O2 and CO2 Activation

Dr. Shengfa Ye joined the State Key Laboratory of Catalysis Dalian Institute of Chemical Physics in 2020. This homepage documents his research in the department of Molecular Theory and Spectroscopy until 2020.

Metalloenzymes play a vital role in metabolism; in particular, they are capable of functionalizing difficult substrates. These processes are remarkable because these transformations proceed with unprecedented level of regio-, chemo- and stereospecificity and, more importantly at mild conditions that can be hardly achieved by any industrial processes. Understanding the catalytic mechanisms of enzymatic reactions at the atomic level will enhance our knowledge for further design and synthesis of novel environmentally benign catalysts. Quantum chemical calculations contribute key information to this important field of investigation.

  1. Calculation of the spectroscopic parameters of potential reaction intermediates and comparison with experimentally determined properties is vital for the structural identification of short-lived species that are inaccessible to X-ray crystallography.
  2. Optimization of the structures of transition states in order to “connect” important intermediates and to predict reaction rates and kinetic isotope effects.
  3. Qualitative analysis of the electronic structures of the intermediates and transition states provides deep chemical insights into catalytic mechanisms and complicated electron transfer processes.

The combined theoretical and spectroscopic analyses trigger new ideas for conclusive experiments that probe the intricate details of the catalytic mechanisms.

Research Topics:

Metalloenzymes can catalyze a range of oxidation reactions utilizing an ultimate "green" oxidant, dioxygen. The reactions are typically initiated by O2 binding at a reduced, electron-rich metal center, such as Cu(I) or Fe(II). The resulting dioxygen adducts often contain a coordinated superoxide.1 Subsequent reduction of O2 takes place along a well-defined reaction pathway and leads to formation of metal-peroxo and -oxo intermediates. More importantly, nature has developed various enzymes to employ all reduced forms of O2 to functionalize substrates.2 [more]
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