Identification of Ni3Fe alloy as a candidate catalyst for quinoline selective hydrogenation with computations†
Abstract
The 1,2,3,4-tetrahydroquinoline (py-THQL) is a crucial intermediate and fragment in chemical synthesis, but its production from quinoline (QL) selective hydrogenation in heterogeneous catalysis mainly relies on noble-metal-based catalysts. Therefore, the design of catalysts composed of earth-abundant elements for this reaction is meaningful. In this work, using density functional theory (DFT) calculations, we found the binding energy of QL to be a suitable descriptor to illustrate the general activity trend of metallic catalysts for QL hydrogenation. Among the screened bimetallic alloys composed of Fe, Co, Ni, and Cu, we computationally identified Ni3Fe as a promising candidate catalyst with high stability, while our systematic mechanistic calculations showed the low energy barriers for each hydrogenation step. Our established DFT-based mean-field microkinetic model indicates a much higher turnover frequency for py-THQL production on the Ni3Fe(111) surface than on the experimentally reported high-performance AuPd3(111) surface. This work not only identified a valuable descriptor for the rational catalyst screening for the complex QL hydrogenation reaction but also theoretically predicted a cost-effective Ni3Fe catalyst for the hydrogenation reaction.
- This article is part of the themed collection: Digital Catalysis