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Analytische Chemie – Elektroanalytik & Sensorik RUHR-UNIVERSITÄT BOCHUM 1 Perspective pentru un nou biocatod de potenţial ridicat – noi proprietăţi ale.

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Presentation on theme: "Analytische Chemie – Elektroanalytik & Sensorik RUHR-UNIVERSITÄT BOCHUM 1 Perspective pentru un nou biocatod de potenţial ridicat – noi proprietăţi ale."— Presentation transcript:

1 Analytische Chemie – Elektroanalytik & Sensorik RUHR-UNIVERSITÄT BOCHUM 1 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 Analytische Chemie – Elektroanalytik & Sensorik RUHR-UNIVERSITÄT BOCHUM Concept of bienzymatic membrane-less biofuel cell (BFC) laccase cellobiose dehydrogenase (CDH) Potential [mV] vs. Ag/AgCl 3M KCl -+ +150-41+450+530 E cell = 300 anode cathode e-e- e-e- e-e- cellobiose dehydrogenase laccase lactose lactoso- lactone e-e- Os loading H2OH2O O2O2 Stoica L. et al, Fuel Cells (2009), 9 (1), 53-62

3 Analytische Chemie – Elektroanalytik & Sensorik RUHR-UNIVERSITÄT BOCHUM 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. P out =E x I [E]; A; k cat, n E 0‘

4 Analytische Chemie – Elektroanalytik & Sensorik RUHR-UNIVERSITÄT BOCHUM I. Large active area electrode 4

5 Analytische Chemie – Elektroanalytik & Sensorik RUHR-UNIVERSITÄT BOCHUM 5 Graphite electrode surface

6 Analytische Chemie – Elektroanalytik & Sensorik RUHR-UNIVERSITÄT BOCHUM 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 Analytische Chemie – Elektroanalytik & Sensorik RUHR-UNIVERSITÄT BOCHUM 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 Analytische Chemie – Elektroanalytik & Sensorik RUHR-UNIVERSITÄT BOCHUM 8 Various supports

9 Analytische Chemie – Elektroanalytik & Sensorik RUHR-UNIVERSITÄT BOCHUM 9

10 Analytische Chemie – Elektroanalytik & Sensorik RUHR-UNIVERSITÄT BOCHUM II. Exploring specific bio-nano interactions 10

11 Analytische Chemie – Elektroanalytik & Sensorik RUHR-UNIVERSITÄT BOCHUM 11 250 results HRP-CNT Y. Yan et al., Langmuir 2005, 21, 6560-6566...only at low potentials!!

12 Analytische Chemie – Elektroanalytik & Sensorik RUHR-UNIVERSITÄT BOCHUM 12 Supervalent iron-oxo-porphyrin cation radical Document Title : Hypervalent Iron-Oxo Porphyrin Cation Radical Formation on Reaction of H 2 o 2 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 Analytische Chemie – Elektroanalytik & Sensorik RUHR-UNIVERSITÄT BOCHUM 13 Thermodynamic potential for reduction = +750 mV

14 Analytische Chemie – Elektroanalytik & Sensorik RUHR-UNIVERSITÄT BOCHUM 14 Any specific bioelectrochemistry of HRP @ these new materials?

15 Analytische Chemie – Elektroanalytik & Sensorik RUHR-UNIVERSITÄT BOCHUM 15 Bioelectrochemistry of HRP-heme -53 mV / pH unit PHA-pyrene-hexanoic acid

16 Analytische Chemie – Elektroanalytik & Sensorik RUHR-UNIVERSITÄT BOCHUM 16 Bioelectrocatalytic current for H 2 O 2 reduction at +600 mV

17 Analytische Chemie – Elektroanalytik & Sensorik RUHR-UNIVERSITÄT BOCHUM 17 Optimum pH @ +400 mV vs. Ag/AgCl Bioelectrocatalytic current for H 2 O 2 reduction at +600 mV PHA-pyrene-hexanoic acid

18 Analytische Chemie – Elektroanalytik & Sensorik RUHR-UNIVERSITÄT BOCHUM 18 Hydrodynamic voltammogram H 2 0 2 oxidation H 2 0 2 reduction at electrode at HRP High potential reduction of Cmp-I/II-HRP

19 Analytische Chemie – Elektroanalytik & Sensorik RUHR-UNIVERSITÄT BOCHUM 19 Scheme of H 2 O 2 involvement H2O2H2O2 H2OH2O HRP ox HRP red Biocathode @ +600 mV 1e - + 1e - W. Jia, S. Schwamborn, C. Jin, W. Xia, M. Muhler, W. Schuhmann, L. Stoica PCCP 12 (2010) 10088.

20 Analytische Chemie – Elektroanalytik & Sensorik RUHR-UNIVERSITÄT BOCHUM 20 H 2 O 2 biosensor at +400 mV @ no O 2 involvement Amperometric responses of the HRP/PHA-CNTs/CF/GR biosensor were recorded by additions of H 2 O 2 in N 2 -saturated PBS (pH 7.0) at +400 mV I max = 220 µA (~ 1.5 mM H 2 O 2 )K M = 320 µM H 2 O 2

21 Analytische Chemie – Elektroanalytik & Sensorik RUHR-UNIVERSITÄT BOCHUM 21 HRP loading E appl =+300 mV

22 Analytische Chemie – Elektroanalytik & Sensorik RUHR-UNIVERSITÄT BOCHUM 22 Is „glucose based cathode“ a promising candidate? Biocathodes based on... E onset pH opt Cl - inhibition e - / O 2 yield Laccase +6504YES4 e- Bilirubin oxidase +2006-7NO4 e- Glucose/HRP +6007NO2 e- P out =E x I [E]; A; k cat, nE 0‘

23 Analytische Chemie – Elektroanalytik & Sensorik RUHR-UNIVERSITÄT BOCHUM 23 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 Analytische Chemie – Elektroanalytik & Sensorik RUHR-UNIVERSITÄT BOCHUM 24 Acknowledgements go to... EU-FP7 funds (project no. FP7-NMP-2008-SMALL-2 ) to ELANOS

25 Analytische Chemie – Elektroanalytik & Sensorik RUHR-UNIVERSITÄT BOCHUM 25 for your attention! Thank you


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