Ainara Nova Flores

• Bai, Yunfei; Cordero-Lanzac, Tomás; Nova Flores, Ainara; Olsbye, Unni; Taarning, Esben & Martinez-Espin, Juan S. (2024). Selective linear ethylene oligomerization over nickel-containing zeotypes with tetravalent framework heteroatoms. Catalysis Science & Technology. ISSN 2044-4753. doi: 10.1039/d3cy01736b.
• Kneiding, Hannes; Nova Flores, Ainara & Balcells Badia, David (2024). Directional multiobjective optimization of metal complexes at the billion-system scale. Nature Computational Science. ISSN 2662-8457. doi: 10.1038/s43588-024-00616-5.
• Gadde, Karthik; Reddy Bheemireddy, Narendraprasad; Heitkämper, Juliane; Nova Flores, Ainara & Maes, Bert (2024). Directed Palladium-Catalyzed γ-C(sp³)-H Alkenylation of (Aza and Oxa) Cyclohexanamines with Bromoalkenes: Bromide Precipitation as an Alternative to Silver Scavenging. ACS Catalysis. ISSN 2155-5435. 14(2), p. 1157–1172. doi: 10.1021/acscatal.3c04152.
• Sun, Hongwei; Ahrens, Alexander; Batista, Gabriel Martins Ferreira; Donslund, Bjarke S.; Ravn, Anne K. & Schwibinger, Emil Vincent [Show all 8 contributors for this article] (2024). Solvent-base mismatch enables the deconstruction of epoxy polymers and bisphenol A recovery. Green Chemistry. ISSN 1463-9262. doi: 10.1039/d3gc03707j. Full text in Research Archive
• Pulumati, Sri Harsha; Sannes, Dag Kristian; Jabbour, Christia R.; Mandemaker, Laurens D. B.; Weckhuysen, Bert M. & Olsbye, Unni [Show all 8 contributors for this article] (2023). Mechanistic Insights in the Catalytic Hydrogenation of CO<inf>2</inf> over Pt Nanoparticles in UiO-67 Metal-Organic Frameworks. ACS Catalysis. ISSN 2155-5435. 14(1), p. 382–394. doi: 10.1021/acscatal.3c03401. Full text in Research Archive
• Holmsen, Marte Sofie Martinsen; Nova Flores, Ainara & Tilset, Mats (2023). Cyclometalated (N,C) Au(III) Complexes: The Impact of Trans Effects on Their Synthesis, Structure, and Reactivity. Accounts of Chemical Research. ISSN 0001-4842. 56(24), p. 3654–3664. doi: 10.1021/acs.accounts.3c00595. Full text in Research Archive
• Berntsen, Linn Neerbye & Nova Flores, Ainara (2023). A Mechanistic Study of the Cu-catalyzed N-arylation of Hydantoin with Aryl(TMP)iodonium Salts. ChemCatChem. ISSN 1867-3880. doi: 10.1002/cctc.202301057. Full text in Research Archive
• Jenny, Sarah; Serviano, Juan M.; Nova Flores, Ainara & Dobereiner, Graham E. (2023). A Hydride Migration Mechanism for the Mo-Catalyzed Z-2-Selective Isomerization of Terminal Alkenes. ChemCatChem. ISSN 1867-3880. 15. doi: 10.1002/cctc.202301052.
• Kneiding, Hannes; Nova Flores, Ainara & Balcells Badia, David (2023). Directional Multiobjective Optimization of Metal Complexes at the Billion-Scale with the tmQMg-L Dataset and PL-MOGA Algorithm. ChemRxiv. ISSN 2573-2293. doi: 10.26434/chemrxiv-2023-k3tf2-v2. Show summary

  Transition metal complexes (TMCs) play a key role in several areas of high interest, including medicinal chemistry, renewable energies, and nanoporous materials. The development of TMCs enabling these technologies remains challenged by the need to optimize multiple properties within very large chemical spaces, in which the thirty transition metals can be combined with a virtually infinite number of ligands. In this work, we provide the open tmQMg-L dataset including 30K TMC ligands, which combines large chemical diversity with synthesizability. The charge and metal-coordination mode of the ligands were robustly defined with a novel algorithm based on graph and natural bond orbital theories. The tmQMg-L dataset was leveraged in the automated generation of 1.37M TMCs resulting from all possible combinations between a square planar palladium(II) scaffold and a pool of 50 different ligands. This TMC space was used to benchmark a multiobjective genetic algorithm (MOGA) that optimized two properties over a Pareto front; namely the polarizability (alpha) and the HOMO-LUMO gap (epsilon). The MOGA evolved 130 TMC hits with maximal (alpha, epsilon) values in a way that could be easily rationalized by analyzing the nature of the ligands selected. Instead of the traditional mutation and crossover of fragments within a single ligand, this MOGA implemented full-ligand genetic operations acting on all coordination sites, maximizing chemical diversity. Further, we extended this MOGA algorithm with the Pareto-Lighthouse functionality (PL-MOGA), which allows for controlling both the aim and scope of the multiobjective optimization over the Pareto front. In explicit spaces containing billions of TMCs, the PL-MOGA enabled the explainable generation of thousands of novel and highly diverse TMC hits. We believe that the combined use of the tmQMg-L dataset and PL-MOGA algorithm will facilitate the discovery of TMCs with optimal properties within untapped chemical spaces.

