% IMPORTANT: The following is UTF-8 encoded.  This means that in the presence
% of non-ASCII characters, it will not work with BibTeX 0.99 or older.
% Instead, you should use an up-to-date BibTeX implementation like “bibtex8” or
% “biber”.

@ARTICLE{RezaeiGhaleh:996127,
      author       = {Rezaei-Ghaleh, Nasrollah and Agudo-Canalejo, Jaime and
                      Griesinger, Christian and Golestanian, Ramin},
      title        = {{M}olecular {D}iffusivity of {C}lick {R}eaction
                      {C}omponents: {T}he {D}iffusion {E}nhancement {Q}uestion},
      journal      = {Journal of the American Chemical Society},
      volume       = {144},
      number       = {3},
      issn         = {0002-7863},
      address      = {Washington, DC},
      publisher    = {ACS Publications},
      reportid     = {FZJ-2023-01124},
      pages        = {1380 - 1388},
      year         = {2022},
      abstract     = {Micrometer-sized objects are widely known to exhibit
                      chemically driven motility in systems away from equilibrium.
                      Experimental observation of reaction-induced motility or
                      enhancement in diffusivity at the much shorter length scale
                      of small molecules is, however, still a matter of debate.
                      Here, we investigate the molecular diffusivity of reactants,
                      catalyst, and product of a model reaction, the
                      copper-catalyzed azide-alkyne cycloaddition click reaction,
                      and develop new NMR diffusion approaches that allow the
                      probing of reaction-induced diffusion enhancement in
                      nanosized molecular systems with higher accuracy than the
                      state of the art. Following two different approaches that
                      enable the accounting of time-dependent concentration
                      changes during NMR experiments, we closely monitored the
                      diffusion coefficient of reaction components during the
                      reaction. The reaction components showed distinct changes in
                      the diffusivity: while the two reactants underwent a
                      time-dependent decrease in their diffusivity, the diffusion
                      coefficient of the product gradually increased and the
                      catalyst showed only slight diffusion enhancement within the
                      range expected for reaction-induced sample heating. The
                      decrease in diffusion coefficient of the alkyne, one of the
                      two reactants of click reaction, was not reproduced during
                      its copper coordination when the second reactant, azide, was
                      absent. Our results do not support the catalysis-induced
                      diffusion enhancement of the components of the click
                      reaction and, instead, point to the role of a relatively
                      large intermediate species within the reaction cycle with
                      diffusivity lower than that of both the reactants and
                      product molecule.},
      cin          = {IBI-7},
      ddc          = {540},
      cid          = {I:(DE-Juel1)IBI-7-20200312},
      pnm          = {5241 - Molecular Information Processing in Cellular Systems
                      (POF4-524)},
      pid          = {G:(DE-HGF)POF4-5241},
      typ          = {PUB:(DE-HGF)16},
      pubmed       = {35078321},
      UT           = {WOS:000752924300038},
      doi          = {10.1021/jacs.1c11754},
      url          = {https://juser.fz-juelich.de/record/996127},
}