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Former personnel - MPI

Former personnel

Benedikt Floeser – Postdoctoral researcher

UiO former personnel

Chiara Negri – Postdoctoral researcher

Kaiqi Xu – Postdoctoral researcher

Isabelle Gerz – PhD

The 19th International Symposium on Relations between Homogeneous and Heterogeneous Catalysis
Oslo, June 27 – 30, 2022

IZC-2022 – 20th International Zeolite Conference
Valencia 3-8 July 2022

8th International Conference on Metal-Organic Frameworks and Open Framework Compounds
Dresden 4-7 September 2022

9th World Congress on Oxidation Catalysis
Cardiff 4-8 September 2022

SURFCAT Summer school 2022
Kysthusene Gilleleje 7-12 August 2022

Former personnel

Andrea Martini – Postdoctoral researcher

Emilia Sannino – Administrative staff

UniTo Master students

Silvia Porporato – Synthesis and characterization of protein-bioconjugates towards the catalytic conversion of methane into methanol – Supervisor: C.Barolo CoSupervisor: S.Bordiga; M.Bonomo – April 2021

Davide Brignone – Synthetis and characterization of copper complexes as model systems for new catalysts in direct methane-methanol conversion (DMTM) – Supervisor: S.Bordiga CoSupervisor: C.Barolo – June 2021

Laura Leonardi – Polymers-protein bioconjugation as a stable and effective platform for the partial oxygenation of methane – Supervisor: M.Bonomo CoSupervisors: C.Barolo; C.Pontremoli – October 2021

Daniele Bonavia – Multi-technique characterization of Cu-complexes for the direct oxidation of light hydrocarbons – Supervisor: E.Borfecchia; M.Signorile – October 2021

What is the mechanism of C-H activation, and does the Cu monomer versus Cu dimer site promote a different reaction mechanism?
What is the influence of the ligands in the first coordination sphere on oxidant activation and ultimately reactivity?
To what exent is catalyst activity, specificity and selctivity influenced by the second coordination sphere and confinement effects?

Recent NMBU publications on LPMOs that are relevant for CuBE:

The impact of reductants on the catalytic efficiency of a lytic polysaccharide monooxygenase and the special role of dehydroascorbic acid. Stepnov AA, Christensen IA, Forsberg Z, Aachmann FL, Courtade G, Eijsink VGH. FEBS Lett. 2021 Nov 29.
Characterization of a lytic polysaccharide monooxygenase from Aspergillus fumigatus shows functional variation among family AA11 fungal LPMOs. Støpamo FG, Røhr ÅK, Mekasha S, Petrović DM, Várnai A, Eijsink VGH. J Biological Chemistry 2021 Dec;297(6):101421.
Fast and Specific Peroxygenase Reactions Catalyzed by Fungal Mono-Copper Enzymes. Rieder L, Stepnov AA, Sørlie M, Eijsink VGH. Biochemistry. 2021 Nov 30;60(47):3633-3643.
Kinetic Characterization of a Putatively Chitin-Active LPMO Reveals a Preference for Soluble Substrates and Absence of Monooxygenase Activity. Rieder L, Petrović D, Väljamäe P, Eijsink VGH, Sørlie M. ACS Catalysis 2021 Sep 17;11(18):11685-11695.
Unraveling the roles of the reductant and free copper ions in LPMO kinetics. Stepnov AA, Forsberg Z, Sørlie M, Nguyen GS, Wentzel A, Røhr ÅK, Eijsink VGH. Biotechnology for Biofuels. 2021 Jan 21;14(1):28.

Open questions

What is the rate-limiting step in LPMO catalysis and what is the nature of the catalytic Cu-oxygen species?
What are the functional implications of the huge variation among LPMO sequences and how does this variation affect copper reativity?
What is the relative importance and O₂ and H₂O₂ as co-substrate and how does the nature of the co-substrate affect the catalytic mechanism and its intermediates?
What factors determine substrate specificity?
What is the role of confinement in LPMO performance?
How can autocatalytic oxidative damage to the LPMO active site be prevented?
Can we, by looking into nature and, more so, by clever design, expand the substrate range of LPMOs to include alkanes or other polymers such as plastics?

Open questions

What is the effect of the redox/coordinative environment on the formation of (multimeric) active sites?
What is the role of framework protons on the reaction?
What is the role of water on the reaction?
What is the rate-determining step? Is it the same for all materials?
How much of the Cu is available for active site formation? How does this vary in different zeolites?
Can structure-activity relationships be described by simple parameters?

Department of Chemistry University of Turin

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