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- W2021015840 abstract "Abstract It is argued that the titled non-linear effects (NLE) may arise whenever the order of the reaction in the chiral catalyst in greater than 1. In a fundamental departure from previous approaches, this is mathematically elaborated for the second order case. (NLE may also be observed if the chiral catalyst forms non-reacting dimers in a competing equilibrium; practically, however, this implies the in situ resolution of the catalyst.) The amplification of enantiomeric excess by NLE implies a relative (although modest) reduction in the entropy of mixing. The consequent increase in free energy apparently indicates a non-equilibrium process. It is suggested, based on arguments involving the chemical potential, that kinetically-controlled reactions lead to a state of “quasi-equilibrium”: in this, although overall equilibrium is attained, the product-spread is far from equilibrium. Thus, both the linear and NLE cases of chiral catalysis represent departures from equilibrium (which requires that the product e.e. = 0). Interesting similarities exist with models of non-equilibrium systems, the NLE cases apparently being analogs of open systems just after the bifurcation point has been crossed." @default.
- W2021015840 created "2016-06-24" @default.
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- W2021015840 date "2012-02-27" @default.
- W2021015840 modified "2023-09-25" @default.
- W2021015840 title "Non-linear Effects in Asymmetric Catalysis: Whys and Wherefores" @default.
- W2021015840 doi "https://doi.org/10.1038/npre.2012.6947.1" @default.
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