Det 21. Landsmøte i kjemi

Foredrag - Abstracts

Fellesarrangemnetet står først, ellers er foredragene nummerert etter faggruppe:

FE - Fellesarrangement

AN - Analytisk kjemi

KA - Katalyse

HI - Kjemiens historie

KI - Kjemometri

UN - Kjemiundervisning

KM - Kvantekjemi og modellering

MK - Makromolekyl- og kolloidkjemi

MA - Matkjemi

OR - Organisk kjemi

UM - Uorganisk kjemi og materialkjemi

Postere (kommer)


Dette dokumentet oppdateres etterhvert som abstractene kommer inn.



FE - Fellesarrangement


GW

Guldberg-Waage-foredrag

Hydrogen

Truls Norby

Kjemisk Institutt, Universitetet i Oslo

Starting my first research in inorganic chemistry, I stumbled across hydrogen where and when I and everyone else did not expect to find it – it is so common and yet so un-common. It makes bonds more different than any other element – polar and purely covalent as protons and atoms, metallic when it pleases, and ionic as hydride ions. Consequently, it shows up in very different forms and locations and has taken me for a journey to my roots in physical chemistry and to electrochemistry – some things discovered and some mysteries remaining. Hydrogen holds a historical role in the establishment of major Norwegian industry, and we today host world-leading production of electrolyzers for the emerging markets of hydrogen for storage and as carrier of renewable electrical energy.

Many different types of solids contain or may take up water and become solid-state proton conductors by various mechanisms of transport. They may be used as electrolytes in novel types of fuel cells and electrolyzers for hydrogen and renewable energy, as well as in electrocatalytic reactors for upgrading natural gas to liquids or hydrogen with minimal carbon emissions or with carbon capture and storage. The research involves experimental and ab initio computational methods to understand hydrogen in its various forms from gas phase, via surfaces and charge transfer at electrode interfaces, into mobile ions in crystalline or liquid-like condensed phases.



FE1

Bottom-up Assembly of Active, Autonomous and Complex Bioinspired Systems with Adaptive Behaviour

Daniela Wilson

Systems Chemistry, Radboud University Nijmegen, Institute for Molecules and Materials Nijmegen, The Netherlands
d.wilson@science.ru.nl

Self-powered artificial motile systems are currently attracting increased interest as mimics of biological motors but also as potential components of nanomachinery, robotics, and sensing devices [1]. We have recently demonstrated a supramolecular approach to design synthetic nanomotors using self-assembly of amphiphilic block copolymers into polymersomes and the controlled folding of the vesicles under osmotic stress into a bowl shape morphology [2]. The folding process can be precisely controlled to generate different complex architectures [3] with adjustable openings and selective entrapment of inorganic catalysts [4,5] enzymes or multiple enzymes working together in a metabolic pathway [6,7]. Control of the speed and behaviour of the nanomotors is possible due to integration of regulatory feedback and feedforward loops in the enzyme networks designed to preserve energy and run the motors at even lower concentrations of fuel eg. 0.05 mM Glucose. Movement in both blood serum and plasma at physiological concentrations of substrates is consequently demonstrated. The nanomotor is now not only running at low concentrations of fuel but also able to regulate it's fuel consumption to achieve the same output speed showing adaptive behaviour. Recent developments on greater control over the movement of the nanomotors under chemical gradients or temperature will be presented [4,7]. Additional manipulation of the nanomotors under external stimuli and their biomedical applications will be discussed [6,7].

Acknowledgement. This work was supported in part by the European Research Council under the European Union's Seventh Framework Programme (FP7/2007-20012)/ERC-StG 307679 "StomaMotors".

Acknowledgement

This work was supported in part by the European Research Council under the European Union's Seventh Framework Programme (FP7/2007-20012)/ERC-StG 307679 (StomaMotors).

