Growth kinetics of humins studied via X-ray scattering

被引:34
作者
Cheng, Ziwei [1 ,2 ]
Goulas, Konstantinos A. [2 ,3 ]
Rodriguez, Natalia Quiroz [1 ,2 ]
Saha, Basudeb [2 ]
Vlachos, Dionisios G. [1 ,2 ]
机构
[1] Univ Delaware, Dept Chem & Biomol Engn, Newark, DE 19716 USA
[2] Univ Delaware, Catalysis Ctr Energy Innovat, Newark, DE 19716 USA
[3] Oregon State Univ, Sch Chem Biol & Environm Engn, 105 SW 26th St,116 Johnson Hall, Corvallis, OR 97331 USA
关键词
D-FRUCTOSE FORMATION; LEVULINIC ACID; MOLECULAR-STRUCTURE; BIOMASS CONVERSION; SILICA PARTICLES; BY-PRODUCTS; DEHYDRATION; 5-HYDROXYMETHYL-2-FURALDEHYDE; GLUCOSE; MECHANISMS;
D O I
10.1039/c9gc03961a
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
We use ultra-Small Angle X-ray Scattering (USAXS) to investigate the evolution of size, morphology, volume fraction and number concentration of humins formed during dehydration of fructose to 5-hydroxymethylfurfural (HMF), and the further polymerization of HMF between 80-95 degrees C in 1 M hydrochloric acidic solutions. The radius of gyration (R-g) of suspended humins particles grows linearly with time and is accompanied by an increase in polydispersity (PD), before possible precipitation occurs. The scattering patterns indicate fractal-like structures. The apparent activation energy of humins growth is 102 +/- 0.4 kJ mol(-1). The trends in the number of particles over time reveal competing processes entailing the continuous formation of new particles (nucleation) leading to increasing polydispersity with time and the aggregation of existing particles and possible precipitation. The direct observation of growth of humins indicates that humins form primarily from HMF rather than fructose.
引用
收藏
页码:2301 / 2309
页数:9
相关论文
共 29 条
[1]   UNIFORM SILICA PARTICLE-PRECIPITATION - AN AGGREGATIVE GROWTH-MODEL [J].
BOGUSH, GH ;
ZUKOSKI, CF .
JOURNAL OF COLLOID AND INTERFACE SCIENCE, 1991, 142 (01) :19-34
[2]   Small-angle X-ray scattering study of the formation of colloidal silica particles from alkoxides: Primary particles or not? [J].
Boukari, H ;
Lin, JS ;
Harris, MT .
JOURNAL OF COLLOID AND INTERFACE SCIENCE, 1997, 194 (02) :311-318
[3]   Probing the dynamics of the silica nanostructure formation and growth by SAXS [J].
Boukari, H ;
Lin, JS ;
Harris, MT .
CHEMISTRY OF MATERIALS, 1997, 9 (11) :2376-2384
[4]   Production of levulinic acid and use as a platform chemical for derived products [J].
Bozell, JJ ;
Moens, L ;
Elliott, DC ;
Wang, Y ;
Neuenscwander, GG ;
Fitzpatrick, SW ;
Bilski, RJ ;
Jarnefeld, JL .
RESOURCES CONSERVATION AND RECYCLING, 2000, 28 (3-4) :227-239
[5]   Polymers and polyfunctionality. [J].
Carothers, WH .
TRANSACTIONS OF THE FARADAY SOCIETY, 1936, 32 (01) :0039-0053
[6]   Quantification and Classification of Carbonyls in Industrial Humins and Lignins by 19F NMR [J].
Constant, Sandra ;
Lancefield, Christopher S. ;
Weckhuysen, Bert M. ;
Bruijnincx, Pieter C. A. .
ACS SUSTAINABLE CHEMISTRY & ENGINEERING, 2017, 5 (01) :965-972
[7]   The Role of Metal Halides in Enhancing the Dehydration of Xylose to Furfural [J].
Enslow, Kristopher R. ;
Bell, Alexis T. .
CHEMCATCHEM, 2015, 7 (03) :479-489
[8]   Critical Influence of 5-Hydroxymethylfurfural Aging and Decomposition on the Utility of Biomass Conversion in Organic Synthesis [J].
Galkin, Konstantin I. ;
Krivodaeva, Elena A. ;
Romashov, Leonid V. ;
Zalesskiy, Sergey S. ;
Kachala, Vadim V. ;
Burykina, Julia V. ;
Ananikov, Valentine P. .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2016, 55 (29) :8338-8342
[9]   Size, volume fraction, and nucleation of Stober silica nanoparticles [J].
Green, DL ;
Lin, JS ;
Lam, YF ;
Hu, MZC ;
Schaefer, DW ;
Harris, MT .
JOURNAL OF COLLOID AND INTERFACE SCIENCE, 2003, 266 (02) :346-358
[10]  
Hammouda B., PROBING NANOSCALE ST