• Bai, Yunfei; Taarning, Esben; Luthra, Mahika; Lundegaard, Lars F.; Katerinopoulou, Anna & Falsig, Hanne [Show all 8 contributors for this article] (2023). Tracking Lattice Distortion Induced by Defects and Framework Tin in Beta Zeotypes. Journal of Physical Chemistry C. ISSN 1932-7447. 127(38), p. 19278–19289. doi: 10.1021/acs.jpcc.3c04751. Full text in Research Archive
• Rama, Raquel J.; Maya, Celia; Molina, Francisco; Nova Flores, Ainara & Nicasio, M. Carmen (2023). Important Role of NH-Carbazole in Aryl Amination Reactions Catalyzed by 2-Aminobiphenyl Palladacycles. ACS Catalysis. ISSN 2155-5435. 13(6), p. 3934–3948. doi: 10.1021/acscatal.3c00075. Full text in Research Archive
• Sannes, Dag Kristian; Øien-Ødegaard, Sigurd; Aunan, Erlend ; Nova, Ainara & Olsbye, Unni (2023). Quantification of Linker Defects in UiO-Type Metal-Organic Frameworks. Chemistry of Materials. ISSN 0897-4756. 35(10), p. 3793–3800. doi: 10.1021/acs.chemmater.2c03744. Full text in Research Archive
• Hong, Wanwan; Luthra, Mahika; Jakobsen, Joakim B.; Madsen, Monica R.; Castro, Abril C & Hammershøj, Hans Christian D. [Show all 11 contributors for this article] (2023). Exploring the Parameters Controlling Product Selectivity in Electrochemical CO<inf>2</inf> Reduction in Competition with Hydrogen Evolution Employing Manganese Bipyridine Complexes. ACS Catalysis. ISSN 2155-5435. p. 3109–3119. doi: 10.1021/acscatal.2c05951. Full text in Research Archive
• Somerville, Rosie J.; Borys, Andryj M.; Perez-Jimenez, Marina; Nova, Ainara; Balcells Badia, David & Malaspina, Lorraine A. [Show all 10 contributors for this article] (2022). Unmasking the constitution and bonding of the proposed lithium nickelate “Li3NiPh3(solv)3”: revealing the hidden C6H4 ligand† . Chemical Science. ISSN 2041-6520. 13. doi: 10.1039/d2sc01244h. Full text in Research Archive
• Pizarro, Juan Diego; Schmidtke, Inga; Nova, Ainara; Fructos, Manuel R. & Pérez, Pedro J. (2022). Selective Functionalization of Arene C(sp2)-H Bonds by Gold Catalysis: The Role of Carbene Substituents. ACS Catalysis. ISSN 2155-5435. 12(12), p. 6851–6856. doi: 10.1021/acscatal.2c01713. Full text in Research Archive
• Hylland, Knut Tormodssønn; Schmidtke, Inga; Wragg, David Stephen; Nova, Ainara & Tilset, Mats (2022). Synthesis of substituted (N,C) and (N,C,C) Au(iii) complexes: the influence of sterics and electronics on cyclometalation reactions. Dalton Transactions. ISSN 1477-9226. 51(13), p. 5082–5097. doi: 10.1039/d2dt00371f. Full text in Research Archive
• Artús Suàrez, Lluís; Balcells Badia, David & Nova, Ainara (2021). Computational Studies on the Mechanisms for Deaminative Amide Hydrogenation by Homogeneous Bifunctional Catalysts. Topics in catalysis. ISSN 1022-5528. 65, p. 82–95. doi: 10.1007/s11244-021-01542-w. Full text in Research Archive
• Berntsen, Linn Neerbye; Nova, Ainara; Wragg, David & Sandtorv, Alexander Harald (2020). Cu-catalyzed N-3-Arylation of Hydantoins Using Diaryliodonium Salts. Organic Letters. ISSN 1523-7060. 22(7), p. 2687–2691. doi: 10.1021/acs.orglett.0c00642. Full text in Research Archive Show summary

  A general Cu-catalyzed, regioselective method for the N-3-arylation of hydantoins is described. The protocol utilizes aryl(trimethoxyphenyl)iodonium tosylate as the arylating agent in the presence of triethylamine and a catalytic amount of a simple Cu-salt. The method is compatible with structurally diverse hydantoins and operates well with neutral aryl groups or aryl groups bearing weakly donating/withdrawing elements. It is also applicable for the rapid diversification of pharmaceutically relevant hydantoins.