References
  1. a) Abdelmohsen, L. K. E. A., Peng, F., Tu, Y. Wilson, D. A., J. Mater. Chem. B., 2014, 2, 2395-2408. (b) Tu, Y. Peng, F. Adawy, A. Men, Y.; Abdelmohsen, L.K.E.A.; Wilson, D. A. Chem. Rev. 2016, doi: 10.1021/acs.chemrev.5b00344 c) Fei Peng, Yingfeng Tu, Daniela A. Wilson Chem. Soc. Rev. 2017, DOI: 10.1039/C6CS00885B
  2. (a) Wilson, D.A., Nolte, R, J. M., van Hest, J.C.M. Nature Chem. 2012, 4, 268-274. b) Wilson, D.A., Nolte, R, J. M., van Hest, J.C.M. J. Am. Chem. Soc., 134, 9894, (2012). (b) Wilson, D.A., de Nijs, B., van Blaaderen, A., Nolte, R, J. M., van Hest, J.C.M., Nanoscale, 2013, 5, 1315.
  3. (a) R.S.M. Rikken, H. Engelkamp, R.J.M. Nolte, J.C. Maan, J.C.M. van Hest, D.A. Wilson& P.C.M. Christianen "Shaping polymersomes into predictable morphologies via out-of-equilibrium self-assembly", Nat. Commun 2016, doi:10.1038/NCOMMS12606 (b) Fei Peng, Nannan Deng, Yingfeng Tu, Jan C.M. van Hest, Daniela A. Wilson, Nanoscale 2017 DOI: 10.1039/C7NR00142H (b) 
  4. a) Abdelmohsen, L. K. E. A., Nijemeisland, M, Pawar, G. M. Janssen, G.-J. A. Nolte, R. J. M., van Hest,  J. C. M. & Wilson, D.A. *, ACS Nano, 2016, 10 (2), pp 2652-2660. b) Peng, F. Tu, Y. Pierson, L., van Hest, J. C. M., Wilson, D. A.*, Angew. Chem. Int. Ed. 2015, 54 (40) 11662-11665
  5. a) R. Rikken, R.J.M. Nolte, J.C. Maan, J.C M van Hest, D. A. Wilson P.C.M. Christianen, Soft Matter, 2013, DOI: 10.1039/C3SM52294F R. Rikken, R.J.M. Nolte, J.C. Maan, J.C M van Hest, P.C.M. Christianen, D. A. Wilson Chem Commun, 2013, DOI:10.1039/C3CC47483F
  6. a) Rhee, P. G.; Rikken, R. S.; Nolte, R. J. M., Maan, J. C., van Hest, J. C. M., Christianen, P. C. M. and Wilson, D. A.* Nature Commun. 5, 2014, doi: 10.1038/ncomms6010. b) Fei Peng, Yingfeng Tu, Jan C.M. van Hest, Wilson, D. A.*, Adv. Mater., 2016, DOI: 10.1002/adma.201604996.
  7. (a) Yingfeng Tu, Fei Peng, Xiaofeng Sui, Paul White, Jan C.M. van Hest, Wilson, D. A. Nature. Chem. 2017 DOI: 10.1038/nchem.2674. (b) Yingfeng Tu, Fei Peng, Alain Andre, Yongjun Men, Daniela A. Wilson*, ACS Nano 2017, DOI:10.1021/acsnano.6b08079 (c) Fei Peng, Yingfeng Tu, Ashish Adhikari, Jordi J.C.J Hintzen, Dennis Lowik, Daniela A. Wilson* Chem Commun 2017, 53, 1088-1091. (d) Fei Peng, Yongjun Men, Yingfeng Tu, Daniela A. Wilson, Adv. Funct. Mater. 2018, 10.1002/adfm.201706117 (e) Yingfeng Tu, Fei Peng, Paul B. White, Daniela A. Wilson, Angew. Chem. Int. Ed. 2017, doi: 10.1002/anie.201703276, 56 (26), 7620-7624

