectroscopy measurements at the APS synchrotron in Chicago in March He also spent several weeks in Berkeley, CA, with Dr. Salmeron's group to learn about their advanced measurement technique and to perform a few preliminary test measurements that were instrumental in obtaining beam time. It is expected that the projects will start to produce the first interesting and publishable results in the course of The primary concern at present is the lack of a PhD student on the AMOLF project. Prof. Bakker promised to intensify his search. In view of his obligations as director of AMOLF, he involved his senior co-worker Dr. J. Versluis to support him on the project. 2. Added value of the programme The individual subprojects are gradually merging together and links also on the personal level are being intensified. A first kick-off meeting was held on September 2015, in Windsor, UK, with all participants of the (CH)IPP and the broader consortium led by BP and including the researchers from Copenhagen University (group Prof. S. Stipp) and the Max-Planck Institute for Dynamics and Self-Organization Göttingen (Prof. S. Herminghaus). BP researchers gave a tutorial introduction into the background of (enhanced) oil recovery to the participating students and first contacts were established. The Dutch team held a second national kick-off meeting on 15 January 2016 in Utrecht at the FOM office. Moreover, two meetings with all PhD students and postdocs of the network were held in Twente on 6 November and 4 December 2015 with introductory training lectures by the staff and subsequent progress presentations by the participants. Moreover, four out of the five - 3 -
4 PhD students attended the traditional Physical Chemistry winter school in Han-sur-Lesse in January At this stage, the primary added value of the programme is to provide joint training and to establish links and stimulate exchange between the students. B. Werkhoven (UU) already adjusts his numerical calculations to match the experimental conditions of the experiments of S. van Lin (UT). Ideas for choices of systems (types of ions) were also coordinated between the Twente team and S. Brugman (RU) to guarantee complementarity between the upcoming synchrotron beam time and the existing and running AFM experiments at UT. The PhD and postdoc meetings will be continued on a monthly basis to further stimulate exchange and collaboration between all team members. The next meeting is planned in March in Nijmegen. Once experimental results emerge, they can be analyzed immediately from different perspectives. 3. Personnel - 5 PhD students were hired: M. Haagh (UT; starting date: February 2015), Simone van Lin (UT; September 2015), Edoardo Mazzi (UT; December 2015), Ben Werkhoven (UU; September 2015), Sander Brugman (RU; September 2015) - 1 postdoc was hired: Dr. Stelian Pintea (UT; April 2015) - 1 tenure tracker was hired: Dr. Igor Siretanu (UT; April 2015) - 1 postdoc position is vacant at UT. Dr. Samaneh Mashagi accepted the offer; start date: 1 July - 1 PhD position is still vacant at AMOLF. Several candidates are being screened. - 1 position technical support (0.5 fte; UT) is vacant. Implementation with existing technician is under discussion. Almost all subprojects thus started. Initial experiments (and in particular numerical calculations) are very promising. Collaborations between PhD students start to develop. First beam times at synchrotrons are coming up in March 2016 (Pintea at APS; Brugman at ESRF). 4. Publications - Naveen Kumar, Cunlu Zhao, Aram Klaassen, Dirk van den Ende, Frieder Mugele, Igor Siretanu, Characterization of the surface charge distribution on kaolinite particles using high resolution atomic force microscopy, Geochim.Cosmochim. Acta 175 (2016) Frieder Mugele, Igor Siretanu, Naveen Kumar, Bijoy Bera, Lei Wang, Rielle de Ruiter, Armando Maestro, Michel Duits, Dirk van den Ende, University of Twente and Ian Collins, Insights from Ion Adsorption and Contact Angle Alteration at Mineral Surfaces for Low Salinity Water Flooding, SPE Journal, DOI / PA, (Both publications were initiated under an earlier programme with BP, but completed by I. Siretanu and F. Mugele within the present (CH)IPP.) 5. Valorisation and outreach At this stage, the project has not produced significant results nor patents. The progress was featured though on the front page of the report of the Commissie Breimer to the minister OCW as an example of a collaborative research programme between physics, chemistry, and industry. Moreover, a short new was presented in the national C2W newsletter of chemical sciences. 6. Vacancies One PhD position (AMOLF), one PD position (UT), one technician (UT) have not yet started. A candidate of the PD position at UT is identified and is expected to start on 1 July
