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Hammett σ from composition predicts SN2 barriers

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A data-enhanced Hammett model maps SN2 barrier heights across substituent and leaving-group space using additive σ values that depend only on group identity and distance to the reacting carbon.

Source

Data enhanced Hammett-equation: reaction barriers in chemical space

Bragato M, von Rudorff GF, von Lilienfeld OA · Chemical science · 2020

doi.org/10.1039/d0sc04235hRead the full paper ↗30 citationscc by

What they did

The authors compressed quantum SN2 potential-energy changes into reaction constants ρ and substituent constants σ, tested additivity versus resonance, compared Theil–Sen averaging with the classical one-reference Hammett fit, and benchmarked against kernel ridge regression.

What they found

Substituent effects are largely additive without resonance; SN2 σ values follow composition and distance to the reaction center (6 parameters vs 20 in a dummy encoding). Their robust fit beats a single-reference Hammett model (errors ≤3.8 vs up to 5.2 kcal mol−1).

The limits

What it doesn't show

The linear model cannot capture strong resonance coupling of substituents, and barriers are electronic-structure estimates rather than experimental condensed-phase rates.

Key terms

Hammett equation
Linear free-energy relation log(K/K0)=ρσ separating reaction and substituent effects.
σ
Substituent constant encoding electron-donating or -withdrawing power.
ρ
Reaction constant measuring sensitivity of the reaction to substituents.
Theil–Sen regressor
Robust linear fit used to avoid overfitting a single reference reaction.
KRR
Kernel ridge regression ML baseline for the same SN2 energies.

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Hammett σ in this SN2 space depends mainly on:

Common questions

How many SN2 reactions were treated?

12 combinations of nucleophile and leaving group.

What substituents sat at R1–R4?

–H, –NO2, –CN, –NH3, –CH3.

How many parameters describe molecular σ with distance decay?

NG+1 = 6.

Worst-case MAE vs original Hammett?

3.8 vs up to 5.2 kcal mol−1.

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