PbCl<sub>2</sub>在缺陷Zigzag未燃尽碳的吸附机理

花桥建; 吴国兴; 徐卫; 周晓韡; 李冬; 董瑞信

PbCl₂在缺陷Zigzag未燃尽碳的吸附机理

1.
国家能源集团泰州发电有限公司, 江苏泰州 225327
2.
山东上奥电力科技有限公司, 山东济南 250101

基金项目: 锅炉吹灰优化项目（标准编码：F646100001，项目编码：10049876BC190037）资助。

详细信息

作者简介:
花桥建（1979.10.09），男，本科，工程师，研究方向：火力发电厂安全生产，E-mail：1109589@chnenergy.com.cn

通讯作者:
董瑞信（1965.12.10），男，本科，高级工程师，研究方向：火力发电厂安全生产，E-mail：957715624@qq.com，电话：18653156596

中图分类号: TK16
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- 被引次数: 0
出版历程
- 录用日期: 2022-03-28
- 网络出版日期: 2022-04-15

Adsorption Mechanism of PbCl₂ on Defect Zigzag Unburned Carbon

1.
CHN ENERGY TAIZHOU POWER GENERATION CO., LTD., Taizhou, 225327, China
2.
Shandong Shangao Power Technology Co., Ltd., Jinan, 250101, China

Funds: The project was supported by the Boiler ash blowing optimization project (Standard Code: F646100001, Project Code: 10049876BC190037).

摘要

摘要: 燃煤电厂排放的PbCl₂毒性极强，且在全球的迁移和积累而受到广泛关注。未燃尽碳被认为是有效去除PbCl₂的一种有前景的吸附剂。然而，现有的未燃尽碳模型不能反映实际未燃尽碳表面上的碳缺陷的结构。因此，建立缺陷未燃尽碳模型具有重要的现实意义。此外，碳模型对PbCl₂的吸附研究还不够深入，反应机理也不清楚。这极大地阻碍了高效吸附剂的发展。为了揭示PbCl₂在缺陷未燃尽碳表面上的吸附机理，利用密度泛函理论(DFT)系统地研究了PbCl₂在不同缺陷未燃尽碳表面上的吸附过程，并分析了PbCl₂在缺陷未燃烧碳表面上的吸附机理。结果表明：缺陷吸附位点是PbCl₂吸附的最佳位点。这项工作将为燃煤电厂碳基吸附剂的开发和脱除PbCl₂提供理论指导。
- 量子化学 /
- 未燃尽碳 /
- 吸附 /
- 铅
Abstract: PbCl₂ emitted from coal-fired power plants is of great concern due to its extreme toxicity and global migration and accumulation. Unburned carbon is considered as a promising adsorbent for effective PbCl₂ removal. However, existing models of unburned carbon do not reflect the structure of carbon defects on the surface of actual unburned carbon. Therefore, it is of great practical importance to develop a defective unburned carbon model. In addition, the carbon model is not deep enough for the adsorption of PbCl₂, and the reaction mechanism is not clear. This greatly hinders the development of efficient adsorbents. In order to reveal the adsorption mechanism of PbCl₂ on the surface of defective unburned carbon, the adsorption process of PbCl₂ on different defective unburned carbon surfaces was systematically investigated by using density functional theory (DFT). The results show that the defective adsorption sites are the best sites for PbCl₂ adsorption. This work will provide theoretical guidance for the development of carbon-based adsorbents for coal-fired power plants and the removal of PbCl₂.
- Quantum Chemistry /
- Unburned Carbon /
- Adsorption /
- Lead

HTML全文

图 1 Zigzag型缺陷未燃尽碳模型

Figure 1 Zigzag type defect unburned carbon model

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图 2 (a) Zigzag型缺陷未燃尽碳模型ELF图, (b)Zigzag型缺陷未燃尽碳模型电子密度变形图

Figure 2 (a) ELF diagram of Zigzag type defective unburned carbon model, (b) Electron density deformation diagram of Zigzag type defective unburned carbon model

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图 3 (a) PbCl₂在未燃尽碳模型表面的吸附构型 (b) PbCl₂在未燃尽碳模型上的吸附能

Figure 3 (a) Adsorption configuration of PbCl₂ on the surface of unburned carbon model (b) Adsorption Energy of PbCl₂ on Unburned Carbon Model

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图 4 Mayer键级与吸附能之间的相关性分析图

Figure 4 Correlation analysis diagram between Mayer bond level and adsorption energy

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图 5 (a) Zig-D1-1-PbCl₂构型ELF图, (b) Zig-D1-1-PbCl₂构型电子密度差分图

Figure 5 (a) Zig-D1-1-PbCl₂ conformation ELF diagram, (b) Zig-D1-1-PbCl₂ conformation electron density difference diagram

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表 1 Zigzag缺陷模型结构的表面优化参数及基态能量

Table 1 Surface optimization parameters and ground state energy of Zigzag defect model structure

	Zigzag	Zig-D1-1	Zig-D1-2	Zig-D2-1	Zig-D2-2	Zig-D2-3	Zig-D3-1	Zig-D3-2
C-C(Å)	1.41	1.41	1.4	1.41	1.43	1.44	1.44	1.39
C-H(Å)	1.09	1.09	1.09	1.09	1.09	1.09	1.09	1.09
∠C-C-C(deg)	120.31	120.31	121.09	120.47	121.65	123.85	120.71	121.88
∠C-C-H(deg)	119.29	119.29	119.46	120.91	120.63	120.8	119.55	119.45
Energy (a.u.)	−921.05	−920.25	−920.15	−881.13	−881.01	−881.9	−845.88	−845.85

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表 2 PbCl₂在Zigzag缺陷未燃尽碳表面吸附构型的MBO值

Table 2 The MBO value of the adsorption configuration of PbCl₂ on the surface of unburned carbon with Zigzag defects

Structure	Bonding Type	Bonding length (Å)	MBO
Zigzag-PbCl₂	C6-Pb35	2.46	0.64
	C9-Pb35	2.47	0.55
	C11-Cl35	1.73	1.27
Zig-D1-1-PbCl₂	C9-Pb34	2.35	0.74
Zig-D1-1-PbCl₂	C14-Cl36	1.77	0.97
Zig-D1-2-PbCl₂	C9-Cl36	1.78	1.04
Zig-D1-2-PbCl₂	C11-Pb34	2.36	0.68
Zig-D2-1-PbCl₂	C8-Pb33	2.36	0.69
Zig-D2-1-PbCl₂	C10-Cl35	1.78	0.97
Zig-D2-2-PbCl₂	C11-Pb1	2.34	0.7
Zig-D2-2-PbCl₂	C16-Cl3	1.77	0.97
Zig-D2-3-PbCl₂	C6-Pb33	2.33	0.81
Zig-D2-3-PbCl₂	C13-C34	1.76	0.97
Zig-D3-1-PbCl₂	C9-Pb32	2.43	0.45
Zig-D3-2-PbCl₂	C12-Pb32	2.4	0.5

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