Spatiotemporal Organization of Catalysts Driven by Enhanced Diffusion.

Recently, both microfluidic and fluorescence correlation spectroscopy experiments have revealed that diffusion coefficients of active biological catalysts (enzymes) rise proportionately to their catalytic rate. Similar effects have also been observed for active material catalysts, such as platinum nanocatalysts in hydrogen peroxide solution. While differences in diffusion coefficients have recently been cleverly exploited to spatially separate active from inactive catalysts, here we investigate the consequences of these novel findings on the spatiotemporal organization of catalysts. In particular, we show that chemical reactions-such as coupled catalytic reactions-may drive effective attraction or repulsion between catalysts which in turn drives their spatiotemporal organization. This, we argue, may have implications for internal cell signaling.

[1]  D. Koshland,et al.  An amplified sensitivity arising from covalent modification in biological systems. , 1981, Proceedings of the National Academy of Sciences of the United States of America.

[2]  Ayusman Sen,et al.  Chemotactic separation of enzymes. , 2014, ACS nano.

[3]  F. Tostevin,et al.  Optimization of collective enzyme activity via spatial localization. , 2013, The Journal of chemical physics.

[4]  Walter F Paxton,et al.  Motility of catalytic nanoparticles through self-generated forces. , 2005, Chemistry.

[5]  J. Stone,et al.  Hydrogen peroxide: a signaling messenger. , 2006, Antioxidants & redox signaling.

[6]  Walter F Paxton,et al.  Chemical locomotion. , 2006, Angewandte Chemie.

[7]  Y. Rondelez Competition for catalytic resources alters biological network dynamics. , 2012, Physical review letters.

[8]  S. Isaacson A convergent reaction-diffusion master equation. , 2012, Journal of Chemical Physics.

[9]  Kambiz M. Hamadani,et al.  The heat released during catalytic turnover enhances the diffusion of an enzyme , 2014, Nature.

[10]  K. Ghosh,et al.  Competition enhances stochasticity in biochemical reactions. , 2013, The Journal of chemical physics.

[11]  Fei Wu,et al.  Krebs cycle metabolon formation: metabolite concentration gradient enhanced compartmentation of sequential enzymes. , 2015, Chemical communications.

[12]  Alan Benesi,et al.  A catalytically driven organometallic molecular motor. , 2013, Nanoscale.

[13]  S. An,et al.  Spatial Organization of Metabolic Enzyme Complexes in Cells. , 2017, Biochemistry.

[14]  E. Cadenas,et al.  Estimation of H2O2 gradients across biomembranes , 2000, FEBS letters.

[15]  A. Szabó,et al.  Theory of the statistics of kinetic transitions with application to single-molecule enzyme catalysis. , 2006, The Journal of chemical physics.

[16]  Samudra Sengupta,et al.  Substrate catalysis enhances single-enzyme diffusion. , 2010, Journal of the American Chemical Society.

[17]  James B. Anderson,et al.  Monte Carlo simulations of single- and multistep enzyme-catalyzed reaction sequences: effects of diffusion, cell size, enzyme fluctuations, colocalization, and segregation. , 2010, The Journal of chemical physics.

[18]  Dennis Bray,et al.  The Chemotactic Behavior of Computer-Based Surrogate Bacteria , 2007, Current Biology.

[19]  W. Ebeling,et al.  Active Brownian particles , 2012, The European Physical Journal Special Topics.

[20]  J. Tour,et al.  Unimolecular Submersible Nanomachines. Synthesis, Actuation, and Monitoring , 2015, Nano letters.

[21]  David Reguera,et al.  Key parameters controlling the performance of catalytic motors. , 2016, The Journal of chemical physics.

[22]  Hartmut Löwen,et al.  Non-Gaussian statistics for the motion of self-propelled Janus particles: experiment versus theory. , 2013, Physical review. E, Statistical, nonlinear, and soft matter physics.

[23]  K. Kaibuchi,et al.  Small GTP-binding proteins. , 1992, International review of cytology.

[24]  Stefan Hellander,et al.  Reaction rates for reaction-diffusion kinetics on unstructured meshes. , 2016, The Journal of chemical physics.

[25]  N. Agmon,et al.  Theory of reversible diffusion‐influenced reactions , 1990 .

[26]  Tristan Tabouillot,et al.  Enzyme molecules as nanomotors. , 2013, Journal of the American Chemical Society.

[27]  Ashutosh Kumar,et al.  Emergence of dynamic cooperativity in the stochastic kinetics of fluctuating enzymes. , 2016, The Journal of chemical physics.

[28]  Ramin Golestanian,et al.  Micromotors Powered by Enzyme Catalysis. , 2015, Nano letters.

[29]  G. Gangopadhyay,et al.  Power law kinetics in reversible enzyme-catalyzed reaction due to diffusion , 2003 .