5 Fact sheet as of 1 January 2016 FOM /1 datum: APPROVED INDUSTRIAL PARTNERSHIP PROGRAMME Number i40. Title (code) Executive organisational unit Programme management Rock-on-a-Chip: Salt-controlled wettability alteration in oilwater-solid systems for applications in enhanced oil recovery (ROAC) BUW Duration Cost estimate M 3,2 Partner(s) NWO-CW, BP, TKI-NCI Concise programme description a. Objectives The purpose of the present programme is to obtain a fundamental understanding of salt-mediated wetting alteration in sandstone-based oil reservoirs by performing experiments with well-defined model systems, starting from idealized solid and fluid compositions and gradually evolving towards more complex systems. b. Background, relevance and implementation Oil recovery is a complex process involving physical and chemical phenomena at multiple length scales ranging from molecular dimensions to the macroscopic extensions of an oil field. State-ofthe-art water flooding technology using sea water is able to recover only percent of the oil that is originally present in the reservoir. A substantial fraction of the residual oil remains trapped in microscopic pores due to the strong adhesion and wettability of crude oil on the reservoir rock. Empirical research, including laboratory tests and field trials, in the past years has demonstrated that the efficiency of the oil recovery in sandstone reservoirs can be potentially increased by several percentage points by reducing the salinity of the water that is injected into the reservoir. While the potential economic impact of this Low Salinity Water Flooding (LSWF) technology is large, the fundamental understanding of the underlying microscopic processes is poor. According to wide spread models, wettability alteration caused by salt-mediated adsorption and desorption of polar components from the crude oil onto the (heterogeneous) rock surface plays an important role. However, a detailed understanding of these complex phenomena has been hampered by a) the complexity of the crude oil-rock system and b) by the absence of systematic investigations using complementary microscopic probes of the relevant molecular interactions and their relation to macroscopic wettability. Key feature of our effort is to combine a series of complementary high resolution experimental techniques along with numerical modeling - 5 -
6 of molecular scale processes. In this manner, we aim at identifying the dominant molecular mechanisms controlling wettability alteration for a variety of typical components of both the aqueous and the oil phase. Funding salarispeil cao per bedragen in k Totaal FOM-basisexploitatie FOM-basisinvesteringen Doelsubsidies NWO - - NWO-CW Doelsubsidies derden - - BP TKI-toeslag 1) ) Totaal ) Voor dit (CH)IPP wordt door het TKI NCI een TKI-projecttoeslag aangevraagd ter hoogte van k 355, hierover berekent TKI NCI k 11 overhead. 2) De verdeling over de jaren wordt bepaald bij de toekenning door RVO. Source documents and progress control a) Original programme proposal: FOM /D b) Ex ante evaluation: FOM , FOM , FOM c) Decision Executive Board: FOM d) Contract: FOM Remarks A programme committee consisting of the programme leader, and the PI's of the other academic groups, as well as one or two representatives from BP will monitor the progress of the individual projects, advise and adjust the scientific direction if necessary. Meetings of the programme committee will take place at each of the six-monthly progress meetings. Proposals for changes in the programme content and/or budget have to be granted by the steering committee. The chair of the programme committee acts as the programme leader. The final evaluation of this programme will consist of a self evaluation initiated by the programme leader and is foreseen in MS par. HOZB Subgebieden: 70% FeF; 30% COMOP - 6 -
7 Historical overview of input eand output personnel (in fte) finances* (in k ) Input WP/V WP/T PhD NWP PhD theses refereed publications other publications & patents Output presentations * After closing the financial year. PhD defences 2015 None. Patents (new/changes) 2015 None
8 Overview of projects and personnel Workgroup FOM-N-10 Prof.dr. E. Vlieg Radboud University Nijmegen In situ surface X-ray diffraction for the structure determination of mineral-solution interfaces (15ROAC03) S.J.T. Brugman PhD 1 September August 2019 Workgroup FOM-T-17 High-resolution Atomic Force Microscopy and Spectroscopy (15ROAC01) I. Siretanu WP/T 1 March February 2019 Adsorption and desorption of ions and polar organic molecules studied by Atomic Force Microscopy (15ROAC02) S.R. van Lin PhD 1 September August 2019 Distribution of inorganic and organic matter at solid-electrolyte interfaces studied by Confocal Raman Microscopy (15ROAC06) - 8 -
9 E. Mazzi PhD 1 December November 2019 Mesoscopic characterization of oil- and water-thin film (de)wetting and adhesion (15ROAC07) M.E.J. Haagh PhD 2 February February 2019 In situ surface X-ray absorption spectroscopy for the structure determination of mineral-solution interfaces (15ROAC09) G.S. Pintea WP/T 1 April March 2016 Workgroup FOM-U-31 Prof.dr. R.H.H.G. van Roij Utrecht University Theory for ions, oil, and water near surfaces: screening, chemistry, and adsorption (15ROAC05) B.L. Werkhoven PhD 1 September August
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