长焰煤热解过程中孔的演变及其对挥发分传质影响

doi:10.11949/0438-1157.20250512

化工学报 ›› 2025, Vol. 76 ›› Issue (10): 5300-5310.DOI: 10.11949/0438-1157.20250512

长焰煤热解过程中孔的演变及其对挥发分传质影响

崔诣¹(), 胡耀伟¹^,², 宋云彩¹^,²^,³(), 冯杰¹^,²^,³(), 李文英¹^,²^,³

^1.太原理工大学省部共建煤基能源清洁高效利用国家重点实验室，山西太原 030024
^2.怀柔实验室山西研究院，山西太原 030024
^3.北京怀柔实验室，北京 101499

收稿日期:2025-05-09 修回日期:2025-07-10 出版日期:2025-10-25 发布日期:2025-11-25
通讯作者: 宋云彩,冯杰
作者简介:崔诣（1999—），男，硕士研究生，cuiyi0980@link.tyut.edu.cn
基金资助:
国家重点研发计划战略性科技创新合作项目(2022YFE0208400);山西省重点研发计划项目(202202090301002);怀柔实验室项目(ZD2023012A);山西省自然科学基金项目(20210302124096)

Pore evolution and its influence on volatile mass transfer during long-flame coal pyrolysis

Yi CUI¹(), Yaowei HU¹^,², Yuncai SONG¹^,²^,³(), Jie FENG¹^,²^,³(), Wenying LI¹^,²^,³

^1.State Key Laboratory of Clean and Efficient Coal Utilization, Taiyuan University of Technology, Taiyuan 030024, Shanxi, China
^2.Shanxi Research Institute of Huairou Laboratory, Taiyuan 030024, Shanxi, China
^3.Beijing Huairou Laboratory, Beijing 101499, China

Received:2025-05-09 Revised:2025-07-10 Online:2025-10-25 Published:2025-11-25
Contact: Yuncai SONG, Jie FENG

摘要/Abstract

摘要：

孔隙结构是影响热解脱挥发分的重要因素之一。为了研究煤热解过程中孔隙的演变规律和分形特征及其对挥发分传质行为的影响，本文通过N₂吸附法和分形理论对不同热解终温（393~1073 K）下半焦的孔隙结构进行了分析和定量描述。并基于半焦孔隙的演变规律和分形特征，从颗粒尺度上对热解过程中孔结构的演变进行了建模，模型考虑了焦油的二次裂解反应、挥发分在分形孔隙内的扩散，同时能预测煤颗粒的瞬态温度分布、挥发分的生成以及孔隙结构的变化。结果表明，半焦热解过程中以狭缝状介孔为主；影响孔隙演变的机制包括干燥脱气、有机质裂解与孔隙收缩；微孔存在增加了半焦孔结构的非均质性。孔结构主要通过改变焦油的扩散机制来影响挥发分的产率，对轻质气体的产率影响不大。

关键词: 低阶煤热解, 多孔介质, 孔隙结构, 分形维数, 扩散, 数值模拟

Abstract:

Pore structure is one of the important factors affecting pyrolytic devolatiles. This study systematically investigates the evolution and fractal characteristics of semicoke pores at different pyrolysis final temperatures (393—1073 K) using integrated N₂ adsorption and fractal dimension analysis. A particle-scale model was developed based on pore evolution patterns, incorporating tar secondary cracking, volatile diffusion in fractal pores, and predicting transient temperature distribution, volatile yields, and pore structure changes. The results show that slit-shaped mesopores dominate during semi-coke pyrolysis, with pore evolution driven by drying degassing, organic decomposition with pore shrinkage, and increased heterogeneity from micropores. Pore structure mainly influences volatile yields by modifying tar diffusion pathways, while showing negligible effects on light gas production. This work provides fundamental insights into pore-volatile interactions that are crucial for pyrolysis reactor design and process optimization.

Key words: low-rank coal pyrolysis, porous media, pore distribution, fractal dimension, diffusion, numerical simulation

中图分类号:

TQ 021.4

崔诣, 胡耀伟, 宋云彩, 冯杰, 李文英. 长焰煤热解过程中孔的演变及其对挥发分传质影响[J]. 化工学报, 2025, 76(10): 5300-5310.

