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]
  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
4. [4]
  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
5. [5]
  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
6. [6]
  Hui Wang , Abdelkader Labidi , Menghan Ren , Feroz Shaik , Chuanyi Wang . 微观结构调控的g-C₃N₄在光催化NO转化中的最新进展：吸附/活化位点的关键作用. Acta Physico-Chimica Sinica, 2025, 41(5): 100039-. doi: 10.1016/j.actphy.2024.100039
7. [7]
  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
8. [8]
  Xiaochen Zhang , Fei Yu , Jie Ma . 多角度数理模拟在电容去离子中的前沿应用. Acta Physico-Chimica Sinica, 2024, 40(11): 2311026-. doi: 10.3866/PKU.WHXB202311026
9. [9]
  Weina Wang , Lixia Feng , Fengyi Liu , Wenliang Wang . Computational Chemistry Experiments in Facilitating the Study of Organic Reaction Mechanism: A Case Study of Electrophilic Addition of HCl to Asymmetric Alkenes. University Chemistry, 2025, 40(3): 206-214. doi: 10.12461/PKU.DXHX202407022
10. [10]
  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
11. [11]
  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
12. [12]
  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
13. [13]
  Guang Huang , Lei Li , Dingyi Zhang , Xingze Wang , Yugai Huang , Wenhui Liang , Zhifen Guo , Wenmei Jiao . Cobalt’s Valor, Nickel’s Foe: A Comprehensive Chemical Experiment Utilizing a Cobalt-based Imidazolate Framework for Nickel Ion Removal. University Chemistry, 2024, 39(8): 174-183. doi: 10.3866/PKU.DXHX202311051
14. [14]
  Fugui XI , Du LI , Zhourui YAN , Hui WANG , Junyu XIANG , Zhiyun DONG . Functionalized zirconium metal-organic frameworks for the removal of tetracycline from water. Chinese Journal of Inorganic Chemistry, 2025, 41(4): 683-694. doi: 10.11862/CJIC.20240291
15. [15]
  Fei Xie , Chengcheng Yuan , Haiyan Tan , Alireza Z. Moshfegh , Bicheng Zhu , Jiaguo Yu . d带中心调控过渡金属单原子负载COF吸附O₂的理论计算研究. Acta Physico-Chimica Sinica, 2024, 40(11): 2407013-. doi: 10.3866/PKU.WHXB202407013
16. [16]
  Shuanglin TIAN , Tinghong GAO , Yutao LIU , Qian CHEN , Quan XIE , Qingquan XIAO , Yongchao LIANG . First-principles study of adsorption of Cl₂ and CO gas molecules by transition metal-doped g-GaN. Chinese Journal of Inorganic Chemistry, 2024, 40(6): 1189-1200. doi: 10.11862/CJIC.20230482
17. [17]
  Yifeng TAN , Ping CAO , Kai MA , Jingtong LI , Yuheng WANG . Synthesis of pentaerythritol tetra(2-ethylthylhexoate) catalyzed by h-MoO₃/SiO₂. Chinese Journal of Inorganic Chemistry, 2024, 40(11): 2155-2162. doi: 10.11862/CJIC.20240147
18. [18]
  Guang-Xu Duan , Queting Chen , Rui-Rui Shao , Hui-Huang Sun , Tong Yuan , Dong-Hao Zhang . Encapsulating lipase on the surface of magnetic ZIF-8 nanosphers with mesoporous SiO₂ nano-membrane for enhancing catalytic performance. Chinese Chemical Letters, 2025, 36(2): 109751-. doi: 10.1016/j.cclet.2024.109751
19. [19]
  Maitri Bhattacharjee , Rekha Boruah Smriti , R. N. Dutta Purkayastha , Waldemar Maniukiewicz , Shubhamoy Chowdhury , Debasish Maiti , Tamanna Akhtar . Synthesis, structural characterization, bio-activity, and density functional theory calculation on Cu(Ⅱ) complexes with hydrazone-based Schiff base ligands. Chinese Journal of Inorganic Chemistry, 2024, 40(7): 1409-1422. doi: 10.11862/CJIC.20240007
20. [20]
  Zhengkun QIN , Zicong PAN , Hui TIAN , Wanyi ZHANG , Mingxing SONG . A series of iridium(Ⅲ) complexes with fluorophenyl isoquinoline ligand and low-efficiency roll-off properties: A density functional theory study. Chinese Journal of Inorganic Chemistry, 2025, 41(6): 1235-1244. doi: 10.11862/CJIC.20240429

Get Citation

PDF

XML

Metrics

PDF Downloads(9)
Abstract views(1118)
HTML views(202)

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