• Gutterød, Emil Sebastian; Pulumati, S.H.; Kaur, Gurpreet; Lazzarini, Andrea; Solemsli, Bjørn Garding & Gunnæs, Anette Eleonora [Show all 13 contributors for this article] (2020). Influence of Defects and H2O on the Hydrogenation of CO2 to Methanol over Pt Nanoparticles in UiO-67 Metal-Organic Framework. Journal of the American Chemical Society. ISSN 0002-7863. 142(40), p. 17105–17118. doi: 10.1021/jacs.0c07153. Full text in Research Archive
• Levchenko, Vladimir; Nova, Ainara; Øien-Ødegaard, Sigurd; Balcells, David & Tilset, Mats (2020). Synthesis, Characterization, and Reactivity of Cyclometalated Gold(III) Dihalide Complexes in Aqua Regia. European Journal of Inorganic Chemistry (EurJIC). ISSN 1434-1948. 2020(34), p. 3249–3258. doi: 10.1002/ejic.202000529. Full text in Research Archive
• Artús Suàrez, Lluís; Jayarathne, Upul; Balcells, David; Bernskoetter, Wesley H.; Hazari, Nilay & Jaraiz, Martin [Show all 7 contributors for this article] (2020). Rational selection of co-catalysts for the deaminative hydrogenation of amides. Chemical Science. ISSN 2041-6520. 11(8), p. 2225–2230. doi: 10.1039/c9sc03812d. Full text in Research Archive
• Gutterød, Emil Sebastian; Lazzarini, Andrea; Fjermestad, Torstein; Kaur, Gurpreet; Manzoli, Maela & Bordiga, Silvia [Show all 12 contributors for this article] (2019). Hydrogenation of CO2 to Methanol by Pt Nanoparticles Encapsulated in UiO-67: Deciphering the Role of the Metal−Organic Framework. Journal of the American Chemical Society. ISSN 0002-7863. 142. doi: 10.1021/jacs.9b10873. Full text in Research Archive Show summary

  Metal-organic frameworks (MOFs) show great prospect as catalysts and catalyst support materials. Yet, studies that address their dynamic, kinetic and mechanistic role in target reactions are scarce. In this study, an exceptionally stable MOF catalyst consisting of Pt nanoparticles (NPs) embedded in a Zr-based UiO-67 MOF was subject to steady-state and transient kinetic studies involving H/D and 13C /12C exchange, coupled with operando infrared spectroscopy and density functional theory (DFT) modeling, targeting methanol formation from CO2/H2 feeds at 170 C and 1-8 bar pressure. The study revealed that methanol is formed at the interface between the Pt NPs and defect Zr nodes, via formate species attached to the Zr nodes. Methanol formation is mechanistically separated from the formation of co-products CO and methane, except for hydrogen activation on the Pt NPs. Careful analysis of transient data revealed that the number of intermediates was higher than the number of open Zr sites in the MOF lattice around each Pt NP. Hence, additional Zr sites must be available to formate formation. DFT modelling revealed that Pt NP growth is sufficiently energetically favored to enable displacement of linkers and creation of open Zr sites during pretreatment. However, linker displacement during formate formation is energetically disfavored, in line with the excellent catalyst stability observed experimentally. Overall, the study provides firm evidence that methanol is formed at the interface of Pt NPs and linker-deficient Zr6O8 nodes resting on the Pt NP surface.

• Holmsen, Marte Sofie; Nova, Ainara; Øien-Ødegaard, Sigurd; Heyn, Richard H. & Tilset, Mats (2019). A highly asymmetric gold(III) η3‐allyl complex. Angewandte Chemie International Edition. ISSN 1433-7851. 59(4), p. 1516–1520. doi: 10.1002/anie.201912315. Full text in Research Archive Show summary

  A highly asymmetric AuIII η3‐allyl complex has been generated by treating Au(η1‐allyl)Br(tpy) (tpy=2‐(p‐tolyl)pyridine) with AgNTf2. The resulting η3‐allyl complex has been characterized by NMR spectroscopy and X‐ray crystallography. DFT calculations and variable temperature 1H NMR suggest that the allyl ligand is highly fluxional.

• Leischner, Thomas; Artus Suarez, Lluis; Spannenberg, Anke; Junge, Kathrin; Nova, Ainara & Beller, Matthias (2019). Highly selective hydrogenation of amides catalysed by a molybdenum pincer complex: scope and mechanism. Chemical Science. ISSN 2041-6520. 10(45), p. 10566–10576. doi: 10.1039/c9sc03453f. Full text in Research Archive
• Holmsen, Marte Sofie; Nova, Ainara; Hylland, Knut Tormodssønn; Wragg, David; Øien-Ødegaard, Sigurd & Heyn, Richard H. [Show all 7 contributors for this article] (2018). Synthesis of a (N,C,C) Au(III) pincer complex via Csp3–H bond activation: increasing catalyst robustness by rational catalyst design. Chemical Communications. ISSN 1359-7345. 54(79), p. 11104–11107. doi: 10.1039/c8cc05489d.
• Artus Suarez, Lluis; Culakova, Zuzana; Balcells, David; Bernskoetter, Wesley H; Eisenstein, Odile & Goldberg, Karen I. [Show all 9 contributors for this article] (2018). The Key Role of the Hemiaminal Intermediate in the Iron-Catalyzed Deaminative Hydrogenation of Amides. ACS Catalysis. ISSN 2155-5435. 8(9), p. 8751–8762. doi: 10.1021/acscatal.8b02184.
• Grajeda, Javier; Nova, Ainara; Balcells, David; Bruch, Quinton J.; Wragg, David & Heyn, Richard H. [Show all 8 contributors for this article] (2018). Synthesis and characterization of stable gold(III) PNP pincer complexes. European Journal of Inorganic Chemistry (EurJIC). ISSN 1434-1948. 2018(26), p. 3113–3117. doi: 10.1002/ejic.201800019.
• Balcells, David & Nova, Ainara (2018). Designing Pd and Ni Catalysts for Cross-Coupling Reactions by Minimizing Off-Cycle Species. ACS Catalysis. ISSN 2155-5435. 8(4), p. 3499–3515. doi: 10.1021/acscatal.8b00230. Full text in Research Archive
• Melvin, Patrick R.; Nova, Ainara; Balcells, David; Hazari, Nilay & Tilset, Mats (2017). DFT Investigation of Suzuki-Miyaura Reactions with Aryl Sulfamates Using a Dialkylbiarylphosphine-Ligated Palladium Catalyst. Organometallics. ISSN 0276-7333. 36(18), p. 3664–3675. doi: 10.1021/acs.organomet.7b00642.
• Vaitla, Janakiram; Guttormsen, Yngve; Mannisto, Jere K.; Nova, Ainara; Repo, Timo & Bayer, Annette [Show all 7 contributors for this article] (2017). Enantioselective incorporation of CO2: status and potential. ACS Catalysis. ISSN 2155-5435. 7(10), p. 7231–7244. doi: 10.1021/acscatal.7b02306. Full text in Research Archive Show summary

