Dissertation Docteur De L'université Du Luxembourg
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PhD-FSTM-2020-079 The Faculty of Science, Technology and Medicine DISSERTATION Defence held on 10/12/2020 in Esch-sur-Alzette to obtain the degree of DOCTEUR DE L’UNIVERSITÉ DU LUXEMBOURG EN SCIENCES DE L’INGÉNIEUR by Vishojit Bahadur THAPA Born on 6th October 1991 in Luxembourg City (Luxembourg) RECYCLING OF GRAVEL WASH MUD FOR MANUFACTURING CO2-REDUCED CEMENT Dissertation defence committee A-Prof. Dr.-Ing. Joachim Hansen, Chairman Associate Professor, University of Luxembourg, Faculty of Science, Technology and Medicine Prof. Dr. André Lecomte, Vice-Chairman Professor, University of Lorraine, Institut Jean Lamour Prof. Dr.-Ing. Danièle Waldmann, Dissertation supervisor Professor, University of Luxembourg, Faculty of Science, Technology and Medicine Prof. Dr. Jean-Frank Wagner Professor, University of Trier, Department of Geology Dr. Claude Simon Expert, Head of Quality Management, Cimalux S.A. Preface and acknowledgements This doctoral dissertation presents the results of my investigations on the topic of “Recycling of gravel wash mud for manufacturing CO2-reduced cement”, which were realised during my PhD journey at the Institute of Civil and Environmental Engineering (INCEEN) of the University of Luxembourg. This research project was mainly carried out at the Laboratory of Solid Structures (LSS) of the University of Luxembourg. It deals with the revalorisation of an unused industrial waste product, namely gravel wash mud (GWM) and its utilisation for the conceptualisation of potential “low carbon” cements. The execution of the present project and the writing of this dissertation were carried out in the period from the 1st of September 2016 to the 10th of November 2020. My sincere and special thanks go to Prof. Dr.-Ing. Danièle Waldmann for her trust and her confidence in my actual potential and capabilities in the scientific field by offering me this unique opportunity to carry out a doctorate under her supervision. I want to express my profound gratitude to Prof. Dr.-Ing. Danièle Waldmann for her clear and continuous guidance throughout my PhD journey, her permanent availability for any exchange (very appreciated as this is not always obvious), her trust on the quality of my independent work, her constructive feedback and criticisms, her understanding for personal concerns, and her professionalism and efforts to provide an inspiring and motivating working environment. i I want to express my sincere thanks to Prof. Dr. Jean-Frank Wagner, Professor and Head of the Department of Geology at the University of Trier, for his support during the elaboration of the actual research question of this project. Furthermore, his contributions and inputs to extend my understanding of the geological origin and the mineralogy of the gravel wash muds were precious for the progress of the project. My sincere thanks and appreciations go to A-Prof. Dr.-Ing. Joachim Hansen, Professor in Engineering Science in the field of Hydraulic Engineering and Urban Water Engineering at the University of Luxembourg, and to Prof. Dr.-Ing.André Lecomte, Professor at the Department of Chemistry and Physics of Solids and Surfaces (Institut Jean Lemour) of the University of Lorraine, for their participation as Chairman, respectively, Vice Chairman in my dissertation defence committee. Their remarks and comments on the content of my PhD work during the different meetings of the thesis supervision committee (CET) and their detailed communication of their expectations on the final work were extremely valuable and allowed to improve my final dissertation. I am deeply grateful to Dr. Claude Simon from Cimalux S.A. for his willingness to participate as a member of my thesis supervision committee (CET). Without his eagerness to support this research project actively, major milestones and some of the significant findings would have been difficult or more time-consuming to reach. I consider his unique contributions by giving me access to various high sensitive and cost-intensive characterisation methods at his company’s expenses and linking me up with different topic-related experts as a key factor to the success of this project. His expertise and his suggestions were a precious contribution to the work and allowed me to clarify my doubts by bringing me back to the right track to succeed at fulfilling my research goals. ii Furthermore, I am sincerely thankful to Carlo Spina from Contern S.A. and Paul Wertz, from Carrières Feidt S.A., for the supply of various raw materials and tools used in the realisation of this research work, and their valuable inputs and feedback on the progress of my research work during our regular meetings. Especially, I am grateful to Paul Wertz for his valuable inputs and responses