报告摘要：

 

Advanced self-assembly strategies enable the targeted synthesis of supramolecular systems and materials with increasing structural and functional complexity. We react bis-monodentate ligands with transition metal cations to coordination compounds showing a broad range of topologies. To combine different functionalities in the same structure, we develop non- statistical assembly strategies based on “shape complementary assembly” (SCA), “coordination sphere engineering” (CSE) and “adjacent backbone interactions” (ABI).¹

With a focus on multi-chromophore systems,² we investigate the suitability of modular assemblies for light-induced charge separation, vectorial excitation transport and as potential photo-redox catalysts. By combining chiral with emissive ligands, heteroleptic cages showing guest-modulated circularly polarized luminescence (CPL) were obtained.³ We further introduce stimuli-responsive behavior in photochromic cages⁴ allowing to control guest affinity⁵ and established a light-fueled dissipative system.⁶ Cages capable of fullerene encapsulation⁷ give rise to confinement-controlled reactivity, such as long-term C60 radical anion stabilization.⁸ Recently, we mastered the non-statistical and robust assembly of dinuclear Pd(II) cages containing four chemically different ligands [Pd2ABCD].⁹ Such structures can also be obtained with kinetically more inert Co(III)salphen complexes.¹⁰ The collected results now set the stage for creating ‘complex systems’ behaviour by following the stimuli-responsive population and evolution of co-existing species in mixtures.¹¹ In this direction, we study multi-step cage interconversions, guest-binding/release cascades and propagation of chiral information.

 

Figure 1. Non-statistical multicomponent self-assembly (left) and complex systems behavior (right)

References

[1] Pullen, S.; Tessarolo, J.; Clever, G. H. Chem. Sci. 2021, 12, 7269.

[2] Regeni, I.; Chowdhury, R.; Terlinden, K.; Horiuchi, S.; Holstein, J. J.; Feldmann, S.; Clever, G. H. Angew. Chem. Int. Ed. 2023, e202308288.

[3] Wu, K.; Tessarolo, J.; Baksi, A.; Clever, G. H. Angew. Chem. Int. Ed. 2022, 61, e202205725.

[4] Benchimol, E.; Tessarolo, J.; Clever, G. H. Nat. Chem. 2024. (Perspective Article)

[5] Li, R.-J.; Tessarolo, J.; Lee, H.; Clever, G. H. J. Am. Chem. Soc. 2021, 143, 3865.

[6] Lee, H.; Tessarolo, J.; Langbehn, D.; Baksi, A.; Herges, R.; Clever, G. H. J. Am. Chem. Soc. 2022, 144, 3099.

[7] Chen, B.; Holstein, J. J.; Platzek, A.; Schneider, L.; Wu, K.; Clever, G. H. Chem. Sci. 2022, 13, 1829.

[8] Hasegawa, S.; Meichsner, S. L.; Holstein, J. J.; Baksi, A.; Kasanmascheff, M.; Clever, G. H. J. Am. Chem. Soc. 2021, 143, 9718.

[9] Wu, K.; Benchimol, E.; Baksi, A.; Clever, G. H. Nat. Chem. 2024, 10.1038/s41557-023-01415-7.

[10] Zhang, B.; Lee, H.; Holstein, J. J.; Clever, G. H. Angew. Chem. Int. Ed. 2024, DOI: 10.1002/anie.202404682.

[11] Benchimol, E.; Regeni, I.; Zhang, B.; Kabiri, M.; Holstein, J. J.; Clever, G. H. J. Am. Chem. Soc. 2024, 146, 6905.

 

报告人简介：

 Guido H. Clever studied chemistry in Heidelberg and obtained his PhD in 2006 from LMU Munich. He then joined the lab of Mitsuhiko Shionoya at the University of Tokyo as an Alexander-von-Humboldt/JSPS postdoc and later Assistant Professor. In 2010 he became Junior Professor at Georg-August University Göttingen, where he climbed on a W2 professorship in 2013. In 2015, he became Full Professor at TU Dortmund University, holding the chair of Bioinorganic Chemistry. He obtained the ADUC Young Investigator Award (German Chemical Society), the Dozenten Award of the Fonds of the German Chemical Industry and an ERC Consolidator grant of the European Union. He is board member of DFG Cluster of Excellence RESOLV EXC2033 and Graduate School “Confinement-controlled chemistry” GRK2376. He serves as vice dean of the department of chemistry. His research interests include the development of non-statistical assembly protocols for low-symmetry metallo-supramolecular cages and the integration of chromophores, e.g. donor/acceptor combinations and light- switchable units. These find application in selective guest binding, chiroptical sensing, light- driven charge separation, cage-confined reactivity and systems chemistry. Furthermore, the Clever Lab studies transition metal-binding DNA G-quadruplexes to serve as a new type of EPR spin labels, enantioselective catalysts and stimuli-responsive protein binders with biomedical relevance.

