Production of γ‐Valerolactone from One‐Pot Transformation of Biomass‐Derived Carbohydrates Over Chitosan‐Supported Ruthenium Catalyst Combined with Zeolite ZSM‐5

Abstract

It remains as a challenge to directly transform the biomass‐derived C5 carbohydrates, such as furfural (FF) and its upstream product xylose and hemicellulose, to γ‐valerolactone (GVL), a versatile renewable chemical platform, due to various restrictions in the current synthetic strategies. Using formic acid as green hydrogen source, we synthesized the recyclable chitosan‐Ru/PPh3 catalyst system, effective for both the hydrogenation of FF to furfuryl alcohol (FAL) and the reduction of levulinic acid (LA) or ethyl levulinate (EL) to GVL, affording up to 99 % product yields. The combination of chitosan‐Ru/PPh3 with ZSM‐5 could successfully achieve up to 79 % yield of GVL from one‐pot conversion of FF under mild condition. Preliminary studies indicated that this method could also be applied to the direct conversion of biomass‐derived C5 carbohydrates such as xylose and hemicellulose to GVL in 37 % or 30 % yield, respectively.

An overview of the obtaining of biomass-derived gamma-valerolactone from levulinic acid or esters without H2 supply

“…However, when alcohol is the H-donor, it goes through a dehydrogenation to produce hydrogen atoms, and the byproducts are an aldehyde or a ketone (ROH to RO in Fig. 2), (Wang et al 2020b). The regeneration of the solvent can restore it, as in the case of alcohol (Geboers et al 2014), which can be reused (Fig.…”

“…3). Hydrogenation is exothermic and depends on the catalyst activity, whereas cyclization is endothermic (Wang et al 2020b). The C-H formation in the γ-carbon to form the alkoxy intermediate is rate-controlling (Mamun et al 2019), whereas the ring closure is easy (Chia and Dumesic 2011;Mamun et al 2019).…”

“…Currently, the CTCH is carried out using commercial high purity reactants (>95%). Experiences with LA or LEs from biomass use molecular hydrogen in the hydrogenation and (or) noble metals as catalysts (Putro et al 2015;Wang et al 2020b). The obtaining of GVL by CTCH using in-situ biomass-obtained LA or LEs is a challenge.…”

Enhanced Device Performance of Perovskite Photovoltaics by Magnetic Field‐Aligned Perovskites‐Magnetic Nanoparticles Composite Thin Film

“…Hybrid perovskites have recently emerged as promising photovoltaic materials for approaching efficient perovskite solar cells (PSCs) [1][2][3][4] and ultrasensitive perovskite photodetectors (PPDs) [5][6][7] due to the low exciton binding energy, long charge carrier diffusion length and high charge carrier mobility of perovskite materials, and the possibility of cost-effective high-throughput manufacturing of perovskite photovoltaics. [8][9][10][11][12][13][14][15][16] An impressive device performance has been reported from the state-of-the-art device architectures through morphological manipulation and generic interface engineering. [17][18][19][20][21][22][23][24] Studies indicated that the defect-assisted charge carrier recombination in perovskite photoactive layer was one of issues needs to be resolved for further boosting device performance.…”

“…[17][18][19][20][21][22][23][24] Studies indicated that the defect-assisted charge carrier recombination in perovskite photoactive layer was one of issues needs to be resolved for further boosting device performance. [8][9][10][11][12][13][14][15][16] Utilization of Lewis acid and/or Lewis base to passivate the surface-defect has been attempted to address above issues, and boosted device performance was indeed observed from perovskite photovoltaics. [25][26][27] Magnetic nanoparticles (MNPs) and external magnetic field (EMF) have been applied for enhancing electroluminescence and photoluminescence efficiencies, and photocurrent in optoelectronics.…”