Yi CUI, Yaowei HU, Yuncai SONG, Jie FENG, Wenying LI. Pore evolution and its influence on volatile mass transfer during long-flame coal pyrolysis[J]. CIESC Journal, 2025, 76(10): 5300-5310.

图/表 15

表1 曹家滩长焰煤的工业分析和元素分析

Table 1 Proximate and ultimate analysis of CJT

工业分析w_ad/%				元素分析w_daf/%
M	A	V	FC	C	H	N	S	O
2.80	7.80	35.38	54.02	81.62	5.64	1.05	0.82	9.81

图1 单颗粒煤热解模型示意图

Fig.1 Illustration of single-particle coal pyrolysis model

表2 反应过程中涉及到的数学模型

Table 2 Mathematical modeling involved in the reaction process

方程类别	方程
能量守恒方程^[19]	$ρ c p e f f ∂ T ∂ t ︸累积项 + ρ c p g, m i x 1 r 2 ∂ ∂ r r 2 u T ︸对流项 + 1 r 2 ∂ ∂ r - r 2 λ e f f ∂ T ∂ t ︸传热项 = Q t o t ︸热源项$
有效比热容(ρc_p )_eff	$ρ c p e f f = 1 - ε c p, a ρ a + c p, i s ρ i s + c p, c ρ c + ε ρ c p g, m i x$
有效热导率λ_eff	$λ e f f = 1 - ε λ a ρ a + λ i s ρ i s + λ c ρ c ρ a + ρ i s + ρ c + ε λ g, m i x + 13.5 σ T 3 d p e w$
热源项Q_tot^[20]	$Q t o t = - k t Δ H t + k g Δ H g + k i s Δ H i s ρ a - k c Δ H c ρ i s - k g 1 Δ H g 1 + k c 1 Δ H c 1 ρ t$
局部热通量q^[21]	$q = - λ e f f ∇ T + h d Δ T$
动量传递控制方程^[22]	$∂ ε ρ g, m i x ∂ t + ∇ ⋅ ρ g, m i x u = Q m$
气体流速u	$u = - κ μ g, m i x ∂ p ∂ r$
多孔基体的渗透率κ^[23]	$κ = ε 3 180 1 - ε 2 d p e 2$
理想气体状态方程^[24]	$ρ g, m i x = ∑ i ρ i$ , $p = ρ g, m i x R T M g, m i x$ , $M g, m i x = ∑ i ρ i ρ g, m i x M i - 1$
质量传递方程^[25]	$∂ ε c i ∂ t ︸累积项 + 1 r 2 ∂ r 2 c i u ∂ r ︸对流项 + 1 r 2 ∂ r 2 J i ∂ r ︸扩散项 = R i ︸源项$
对流质量通量^[20]	$T a r : ∂ ε ρ t ∂ t + 1 r 2 ∂ r 2 V ρ t ∂ t = k t ρ a - k c 1 + k g 1 ρ t$ , $G a s : ∂ ε ρ g ∂ t + 1 r 2 ∂ r 2 V ρ g ∂ t = k g ρ a + k g 1 ρ t$
扩散通量J_i^[26]	$J i = - D i ∇ c i$
分形扩散系数D_i^[27]	$D i = v 3 d p 0.0033 d p δ + 0.57 e - 7.05 - 0.054 D f d p δ ε 2.97 - 0.17 d p δ$
分子运动的平均速率v^[27]	$v = 8 R T π M i$
分子平均自由程δ^[28]	$δ = κ B T 2 p π d m 2$
孔隙结构演变模型^{[14, 19, 27, 29]}	$V s o l i d V 0, a = ρ a + α ρ i s + ρ c ρ 0, a$ , $V p = V 0, p + β V 0, a - V s o l i d$ , $V f i n a l, p = γ V 0, p 0$ $V 0 . p = θ V 0, p 0 + 1 - θ V f i n a l, p$ , $θ = ρ a ρ 0, a$ , $V p e = V + s o l i d V p$ , $ε = V p V p e$ $d p = d 0, p ε 1 / 3$ , $l p = χ d p 2 ε 1 / 3$ , $D f = - l n d S p d r p l n r p$ , $S p = 4 ε V p e d p 1 - ε$
Nusselt数^[30-31]	$N u = 2.0 + f × R e 1 / 2 P r 1 / 3$
Reynolds数^[32]	$R e = ρ g d p u μ g$
Prandtl数^[32]	$P r = μ g c p, g λ g$
反应速率常数k^[18]	$k = A i e - E i R T$

