化工学报 ›› 2023, Vol. 74 ›› Issue (7): 2935-2946.DOI: 10.11949/0438-1157.20230207
陈吉1(), 洪泽3, 雷昭1,2(), 凌强1,2, 赵志刚1,2, 彭陈辉3, 崔平1,2()
收稿日期:
2023-03-08
修回日期:
2023-07-06
出版日期:
2023-07-05
发布日期:
2023-08-31
通讯作者:
雷昭,崔平
作者简介:
陈吉(1993—),男,博士研究生,chenjiahut@126.com
基金资助:
Ji CHEN1(), Ze HONG3, Zhao LEI1,2(), Qiang LING1,2, Zhigang ZHAO1,2, Chenhui PENG3, Ping CUI1,2()
Received:
2023-03-08
Revised:
2023-07-06
Online:
2023-07-05
Published:
2023-08-31
Contact:
Zhao LEI, Ping CUI
摘要:
为从分子层面研究焦炭溶损反应及其机理,借助分子动力学和第一性原理构建了一种包含石墨化碳和非石墨化碳的焦炭分子模型,研究了电荷密度和孔径大小对焦炭溶损反应及其机理的影响,并通过实验对模拟结果加以验证。结果表明,所建模型真密度在焦炭实测密度范围内;焦炭石墨化程度越高,碳原子周边电荷密度越小,其溶损反应程度越低,实验结果与模拟结果相近;CO2在孔径大于50 Å(1 Å=1×10-10 m)气孔内以扩散为主,其扩散表观活化能最小,为131.24 kJ/mol;在孔径小于2 Å气孔内以吸附为主,其吸附能的绝对值最大,为192.54 kJ/mol;焦炭溶损反应机理包括焦炭分子生成石墨化碳和非石墨化碳原子的裂解反应、碳原子之间的异构化反应以及碳原子与CO2的氧化反应,在氧化反应过程中,碳原子与CO2反应生成的烯酮式结构会因其稳定性差裂解成CO,完成反应过程。
中图分类号:
陈吉, 洪泽, 雷昭, 凌强, 赵志刚, 彭陈辉, 崔平. 基于分子动力学的焦炭溶损反应及其机理研究[J]. 化工学报, 2023, 74(7): 2935-2946.
Ji CHEN, Ze HONG, Zhao LEI, Qiang LING, Zhigang ZHAO, Chenhui PENG, Ping CUI. Study on coke dissolution loss reaction and its mechanism based on molecular dynamics simulations[J]. CIESC Journal, 2023, 74(7): 2935-2946.
样品编号 | JM/kg | FM/kg | 1/3JM/kg | SM/kg | QM/kg | Ad/% | Vdaf/% | St,d/% | G | Y/mm |
---|---|---|---|---|---|---|---|---|---|---|
c1 | 28 | 11 | 17 | 7 | 7 | 9.30 | 28.27 | 0.83 | 80 | 16.4 |
c2 | 28 | 11 | 15 | 7 | 9 | 9.42 | 28.85 | 0.84 | 79 | 16.1 |
c3 | 28 | 11 | 13 | 7 | 11 | 9.61 | 29.34 | 0.86 | 76 | 15.6 |
c4 | 28 | 11 | 10 | 7 | 14 | 9.74 | 29.78 | 0.89 | 77 | 15.2 |
表1 配煤及基本性质
Table 1 Schemes of blending coal and quality of blending coal
样品编号 | JM/kg | FM/kg | 1/3JM/kg | SM/kg | QM/kg | Ad/% | Vdaf/% | St,d/% | G | Y/mm |
---|---|---|---|---|---|---|---|---|---|---|
c1 | 28 | 11 | 17 | 7 | 7 | 9.30 | 28.27 | 0.83 | 80 | 16.4 |
c2 | 28 | 11 | 15 | 7 | 9 | 9.42 | 28.85 | 0.84 | 79 | 16.1 |
c3 | 28 | 11 | 13 | 7 | 11 | 9.61 | 29.34 | 0.86 | 76 | 15.6 |
c4 | 28 | 11 | 10 | 7 | 14 | 9.74 | 29.78 | 0.89 | 77 | 15.2 |
样品编号 | 性质/%(质量分数) | |||||
---|---|---|---|---|---|---|
Ad | Vdaf | M40 | M10 | CRI | CSR | |
c1 | 12.59 | 1.06 | 78.2 | 6.3 | 22.9 | 60.7 |
c2 | 12.61 | 1.08 | 76.7 | 6.5 | 23.3 | 60.2 |
c3 | 12.65 | 1.07 | 75.2 | 6.7 | 23.8 | 59.9 |
c4 | 12.73 | 1.05 | 74.3 | 6.7 | 24.3 | 59.4 |
表2 四种焦炭的基本性质
Table 2 Basic properties of four kinds of coke
样品编号 | 性质/%(质量分数) | |||||
---|---|---|---|---|---|---|
Ad | Vdaf | M40 | M10 | CRI | CSR | |
c1 | 12.59 | 1.06 | 78.2 | 6.3 | 22.9 | 60.7 |
c2 | 12.61 | 1.08 | 76.7 | 6.5 | 23.3 | 60.2 |
c3 | 12.65 | 1.07 | 75.2 | 6.7 | 23.8 | 59.9 |
c4 | 12.73 | 1.05 | 74.3 | 6.7 | 24.3 | 59.4 |
样品编号 | 含量/%(质量分数) | |||||
---|---|---|---|---|---|---|
Cd | Hd | Od① | Nd | Sd | Pd | |
c1 | 97.04 | 0.56 | 0.49 | 1.11 | 0.79 | 0.01 |
c2 | 97.18 | 0.49 | 0.54 | 0.99 | 0.78 | 0.02 |
