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Designing Novel Efficient Catalytic Strategies for the Transformation of Lignocellulose into Lignin-derived Chemicals and Valorisable Carbohydrates

Periodic Reporting for period 1 - CATLIGCAR (Designing Novel Efficient Catalytic Strategies for the Transformation of Lignocellulose into Lignin-derived Chemicals and Valorisable Carbohydrates)

Reporting period: 2017-10-01 to 2019-09-30

Summary of the project:

This project aims to develop various multifunctional nanostructured catalysts for efficient conversion of lignocellulosic biomass into aromatic platform molecules and valorizable carbohydrates fraction. Efficient valorization of renewable lignocellulose biomass (composed of cellulose, hemicellulose and lignin) is essential in view of increasing concerns on fossil fuel reserves and the detrimental effects of surplus consumption of fossil fuels on the environment. In this context, the reductive fractionation of lignocellulose using appropriate catalysts is a promising route to fully unlock its potentiality for sustainable chemicals production. This strategy enables one-pot conversion of lignocellulose into useful lignin-derived chemicals while retaining a solid (hemi)cellulose fraction that can be used for the production of fuels, chemicals or paper.


• Designing novel, multifunctional heterogeneous M-Ni (M = Cu, Fe, and Co) catalysts supported on shape-controlled TiO2 nanomaterials.
• Investigating the structural, morphological, acid, and redox properties of the catalysts using a range of advanced microscopy, spectroscopy, and thermal programmed techniques. This fundamental understanding will provide useful information for the design of state-of-the-art catalysts with advanced properties.
• Developing a one-pot catalytic lignocellulose biomass fractionation process for exploiting the full potential of lignin into valuable chemicals, while retaining a useful solid (hemi)cellulose fraction that can be used for the synthesis of chemicals, fuels or paper.
• Conducting catalysts’ reusability and kinetic/mechanistic studies for estimating the catalysts’ stability, rate of chemical reactions, identification of catalytically active species, and the mechanism of catalytic reactions, aiming to determine structure-activity relationships in the lignocellulose catalytic fractionation process.
Work performed: During this project, several nanostructured catalysts consisting of Ni and TiO2 were successfully synthesized using wet-chemical methods. The structural and catalytic properties of Ni/TiO2 materials were tuned by changing the shape of TiO2 nanomaterial. Various reducible metals, such as Cu, Fe, and Co were added to Ni/TiO2 catalysts with the aim of improving their catalytic efficiencies for lignocellulose conversion. Various parameters were optimized including catalyst wt%, catalyst’s calcination temperature, reaction temperature/pressure, pre-activation variables (H2 flow rate/temperature/time), etc. to achieve higher yields of lignin-derived monomers. The obtained reaction mixture is fully characterized using NMR, GC, and GPC techniques. In-depth catalysts’ reusability and kinetic/mechanistic studies were conducted to determine structure-activity relationships in the process.

Main Results:
Among all the catalysts investigated, the Ni catalyst dispersed on TiO2 nanotubes (pre-reduced at the desirable temperature) showed higher catalytic performance in terms of lignin-derived monomer yields and their selectivity. The TiO2 shape played a major role in tuning the catalytic performance and the selectivity of Ni/TiO2 catalysts. Surprisingly, the addition of second metal (Cu, Fe and Co) to Ni/TiO2 catalyst led to low catalytic performance. The kinetics/mechanistic and catalyst’s reusability studies were performed using the best catalyst. The physicochemical characterization of the catalysts was completed and the results were analyzed and summarized.
This fellowship provided me (Dr Putla Sudarsanam) a great opportunity to work at KU Leuven and allowed me to acquire additional disciplinary skills in several fields, including catalysis, materials science, and biomass valorization. I believe that the experience and expertise achieved from this project would be useful for my long-term career prospects. I have achieved the following skills (training and research) and benefits/opportunities (mainly collaboration) during this project.
• In-depth knowledge of developing multifunctional nanostructured catalysts
• Experience in developing and handling catalysis and biomass projects
• Experience in handling of NMR and GPC techniques
• Took a teaching course (Basics of Biological Chemistry) for master students, which helped me to gain the necessary experience in the educational requirements and delivery standards of modern Universities, preparing me for a career in academia
• Participated at three international conferences, which helped me to expand my research network with NUS (Singapore), Vito (Belgium), and TIFR (Mumbai, India) institutes
• Being part of Prof. Sels’ group enabled me to establish new connections with leading scientists, namely Prof. Kiyotaka Nakajima (Institute for Catalysis, Hokkaido University, Kita 21 Nishi 10, Kita-ku, Sapporo 001-0021, Japan) and Prof. Tao Ghang (Dalian Institute of Chemical Physics, Chinese Academy of Sciences, China)
• Observation of implementation methods of Prof. Sels group enabled me to gain experience in the management of financial/scientific project measurements.
• Published two review articles based on this project: (1) P. Sudarsanam,* E. Peeters, E.V. Makshina, V.I. Parvulescu, B.F. Sels*. Advances in porous and nanoscale catalysts for viable biomass conversion. Chemical Society Reviews, Chem. Soc. Rev., 2019, 48, 2366-2421. [IF = 40.443] and (2) P. Sudarsanam,* R. Zhong, S.V. den Bosch, S.M. Coman, V.I. Parvulescu,* B.F. Sels*. Functionalised heterogeneous catalysts for sustainable biomass valorisation. Chemical Society Reviews, 47 (2018) 8349-8402. [IF = 40.443]. These publications are value-added to my CV.

Impact of this project on the economy and society:

• In 2008, the EU agreed to the 20-20-20 objectives: a 20% reduction in greenhouse gases compared with 1990 levels, a 20% renewable energy market share, and a 20% improvement in energy efficiency. This project will help to achieve at least two objectives: reduction of greenhouse gases and increased renewable energy market share.
• Use of biomass as fuel will improve air quality and ultimately reduce pollution levels in major European cities. Normally, biomass has less sulphur content (a major component in the European fuel mix) than diesel. Estimated asthma prevalence rates in European countries range from 1.6% in Romania to 7% in France. Cleaner air as a result of cleaner-burning biofuels will help to reduce these statistics, thus improving the health of European citizens.
• Application of green solid catalysts instead of hazardous liquid catalysts reduces a heavy environmental burden to the European Union. The advantages of solid catalysts will improve the efficiency, economy and green credentials of current European chemical industries.
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