  CO2 is a promising and sustainable carbon feedstock for organic synthesis. New catalytic protocols for efficient incorporation of CO2 into organic molecules are continuously reported. However, little progress has been made in the enantioselective conversion of CO2 to form enantioenriched molecules. In order to allow CO2 to become a versatile carbon source in academia, and in the fine chemical and pharmaceutical industries, the development of enantioselective approaches is essential. Here we discuss general strategies for CO2 activation and for generation of enantioenriched molecules, alongside selected examples of reactions involving asymmetric incorporation of CO2. Main product classes considered are carboxylic acids and derivatives (C-CO2 bonds), and carbonates, carbamates, and polycarbonates (C-OCO bonds). Similarities to asymmetric hydrogenation are discussed, and some strategies for developing novel enantioselective CO2 reactions are outlined.

• Holmsen, Marte Sofie; Nova, Ainara; Balcells, David; Langseth, Eirin; Øien-Ødegaard, Sigurd & Heyn, Richard H. [Show all 8 contributors for this article] (2017). trans-Mutation at Gold(III): A mechanistic study of a catalytic acetylene functionalization via a double insertion pathway. ACS Catalysis. ISSN 2155-5435. 7(8), p. 5023–5034. doi: 10.1021/acscatal.7b01364. Full text in Research Archive
• Campos, Jesús; Nova, Ainara; Kolychev, Eugene L. & Aldridge, Simon (2017). A Combined Experimental/Computational Study of the Mechanism of a Palladium-Catalyzed Bora-Negishi Reaction. Chemistry - A European Journal. ISSN 0947-6539. 23(51), p. 12655–12667. doi: 10.1002/chem.201702703.
• Beromi, Megan Mohadjer; Nova, Ainara; Balcells, David; Brasacchio, Ann M; Brudvig, Gary W. & Guard, Louise M. [Show all 8 contributors for this article] (2017). Mechanistic study of an improved Ni precatalyst for Suzuki-Miyaura reactions of aryl sulfamates: Understanding the role of Ni(I) species. Journal of the American Chemical Society. ISSN 0002-7863. 139(2), p. 922–936. doi: 10.1021/jacs.6b11412.
• Peltzer, Raphael Mathias; Eisenstein, Odile; Nova, Ainara & Cascella, Michele (2017). How Solvent Dynamics Controls the Schlenk Equilibrium of Grignard Reagents: A Computational Study of CH3MgCl in Tetrahydrofuran. Journal of Physical Chemistry B. ISSN 1520-6106. 121(16), p. 4226–4237. doi: 10.1021/acs.jpcb.7b02716. Full text in Research Archive
• Holmsen, Marte Sofie; Nova, Ainara; Balcells, David; Langseth, Eirin; Øien-Ødegaard, Sigurd & Tråseth, Eline Aasen [Show all 8 contributors for this article] (2016). Small-molecule activation at Au(III): metallacycle construction from ethylene, water and acetonitrile. Dalton Transactions. ISSN 1477-9226. 45(37), p. 14719–14724. doi: 10.1039/c6dt01648k. Show summary

  Incorporation of the simple, readily available, building blocks ethylene, water and acetonitrile into Au(tpy)(OCOCF3)2 (tpy = 2-(p-tolyl)pyridine) in a one-step reaction leads to high yields of a new 6-membered ring gold(III) metallacycle complex. The metallacycle has been characterized spectroscopically and crystallographically, and the mechanism of its formation has been investigated with the aid of DFT calculations.

• Balcells, David; Clot, Eric; Eisenstein, Odile; Nova, Ainara & Perrin, Lionel (2016). Deciphering Selectivity in Organic Reactions: A Multifaceted Problem. Accounts of Chemical Research. ISSN 0001-4842. 49(5), p. 1070–1078. doi: 10.1021/acs.accounts.6b00099.
• Balcells, David; Eisenstein, Odile; Tilset, Mats & Nova, Ainara (2016). Coordination and insertion of alkenes and alkynes in AuIII complexes: nature of the intermediates from a computational perspective. Dalton Transactions. ISSN 1477-9226. 45(13), p. 5504–5513. doi: 10.1039/c5dt05014f.

