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Elektroanalytik & Sensorik • Elektroanalytik & Sensorik •

Elektroanalytik & Sensorik • Elektroanalytik & Sensorik •. Perspective pentru un nou biocatod de potenţial ridicat – noi proprietăţi ale enzimelor redox imobilizate pe nanostructuri compozite de grafit - Wenzhi Jia, Yvonne Ackermann, Wolfgang Schuhmann, Leonard Stoica

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Elektroanalytik & Sensorik • Elektroanalytik & Sensorik •

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  1. Elektroanalytik & Sensorik • Elektroanalytik & Sensorik • Perspective pentru un nou biocatod de potenţial ridicat – noi proprietăţi ale enzimelor redox imobilizate pe nanostructuri compozite de grafit - Wenzhi Jia, Yvonne Ackermann, Wolfgang Schuhmann, Leonard Stoica Anal. Chem. - Elektroanalytik & Sensorik (ELAN) Universitätsstr. 150, Bochum 44780 Ruhr-University Bochum Germany

  2. Concept of bienzymatic membrane-less biofuel cell (BFC) loading cellobiose dehydrogenase laccase e- e- anode cathode Os lactose Os O2 Os Os Os Os Os Os lactoso- lactone Os H2O Os Os e- e- - + -41 +150 +450 +530 Ecell = 300 Potential [mV] vs. Ag/AgCl 3M KCl cellobiose dehydrogenase (CDH) laccase Stoica L. et al, Fuel Cells (2009), 9 (1), 53-62

  3. Motivation for new material electrode • High catalytic coverage: • large amount of active enzyme; • Large active area of electrode: • using hierarchical carboneous materials two-generations CNT‘s • Exploring specific properties of bio-nano interactions. [E]; A; kcat, n Pout=E x I E0‘

  4. I. Large active area electrode

  5. Graphite electrode surface

  6. Composite material:CNT/CMF onto carbon paper Preparation: N. Li, X. Chen, L. Stoica, W. Xia, J. Qian, J. Aßmann, W. Schuhmann, M. Muhler Adv. Mater. (2007), 19, 2957-2960

  7. EIS characterisation of CNT/CMF • Properties: • Low ohmic resistance => no potential loss; • Ratio active/geometric area=200; • Non-restrictive diffusion of enzyme substrate. N. Li, X. Chen, L. Stoica, W. Xia, J. Qian, J. Aßmann, W. Schuhmann, M. Muhler Adv. Mater. (2007), 19, 2957-2960

  8. Various supports

  9. II. Exploring specific bio-nano interactions

  10. 250 results HRP-CNT ...only at low potentials!! Y. Yan et al., Langmuir 2005, 21, 6560-6566

  11. Thermodynamic potential for reduction = +750 mV

  12. Anyspecific bioelectrochemistry of HRP @ these new materials?

  13. Bioelectrochemistry of HRP-heme -53 mV / pH unit PHA - pyrene-hexanoic acid

  14. Bioelectrocatalytic current forH2O2 reduction at +600 mV

  15. Bioelectrocatalytic current forH2O2 reduction at +600 mV Optimum pH @ +400 mV vs. Ag/AgCl PHA - pyrene-hexanoic acid

  16. Hydrodynamic voltammogram H202 oxidation at electrode High potential reduction of Cmp-I/II-HRP H202 reduction at HRP

  17. Scheme of H2O2 involvement Biocathode @ +600 mV H2O2 HRPred 1e- + 1e- HRPox H2O W. Jia, S. Schwamborn, C. Jin, W. Xia, M. Muhler, W. Schuhmann, L. Stoica PCCP12 (2010) 10088.

  18. H2O2 biosensor at +400 mV@ no O2 involvement Imax= 220 µA (~ 1.5 mM H2O2) KM= 320 µM H2O2 Amperometric responses of the HRP/PHA-CNTs/CF/GR biosensor were recorded by additions of H2O2 in N2-saturated PBS (pH 7.0) at +400 mV

  19. HRP loading Eappl=+300 mV

  20. Is „glucose based cathode“ a promising candidate? Pout=E x I [E]; A; kcat, n E0‘

  21. Conclusions 3D-hierachical carbon nanostructures: • present excellent characteristics for large active area and enhanced/”novel” bioelectrocatalysis of known redox enzymes; Biocathode enzyme: • Yes, indeed, high potential biocathode functioning on glucose/oxygen is feasible at in-vivo conditions (pH, Cl-)

  22. Acknowledgements go to... • EU-FP7 funds (project no. FP7-NMP-2008-SMALL-2) • to ELANOS

  23. Thank you for your attention!

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