Ni/HZSM-5 catalyst preparation by deposition-precipitation. Part 2. Catalytic hydrodeoxygenation reactions of lignin model compounds in organic and aqueous systems

被引:45
作者
Barton, R. R. [1 ]
Carrier, M. [2 ,3 ]
Segura, C. [2 ]
Fierro, J. L. G. [4 ]
Park, S. [5 ]
Lamb, H. H. [1 ]
Escalona, N. [6 ,7 ,8 ]
Peretti, S. W. [1 ]
机构
[1] North Carolina State Univ, Dept Chem & Biomol Engn, Campus Box 7905, Raleigh, NC 27695 USA
[2] Univ Concepcion, Unidad Desarrollo Tecnol, Coronel, Chile
[3] Aston Univ, European Bioenergy Res Inst, Birmingham B4 7ET, W Midlands, England
[4] CSIC, Inst Catalisis & Petroquim, Plaza Murillo 2, E-28049 Madrid, Spain
[5] North Carolina State Univ, Dept Forest Biomat, Raleigh, NC USA
[6] Pontificia Univ Catolica Chile, Dept Ingn Quim & Bioproc, Santiago, Chile
[7] Pontificia Univ Catolica Chile, Fac Quim, Santiago, Chile
[8] Pontificia Univ Catolica Chile, Ctr Invest Nanotecnol & Mat Avanzados CIEN UC, Santiago, Chile
基金
美国国家科学基金会; 美国食品与农业研究所;
关键词
Hydrodeoxygenation; Lignin; Depolymerization; HZSM-5; Deposition-Precipitation; O BOND-CLEAVAGE; ACID SITES; ORGANOSOLV LIGNIN; NI NANOPARTICLES; ARYL ETHERS; NICKEL; CONVERSION; GUAIACOL; PHASE; DEPOLYMERIZATION;
D O I
10.1016/j.apcata.2018.06.012
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Nickel metal supported on HZSM-5 (zeolite) is a promising catalyst for lignin depolymerization. In this work, the ability of catalysts prepared via deposition-precipitation (DP) to perform hydrodeoxygenation (HDO) on two lignin model compounds in organic and aqueous solvents was evaluated; guaiacol in dodecane and 2-phenoxy-1-phenylethanol (PPE) in aqueous solutions. All Ni/HZSM-5 catalysts were capable of guaiacol HDO into cyclohexane at 523 K. The role of the HZSM-5 acid sites was confirmed by comparison with Ni/SiO2 (inert support) which exhibited incomplete deoxygenation of guaiacol due to the inability to perform the cyclohexanol dehydration step. The catalyst prepared with 15 wt% Ni, a DP time of 16 h, and a calcination temperature of 673 K (Ni (15)/HZSM-5 DP16_Cal673), performed the guaiacol conversion with the greatest selectivity towards HDO products, with an intrinsic rate ratio (HDO rate to conversion rate) of 0.31, and 90% selectivity to cyclohexane. Catalytic activity and selectivity of Ni/HZSM-5 (15 wt%) in aqueous environments (water and 0.1 M NaOH solution) was confirmed using PPE reactions at 523 K. After 30 min reaction time in water, Ni/HZSM-5 exhibited similar to 100% conversion of PPE, and good yield of the desired products; ethylbenzene and phenol (similar to 35% and 23% of initial carbon, respectively). Ni/HZSM-5 in NaOH solution resulted in significantly higher ring saturation compared to the Ni/HZSM-5 in water or the NaOH solution control.
引用
收藏
页码:294 / 309
页数:16
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