View all works in Cristin

• Schmidtke, Inga; Erken, Christina; Repo, Timo & Nova Flores, Ainara (2023). Mechanistic DFT studies of the formation of a novel Rh(I)-ethylene complex.
• Schmidtke, Inga; Erken, Christina; Repo, Timo & Nova Flores, Ainara (2023). Mechanistic DFT studies on the formation of a novel Rh(I)-ethylene complex.
• Nova Flores, Ainara (2023). Modelling (De-)Hydrogenation Reactions using Bifunctional Catalysts.
• Nova Flores, Ainara (2023). Modelling reaction mechanisms of multicomponent catalytic systems .
• Nova Flores, Ainara (2023). Recycling CO2 will help minimising climate effects. NordForsk Rapporter. ISSN 1890-3258.
• Kneiding, Hannes; Nova Flores, Ainara & Balcells Badia, David (2023). Evolutionary Multiobjective Optimization for Transition Metal Complexes.
• Kneiding, Hannes; Nova Flores, Ainara & Balcells Badia, David (2023). Evolutionary Multiobjective Optimization for Transition Metal Complexes.
• Sannes, Dag Kristian; Øien-Ødegaard, Sigurd; Aunan, Erlend; Nova Flores, Ainara & Olsbye, Unni (2023). Quantification of linker defects in UiO-type metal-organic frameworks.
• Nova Flores, Ainara; Skrydstrup, Troels; Daasbjerg, Kim; Bayer, Annette & Karulf, Liselotte (2023). Recommendations for Future CO2 Management in the Nordic Countries.
• Jimenez Rama, Raquel & Nova, Ainara (2022). Synthesis and characterization of linker-based ligands for the CO2 hydrogenation to methanol.
• Jimenez Rama, Raquel; Maya, Celia; Nova, Ainara & Nicasio, M. Carmen (2022). Mechanistic study of palladium-catalyzed C-N couplings supported by terphenyl phosphane ligands.
• Jimenez Rama, Raquel; Maya, Celia; Nova, Ainara & Nicasio, M. Carmen (2022). Mechanistic study of Pd-catalyzed C-N couplings supported by terphenyl phosphane ligands.
• Safy, Mohamed E. A.; Balcells, David & Nova, Ainara (2022). COMBINING DFT AND MACHINE LEARNING TOWARDS DISCOVERING OF NEW CATALYSTS FOR CO2 REDUCTION TO METHANOL.
• Safy, Mohamed E. A.; Balcells, David & Nova, Ainara (2022). Hydrogenation of CO2 to methanol: What is beyond Ru-MACHO? .
• Schmidtke, Inga; Pizarro, Juan Diego; Fructos, Manuel R.; Pérez, Pedro J. & Nova, Ainara (2022). Selective functionalization of arene C(sp2)-H bonds by gold catalysis.
• Schmidtke, Inga; Pizarro, Juan Diego; Fructos, Manuel R.; Pérez, Pedro J. & Nova, Ainara (2022). Selective functionalization of arene C(sp2)-H bonds by gold catalysis.
• Schmidtke, Inga; Pizarro, Juan Diego; Fructos, Manuel R.; Pérez, Pedro J. & Nova, Ainara (2022). Computational study on the role of carbene substituents in a Au(I)-catalyzed C-H-functionalization reaction.
• Das, Tamal & Nova, Ainara (2022). The Multiple Configurations of μ3-OH Functionalized UiO-MOFs and its Potential Relevance in carbon capture and conversion. Show summary

  One strategy to incorporate metal catalysts (MX) into the Zr6O8 nodes of UiO-type metal organic frameworks (MOF) is by μ3-OH proton exchange. In this approach, the relative position of the μ3−OH or μ3−OMX (after functionalization) in the tetrahedral (Td) pore become very relevant since it defines the chemical environment of the reaction. In this work, DFT methods have been used to study the different configurations of UiO MOFs, denoted as [4,0], [3,1] and [2,2] depending on the number of μ3−OH or μ3−OMX pointing into the tetrahedral (Td) pores. Periodic gas phase  DFT calculations on UiO-66 and UiO-67 show that the [4,0] configuration is the most stable and [2,2] is the least stable for the functionalized μ3−OH sites with MX groups being M=Mg, Ca, or Zn, and X=Me, Cl and Br. Furthermore, ab initio molecular dynamics (AIMD) study reveals that node de-metalation occurs from the μ3−OMgMe sites of less stable conformers under explicit solvation (THF) suggesting that the relocation of the catalyst during a postsynthetic metalation is feasible. Calculations also showed a largest compression of the unit cell volume for the UiO-67 [4,0] configuration after metalation. These results should help to understand the reactivity of μ3-OMX single-site catalysts and exploit the potential of this type of functionalization.  