to diverse questions related to the current, historical and regional availability of gravel wash muds and the regional occurrence of similar products. Moreover, I would like to express my gratitude to Dr. Marcus Paul and Astrid Becker from the Wilhelm Dyckerhoff Institut (WDI) for their valuable contributions to various applied characterisation techniques. Additionally, I am grateful to Dr. Oscar Baeza-Urrea from the University of Trier and Zornitza Tosheva from the Department of Physics and Materials Science at the University of Luxembourg for providing support to the microstructural analysis. I would also like to thank my colleagues and friends from the laboratories in Campus Kirchberg of the University of Luxembourg, Gilbert Klein, Marc Seil, Claude Collé, Logan Freitas, Vicente Reis Adonis, Ed Weyer, Markus Schlienz, Ralph Reiter, Ken Adam, Cédric Bruyère, Grace Ligbado and Remi Radinovic for sharing their valuable time at countless occasions for technical support or memorable discussions as short distractions from everyday work. Special thanks go to Marc Seil and Gilbert Klein for their excellent and experienced research support capabilities in a friendly, pleasant and cooperative atmosphere. I could contact them at any time, and I always found appreciative advice and help regarding the provision of materials or tools, the appropriate setup of the experiments, the introduction to the operation of new machines and tools, and much more. Heartfelt thanks and highest appreciations go to my fellow PhD and Post-doc colleagues, Dr.-Ing. Michel Weiler, Dr.-Ing. Dolgion Erdenebat, Patrick Pereira Dias, Dr.-Ing. Gael Chewe Ngapeya, iii Lorenc Bogoviku, Hooman Eslami, Dr.-Ing. Laddu Bhagya Jayasinghe, Dr.-Ing.Thanh Tung Nguyen and Tarik Camo, for the numerous and endless rounds of discussions on professional and private matters, for the share of knowledge as well as for getting me out of my monotonous work routines throughout my PhD journey. I am also grateful to the staff members of the University of Luxembourg for their helpful administrative support, especially Simone Drees, Annabella Simon, Marielle Mabille, Mike Hansen, Shayan Weber, Inmaculada Peral Alonso, Silvia Vendetti, Berta Rato, Rita Giannini and Suzanne Biwer. Furthermore, I would like to thank the students Sinan Kaassamani, Alejandra Mora Rincón (University of Trier), Jasmin Riem (University of Trier), Stefan Habetz (University of Trier), Nico Moes, Vincent Bamberg, Joe Gengler, Kristian Vidovic, Gilles Kayser, Jérome Pauly and Kauyne Parise for their active contributions to the global project through their successful Bachelor’s theses, Master’s theses and semester projects under my personal supervision. The greatest and deepest thanks go to my parents, for their admirable and selfless love, support, trust, and patience in all stages throughout my life without ever expecting anything in return. Luxembourg, 10th November 2020 Vishojit Bahadur THAPA iv Abstract The present research project “CO2REDCEM” is carried out at the Laboratory of Solid Structures (LSS) of the University of Luxembourg, in close collaboration with Luxembourgish industrial partners (Cimalux S.A., Carrières Feidt S.A. and Contern S.A.). This project aims at reducing the generation of CO2 emissions during cement production by minimisation of the use of cement clinker or its complete replacement by new binder compositions and concepts, containing novel material resources derived from local unused industrial waste products. Such a potential raw material is gravel wash mud (GWM), which occurs as a waste product from gravel mining. This clayey mud is collected from a sludge reservoir, located in the North West of Luxembourg. Currently, this waste product is landfilled without any further use. However, this prime material offers very promising properties, which require a thorough characterisation and verification before its revalorisation as a viable supplementary cementitious material (SCMs). Reusing or recycling of waste elements into goods has been among the greatest ambitions of our and earlier generations, and it will take a more important role in the future economy. One primary goal of this project is to replace the “end-of-life” concept of gravel wash mud by reusing it as new raw material. This endeavour will bring double benefit to environment as the waste is prevented from landfilling, and it is revalorised as a prime resource in another system. v This research work shares the outcomes from the assessment of the performance of the prime material GWM within the following binder concepts and binder reaction mechanisms: • The use of gravel wash mud (GWM) powders as a precursor material for the synthesis of alkali-activated binders: A “cementless” binder is synthesised by alkaline activation of processed and calcined GWM powders. The