Citation: DONG Jing-lan, GENG Xiao, GAO Zheng-yang, LIU Yan-feng. Adsorption mechanism of trace As on the defect sites of SiO₂ in fly ash[J]. Journal of Fuel Chemistry and Technology, ;2018, 46(11): 1401-1408. shu

Adsorption mechanism of trace As on the defect sites of SiO₂ in fly ash

School of Energy Power and Mechanical Engineering, North China Electric Power University, Baoding 071003, China

Corresponding author: DONG Jing-lan, jinglan_dong@163.com
Received Date: 15 May 2018
Revised Date: 15 August 2018

Fund Project: the Fundamental Research Funds for the Central Universities 2018MS099The project was supported by the Fundamental Research Funds for the Central Universities(2018MS099)

Figures(5)

To understand the enrichment characteristics of trace As in fly ash, the adsorption mechanism of AsO, a typical arsenic oxide, in SiO₂, the main component of fly ash, was investigated by using density functional theory; energy calculation, AIM theory, Mulliken charge analysis and Localized Orbital Locator(LOL) color map were performed on the optimized adsorption configuration, in order to analyze the interaction between AsO and SiO₂. The results show that the adsorption energy of AsO on the defect sites of amorphous SiO₂ is higher than 50 kJ/mol, typical for the configuration of chemical adsorption. The bonds of As-Si, Si-O and As-O formed at the active defect sites of the amorphous SiO₂ have high strength, belonging to the covalent bond; that is, the interaction between SiO₂ and AsO is covalent.
- density functional theory,
- adsorption,
- AsO,
- SiO₂,
- AIM theory,
- LOL
1. [1]
  ZHAO Yong-chun, MA Si-ming, YANG Jian-ping. Development and status quo of ultra-clean pollutant emissions from coal-fired power plants[J]. J China Coal Soc, 2015,40(11):2629-2640.
2. [2]
  GUO Xin, ZHENG Chu-guang, CHEN Dan. Experimental Study on arsenic emission characteristics of 300MW pulverized coal-fired boiler[J]. J Environ Sci-China, 2006,27(4):631-634.
3. [3]
  WANG Quan-hai, QIU Jian-rong, WUN Cun. Experimental and simulation study on morphological transformation of trace elements under oxygen combustion[J]. J Eng Thermophys, 2006,27(s2):199-202.
4. [4]
  DING Z H, ZHENG B S, ZHUANG M. Mode of occurrence of arsenic in high-As coals from endemic arsenicosis areas in southwestern Guizhou Province, China[J]. J Coal Sci Eng, 2007,13(2):194-198.
5. [5]
  DONG Jing-lan, MA Kai. Study on arsenic release from coal-biomass combustion under oxygen-enriched atmosphere[J]. Chin J Power Eng, 2017,37(3):237-241.
6. [6]
  GAO Zheng-yang, LÜ Shao-kun, JI Shuo. Mechanism of lead adsorption on carbon-based surfaces[J]. J Chin Environ Eng, 2016,10(7):3848-3852.
7. [7]
  GAO Zheng-yang, LÜ Shao-kun. Mechanism of adsorption of mercury by manganese dioxide modified activated carbon[J]. Chin J Power Eng, 2015,35(11):923-928. doi: 10.3969/j.issn.1674-7607.2015.11.010
8. [8]
  GUO Xin, ZHENG Chu-guang, LÜ Nai-xia. Density functional theory study of adsorption of mercury and mercury over the CaO(001) Surface of cluster model[J]. Proc CSEE, 2005,25(13):101-104. doi: 10.3321/j.issn:0258-8013.2005.13.019