FE2

Molecular Spin Switches

R. Herges

Otto-Diels Institute for Organic Chemistry, University of Kiel, Germany
Magnetic bistability at room temperature, such as the orientation of magnetization used in magnetic storage media, or spin flips in spin crossover transition metal complexes are typical solid-state phenomena. Six years ago, we published the first bistable molecular system [1]. Our spin switches are based on a Ni-porphyrin equipped with a photochromic azogroup that moves an axial ligand up and down upon irradiation with violet (430 nm), and green light (530 nm). By changing the coordination number, the Ni2+ reversibly changes its spin state from singlet (diamagnetic) to triplet (paramagnetic). The switching efficiency in both directions is 100% within the accuracy of NMR and UV spectroscopy, and there is no fatigue after more than 100 000 switching cycles. Potential applications are the use as switchable contrast agents for MRI in interventional radiology for patients suffering from stroke or myocardial infarction [2]. Further developments are aiming at measuring temperatures or pH with high spatial 3D resolution by MRI in deep tissue.

To replace Ni2+ by physiologically benign Fe3+, and to increase the change in magnetic moment (Ni2+ : ΔS=1, Fe3+ : ΔS=2) we developed a molecular spin switch based on Fe(III) tetraphenyl porphyrin and a custom-build azopyridine ligand. Again switching between low-spin (S=1/2) and high-spin (5/2) is close to quantitative, and no fatigue was observed after several hundred cycles [3].

Spin switching in iron porphyrins is the key step in a number of enzymatic reactions, particularly in C-H activation (e.g. cytochrome P450). Our system provides the basis for the development of artificial cytochrome type complexes.

Figure 1

Figure 1: Spin switching with iron.

References
  1. S. Venkataramani, U. Jana, M. Dommaschk, F. D. Sšnnichsen, F. Tuczek, R. Herges, Science 2011, 331, 445.
  2. M. Dommaschk, M. Peters, F.Gutzeit, C. Schuett, C. Naether, F.D. Soennichsen, S. Tiwari,C. Riedel, S. Boretius, R. Herges, J. Am. Chem. Soc. 2015, 137, 7552.
  3. unpublished.

FE3

Industry lecture

Radionuclides and cancer treatment: How to succeed

Roy Larsen

Oncoinvent AS

Radionuclides have been used for cancer treatment for almost a century. Initially gamma and beta emitters were used but later alpha emitters attracted a substantial attention. Criterion for successful product development should be determined before initiation of the clinical phase of product development. The product candidate’s chemical and physical properties must be carefully considered, and synthesis route should be adaptable to industrial scale. The product candidate must show consistent antitumor activity and acceptable safety profile in the preclinical tests and dosimetry estimates for human use should indicate appropriate benefit to risk ratio. Sufficient patent protection is needed to attract investors.

Radionuclides and properties are addressed, and examples of clinical products are presented.

Norwegian inventions in the field are presented and the international trends in the field are discussed. 
 
 


FE4

Integrating cryogenic ion chemistry and spectroscopy: Capture and characterization of reaction intermediates in homogeneous catalysis

Mark Johnson

Yale Univerisity
The coupling between ambient ionization sources, developed for mass spectrometric analysis of biomolecules, and cryogenic ion processing, originally designed to study astrochemistry, creates a new and general way to capture transient chemical species and elucidate their structures with optical spectroscopies. Advances in non-linear optics over the past decade allow single-investigator, table top lasers to access radiation from 550 cm-1 in the infrared to the vacuum ultraviolet. When spectra are acquired using predissociation of weakly bound rare gas "tags", the resulting patterns are equivalent to absorption spectra and correspond to target ions at temperatures below 10K. Taken together, what emerges is a new and powerful structural component to traditional mass spectrometric analysis. Recent applications ranging from the mechanisms of small molecule activation by homogeneous catalysts to the microscopic mechanics underlying the Grotthuss proton relay mechanism in water emphasize the generality and utility of the methods in contemporary chemistry.


