AbstractThe status of surface species on solid catalysts during heterogeneous catalysis is often mysterious. Investigations of these surface species are crucial to deconvolute the reaction network and design more efficient catalysts. Vibrational spectroscopy is a powerful technique to study the interactions between surface species and the catalysts and infrared (IR) and Raman spectroscopies have been widely applied to study reaction mechanisms in heterogeneous catalysis. However, IR/Raman spectra are difficult to model computationally and important vibrational modes may be IR-, Raman- (or both) inactive due to restrictions by optical selection rules. Inelastic neutron scattering (INS) is another form of vibrational spectroscopy and relies on the scattering of neutrons by the atomic nucleus. A consequence of this is that INS is not subject to any optical selection rules and all vibrations are measurable in principle. INS spectroscopy has been used to investigate surface species on catalysts in a wide range of heterogeneous catalytic reactions. In this mini-review, we focus on applications of INS in two important fields: petrochemical reactions and C1 chemistry. We introduce the basic principles of the INS technique, followed by a discussion of its application in investigating two key catalytic systems: (i) the behaviour of hydrocarbons on metal-oxide and zeolite catalysts and (ii) the formation of hydrocarbonaceous species on methane reforming and Fischer–Tropsch catalysts. The power of INS in studying these important catalytic systems is demonstrated.