Computers 1967-2013: a personal perspective. Part 5. Network bandwidth.

June 5th, 2013

In a time of change, we often do not notice that Δ = ∫δ. Here I am thinking of network bandwidth, and my personal experience of it over a 46 year period.

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Mechanism of the Van Leusen reaction.

May 29th, 2013

This is a follow-up to comment posted by Ryan, who asked about isocyanide’s role (in the form of the anion of tosyl isocyanide, or TosMIC): “In Van Leusen, it (the isocyanide) acts as an electrophile”. The Wikipedia article (recently updated by myself) shows nucleophilic attack by an oxy-anion on the carbon of the C≡N group, with the isocyanide group acting as the acceptor of these electrons (in other words, the electrophile). In the form shown below, one negatively charged atom appears to be attacking another also carrying a negative charge. Surely this breaks the rules that like charges repel? So we shall investigate to see if this really happens.

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How should one represent the anion of TosMIC?

May 24th, 2013

The title of this post comes from a comment posted by Ryan, who asks about isocyanide’s role (in the form of the anion of tosyl isocyanide, or TosMIC) in two named reactions, Van Leusen and Ugi FCR.  “In Van Leusen, it (the isocyanide) acts as an electrophile: however, in Ugi, it acts as a nucleophile”. Here are some valence bond forms for this species;

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Another Woodward pericyclic example dissected: all is not what it seems.

May 22nd, 2013

Here is another example gleaned from that Woodward essay of 1967 (Chem. Soc. Special Publications (Aromaticity), 1967, 21, 217-249), where all might not be what it seems.

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Woodward’s symmetry considerations applied to electrocyclic reactions.

May 20th, 2013

Sometimes the originators of seminal theories in chemistry write a personal and anecdotal account of their work. Niels Bohr[cite]10.1007/BF01326955[/cite] was one such and four decades later Robert Woodward wrote “The conservation of orbital symmetry” (Chem. Soc. Special Publications (Aromaticity), 1967, 21, 217-249; it is not online and so no doi can be given). Much interesting chemistry is described there, but (like Bohr in his article), Woodward lists no citations at the end, merely giving attributions by name. Thus the following chemistry (p 236 of this article) is attributed to a Professor Fonken, and goes as follows (excluding the structure in red):

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Au and Pt π-complexes of cyclobutadiene.

May 15th, 2013

In the preceding post, I introduced Dewar’s π-complex theory for alkene-metal compounds, outlining the molecular orbital analysis he presented, in which the filled π-MO of the alkene donates into a Ag+ empty metal orbital and back-donation occurs from a filled metal orbital into the alkene π* MO. Here I play a little “what if” game with this scenario to see what one can learn from doing so.

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The π-complex theory of metal-alkene compounds.

May 13th, 2013

The period 1951–1954 was a golden one for structural chemistry; proteins, DNA, Ferrocene (1952) and the one I discuss here, a bonding model for Zeise’s salt (3).

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Concerted 1,4-addition of thioacetic acid: a (requested) reality check.

May 11th, 2013

Lukas, who occasionally comments on this blog, sent me the following challenge. In a recent article[cite]10.1021/jo3021709[/cite] he had proposed that the stereochemical outcome (Z) of reaction between a butenal and thioacetic acid as shown below arose by an unusual concerted cycloaddtion involving an S-H bond. He wrote in the article “…this scheme … recommends itself for evaluation by in silico methods“. I asked if the answer could be posted here, and he agreed. So here it is.

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Transition states for the (base) catalysed ring opening of propene epoxide.

May 8th, 2013

The previous post described how the acid catalysed ring opening of propene epoxide by an alcohol (methanol) is preceded by pre-protonation of the epoxide oxygen to form a “hidden intermediate” on the concerted intrinsic reaction pathway to ring opening. Here I take a look at the mechanism where a strong base is present, modelled by tetramethyl ammonium methoxide (R4N+.OMe), for the two isomers R=Me; R’=Me, R”=H and R’=H, R”=Me.

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