c3 | 97.20 | 0.51 | 0.50 | 1.02 | 0.76 | 0.01 |
c4 | 97.17 | 0.54 | 0.48 | 1.04 | 0.75 | 0.02 |
表3 四种焦炭的元素分析
Table 3 Element analysis of four coke
样品编号 | 含量/%(质量分数) | |||||
---|---|---|---|---|---|---|
Cd | Hd | Od① | Nd | Sd | Pd | |
c1 | 97.04 | 0.56 | 0.49 | 1.11 | 0.79 | 0.01 |
c2 | 97.18 | 0.49 | 0.54 | 0.99 | 0.78 | 0.02 |
c3 | 97.20 | 0.51 | 0.50 | 1.02 | 0.76 | 0.01 |
c4 | 97.17 | 0.54 | 0.48 | 1.04 | 0.75 | 0.02 |
项目 | 石墨化碳 | 非石墨化碳 |
---|---|---|
实验值 | 72.1% | 27.9% |
模拟值 | 71.5% | 28.5% |
误差 | -0.83% | 2.15% |
表4 分子模型、焦炭中石墨化碳原子与非石墨化碳原子含量对比
Table 4 Contents of graphitized carbon atoms and non-graphitized carbon atoms in the model and coke
项目 | 石墨化碳 | 非石墨化碳 |
---|---|---|
实验值 | 72.1% | 27.9% |
模拟值 | 71.5% | 28.5% |
误差 | -0.83% | 2.15% |
类别 | 0~5 Å/% | 5~10 Å/% | 10~15 Å/% | 15~25 Å/% |
---|---|---|---|---|
5A | 54.21 | 45.79 | 0 | 0 |
5B | 61.79 | 33.21 | 3.57 | 1.43 |
5C | 65.61 | 25.39 | 5.11 | 3.89 |
表5 三种模型的气孔大小与分布
Table 5 Pore size distribution of three models
类别 | 0~5 Å/% | 5~10 Å/% | 10~15 Å/% | 15~25 Å/% |
---|---|---|---|---|
5A | 54.21 | 45.79 | 0 | 0 |
5B | 61.79 | 33.21 | 3.57 | 1.43 |
5C | 65.61 | 25.39 | 5.11 | 3.89 |
基元反应 | 频率 |
---|---|
cokesp3C | 104 |
cokesp2C | 67 |
sp3C—sp3C 2sp3C | 89 |
2sp3C sp2C | 7 |
sp2C sp2C sp3C + sp2C | 8 |
sp3C + CO2 sp3CO + CO | 38 |
sp2C + CO2 sp2CO + CO | 11 |
sp3C + CO2 sp3CCO | 94 |
sp2C + CO2 sp2CCO | 36 |
sp3CCO sp3C + CO | 92 |
sp2CCO sp2C + CO | 31 |
表6 焦炭溶损反应机理
Table 6 Reaction mechanisms of coke solution loss
基元反应 | 频率 |
---|---|
cokesp3C | 104 |
cokesp2C | 67 |
sp3C—sp3C 2sp3C | 89 |
2sp3C sp2C | 7 |
sp2C sp2C sp3C + sp2C | 8 |
sp3C + CO2 sp3CO + CO | 38 |
sp2C + CO2 sp2CO + CO | 11 |
sp3C + CO2 sp3CCO | 94 |
sp2C + CO2 sp2CCO | 36 |
sp3CCO sp3C + CO | 92 |
sp2CCO sp2C + CO | 31 |
样品 | 状态 | 2θ002/(o) | d002/nm | La/nm | Lc/nm | 石墨化度 |
---|---|---|---|---|---|---|
c1 | 反应前 | 26.41 | 0.34 | 5.81 | 3.07 | 0.62 |
失重30% | 26.38 | 0.34 | 6.19 | 3.01 | 0.71 | |
c2 | 反应前 | 26.03 | 0.34 | 5.76 | 2.62 | 0.61 |
失重30% | 26.26 | 0.34 | 5.56 | 2.68 | 0.69 | |
c3 | 反应前 | 26.30 | 0.34 | 6.23 | 3.46 | 0.63 |
失重30% | 26.37 | 0.34 | 6.07 | 3.58 | 0.71 | |
c4 | 反应前 | 26.22 | 0.34 | 5.01 | 2.46 | 0.60 |
失重30% | 26.27 | 0.34 | 5.31 | 2.62 | 0.72 |
表7 焦炭的晶格参数
Table 7 Lattice parameters of coke
样品 | 状态 | 2θ002/(o) | d002/nm | La/nm | Lc/nm | 石墨化度 |
---|---|---|---|---|---|---|
c1 | 反应前 | 26.41 | 0.34 | 5.81 | 3.07 | 0.62 |
失重30% | 26.38 | 0.34 | 6.19 | 3.01 | 0.71 | |
c2 | 反应前 | 26.03 | 0.34 | 5.76 | 2.62 | 0.61 |
失重30% | 26.26 | 0.34 | 5.56 | 2.68 | 0.69 | |
c3 | 反应前 | 26.30 | 0.34 | 6.23 | 3.46 | 0.63 |
失重30% | 26.37 | 0.34 | 6.07 | 3.58 | 0.71 | |
c4 | 反应前 | 26.22 | 0.34 | 5.01 | 2.46 | 0.60 |
失重30% | 26.27 | 0.34 | 5.31 | 2.62 | 0.72 |
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