• Das, Tamal & Nova, Ainara (2022). The Multiple Configurations of μ3-OH Functionalized UiO-MOFs and its Potential Relevance in Catalysis . Show summary

  One strategy to incorporate metal catalysts (MX) into the Zr6O8 nodes of UiO-type metal organic frameworks (MOF) is by μ3-OH proton exchange. In this approach, the relative position of the μ3−OH or μ3−OMX (after functionalization) in the tetrahedral (Td) pore become very relevant since it defines the chemical environment of the reaction. In this work, DFT methods have been used to study the different configurations of UiO MOFs, denoted as [4,0], [3,1] and [2,2] depending on the number of μ3−OH or μ3−OMX pointing into the tetrahedral (Td) pores. Periodic gas phase  DFT calculations on UiO-66 and UiO-67 show that the [4,0] configuration is the most stable and [2,2] is the least stable for the functionalized μ3−OH sites with MX groups being M=Mg, Ca, or Zn, and X=Me, Cl and Br. Furthermore, ab initio molecular dynamics (AIMD) study reveals that node de-metalation occurs from the μ3−OMgMe sites of less stable conformers under explicit solvation (THF) suggesting that the relocation of the catalyst during a postsynthetic metalation is feasible. Calculations also showed a largest compression of the unit cell volume for the UiO-67 [4,0] configuration after metalation. These results should help to understand the reactivity of μ3-OMX single-site catalysts and exploit the potential of this type of functionalization.  

• Das, Tamal & Nova, Ainara (2022). Insights Into Multi Configuration Single Metal-Site MOF Based Catalysts: Structure, Stability and Dynamics Study . Show summary

  One strategy to incorporate metal catalysts (MX) into the Zr6O8 nodes of UiO-type metal organic frameworks (MOF) is by μ3-OH proton exchange. In this approach, the relative position of the μ3−OH or μ3−OMX (after functionalization) in the tetrahedral (Td) pore become very relevant since it defines the chemical environment of the reaction. In this work, DFT methods have been used to study the different configurations of UiO MOFs, denoted as [4,0], [3,1] and [2,2] depending on the number of μ3−OH or μ3−OMX pointing into the tetrahedral (Td) pores. Periodic gas phase  DFT calculations on UiO-66 and UiO-67 show that the [4,0] configuration is the most stable and [2,2] is the least stable for the functionalized μ3−OH sites with MX groups being M=Mg, Ca, or Zn, and X=Me, Cl and Br. Furthermore, ab initio molecular dynamics (AIMD) study reveals that node de-metalation occurs from the μ3−OMgMe sites of less stable conformers under explicit solvation (THF) suggesting that the relocation of the catalyst during a postsynthetic metalation is feasible. Calculations also showed a largest compression of the unit cell volume for the UiO-67 [4,0] configuration after metalation. These results should help to understand the reactivity of μ3-OMX single-site catalysts and exploit the potential of this type of functionalization.  

• Cao, Ning; Nova, Ainara; Olsbye, Unni & Balcells, David (2022). Structural characterization of Cu-UiO MOFs by DFT methods.
• Das, Tamal & Nova, Ainara (2022). Insight Into the Multiple Configurations of MOF based Single-Site Catalysts: Structure, Stability and Dynamics. Show summary

  One strategy to incorporate metal catalysts (MX) into the Zr6O8 nodes of UiO-type metal organic frameworks (MOF) is by μ3-OH proton exchange. In this approach, the relative position of the μ3−OH or μ3−OMX (after functionalization) in the tetrahedral (Td) pore become very relevant since it defines the chemical environment of the reaction. In this work, DFT methods have been used to study the different configurations of UiO MOFs, denoted as [4,0], [3,1] and [2,2] depending on the number of μ3−OH or μ3−OMX pointing into the tetrahedral (Td) pores. Periodic gas phase  DFT calculations on UiO-66 and UiO-67 show that the [4,0] configuration is the most stable and [2,2] is the least stable for the functionalized μ3−OH sites with MX groups being M=Mg, Ca, or Zn, and X=Me, Cl and Br. Furthermore, ab initio molecular dynamics (AIMD) study reveals that node de-metalation occurs from the μ3−OMgMe sites of less stable conformers under explicit solvation (THF) suggesting that the relocation of the catalyst during a postsynthetic metalation is feasible. Calculations also showed a largest compression of the unit cell volume for the UiO-67 [4,0] configuration after metalation. These results should help to understand the reactivity of μ3-OMX single-site catalysts and exploit the potential of this type of functionalization.  

