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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 lactose Os Os Os Os O2 Os Os Os Os lactoso- lactone Os H2O Os Os e- e- - + -41 +150 +450 +530 Ecell = 300 cellobiose dehydrogenase (CDH) Potential [mV] vs. Ag/AgCl 3M KCl 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,

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,

8 Various supports


10 II. Exploring specific bio-nano interactions

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

12 Supervalent iron-oxo-porphyrin cation radical
Document Title : Hypervalent Iron-Oxo Porphyrin Cation Radical Formation on Reaction of H2o2 with The Cytochrome-c-Derived Heme Octapeptide Microperoxidase-8 (Mp-8) in Aqueous-Solution Published in : JOURNAL OF THE CHEMICAL SOCIETY-CHEMICAL COMMUNICATIONS year: 1990 issue: 2 pages: 97-98

13 Thermodynamic potential for reduction = +750 mV

14 Any specific bioelectrochemistry of HRP @ these new materials?

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

16 Bioelectrocatalytic current for H2O2 reduction at +600 mV

17 Bioelectrocatalytic current for H2O2 reduction at +600 mV
Optimum pH @ +400 mV vs. Ag/AgCl PHA - pyrene-hexanoic acid

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

19 Scheme of H2O2 involvement
Biocathode @ +600 mV H2O2 HRPred 1e- + H2O HRPox W. Jia, S. Schwamborn, C. Jin, W. Xia, M. Muhler, W. Schuhmann, L. Stoica PCCP 12 (2010)

20 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

21 HRP loading Eappl=+300 mV

22 Is „glucose based cathode“ a promising candidate?
Biocathodes based on... Eonset pHopt Cl- inhibition e- / O2 yield Laccase +650 4 YES 4 e- Bilirubin oxidase +200 6-7 NO Glucose/HRP +600 7 2 e- Pout=E x I [E]; A; kcat, n E0‘

23 3D-hierachical carbon nanostructures:
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-)

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

25 Thank you for your attention!

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