From Manipulated Enzymes to Solid State Electrodes: Towards the Reduction of Protons and CO₂

Résumé

The efficient reduction of protons as well as direct conversion of CO₂ under mild conditions and catalyzed by non-noble metals is a current challenge and a need of modern society. While nature possesses very sophisticated machineries to perform such conversions, rationally designed catalytic materials are rare [1]. To find suitable compounds for the activation of such small molecules, new strategies have to be found to design superior electrocatalysts. Herein the manipulation of [FeFe]-enzymes with synthetic inorganic cofactors will be presented [2]. Based on such experiments, 1) a strategy to apply biological principles (e.g. cooperative metal-metal interactions) in small homogenous electrocatalysts and 2) an attempt to obtain heterogeneous electrocatalysts, revealing comparable built-in Fe/Ni-moieties, will be presented [3].  We herein aim to raise the awareness of the overall common design and working principles of catalysts incorporating aspects of biology, chemistry, and material sciences.

References

[1] See F. Möller, S. Piontek, R. G. Miller, U.-P. Apfel, Chem. Eur. J. 2018, 24, 1471-1493 and references cited herein.

[2] F. Wittkamp, M. Senger, S. T. Stripp, U.-P. Apfel, Chem. Commun. 2018, 54, 5934-5942.

[3] B. Konkena, K. junge Puring, O. Khavryuchenko, I. Sinev, S. Piontek, M. Muhler, W. Schuhmann, U.-P. Apfel, Nature Commun. 2016, 7:12269.

[4] S. Piontek, C. Andronescu, A. Zaichenko, B. Konkena, K. junge Puring, B. Marler, H. Antoni, I. Sinev, M. Muhler, D. Mollenhauer, B. Roldan Cuenya, W. Schuhmann, U.-P. Apfel, ACS Catalysis 2018, 8, 987-966.

[5] C. L. Bentley, C. Andronescu, M. Smialkowski, M. Kang, T. Tarnev, B. Marler, P. R. Unwin, U.-P. Apfel, W. Schuhmann, Angew. Chem. Int. Ed. 2018, 57, 4093-4097.