表2 反应过程中涉及到的数学模型

Table 2 Mathematical modeling involved in the reaction process

方程类别	方程
能量守恒方程^[19]	$ρ c p e f f ∂ T ∂ t ︸累积项 + ρ c p g, m i x 1 r 2 ∂ ∂ r r 2 u T ︸对流项 + 1 r 2 ∂ ∂ r - r 2 λ e f f ∂ T ∂ t ︸传热项 = Q t o t ︸热源项$
有效比热容(ρc_p )_eff	$ρ c p e f f = 1 - ε c p, a ρ a + c p, i s ρ i s + c p, c ρ c + ε ρ c p g, m i x$
有效热导率λ_eff	$λ e f f = 1 - ε λ a ρ a + λ i s ρ i s + λ c ρ c ρ a + ρ i s + ρ c + ε λ g, m i x + 13.5 σ T 3 d p e w$
热源项Q_tot^[20]	$Q t o t = - k t Δ H t + k g Δ H g + k i s Δ H i s ρ a - k c Δ H c ρ i s - k g 1 Δ H g 1 + k c 1 Δ H c 1 ρ t$
局部热通量q^[21]	$q = - λ e f f ∇ T + h d Δ T$
动量传递控制方程^[22]	$∂ ε ρ g, m i x ∂ t + ∇ ⋅ ρ g, m i x u = Q m$
气体流速u	$u = - κ μ g, m i x ∂ p ∂ r$
多孔基体的渗透率κ^[23]	$κ = ε 3 180 1 - ε 2 d p e 2$
理想气体状态方程^[24]	$ρ g, m i x = ∑ i ρ i$ , $p = ρ g, m i x R T M g, m i x$ , $M g, m i x = ∑ i ρ i ρ g, m i x M i - 1$
质量传递方程^[25]	$∂ ε c i ∂ t ︸累积项 + 1 r 2 ∂ r 2 c i u ∂ r ︸对流项 + 1 r 2 ∂ r 2 J i ∂ r ︸扩散项 = R i ︸源项$
对流质量通量^[20]	$T a r : ∂ ε ρ t ∂ t + 1 r 2 ∂ r 2 V ρ t ∂ t = k t ρ a - k c 1 + k g 1 ρ t$ , $G a s : ∂ ε ρ g ∂ t + 1 r 2 ∂ r 2 V ρ g ∂ t = k g ρ a + k g 1 ρ t$
扩散通量J_i^[26]	$J i = - D i ∇ c i$
分形扩散系数D_i^[27]	$D i = v 3 d p 0.0033 d p δ + 0.57 e - 7.05 - 0.054 D f d p δ ε 2.97 - 0.17 d p δ$
分子运动的平均速率v^[27]	$v = 8 R T π M i$
分子平均自由程δ^[28]	$δ = κ B T 2 p π d m 2$
孔隙结构演变模型^{[14, 19, 27, 29]}	$V s o l i d V 0, a = ρ a + α ρ i s + ρ c ρ 0, a$ , $V p = V 0, p + β V 0, a - V s o l i d$ , $V f i n a l, p = γ V 0, p 0$ $V 0 . p = θ V 0, p 0 + 1 - θ V f i n a l, p$ , $θ = ρ a ρ 0, a$ , $V p e = V + s o l i d V p$ , $ε = V p V p e$ $d p = d 0, p ε 1 / 3$ , $l p = χ d p 2 ε 1 / 3$ , $D f = - l n d S p d r p l n r p$ , $S p = 4 ε V p e d p 1 - ε$
Nusselt数^[30-31]	$N u = 2.0 + f × R e 1 / 2 P r 1 / 3$
Reynolds数^[32]	$R e = ρ g d p u μ g$
Prandtl数^[32]	$P r = μ g c p, g λ g$
反应速率常数k^[18]	$k = A i e - E i R T$