• Safy, Mohamed Eid Ahmed; Nova, Ainara & Balcells, David (2022). COMBINING DFT AND MACHINE LEARNING TOWARDS DISCOVERING OF SUPERIOR CATALYSTS FOR CO2 REDUCTION TO METHANOL.
• Nova, Ainara (2022). CO2 Hydrogenation to Methanol via Cooperative Mechanisms.
• Nova, Ainara (2022). The role of amines in the electrochemical reduction of CO2.
• Nova, Ainara (2022). The multiple roles of amines in CO2 conversion reactions.
• Sannes, Dag Kristian; Øien-Ødegaard, Sigurd; Aunan, Erlend; Nova, Ainara & Olsbye, Unni (2022). Reliable determination of linker defects in UiO-type metal-organic frameworks.
• Sannes, Dag Kristian; Øien-Ødegaard, Sigurd; Aunan, Erlend; Nova, Ainara & Olsbye, Unni (2022). Reliable determination of linker defects in UiO-type metal-organic frameworks.
• Luthra, Mahika; Nova, Ainara; Balcells, David & Castro, Abril C (2022). Mechanistic Insight into Electrocatalytic CO2 Reduction with Mn Bipyride complexes using Ab-Initio MD and Static DFT.
• Nova, Ainara (2021). Modelling complex reaction mechanisms of catalytic processes using DFT methods.
• Luthra, Mahika; Nova, Ainara; Castro, Abril C & Balcells, David (2021). Mechanistic Insight into the Electrochemical Reduction of CO2 using Homogenous Molecular Catalysts.
• Nova, Ainara (2021). From C-F activation to CO2 conversion through catalysis: My research career.
• Nova, Ainara (2021). Modelling complex reaction mechanisms of catalytic processes using DFT methods.
• Olsbye, Unni; Gutterød, Emil Sebastian; Lazzarini, Andrea; Fjermestad, Torstein; Pulumati, S.H. & Nova, Ainara [Show all 7 contributors for this article] (2021). Mechanistic studies of CO2 hydrogenation to methanol, methane and CO over Pt-containing Zr-MOFs .
• Nova, Ainara (2020). CO2 hydrogenation reactions on metal-organic frameworks: challenges and opportunities.
• Nova, Ainara (2020). Hydrogenation of CO2 to methanol by PtNP@UiO67.
• Artús Suàrez, Lluís; Balcells, David & Nova, Ainara (2019). Rational Cocatalyst Design for Amide Hydrogenolysis Based on DFT Calculations.
• Nova, Ainara (2019). Can we transform carbon dioxide into something useful?
• Nova, Ainara (2019). Computational design of multivariate MOFs for CO2 conversion to methanol.
• Nova, Ainara (2019). Mechanistic Insight into the Hydrogenation of Amides by Noyori-type Bifunctional Catalysts.
• Nova, Ainara (2019). Rational Design of Homogeneous and Heterogeneous Catalysts for CO2 Hydrogenation to Methanol.
• Artus Suarez, Lluis; Nova, Ainara; Balcells, David & Tilset, Mats (2018). Computational study on the iron-catalyzed hydrogenation of amides to methanol and amines.
• Artus Suarez, Lluis; Nova, Ainara; Balcells, David & Tilset, Mats (2018). Hydrogenation of amides to methanol and amines with an iron-based catalyst. A computational study.
• Nova, Ainara; Balcells, David & Melteig, Elina (2018). Nytt «designer-molekyl» kan spare industrien for store beløp. [Internet]. https://titan.uio.no/node/2909.
• Nova, Ainara (2018). Computational Insight into the Conversion of CO2 to Methanol.
• Nova, Ainara (2018). New Approaches to the Conversion of CO2 to Methanol.
• Nova, Ainara (2018). Towards the Conversion of Carbon Dioxide to Methanol: A Computational Study on the Iron-Catalyzed Hydrogenation of Amides.
• Coenegrachts, Lore; Ralte, Lalrempuia; Nova, Ainara & Le Roux, Erwan (2018). Synthesis and Characterization of Transition Metal Complexes for the Copolymerization of Polar Monomer with CO2.
• Holmsen, Marte Sofie; Nova, Ainara; Ihlefeldt, Franziska Stefanie; Langseth, Eirin; Øien-Ødegaard, Sigurd & Tilset, Mats (2017). Small Molecule Activation at Au(III) Complexes.
• Artus Suarez, Lluis; Nova, Ainara & Balcells, David (2017). Earth-abundant metal catalyst for amide hydrogenation to methanol.
• Nova, Ainara (2017). Mechanistic insight on the Au(III)-catalyzed functionalization of C-C multiple bonds.
• Nova, Ainara (2017). AU(III) CATALYST DESIGN FOR ALKENE AND ALKYNE FUNCTIONALIZATION REACTIONS.
• Holmsen, Marte Sofie; Ihlefeldt, Franziska Stefanie; Nova, Ainara; Wencke, Yannick; Langseth, Eirin & Øien-Ødegaard, Sigurd [Show all 7 contributors for this article] (2016). Au(III) complexes and their reactivity towards alkenes and alkynes.
• Holmsen, Marte Sofie; Nova, Ainara; Wencke, Yannick; Langseth, Eirin; Øien-Ødegaard, Sigurd & Tilset, Mats (2016). NMR and organometallic chemistry – some examples from Au(III) chemistry.
• Holmsen, Marte Sofie; Ihlefeldt, Franziska Stefanie; Nova, Ainara; Wencke, Yannick; Langseth, Eirin & Øien-Ødegaard, Sigurd [Show all 7 contributors for this article] (2016). Au(III) complexes and their reactivity towards alkenes and alkynes.
• Nova, Ainara (2015). Understanding the mechanism of precatalyst activation in Pd Cross-Coupling reactions.
• Berntsen, Linn Neerbye & Nova Flores, Ainara (2023). Development of New Synthetic Methods for the Preparation of N-functionalized Hydantoins. University of Oslo, Faculty of Mathematics and Natural Sciences, Department of Chemistry. ISSN 1501-7710. 2023(2628). Show summary

  Hydantoin is an organic framework of considerable chemical and biological interest as it is encountered in several drugs and natural products with biological activity. Access to synthetic tools for synthesis and modification of the hydantoin framework is therefore of importance both in academia and industry. The current synthetic methods used often include multiple steps, harsh conditions and toxic reagents, and thus have room for improvement. In this work, development of new and improved synthetic processes that allow for more efficient and less toxic production of hydantoins and derivatives is presented. The concept of the methods is direct bond formation between (carbon-based) functional groups and a specific position in the hydantoin framework. It was discovered that the key to solve this challenging task was to use copper as a catalyst. The methods developed allows for synthesis of two different classes of substituted hydantoins, including structures previously not accessible.