FE5

Semi-artificial Photosynthesis

Erwin Reisner

Department of Chemistry, University of Cambridge, Lensfield Road, Cambridge CB2 1EW, UK
E-mail:
reisner@ch.cam.ac.uk
Web:
http://www-reisner.ch.cam.ac.uk/
In photosynthesis, light is used for the production of chemical energy carriers to fuel biological activity and the water oxidation enzyme Photosystem II is the first protein complex in the light-dependent reactions of oxygenic photosynthesis. This presentation will summarise our progress in the development of protein film photoelectrochemistry as a technique for the activity of this enzyme adsorbed onto an electrode surface to be studied.[1] Materials design enabled us to develop 'tailor-made' 3D electrode scaffolds for optimised integration of the 'wired' enzyme and these investigations yielded valuable insights into Photosystem II function. Examples are the identification of unnatural charge transfer pathways to the electrode and the elucidation of O2 reduction pathway that short-circuit the known water-oxidation process.[2]

The integration of Photosystem II in a photoelectrochemical circuit has enabled the in vitro re-engineering of natural photosynthetic pathways. We assembled an efficient semi-artificial water splitting cell driven by light through the rational wiring of Photosystem II to a H2 producing enzyme known as hydrogenase (Figure 1).[3] This hydrogenase displays unique properties for water splitting applications as it displays good H2 evolution activity, little product (H2) inhibition and some tolerance towards O2.[4] The bio-hybrid water splitting cell shows how we can harvest and utilise electrons generated during water oxidation at Photosystem II electrodes for the generation of renewable H2 with a wired hydrogenase through a direct pathway unavailable to biology. Progress in the assembly of bias-free tandem water splitting cells with wired enzymes and the integration of robust live cyanobacteria in 3D structured electrodes will also be discussed.[5]

Figure 1

Figure 1. Schematic representation of a semi-artificial water splitting system. Water is photo-oxidized and O2 generated at a Photosystem II-containing photoanode and aqueous protons are reduced at a hydrogenase-based cathode. Enzyme-integration was optimised by using a hierarchical ITO architecture.

References
  1. Kato, Zhang, Paul & Reisner, Chem. Soc. Rev., 2014, 43, 6485-6497.
  2. Zhang, Sokol, Paul, Romero, van Grondelle, & Reisner, Nature Chem. Biol., 2016, 12, 1046-1052.
  3. Mersch, Lee, Zhang, Brinkert, Fontecilla-Camps, Rutherford & Reisner J. Am. Chem. Soc., 2015, 137, 8541-8549.
  4. Wombwell, Caputo & Reisner, Acc. Chem. Res., 2015, 48, 2858-2865.
  5. Zhang, Bombelli, Sokol, Fantuzzi, Rutherford, Howe & Reisner, J. Am. Chem. Soc., 2018, 140, 6-9.

AN - Analytisk kjemi


AN1


KA - Katalyse


KAi1

Probing Active Species in Catalysis – Application of Advanced X-ray Techniques

Moniek Tromp

Materials Chemistry, Zernike Institute for Advanced Materials, University of Groningen, Groningen, The Netherlands moniek.tromp@rug.nl
Detailed information on the structural and electronic properties of a catalyst or material and how they change during reaction is required to understand their reaction mechanism and performance. An experimental technique that can provide structural as well as electronic analysis and that can be applied in situ/operando and in a time-resolved mode, is X-ray spectroscopy. Extended X-ray Absorption Fine Structure (EXAFS) spectroscopy is powerful in determining the local structure of compounds including amorphous materials and solutions, since long-range order is not required. Combined X-ray Absorption and X-ray Emission spectroscopy (XAS and XES resp.) provides detailed insights in the electronic properties of a material. Detailed information about the materials in their dynamic chemical active environment can thus be obtained and structure/electronic – performance relationships and reaction mechanisms derived. A combination of spectroscopic techniques (e.g. UV-Vis, IR) gives complementary information about the system under investigation.

