Unraveling the Dependence of Critical Active Sites of WOx on Rh/WOx Catalysts in Tetrahydrofurfuryl Alcohol Hydrogenolysis

Yang, Man; Jiao, Yu; Duan, Jianglin; Wu, Keying; Song, Hai-Liang; Sun, Shaodong; Ren, Yujing

doi:10.1021/acssuschemeng.3c01461

Cited by 5 publications

(1 citation statement)

References 44 publications

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“…5,6 The optimal Cu 1 Re 0.14 catalyst achieved the highest total yield of combined 2-MF and 2-MTHF at 96.8% under a reaction temperature of 200 °C, H 2 pressure of 20 bar, and reaction time of 6 h. 5 Additionally, under the N 2 atmosphere, accelerating the reaction temperature to 220 °C resulted in the highest yield of 2-MF at 94% under an extended reaction time of 4 h. 6 This enhanced hydrogenolysis activity can be attributed to the presence of Re in oxide states, facilitating the conversion of FAL into the target 2-MF product in both H 2 and N 2 systems. 5,6 To consider an alternative oxophilic metal oxide, tungstate-based oxide species (WO x ) has been applied as a catalyst in various applications such as THFA hydrogenolysis, 17,18 glycerol hydrogenolysis, 19−22 and erythritol hydrogenolysis. 23 Nevertheless, the design of a Cu-WO x catalyst for FAL hydrogenolysis into 2-MF and 2-MTHF products remains unexplored.…”

Section: Introductionmentioning

confidence: 99%

Continuous Furfural Hydrogenolysis into 2-Methylfuran and 2-Methyltetrahydrofuran over Cu/γ–Al₂O₃ with ReO_x and WO_x as Catalyst Boosters

Kalong,

Praikaew,

Ratchahat

et al. 2024

Energy Fuels

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Cu/Al2O3 catalysts, enhanced with ReO x and WO x as catalyst boosters, were employed for the hydrogenolysis of furfural (FAL) into 2-methylfuran (2-MF) and 2-methyltetrahydrofuran (2-MTHF) within a continuous fixed-bed reactor. Comprehensive catalyst analyses revealed that the addition of ReO x and WO x onto Cu/Al2O3 catalysts resulted in reinforced metal–support interactions, while the acidity, in terms of both its strength and quantity, was influenced by these booster additions. Additionally, structural characterizations after H2 reduction via X-ray diffraction, X-ray absorption near-edge structure, and X-ray photoelectron spectroscopy confirmed the coexistence of Cu in the forms of Cu0/CuO x across all of the Cu-containing catalysts, whereas the valence states of Re0/ReO x and WO x were detected for the ReCuAl and WCuAl catalysts, respectively. Operating at a maximum temperature of 220 °C, the ReCuAl catalyst achieved the highest combined yields of 2-MF and 2-MTHF at 80.4%, with the WCuAl catalyst reaching 89.0%, in contrast to the lowest yields of 54.0% obtained with the CuAl catalyst. These results underscore the positive impact of ReO x and WO x additions on Cu/Al2O3 catalysts, in which the catalyst acidity, metal–support interactions, and coexistence of metallic and oxophilic sites influenced the hydrogenolysis process, leading to the enhanced production of 2-MF and 2-MTHF simultaneously from FAL.

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Section: Introductionmentioning

confidence: 99%

Continuous Furfural Hydrogenolysis into 2-Methylfuran and 2-Methyltetrahydrofuran over Cu/γ–Al₂O₃ with ReO_x and WO_x as Catalyst Boosters

Kalong,

Praikaew,

Ratchahat

et al. 2024

Energy Fuels

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Conversion of Penta‐Acetyl‐Xylitol to 3‐Acetoxymethylene‐Tetrahydrofuran by a Combined Hetero‐/Homogeneous Tandem Catalyst System

England,

Slater‐Eddy,

Earnden

et al. 2024

ChemCatChem

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A tandem catalyst system comprised of trifluoromethanesulfonic (triflic acid, HOTf) or Hafnium tetratriflate (Hf(OTf)4) and Ru/C in glacial acetic acid (HOAc) as the solvent at 200 °C and ~ 7 MPa hydrogen pressure in a batch reactor converts penta‐acetyl‐xylitol ((2R,3R,4S)‐Pentane‐1,2,3,4,5‐penta‐acetoxy‐pentane) or unprotected xylitol to 3‐acetoxymethylene‐tetrahydrofuran (3‐AMT) in up to 15 % yield at full conversion. A comparative analysis by SEM‐EDS and XPS of the fresh commercial Ru/C catalyst vs catalyst reused and recovered after 5 cycles shows increasing aggregation of ruthenium to larger particles with a concomitant decrease in yield of 3‐AMT to 8‐9 % for cycles 4 and 5. 3‐AMT or its hydrolysis product 3‐hydroxymethyl‐tetrahydrofuran (3‐HMT) are valuable synthons for the preparation of agrochemicals, pharmaceuticals and specialty polyurethanes and polyesters.