9. [9]
  WANG Peng, WU Jiang, REN Jian-xing. Experimental study on the effect of unburned carbon from fly ash on mercury adsorption in flue gas[J]. Chin J Power Eng, 2012,32(4):332-337. doi: 10.3969/j.issn.1674-7607.2012.04.012
10. [10]
  WANG Jun, JIANG Jian-guo, SUI Ji-chao. Study on the basic properties of waste incineration fly ash[J]. J Environ Sci-China, 2006,27(11):141-145.
11. [11]
  SUN Jun-min, HAN De-xin, YAO Qiang. Microscopic particle types and microstructure characteristics of coal-fired fly ash[J]. J Electron Micro, 2001,20(2):140-147. doi: 10.3969/j.issn.1000-6281.2001.02.012
12. [12]
  WILLIAMS R P, RIESSEN A V. Determination of the reactive component of fly ashes for geopolymer production using XRF and XRD[J]. Fuel, 2010,89(12):3683-3692. doi: 10.1016/j.fuel.2010.07.031
13. [13]
  NURIA L, FRANCESC I, GIANFRANCO P. Adsorption of Cu, Pd, and Cs Atoms on Regular and Defect Sites of the SiO₂ Surface[J]. J Am Chem Soc, 2017,121(4):813-821.
14. [14]
  FERULLO R M, GARDA G R, BELELLI P G. Deposition of small Cu, Ag and Au particles on reduced SiO₂[J]. J Mol Struct (Theochem), 2006(769):217-223.
15. [15]
  LÜ Xin. Cluster-Surface Analogy: Discussion on Metal Oxide Cluster Model[D]. Xiamen: Xiamen University, 2004.
16. [16]
  MUKHOPADHYAY S, SUSHKO P V. Correlation between the atomic structure, formation energies, and optical absorption of neutral oxygen vacancies in amorphous silica[J]. Phys Rev B, 2005,71(23)5204.
17. [17]
  KRISHNAN R, BINKLEY J S, SEEGER R. Self-consistent molecular-orbital methods-A basis set for correlated wave functions[J]. Chem Phys, 1980,72(1):650-654.
18. [18]
  WEIGEND F, AHLRICHS R. Balanced basis sets of split valence, triple zeta valence and quadruple zeta valence quality for H to Rn:Design and assessment of accuracy[J]. Phys Chem Chem Phys, 2005(7):3297-3305.
19. [19]
  GAUSSIAN 09, REVISIOND.01, FRISCH M J, TRUCKS G W, SCHLEGEL H B. Gaussian, Inc., Wallingford CT, 2016.
20. [20]
  LU T. Multiwfn:A multifunctional wavefunction analyzer[J]. J Comput Chem, 2012,33(5):580-592. doi: 10.1002/jcc.v33.5
21. [21]
  TANG T H, CUI Y P. A theoretical study of some X-H-π hydrogen-bonded complexes using the theory of atoms in molecules[J]. Can J Chem, 2011,74(6):1162-1170.
22. [22]
  BADER R F. A quantum theory of molecular structure and its applications[J]. Chem Rev, 1991,91(5):893-928. doi: 10.1021/cr00005a013
23. [23]
  CREMER D, KRAKA E. Chemical bonds without bonding electron density-Does the difference electron density analysis suffice for a description of the chemical bond[J]. Angew Chem, 1984,23(23):627-628.
24. [24]
  ESPINOSA E, ALKORTA I, ELGUERO J. From weak to strong interactions:A comprehensive analysis of the topological and energetic properties of the electron density distribution involving X-H F-Y systems[J]. J Chem Phys, 2002,117(12):5529-5542. doi: 10.1063/1.1501133
25. [25]
  DONG Lan, JIANG Shu-bin, ZHENG Shen-sheng. Density functional theory for hydrogen molecule adsorption of Be_n(n=1~6) clusters[J]. Atomic Energy Sci Technol, 2010,44(12):1414-1419.
26. [26]
