Electron-Rich Ruthenium on Nitrogen-Doped Carbons Promoting Levulinic Acid Hydrogenation to γ-Valerolactone: Effect of Metal–Support Interaction

Abstract

Ru has been found to be a highly efficient catalyst for producing γ-valerolactone from the hydrogenation of levulinic acid. However, the active species on Ru nanoparticles (NPs) are still unclear. Here, we synthesized a series of Ru NPs with tunable chemical states obtained by altering the interaction with carbon-nanotube-based supports, achieved by the strategies of doping carbon nanotubes with N and S atoms, changing the amount of dopants, and varying the loading of Ru. The surface species of the supported Ru NPs, identified by X-ray photoelectron spectroscopy, were linked to the catalytic activities instrinsically. We found that the Ru NPs possessing Ru0 with lower binding energy (Ru 3p) showed higher activity independent of the parameters of synthesis. Theoretical calculations indicated that the electron-rich Ru0 enhanced LA hydrogenation through facilitating R–COOH breaking into R–CO and −OH, suggesting a powerful tool modifying the catalytic activity of carbon-supported metals by manipulating the electronic metal–support interaction.

Editorial: Carbon Catalysis: Focus on Sustainable Chemical Technology

“…For instance, carbon nanotubes (CNTs) are widely used in heterogeneous catalysis due to their chemical stability, relatively low cost and easy recovery of precious metals by means of combustion in recent years (Gao et al, 2018;Zhu et al, 2019). CNTs have been demonstrated effective to support noble metal nanoparticles to catalyze the valorization of biomass-derived platform molecules in the context of sustainable chemistry (Wan et al, 2014;Ning et al, 2015Ning et al, , 2016Meng et al, 2019). However, the separation of CNT-based catalyst usually adds costs particularly for liquid-phase reactions due to its original powder form.…”

Insight into the Metal‐Support Interactions between Ruthenium and Nanodiamond‐derived Carbon material for CO Oxidation

“…Therefore, regulation of MSI is critical for improving the catalytic performance. One significant factor for regulating MSI is through selection of support material [9–12] . It is well known that the reducible oxides, such as TiO 2 , CeO 2 , and FeO x , usually provide a strong MSI given the more tangible effect on the catalytic activity [13–15] .…”

“…One significant factor for regulating MSI is through selection of support material. [9][10][11][12] It is well known that the reducible oxides, such as TiO 2 , CeO 2 , and FeO x , usually provide a strong MSI given the more tangible effect on the catalytic activity. [13][14][15] More recently, non-metal oxide supports (e. g., carbides and nanocarbons) also manifested remarkable result from the strong MSI.…”

NNN Pincer‐functionalized Porous Organic Polymer Supported Ru(III) as a Heterogeneous Catalyst for Levulinic Acid Hydrogenation to γ‐Valerolactone

“…Numerous devotion to improving stabilization of Ru NPs on catalyst supports have been implemented, resulting from the combination of Ru NPs and metal oxide catalyst supports, such as Al 2 O 3 , TiO 2 , ZrO 2 , and heteroatom-doped carbons. [27][28][29][30][31][32][33][34][35][36][37][38][39][40][41][42][43] However, it is still advisable to investigate further the synergetic combination of Ru NPs and catalyst supports to escape from deactivation over subsequent cycles or in continuous flow production.…”