Insights on the Molecular Mechanism for the Recalcitrance of Biochars: Interactive Effects of Carbon and Silicon Components

被引:195
作者
Guo, Jianhua [1 ,2 ]
Chen, Baoliang [1 ,2 ]
机构
[1] Zhejiang Univ, Dept Environm Sci, Hangzhou 310058, Zhejiang, Peoples R China
[2] Zhejiang Prov Key Lab Organ Pollut Proc & Control, Hangzhou 310058, Zhejiang, Peoples R China
基金
中国国家自然科学基金;
关键词
RICE HUSK SILICA; BLACK CARBON; ORGANIC-MATTER; HYDROGEN-PEROXIDE; WASTE BIOMASSES; SOIL; TEMPERATURE; PYROLYSIS; CONTAMINANTS; DEGRADATION;
D O I
10.1021/es405647e
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Few studies have investigated the effects of structural heterogeneity (particularly the interactions of silicon and carbon) on the mechanisms for the recalcitrance of biochar. In this study, the molecular mechanisms for the recalcitrance of biochars derived from rice straw at 300, 500, and 700 degrees C (named RS300, RS500, and RS700, respectively) were elucidated. Short-term (24 h) and long-term (240 h) oxidation kinetics experiments were conducted under different concentrations of H2O2 to distinguish the stable carbon pools in the biochars. We discovered that the stabilities of the biochars were influenced not only by their aromaticity but also through possible protection by silicon encapsulation, which is regulated by pyrolysis temperatures. The aromatic components and recalcitrance of the biochars increased with increasing pyrolysis temperatures. The morphologies of the carbon forms in all of the biochars were also greatly associated with those of silica. Silica-encapsulation protection only occurred for RS500, not for RS300 and RS700. In RS300, carbon and silica were both amorphous, and they were easily decomposed by H2O2. The separation of crystalline silica from condensed aromatic carbon in RS700 eliminated the protective role of silicon on carbon. The effect of the biochar particle size on the stability of the biochar was greatly influenced by C-Si interactions and by the oxidation intensities. A novel silicon-and-carbon-coupled framework model was proposed to guide biochar carbon sequestration.
引用
收藏
页码:9103 / 9112
页数:10
相关论文
共 52 条
[1]  
[Anonymous], 2009, Biochar for Environmental Management: Science and Technology
[2]   HYDROPYROLYSIS: IMPLICATIONS FOR RADIOCARBON PRETREATMENT AND CHARACTERIZATION OF BLACK CARBON [J].
Ascough, P. L. ;
Bird, M. I. ;
Meredith, W. ;
Wood, R. E. ;
Snape, C. E. ;
Brock, F. ;
Higham, T. F. G. ;
Large, D. J. ;
Apperley, D. C. .
RADIOCARBON, 2010, 52 (03) :1336-1350
[3]   The selective dissolution of rice hull ash to form [ OSiO1.5]8[R4N]8 (R= Me, CH2CH2OH) octasilicates.: Basic nanobuilding blocks and possible models of intermediates formed during biosilicification processes [J].
Asuncion, MZ ;
Hasegawa, I ;
Kampf, JW ;
Laine, RM .
JOURNAL OF MATERIALS CHEMISTRY, 2005, 15 (21) :2114-2121
[4]   Synthesis and Characterization of Carbonaceous Materials from Saccharides (Glucose and Lactose) and Two Waste Biomasses by Hydrothermal Carbonization [J].
Aydincak, Kivanc ;
Yumak, Tugrul ;
Sinag, Ali ;
Esen, Bekir .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2012, 51 (26) :9145-9152
[5]   Morphological and chemical properties of black carbon in physical soil fractions as revealed by scanning electron microscopy and energy-dispersive X-ray spectroscopy [J].
Brodowski, S ;
Amelung, W ;
Haumaier, L ;
Abetz, C ;
Zech, W .
GEODERMA, 2005, 128 (1-2) :116-129
[6]   Transitional adsorption and partition of nonpolar and polar aromatic contaminants by biochars of pine needles with different pyrolytic temperatures [J].
Chen, Baoliang ;
Zhou, Dandan ;
Zhu, Lizhong .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2008, 42 (14) :5137-5143
[7]   Fast and Slow Rates of Naphthalene Sorption to Biochars Produced at Different Temperatures [J].
Chen, Zaiming ;
Chen, Baoliang ;
Chiou, Cary T. .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2012, 46 (20) :11104-11111
[8]   Silicon transfers in a rice field in Camargue (France) [J].
Desplanques, V ;
Cary, L ;
Mouret, JC ;
Trolard, F ;
Bourrié, G ;
Grauby, O ;
Meunier, JD .
JOURNAL OF GEOCHEMICAL EXPLORATION, 2006, 88 (1-3) :190-193
[9]   Characterization of biochars to evaluate recalcitrance and agronomic performance [J].
Enders, Akio ;
Hanley, Kelly ;
Whitman, Thea ;
Joseph, Stephen ;
Lehmann, Johannes .
BIORESOURCE TECHNOLOGY, 2012, 114 :644-653
[10]   Silicon: its manifold roles in plants [J].
Epstein, E. .
ANNALS OF APPLIED BIOLOGY, 2009, 155 (02) :155-160