 

Guido H. Clever

Nationality: German

E-Mail: guido.clever@tu-dortmund.de

Web: www.clever-lab.de

ORCID: https://orcid.org/0000-0001-8458-3060

 

EDUCATION

2006 PhD with Prof. T. Carell, LMU Munich, Germany (Chemistry, Summa cum Laude)

2003 Diploma with Prof. T. J. J. Müller, Heidelberg University, Germany (Chemistry and Mol. Biology)

POSITIONS

Since 2015 Full Professor (W3, Inorganic Chemistry), Chair of Bioinorganic Chemistry Faculty of Chemistry and Chemical Biology, TU Dortmund

2013-2015  Professor (W2, Inorganic Chemistry), Georg-August University Göttingen

2010-2013  Junior Professor (W1, Inorganic Chemistry), Georg-August University Göttingen

2009-2010  Assistant Professor (Bioinorganic Chemistry), The University of Tokyo

2007-2009  Postdoctoral Researcher with Prof. M. Shionoya, The University of Tokyo

 

FELLOWSHIPS and AWARDS

2016  ERC Consolidator Grant (RAMSES, 683083) of the European Research Council

2014  Dozenten Prize of the Fonds d. Chemischen Industrie for excellence in research and teaching

2013  ADUC Prize 2012 of the GDCh (Yound Investigators Award of German Chemical Society)

2011  JSPS Bridge Fellowship of the Japanese Society for the Promotion of Science

2007-2009  Postdoctoral fellow of the Japanese Society for the Promotion of Science (JSPS) and the Alexander von Humboldt Foundation

2006  Prize of the “Dr. Klaus Römer Foundation” for PhD thesis

2003-2005  Kekulé Fellow of the Fonds der Chemischen Industrie

2003  Prize of the “Dr. Sophie Bernthsen Fonds” for diploma

2001-2003  Fellow of the Studienstiftung des Deutschen Volkes

1999  Prize of the “Otto Hofmann Foundation” for pre-diploma

 

COMMISSION of TRUST

2023– Dean of the iGSS Graduate School and Board member of DFG Cluster of Excellence RESOLV EXC2033

2019– Graduate program selection committee member of DFG Cluster of Excellence RESOLV EXC2033

2018– Board member of the graduate school GRK2376 “Confinement-Controlled Chemistry”

2017– Vice Dean of the Faculty of Chemistry and Chemical Biology, TU Dortmund

2016– Head of selection committees to fill a W1 Junior-Professorship “InorganicMaterials Chemistry”, a W3 Full-Professorship “Inorganic Transition Metal Chemistry” and a W3 Full-Professorship “NRW One Health Research Center – Hybrid Bionanosystems”; participation > 10 further committees

2016– Scientific Advisory Board member of the Japanese Collaborative Research Center “Asymmetallic”

2017– Selection Committee member of nationwide PhD prize of the Studienstiftung des Deutschen Volkes

2013– Liaison Professor (Vertrauensdozent) of the Studienstiftung des Deutschen Volkes
(Co)Organizer of symposia and workshops, e.g.: Promoting Younger Chemists (2002), JCF Alpenforum (2005), Jap-German HeKKSaGOn meeting (Göttingen 2013, Tohoku 2015), German Science Days (Kyoto 2013), GDCh Sino-German Frontier of Science Meeting (Berlin 2014), ICCC (Sendai 2018), SupraChem (Dortmund 2025).

2010– Acquisition of ∼ 6 Mio € third party funding:

- ERC Consolidator Grant (RAMSES, 683083) of the European Research Council: 2 Mio€

- For past and present DFG (German Science Foundation) Grants (individual grants, large instrumentation, CRCs (i.e. http://www.solvation.de/, http://www.confinement-controlled- chemistry.de/), see: https://gepris.dfg.de/gepris/person/190719587?language=en

- Mercator Foundation Grants „Ko-2023-0011" and "DNA-based Redox Systems 2021"

- Further Grants/ CRC Participations: DAAD 2022 “DNA G-Quadruplex Recognition with Modified Oligonucleotide Probes”, DLR CANTAR, IGNITE Network

 

REVIEWING ACTIVITY

External PhD: Cambridge Univ. (3x), Girona Univ., IIT Madras, IIT Guwahati, JNCASR Bangalore, Univ. Greifswald, EPFL Lausanne, Univ. Trieste; Univ. of Jyvaskyla, Faculty tenure: Univ. Nicosia, Univ. Otago; Journals: Nature Chem., Nat. Commun., JACS, Angew. Chem. (outstanding reviewer 2017, 2018 and 2020), Chem,, Chem. Sci, Chem. Commun....; Other: DFG, ERC, A. v. Humboldt Found., Studienstiftung d. dt. Volkes, Cusanus Werk, German-Israelian Foundation, Israelian Science Foundation, Japanese WPI projects, Nobel Foundation.