表3 热解反应的动力学参数和反应热［20］

Table 3 Kinetic parameters and reaction heat of pyrolysis reactions［20］

反应	指前因子A_i /s^-1	活化能E_i /(kJ·mol^-1)	反应热ΔH/(kJ·kg^-1)
1	4.38×10⁹	152.7	80
2	1.08×10¹⁰	148	80
3	3.75×10⁶	111.7	80
4	4.28×10⁶	108	-42
5	1×10⁵	108	-42
6	1.38×10¹⁰	161	-300

图2 热解反应路径示意图

Fig.2 Pyrolytic reaction pathways

表4 模型中使用的物性参数或关系式［33］

Table 4 Physical property parameters or relationships used in the model［33］

物性参数	数值或表达式
比热容/(J·kg^-1·K^-1)	$c p, a = 1150 T ≤ 573 K 1150 + 2.03 T - 573 - 1.55 × 10 - 3 T - 573 2 T > 573 K$ $c p, i s = c p, c = 1458$ , $c p g, m i x = 1390$
热导率/(W·m^-1·K^-1)	$λ a = 0.23 T ≤ 673 K 0.23 + 2.24 × 10 - 5 T - 673 1.8 T > 673 K$ $λ i s = λ c = 1.89$ , $λ g, m i x = 0.07$
颗粒的初始密度/ (kg·m^-3)	$ρ 0, a = 1250$
环境压力/Pa	$p a m b = 101325$

表4 模型中使用的物性参数或关系式［33］

Table 4 Physical property parameters or relationships used in the model［33］

物性参数	数值或表达式
比热容/(J·kg^-1·K^-1)	$c p, a = 1150 T ≤ 573 K 1150 + 2.03 T - 573 - 1.55 × 10 - 3 T - 573 2 T > 573 K$ $c p, i s = c p, c = 1458$ , $c p g, m i x = 1390$
热导率/(W·m^-1·K^-1)	$λ a = 0.23 T ≤ 673 K 0.23 + 2.24 × 10 - 5 T - 673 1.8 T > 673 K$ $λ i s = λ c = 1.89$ , $λ g, m i x = 0.07$
颗粒的初始密度/ (kg·m^-3)	$ρ 0, a = 1250$
环境压力/Pa	$p a m b = 101325$

表5 煤热解挥发分组分的物性参数［34］

Table 5 Physical parameters of volatiles components of coal pyrolysis［34］

挥发分组成

摩尔质量M/

(kg·mol^-1)

有效分子碰撞

直径d_m/m

3.79×10^-5, T_0,gas=298 K

图3 不同热解温度下半焦的N2吸附-脱附等温曲线

Fig.3 Isothermal curves of N2 adsorption/desorption of semi-coke at different pyrolysis temperature

图4 半焦孔隙结构的演变

Fig.4 Evolution of semi-coke pore structure

表6 不同热解温度下半焦的孔体积

Table 6 Pore volume of semicoke at different pyrolysis temperature

热解温度/K	微孔孔容/ (cm³·g^-1)	介孔孔容/ (cm³·g^-1)	大孔孔容/ (cm³·g^-1)
393	0.0018	0.0185	0.0109
473	0.0017	0.0217	0.0111
573	0.0017	0.0162	0.0094
673	0.0071	0.0240	0.014
773	0.0144	0.0321	0.0161
873	0.0400	0.0428	0.0183
973	0.0543	0.0407	0.0286
1073	0.0216	0.0346	0.0215

图5 不同热解温度下分形维数DFHH-1与DFHH-2的变化

Fig.5 Variation of the fractal dimension DFHH-1 and DFHH-2 at different pyrolysis temperature

图6 不同工况条件下颗粒温度与孔隙率的模型预测值与实验值的对比

Fig.6 Comparison between model predictions and experimental results of particle temperature and porosity under different operating conditions

图7 热解轻质气体与焦油在不同孔径内的Knudsen数

Fig.7 Knudsen number of pyrolyzed light gas and tar in different pore size

图8 分形维数的变化对热解轻质气体与焦油产率的影响

Fig.8 Effect of fractal dimension on pyrolysis of light gases with tar yields

图9 孔隙率对热解轻质气体与焦油产率的影响

Fig.9 Effect of porosity on pyrolysis light gas and tar yields

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长焰煤热解过程中孔的演变及其对挥发分传质影响

Pore evolution and its influence on volatile mass transfer during long-flame coal pyrolysis

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