• Norén, Karl Stefan; Tilset, Mats & Nova Flores, Ainara (2023). Synthesis and characterization of molecules for gold (III) catalysis. Kjemisk Institutt.
• Suàrez, Lluís Artús; Tilset, Mats; Balcells, David & Nova Flores, Ainara (2021). Computational study on the deaminative hydrogenation of amides catalyzed by base metal complexes. Universitetet i Oslo, Det matematisk-naturvitenskapelige fakultet. ISSN 1501-7710. 2021(2388). Show summary

  Catalytic hydrogenation of amides could be an excellent option for the green atom efficient formation of alcohols and amines. However, the low reactivity of amides has been a big drawback for this reaction. In the last decade, the emergence of bifunctional catalysts for hydrogenation reactions improved the conditions for amide hydrogenation and made them feasible on larger scales. Still, the reaction mechanisms remained underinvestigated. In the course of his PhD studies, the candidate has elucidated the reaction mechanisms and bottlenecks by computational simulations at a quantum scale. With that information, the candidate proposed new catalysts that avoided such bottlenecks. Later, experimental studies proved the increased performance of the predicted catalysts.

• Héron, Julie; Balcells, David; Tilset, Mats & Nova Flores, Ainara (2021). C-H Activation and CuAAC Reactions with 1,8-Naphthyridine Based Dicopper Complexes from a Computational Perspective. Universitetet i Oslo, Det matematisk-naturvitenskapelige fakultet. ISSN 1501-7710. 2021(2459). Show summary

  Copper salts are often used to activate the C-H bond of alkynes and to catalyze the cycloaddition of alkynes to azides (CuAAC reaction). While cheap and easily accessible, the copper salts generate many different active species (number of metals and ligands), complicating the study of the reaction mechanism. To overcome this issue, chelating ligands are used to control the number of metal atoms in the active species and to allow only a narrow range of ligand configurations. In the course of her PhD studies, the candidate has elucidated the mechanisms of these reactions for dicopper complexes with an unsymmetrical naphthyridine-based ligand with di (pyridyl) and phosphino side arms (DPEOPN) by computational simulations at a DFT level. With this information, the candidate proposed new potential complexes that could be more efficient in the C-H activation of alkynes.

• Levchenko, Vladimir; Tilset, Mats & Nova, Ainara (2020). Synthesis of Cyclometalated Au (III) Complexes for Catalysis and MOF Functionalization. Matematisk Naturvitenskapelig fakultet, Universitetet i Oslo. ISSN 1501-7710. 2020(2333).
• Brevik, Robert & Nova, Ainara (2020). Rational Design of MOFs for CO2 Capture. Universitetet i Oslo. Show summary

  In this thesis, the structure and reactivity of functionalized UiO MOFs were studied using density functional theory. Specifically, UiO-66 and UiO-67 were the target materials for the metalation with MgMe2reagents. To model the material, both periodic and cluster models were used. The UiO MOFs has the possibility to take different configurations with regards to the μ3−OHgroups within the tetrahedral (Th) pores. These configurations were defined as (4,0) to indicate that Th pores have either 4 OMgMe groups or none; (3,1) to indicate that the Th pores have 3 or 1 MgMe groups; and (2,2) to indicate that all Th pores have 2 MgMe. Periodic gas phase calculations on UiO-66 and UiO-67 show that the (4,0) configuration is the most stable for the functionalized μ3−OHsites with MX groups being M=Mg or Zn, and X=Me and Cl. In contrast, (2,2) was found to be the most stable configuration with MX=MgMe using cluster calculation with implicit THF solvent. Periodic computations showed a compression of the unit cell volume for UiO-67 after the pristine SBUs are metalated due to the bending of the linkers, which is consistent with unpublished experimental results. The geometrical analysis of the metalated structures showed that Mg is three-fold coordinated with oxygen at the bridging site, while Zn is only one-fold coordinated.Calculations on the metalation energy using nodes involving a defect site showed that it is more favorable to metalate a defect site containing a –OH and coordinated H2O than the μ3−OHsite. For both bridging and defect site, the insertion of CO2into the Mg-Me and ZnMe bonds was calculated, and was found to be exergonic with the Mg-Me and Zn-Me located in the defect sites, while endergonic with the Zn-Me located in the bridging site. Lastly the mechanism for the catalytic conversion of pentenylamine to pyrrolidine on the bridging site of the [Zr node]-MgMe model was computed with implicit benzene solvent at room temperature. The computed transition state energy barriers is consisted with experimental results.

• Holmsen, Marte Sofie; Tilset, Mats; Nova, Ainara & Heyn, Richard H. (2019). Small-molecule activation at gold: synthesis, characterization, and reactivity of cyclometalated Au(III) complexes. Department of Chemistry.

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