 

SELECTED PUBLICATIONS (> 135 PAPERS, H-INDEX 49)

1. "Shape-Complementary Multicomponent Assembly of Low-Symmetry Co(III)Salphen-Based Coordination Cages“

B. Zhang, H. Lee, J. J. Holstein, G. H. Clever, Angew. Chem. Int. Ed. 2024, DOI: 10.1002/anie.202404682.

2. "Nonstatistical Assembly of Multicomponent [Pd2ABCD] Cages“

K. Wu, E. Benchimol, A. Baksi, G. H. Clever, Nat. Chem. 2024, 16, 584. (Highlighted in ChemistryViews, Chem, by Springer Nature and in a press release of TU Dortmund)

3. "Heteromeric completive self-sorting in coordination cage systems“

E. Benchimol, I. Regeni, B. Zhang, M. Kabiri, J. J. Holstein, G. H. Clever, J. Am. Chem. Soc. 2024, 146, 6905.

4. "Photoswitchable Coordination Cages“

E. Benchimol, J. Tessarolo, G. H. Clever, Nat. Chem. 2024, 16, 13.

5. "Engineering Soluble Diketopyrrolopyrrole Chromophore Stacks from a Series of Pd(II)-based Ravels“

I. Regeni, R. Chowdhury, K. Terlinden, S. Horiuchi, J. J. Holstein, S. Feldmann, G. H. Clever, Angew. Chem. Int. Ed. 2023, 62,

6. "Maximized axial helicity in a Pd2L4 cage: inverse guest size-dependent compression and mesocate isomerism“

W. M. Bloch, S. Horiuchi, J. J. Holstein, C. Drechsler, A. Wuttke, W. Hiller, R. A. Mata, G. H. Clever, Chem. Sci. 2023, DOI: 10.1039/D2SC06629G

7. "Guest-modulated Circularly Polarized Luminescence by Ligand-to-Ligand Chirality Transfer in Heteroleptic Pd(II) Coordination Cages"
K. Wu, J. Tessarolo, A. Baksi, G. H. Clever, Angew. Chem. Int. Ed. 2022, 61, e202205725. (Hot Paper, Front Cover)

8. "Long-Lived C60 Radical Anion Stabilized inside an Electron-Deficient Coordination Cage"
S. Hasegawa, S. L. Meichsner, J. J. Holstein, A. Baksi, M. Kasanmascheff, G. H. Clever, J. Am. Chem. Soc. 2021, 143, DOI: 10.1021/jacs.1c02860

9. "Integrative Assembly of Heteroleptic Tetrahedra Controlled by Backbone Steric Bulk"
J. Tessarolo, H. Lee, E. Sakuda, K. Umakoshi, G. H. Clever, J. Am. Chem. Soc. 2021, 143, 6339.

10. "Modular Design of G-Quadruplex MetalloDNAzymes for Catalytic C-C Bond Formations with Switchable Enantioselectivity"
P. M. Punt, M. D. Langenberg, O. Altan, G. H. Clever, J. Am. Chem. Soc. 2021, 143, 3555.

11. "Multi-Stimuli Control over Assembly and Guest Binding in Metallo-Supramolecular Hosts based on DTE Photoswitches"

R. Li, J. Tessarolo, H. Lee, G. H. Clever, J. Am. Chem. Soc. 2021, 143, 3865.

12. "Coal-Tar Dye-based Coordination Cages and Helicates"

I. Regeni, B. Chen, M. Frank, A. Baksi, J. J. Holstein, G. H. Clever, Angew. Chem. Int. Ed. 2021, 60, 5673. (Hot Paper)

13. "Precise Distance Measurements in DNA G‐Quadruplex Dimers and Sandwich Complexes by Pulsed Dipolar EPR Spectroscopy"

L. M. Stratmann, Y. Kutin, M. Kasanmascheff, G. H. Clever, Angew. Chem. Int. Ed. 2021, 60, 4939. (VIP Paper)

14. "A New Mechanically-Interlocked [Pd2L4] Cage Motif by Dimerization of two Peptide-based Lemniscates"

T. R. Schulte, J. J. Holstein, L. Schneider, A. Adam, G. Haberhauer, G. H. Clever, Angew. Chem. Int. Ed. 2020, 59, 22489. (Hot Paper, Inside Cover)

15. "Mechanistic Interplay between Light-Switching and Guest-Binding in Photochromic [Pd2Dithienylethene4] Coordination Cages"

R. Li, J. J. Holstein, W. G. Hiller, J. Andréasson, G. H. Clever, J. Am. Chem. Soc. 2019, 141, 2097.