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Recent progress on catalyst development for ring-opening C-O hydrogenolysis of cyclic ethers in the production of biomass-derived chemicals

Tomishige,

Honda,

Sugimoto

et al. 2024

Carb Neutrality

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Catalytic hydrogenolysis systems of C-O bonds in furan ring, tetrahydrofuran ring and tetrahydropyran ring in biomass-derived cyclic compounds are reviewed. Furfural or its hydrogenation products (furfuryl alcohol and tetrahydrofurfuryl alcohol) have been frequently used as substrates for this type of reactions. Ring-opening of furfuryl alcohol over metal catalysts combined with basic components gives a mixture of 1,2-pentanediol, 1,5-pentanediol and other by-products. The selectivity much depends on catalysts and reaction conditions, and good 1,2-pentanediol selectivity can be obtained. For 1,5-pentanediol synthesis, more selective approaches have been reported such as Cu-zeolite catalysts for furfuryl alcohol hydrogenolysis in flow reactor and M-M’Ox-type (M: noble metal; M’: transition metal) supported catalysts or Ni-LnOx (Ln: rare earth element) catalysts for tetrahydrofurfuryl alcohol hydrogenolysis. The metal catalysts and M-M’Ox-type catalysts can be applied to ring-opening hydrogenolysis of other furan- and tetrahydrofuran-based compounds, respectively. Among the products of ring-opening hydrogenolysis of biomass-derived compounds, 1,5-pentanediol seems to be the most important because of the potential use as a monomer. The recent progress and reported properties of polymers using 1,5-pentanediol as a monomer are also summarized.

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Unraveling the Dependence of Critical Active Sites of WO_x on Rh/WO_x Catalysts in Tetrahydrofurfuryl Alcohol Hydrogenolysis

Cited by 5 publications

References 44 publications

Continuous Furfural Hydrogenolysis into 2-Methylfuran and 2-Methyltetrahydrofuran over Cu/γ–Al₂O₃ with ReO_x and WO_x as Catalyst Boosters

Continuous Furfural Hydrogenolysis into 2-Methylfuran and 2-Methyltetrahydrofuran over Cu/γ–Al₂O₃ with ReO_x and WO_x as Catalyst Boosters

Conversion of Penta‐Acetyl‐Xylitol to 3‐Acetoxymethylene‐Tetrahydrofuran by a Combined Hetero‐/Homogeneous Tandem Catalyst System

Recent progress on catalyst development for ring-opening C-O hydrogenolysis of cyclic ethers in the production of biomass-derived chemicals

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Unraveling the Dependence of Critical Active Sites of WOx on Rh/WOx Catalysts in Tetrahydrofurfuryl Alcohol Hydrogenolysis

Cited by 5 publications

References 44 publications

Continuous Furfural Hydrogenolysis into 2-Methylfuran and 2-Methyltetrahydrofuran over Cu/γ–Al2O3 with ReOx and WOx as Catalyst Boosters

Continuous Furfural Hydrogenolysis into 2-Methylfuran and 2-Methyltetrahydrofuran over Cu/γ–Al2O3 with ReOx and WOx as Catalyst Boosters

Conversion of Penta‐Acetyl‐Xylitol to 3‐Acetoxymethylene‐Tetrahydrofuran by a Combined Hetero‐/Homogeneous Tandem Catalyst System

Recent progress on catalyst development for ring-opening C-O hydrogenolysis of cyclic ethers in the production of biomass-derived chemicals

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Resources

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Unraveling the Dependence of Critical Active Sites of WO_x on Rh/WO_x Catalysts in Tetrahydrofurfuryl Alcohol Hydrogenolysis

Continuous Furfural Hydrogenolysis into 2-Methylfuran and 2-Methyltetrahydrofuran over Cu/γ–Al₂O₃ with ReO_x and WO_x as Catalyst Boosters

Continuous Furfural Hydrogenolysis into 2-Methylfuran and 2-Methyltetrahydrofuran over Cu/γ–Al₂O₃ with ReO_x and WO_x as Catalyst Boosters