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Diffusive transport phenomena in artificial enzyme cascades on scaffolds

Nature Nanotechnology volume 7, pages 769–770 (2012)Cite this article

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A variety of artificial enzyme cascade systems have recently been developed that involve the diffusion of substrates between enzymes bound to nanostructured scaffolds1,2,3,4. Wilner et al.1 placed enzyme pairs — glucose oxidase (GOx) and horseradish peroxidase (HRP) — on planar DNA scaffolds, and measured the throughput of the enzymatic cascade as a function of the size of the scaffold. The product formation for a scaffold separating GOx and HRP by approximately 6 nm was 1.2-fold higher than the product formation for a scaffold with an enzyme separation of 23 nm, and 8-fold higher than untethered enzymes1. The increase in throughput was attributed to a higher local concentration of H2O2 at the HRP site due to only partial diffusion to the bulk solution. A quantitative agreement was obtained with a ballistic transport model, which claimed “...the calculated value of V2/V1 = [r12/r22] = 1.16, is in good agreement with the experimented value, 1.2” (from Supplementary Information). V1 and V2 are the maximum rates of the cascades occurring on the larger- and smaller-separation scaffolds, respectively, and r1 and r2 are the distances separating the two enzymes on the respective scaffolds. However, according to this equation the ratio of reaction rates V2/V1 is 15.7 for r1 = 23.4 nm and r2 = 5.9 nm, and the idea that the diffusive flux is proportional to the solid angle subtended by the adsorber has previously been refuted by Berg5.

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Figure 1: Reaction–diffusion simulations for isolated or aggregated enzyme pairs.

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  1. Department of Biomedical Engineering, Columbia University, 351L Engineering Terrace, 1210 Amsterdam Avenue, New York, 10027, New York, USA

    Ofer Idan & Henry Hess

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  1. Ofer Idan
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  2. Henry Hess
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Correspondence to Henry Hess.

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Idan, O., Hess, H. Diffusive transport phenomena in artificial enzyme cascades on scaffolds. Nature Nanotech 7, 769–770 (2012). https://doi.org/10.1038/nnano.2012.222

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