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Progress in Chemistry 2019, Vol. 31 Issue (8): 1075-1085 DOI: 10.7536/PC190213 Previous Articles   Next Articles

Heterogeneous Catalysts for Biomass-Based Molecules Aqueous-Phase Catalytic Hydrogenation

Lihua Qian, Guojun Lan, Xiaoyan Liu, Qingfeng Ye, Ying Li**()   

  1. Institute of Industrial Catalysis, Zhejiang University of Technology, Hangzhou 310014, China
  • Received: Online: Published:
  • Contact: Ying Li
  • About author:
    ** E-mail:
  • Supported by:
    Natural Science Foundation of Zhejiang Province(LY17B030010)
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Transformation of the biomass into platform molecules and further conversion into fuel and chemicals is one of the important ways of biomass utilization. The research progress on aqueous-phase hydrogenation and highly active and stable catalysts for aqueous-phase catalytic reactions are summarized. The challenges of the heterogenous catalysts used in aqueous reaction such as the loss of active components, catalyst surface reconstruction, toxicity, etc., and the preparation strategy of highly active and stable catalysts, such as the surface reconstruction, surface carbon coating, enhancement of the interaction between the support and the metal active components, and new structure catalysts design are summarized. The further research direction on catalysts design for aqueous-phase hydrogenation reaction are discussed.

Key words: aqueous-phase reaction, biomass, hydrogenation, metal catalyst
Fig. 1 Schematic illustration of the simulated water structure at a water/hydrocarbon(oil) interface. Color key: dark gray spheres=C, light gray=H, red=O. Dotted lines are hydrogen bonds. The transparent rectangle depicts the interface between water and the hydrocarbon[14]
Fig. 2 Partial dissociation of H2O on Ru(0001): STM images of(a) intact water stripes after deposition at 145 K and its transformation to(b) partially dissociated H2O-OH stripes after 30 min annealing at 145 K. In the DFT optimized structures shown, the OH group is highlighted by an orange O atom[16]
Fig. 3 Acetone and water co-adsorbed to Ru(0001). This adsorption configuration of acetone is stabilized by 0.18 eV through formation of a hydrogen bond(depicted with annotated line). Dark brown spheres=C, pink=H, red=O, light brown=Ru[22]
Fig. 4 Schematic of mass transfer in a three-phase reaction[27]
Table 1 Summary of catalytic performance of various catalysts in aqueous phase hydrogenation
Type of catalyst Catalyst Substrate Reaction condition Conv./% ref
noble metals Ru-MC-g benzoic acid H2(4 MPa), 120 ℃, 2 h 94 35
Rh/H-Beta diphenyl ether H2(4 MPa), 120 ℃, 3 h 80 37
Pt/H-Beta diphenyl ether H2(4 MPa), 120 ℃, 3 h 64 37
Ru/H-Beta diphenyl ether H2(4 MPa), 120 ℃, 3 h 70 37
Ru/Al2O3 levulinic acid H2(2 MPa), 50 ℃, 1 h 22 49
Ir/CNT levulinic acid H2(2 MPa), 50 ℃, 1 h 96 49
Ru/CNT levulinic acid H2(2 MPa), 50 ℃, 1 h 65 47
Ru/C guaiacol H2(4 MPa), 250 ℃, 2 h 56 50
Rh/C guaiacol H2(4 MPa), 250 ℃, 2 h 15 50
Pt/C guaiacol H2(4 MPa), 250 ℃, 2 h 2 50
Pd/C guaiacol H2(4 MPa), 250 ℃, 2 h 0 50
Pd/C phenol H2(4 MPa), 250 ℃, 2 h 82 50
Ru/CNT cellobiose H2(5 MPa), 185 ℃, 3 h 88 51
metal oxides and metal composites 4%Rh-MoOx/SiO2(Mo/Rh=0.13) levulinic acid H2(6 MPa), 80 ℃, 6 h 100 38
4%Ir-MoOx/SiO2(Mo/Ir=0.13) levulinic acid H2(6 MPa), 80 ℃, 6 h 100 38
4%Ru-MoOx/SiO2(Mo/Ru=0.13) levulinic acid H2(6 MPa), 80 ℃, 6 h 100 38
4%Rh-MoOx/SiO2(Mo/Rh=0.13) lactic acid H2(6 MPa), 80 ℃, 6 h 78 38
Pt-ReOx/C sorbitol H2(6.21 MPa), 245 ℃, WHSV(2.92 h-1) 99 41
Pt-ReOx/Zr-P sorbitol H2(6.21 MPa), 160 ℃, WHSV(0.16 h-1) 92 42
Pd1Fe3/Zr-P sorbitol H2(6.21 MPa), 245 ℃, WHSV(2.92 h-1) 16 44
Pd/WOx/-Al2O3 guaiacol H2(7 MPa), 300 ℃, 150 min 100 52
non-noble metals Raney Ni levulinate esters H-donor(2-PrOH), room temperature, Ar, 2 h 87 40
20%Cu/ZrO2-OG(oxalate-gel) levulinic acid/
formic acid		 formic acid, N2(1 MPa), 180 ℃, 5 h 60 41
5 wt%Ni-HAP levulinic acid H2(0.5 MPa), 70 ℃, 4 h 18 53
10%Ni/Al2O3 levulinic acid H2(3 MPa), 200 ℃, 3 h 29 54
7.9 mol%Co/AC vanillin/formic acid formic acid, N2(0.5 MPa), 180 ℃, 4 h 6 45
Co@NC-700
(7.9 mol%Co)		 vanillin/ formic acid formic acid, N2(0.5 MPa), 180 ℃, 4 h 96 48
Fe@NC-700
(7.9 mol% Fe)		 vanillin/ formic acid formic acid, N2(0.5 MPa), 180 ℃, 4 h 10 48
Ni@NC-700
(7.9 mol% Ni)		 vanillin/ formic acid formic acid, N2(0.5 MPa), 180 ℃, 4 h 37 48
Cu@NC-700
(7.9 mol% Cu)		 vanillin/ formic acid formic acid, N2(0.5 MPa), 180 ℃, 4 h 4 48
4Co/Al2O3(nCo/nAl=4) levulinic acid H2(5 MPa), 180 ℃, 3 h 6 55
Fig. 5 A facile approach for coating supported metal catalysts[67]
Fig. 6 Preparation of graphitic carbon/oxide composites that are applicable to powders as well as pellets[68]
Fig. 7 Schematic illustration of the preparation process of Ru-MC catalyst[72]
Fig. 8 Schematic illustration of the synthesis of the Co@NC-x catalyst[48]
Fig. 9 Schematic illustration of the synthesis of hollow yolk-shell Co@C-N nanoreactors[73]
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