Over the last years, different approaches have been reported to allow operando time resolved XAS on catalytic systems, mostly solid-gas. Our group has developed stopped-flow methodologies allowing simultaneous time-resolved UV–Vis/XAS experimentation on liquid systems down to the millisecond (ms) time resolution [1]. Low X-ray energy systems (light elements) or for low concentrated systems, longer XAS data acquisition times in fluorescence detection are required and therefore a stopped flow freeze-quench procedure has been developed [2]. Pushing the time-resolution has been achieved by synchronizing the synchrotron bunches with an optical laser in order to perform fast pump-probe experiments [3] or micro-reactors for modulation excitation experiments [4].

Developments in XAS using new instrumentation and data acquisition methods while selecting specific X-ray energies provide this more detailed electronic information [5]. High energy resolution XAS, XES and Resonant Inelastic X-ray Scattering (RIXS) provide very detailed electronic information on the systems under investigation. The secondary spectrometer design also opens up lab based spectrometer designs as will be demonstrated.

The methodologies and instrumentation have been developed and applied to a wealth of materials science, for homogeneous and heterogeneous catalysis to batteries and fuel cells as well as art objects. In this lecture, several examples will be given with an emphasis on homogeneous catalysis, providing insights in activated species and reaction mechanisms of selective oligomerisation reaction.

References
  1. e.g. Tromp M. et al. Organometallics 2010, 29, 3085–3097.
  2. Bartlett S.A. et al.  J. Catal. 2011, 284, 247–258; ACS Catalysis 2014, 4, 4201; Catal. Sci. Techn. 2016, 6, 6237; Tromp, M. et al, under review.
  3. Tromp, M. et al. J. Phys. Chem. B 2013, 117(24), 7381–7387.
  4. Tromp, M. manuscript in preparation.
  5. e.g. Thomas, R. J. et al. J. Phys. Chem. C 2015, 119(5), 2419–2426; Tromp M. et al, under review.


KAi2

From Homogeneous to Heterogeneous catalysis: Use of Microporous Solids as Macroligands

Jéróme Canivet

Univ. Lyon, Univ. Claude Bernard Lyon 1, CNRS, IRCELYON - UMR 5256, Villeurbanne, France.  
jerome.canivet@ircelyon.univ-lyon1.fr
At the molecular scale, the integration of the catalytically active centers into a solid support without loss of performance compared to the homogeneous analog is still a major challenge. In this context, a molecularly defined support as macroligand, i.e. a solid acting like the ligand in the corresponding molecular complex, can be considered as a key to bridge the gap between molecular and heterogeneous catalysis. Metal-Organic Frameworks and purely organic microporous polymers are promising candidates. In particular, porous frameworks made by the repetition of a coordinating motif, like the bipyridine motif are of a high interest as far as bipyridines are widely used as chelating ligand for molecular catalysts.[1,2]. We show that both homogeneous and heterogenized catalysts follow the same linear correlation between the electronic effect of the ligand, described by the Hammett parameter, and the catalytic activity as exemplified in two reactions. This correlation highlights the crucial impact of the local electronic environment surrounding the active catalytic center over the long-range framework structure of the porous support. The gap between molecular and heterogeneous catalysis has never been so close to being bridged. This work is carried out within the H-CCAT project that has received funding from the European Union’s Horizon 2020 research and innovation program under grant agreement No 720996. H-CCAT aims at the large scale production of MOF catalysts and at their use in the industrial production of pharmaceuticals.

References
  1. F. M. Wisser, P. Berruyer, L. Cardenas, Y. Mohr, E. A. Quadrelli, A. Lesage, D. Farrusseng, J. Canivet, ACS Catal., DOI: 10.1021/acscatal.7b03998 (2018)
  2. F. M. Wisser, Y. Mohr, E. A. Quadrelli, D. Farrusseng, J. Canivet, ChemCatChem, DOI: 10.1002/cctc.201701836 (2018).


HI - Kjemiens historie



KI - Kjemometri



UN - Kjemiundervisning



KM - Kvantekjemi og modellering



MK - Makromolekyl- og kolloidkjemi



MA - Matkjemi



OR - Organisk kjemi



UM - Uorganisk kjemi og materialkjemi