Neumann Lab

Precision Nickel Coating of Complex Nanostructures with Commercially Available ALD Precursors Atomic Layer Deposition (ALD) is a scalable, solvent-free synthesis technique that is routinely used for the deposition of thin films with sub-Angstrom precision. The coating of nonplanar substrates v...

The group's first paper on atomic layer deposition is now available online! pubs.acs.org/doi/10.1021/...

We report a solvent-free, reproducible and scalable synthesis of nickel-containing core-shell nanoparticles.

Congratulations to authors Neha, Norbert, Claudia and Aamir!

Solid-State NMR Provides Location-Specific Information on the Chemical Environment Inside MOF Pores Solid-state NMR can capture the inequivalence of differently shaped MOF pores. We show that the chemical shifts of reporting substituents that extend a defined distance into a MOF pore reflect the por...

In our most recent work we show how solid-state NMR reveals information about the chemical environment inside MOF pores in the absence and presence of guest molecules.
chemrxiv.org/engage/chemr...

Congratulations to authors Hao Deng, Marco Bengsch, Christophe Fares, Zihang Qiu and Mir Henglin!

www.organic-chemistry.org/Highlights/2...
Douglass features Reduction: The Bisai Synthesis of Oridamycin A

Click Heterogenization of Phosphines Furnishes Recyclable Hydroformylation Catalysts that Reproduce Homogeneous Performance Heterogeneous catalysts confer notable practical advantages for large-scale reactions, while homogeneous catalysts permit targeted performance optimization. A rapid and general method for the heteroge...

Our work on mechanistically homogeneous and functionally heterogeneous catalysis with MOFs is now available in @jacs.acspublications.org

Congrats to authors Junjun Chen, Christophe Fares and Aamir Abbas!

pubs.acs.org/doi/10.1021/...

In Co-catalyzed hydroformylation, where substantial phosphine rearrangement is required to stabilize the precatalyst and structures along the catalytic cycle, MOF-heterogenized phosphines reproduce homogeneous performance while offering recyclability and minimizing leaching (< 0.7 ppm Co).

We show via solid-state NMR studies that the phosphine ligands enjoy a high degree of mobility within the super-cages, which permits them to furnish mechanistically homogeneous and functionally heterogeneous transition-metal catalysts.

Click Heterogenization of Phosphines Furnishes Recyclable Hydroformylation Catalysts that Reproduce Homogeneous Performance Heterogeneous catalysts confer notable practical advantages for large-scale reactions, while homogenous catalysts permit targeted performance optimization. A rapid and general method for the heterogen...

Our new preprint describes a 1-step method for the secure heterogenization of structurally diverse phosphine ligands within spacious MOF super-cages.

chemrxiv.org/engage/chemr...

Congratulations to authors Junjun Chen, Christophe Fares and Aamir Abbas!

#newpaper Preferential 5-endo-trig and 5-exo trig cyclizations of silyl radicals with a MOF-based Rh(II) porphyrin catalyst enables chemoselective 1,3-diol formation for olefins that contain multiple olefins: www.thieme-connect.com/products/ejo...
Congrats to all authors (Gupta, Deng, Ding, Qiu)!

Our mechanistic proposal rationalizes why MOF-supported Rh(II) porphyrins are thermal hydrofunctionalization catalysts while molecular analogues prove unreactive. It also showcases the cooperation that can be achieved within a MOF matrix which precisely arranges Rh(II) centers in 3D space.

Via EPR and NMR spectroscopic analyses, kinetics, isotope labeling, IR spectroscopy, molecular model systems, radical trapping, digestion studies, quantum chemistry and molecular dynamics, we could get a rare level of insight into the mechanistic details of a heterogeneously catalyzed reaction.

3-Center-3-Electron σ-Adduct Enables Silyl Radical Transfer below the Minimum Barrier for Silyl Radical Formation Transition-metal-catalyzed cleavage of the Si–H bond in silanes to yield silyl radicals requires substantial amounts of energy, which are commonly supplied by photons. For Rh(II) porphyrins, efficient...

Our mechanism study of a MOF-catalyzed hydrosilylation reaction is now available in #JACS.

Congratulations to all authors!

Zihang Qiu, Paolo Cleto Bruzzese, Zikuan Wang, Hao Deng, Markus Leutzsch, Christophe Farès, Sonia Chabbra, PhD, Frank Neese, Alexander Schnegg

pubs.acs.org/doi/10.1021/...

Metal‐Organic Framework–Specific Catalysis MOF catalysis is not a successor to either homogeneous or classical heterogeneous catalysis, but rather a distinct domain of catalysis with its own set of advantages and limitations. This concept art...

Our concept paper on "Metal-Organic Framework-Specific Catalysis" is now available online
chemistry-europe.onlinelibrary.wiley.com/doi/10.1002/...
Congratulations Marco!

The graphic shows three regioisomers of diazines in the top row and shows a sketch of a pill with an attached arene. The latter alludes to the fact that the ability to prepare individual regioisomers permits researchers to optimize the position of nitrogen atoms in arene rings for applications in medicinal chemistry. The bottom row shows simplistic representations of four different structomers of metal-organic frameworks. All four structomers have the same composition and are isostructural, but differ in how "active" and "inactive" metal sites are arranged within the structure. Selective preparation of individual structomers thus permits one to optimize metal arrangements in extended structures.

Our work on the development of structomers is now available as a preprint: chemrxiv.org/engage/chemr...
Congratulations to the authors Qiming Jin, Paolo Cleto Bruzzese, Alessandro Vetere, Claudia Weidenthaler, Eko Budiyanto, Mir Henglin, Nils Nöthling and Alexander Schnegg!