  YE Tian-xu, XU Yong-qiang, ZHANG Yu-hui. Quantum chemistry study on hydrogenation desulfurization activity of Co/MoS₂ catalyst[J]. J Chin Univ Pet(Nat Sci Ed), 2005,29(4):119-121. doi: 10.3321/j.issn:1000-5870.2005.04.028
27. [27]
  JACOBSEN H J. Localized-orbital locator (LOL) profiles of transition-metal hydride a[J]. Can J Chem, 2009,87(7):965-973. doi: 10.1139/V09-060
1. [1]
  Jie ZHAO , Sen LIU , Qikang YIN , Xiaoqing LU , Zhaojie WANG . Theoretical calculation of selective adsorption and separation of CO₂ by alkali metal modified naphthalene/naphthalenediyne. Chinese Journal of Inorganic Chemistry, 2024, 40(3): 515-522. doi: 10.11862/CJIC.20230385
2. [2]
  Hao XU , Ruopeng LI , Peixia YANG , Anmin LIU , Jie BAI . Regulation mechanism of halogen axial coordination atoms on the oxygen reduction activity of Fe-N₄ site: A density functional theory study. Chinese Journal of Inorganic Chemistry, 2025, 41(4): 695-701. doi: 10.11862/CJIC.20240302
3. [3]
  Hanyan DAI , Shuwei ZHANG , Han ZENG , Jianfei NIU . Electro-chemiluminescence performance of glucose sensor based on graphene quantum dot nano-complex. Chinese Journal of Inorganic Chemistry, 2026, 42(11): 2475-2492. doi: 10.11862/CJIC.20260044
4. [4]
  Cong JI , Hao WANG , Willie Forkpah DELEAU , Xinxin JING , Dapeng LI , Zhengying WU , Linbing SUN . Magnetic calcium-rich CaFe₂O₄: Synthesis and adsorption performance for phosphates in water bodies. Chinese Journal of Inorganic Chemistry, 2026, 42(6): 1131-1145. doi: 10.11862/CJIC.20260063
5. [5]
  Kaifu Zhang , Shan Gao , Bin Yang . Application of Theoretical Calculation with Fun Practice in Raman Spectroscopy Experimental Teaching. University Chemistry, 2025, 40(3): 62-67. doi: 10.12461/PKU.DXHX202404045
6. [6]
  Jie ZHAO , Huili ZHANG , Xiaoqing LU , Zhaojie WANG . Theoretical calculations of CO₂ capture and separation by functional groups modified 2D covalent organic framework. Chinese Journal of Inorganic Chemistry, 2025, 41(2): 275-283. doi: 10.11862/CJIC.20240213
7. [7]
  Ting YANG , Jia AN , Jinyu ZHANG , Ruonan FAN , Rong YAN , Xiaoxia JING , Panpan CHANG , Wei YAN . Synergistic enhancement of ion migration and sulfur conversion kinetics in lithium-sulfur batteries by CeO₂/g-C₃N₄. Chinese Journal of Inorganic Chemistry, 2026, 42(3): 519-530. doi: 10.11862/CJIC.20250274
8. [8]
  Qin′ai FENG , Jianjun LI , Lili ZHANG , Linxin WU , Huiling WANG , Wenjing HOU , Lei WANG , Mingjie REN . Amphiphilic surface modification of magnetic adsorbents and its adsorption properties of two microplastics. Chinese Journal of Inorganic Chemistry, 2026, 42(4): 789-807. doi: 10.11862/CJIC.20250208
9. [9]
  Hongfei Yin , Mengling Hong , Jinyang Zhang , Wentao Wang , Wei Chen , Guozhi Wu . Oxygen vacancy-mediated 2D/2D Bi₂MoO₆/Bi₂O₂S S-scheme heterojunctions for efficient CO₂ photoreduction. Acta Physico-Chimica Sinica, 2026, 42(9): 100332-0. doi: 10.1016/j.actphy.2026.100332
10. [10]
  Jingke LIU , Jia CHEN , Yingchao HAN . Nano hydroxyapatite stable suspension system: Preparation and cobalt adsorption performance. Chinese Journal of Inorganic Chemistry, 2024, 40(9): 1763-1774. doi: 10.11862/CJIC.20240060
11. [11]
  Peipei DING , Jingying DUAN , Haoran XU , Xinru FANG , Xingyu LIU , Juntao YAN , Chunlei WANG . Preparation and adsorption properties of poplar catkin-derived porous carbon by ethanol solvothermal method. Chinese Journal of Inorganic Chemistry, 2026, 42(6): 1203-1214. doi: 10.11862/CJIC.20250370
12. [12]
  Wei Sun , Yongjing Wang , Kun Xiang , Saishuai Bai , Haitao Wang , Jing Zou , Arramel , Jizhou Jiang . CoP Decorated on Ti₃C₂T_x MXene Nanocomposites as Robust Electrocatalyst for Hydrogen Evolution Reaction. Acta Physico-Chimica Sinica, 2024, 40(8): 2308015-0. doi: 10.3866/PKU.WHXB202308015
13. [13]
  Shuangshuang Mao , Juhua Luo , Bingjie Han , Jiahuan Shi , Yujia Gu . Covalent organic framework-derived Fe₃C/NC/TiO₂ heterostructures for high-performance electromagnetic wave absorption. Acta Physico-Chimica Sinica, 2026, 42(7): 100290-. doi: 10.1016/j.actphy.2026.100290
14. [14]
  Hui Wang , Abdelkader Labidi , Menghan Ren , Feroz Shaik , Chuanyi Wang . Recent Progress of Microstructure-Regulated g-C₃N₄ in Photocatalytic NO Conversion: The Pivotal Roles of Adsorption/Activation Sites. Acta Physico-Chimica Sinica, 2025, 41(5): 100039-0. doi: 10.1016/j.actphy.2024.100039
15. [15]
  Wei ZHANG , Ye LIU , Zehong CHEN . Theoretical investigation of Pb²⁺ adsorption and migration behavior at the α-ZrP/polypyrrole composite interface. Chinese Journal of Inorganic Chemistry, 2026, 42(10): 2232-2244. doi: 10.11862/CJIC.20260054
16. [16]
  Meifeng Zhu , Jin Cheng , Kai Huang , Cheng Lian , Shouhong Xu , Honglai Liu . Classical Density Functional Theory for Understanding Electrochemical Interface. University Chemistry, 2025, 40(3): 148-152. doi: 10.12461/PKU.DXHX202405166
17. [17]
  Yupeng TANG , Haiying YANG , Fan JIN , Nan LI . Hydrogen storage properties of C₆S₆Li₆: A density functional theory study. Chinese Journal of Inorganic Chemistry, 2025, 41(9): 1827-1839. doi: 10.11862/CJIC.20240460
18. [18]
  Peng XU , Shasha WANG , Nannan CHEN , Ao WANG , Dongmei YU . Preparation of three-layer magnetic composite Fe₃O₄@polyacrylic acid@ZiF-8 for efficient removal of malachite green in water. Chinese Journal of Inorganic Chemistry, 2024, 40(3): 544-554. doi: 10.11862/CJIC.20230239
19. [19]
  Zeyu XU , Anlei DANG , Bihua DENG , Xiaoxin ZUO , Yu LU , Ping YANG , Wenzhu YIN . Evaluation of the efficacy of graphene oxide quantum dots as an ovalbumin delivery platform and adjuvant for immune enhancement. Chinese Journal of Inorganic Chemistry, 2024, 40(6): 1065-1078. doi: 10.11862/CJIC.20240099
20. [20]
  Jing Wang , Pingping Li , Yuehui Wang , Yifan Xiu , Bingqian Zhang , Shuwen Wang , Hongtao Gao . Treatment and Discharge Evaluation of Phosphorus-Containing Wastewater. University Chemistry, 2024, 39(5): 52-62. doi: 10.3866/PKU.DXHX202309097

Get Citation

PDF

XML

Metrics

PDF Downloads(9)
Abstract views(2485)
HTML views(375)

通讯作者: 陈斌, bchen63@163.com

1.
沈阳化工大学材料科学与工程学院沈阳 110142

Adsorption mechanism of trace As on the defect sites of SiO2 in fly ash

Metrics

通讯作者: 陈斌, bchen63@163.com

Adsorption mechanism of trace As on the defect sites of SiO₂ in fly ash