Catalyst design and reactor analysis for in-situ purification of organic solid waste syngas

doi:10.16085/j.issn.1000-6613.2022-0977

Abstract

Abstract:

Tar removal from syngas is key for solid waste gasification. Conventional metal-based catalysts, despite their high cracking capabilities, easily deactivate during gasification in tar- and water vapor-laden environments. In this study, a biochar catalyst with a large specific surface area of 1384.2m²/g was prepared and its kinetics of in-situ tar removal were examined in an organic solid waste gasification reactor. The generated biochar could directly be incorporated into the gasification process without regeneration, enabling efficient tar removal at a considerably lower cost. In addition, the deactivation kinetic model of the char catalyst was constructed by measuring its surface properties and evaluating the activity of toluene cracking reaction. On this basis, the tar removal process under the conditions of the demonstration engineering process was simulated using the multi-field coupling software COMSOL. The effects of residence time, catalyst loading amount, and reactor shape on the cracking process were investigated. The results showed that, in a reactor with a height-to-diameter ratio 1.0 and full catalyst loading, the tar concentration at the outlet was reduced to zero within 4—6s, and the H₂ and CO concentrations in the syngas were 0.032kg/m³ and 0.50kg/m³, respectively.

Key words: organic solid waste, biochar, tar, kinetics, numerical simulation

摘要：

焦油脱除是实现有机固废气化制合成气连续运行的关键。常规金属类的焦油裂解催化剂尽管裂解能力强，但在固废气化高焦油、高水的环境下容易失活，催化剂再生和使用成本高。本研究设计并制备了一种比表面积达1384.2m²/g的生物质半焦催化剂，该催化剂用于可原位脱除焦油的有机固废气化反应器中，使用后的生物质半焦无需再生，直接落入气化反应器作为有机固废气化原料，大幅降低了焦油脱除成本。此外，本文通过对生物质半焦表面性质的测定及模型化合物甲苯在生物质半焦上裂解的活性评价，构建了半焦催化剂的失活动力学模型。在此基础上，利用多场耦合软件COMSOL对该催化剂在示范工程工艺条件下的焦油脱除过程进行仿真，考察了催化剂停留时间、装填量以及催化剂反应器形状对裂解过程的影响。结果表明，当脱除焦油的反应器高径比为1.0，全部填充催化剂时，出口焦油浓度可在4~6s内降为0，且合成气中H₂浓度为0.032kg/m³，CO浓度为0.50kg/m³。

关键词: 有机固废, 生物质半焦, 焦油, 动力学, 数值模拟

CLC Number:

TQ524

SONG Ye, CHEN Yuzhuo, SONG Yuncai, FENG Jie. Catalyst design and reactor analysis for in-situ purification of organic solid waste syngas[J]. Chemical Industry and Engineering Progress, 2023, 42(3): 1383-1396.

宋叶, 陈玉卓, 宋云彩, 冯杰. 有机固废合成气原位净化催化剂设计及反应器分析[J]. 化工进展, 2023, 42(3): 1383-1396.

Figures/Tables 27

原料	C	H	O	N	S
核桃壳	51.36	6.16	41.94	0.50	0.05
玉米芯	46.76	4.17	48.45	0.55	0.06
水稻秸秆	39.22	5.27	53.66	1.14	0.71

方程类别	方程
能量守恒方程^[14]	$ρ c p e f f ∂ T ∂ t ︸ a c c u m u l a t i o n t e r m + ρ c p g, m i x u ⋅ ∇ T ︸ c o n v e c t i v e t e r m + ∇ ⋅ - k e f f ∇ T ︸ c o n d u c t i v e t e r m = Q t o t ︸ s o u r c e t e r m$
热源Q_tot	$Q t o t = - ∑ i = 1 7 r i Δ H i$
有效比热容(ρc_p )_eff	$ρ c p e f f = 1 - η c p, C ρ C + η ρ c p g, m i x$
热导率k_eff	$k e f f = 1 - η k C + η k g, m i x$
反应器内的动量传递守恒方程^[15]	$1 η × ρ × ∂ u ∂ t + 1 η × ρ u ⋅ ∇ u × 1 η =$ $∇ ⋅ - p I + K - μ κ - 1 + β ρ u + Q m η 2 u$
催化剂床层内的动量传递守恒方程	$∂ ε ρ g, m i x ∂ t + ∇ ⋅ ρ g, m i x u = Q m$
黏性应力张量K^[16]	$K = μ × 1 η ∇ u + ∇ u T - 23 μ × 1 η ∇ ⋅ u I$
气体流速u^[17-18]	$u = - κ μ g, m i x$
理想气体状态方程^[18]	$ρ g, m i x = ∑ i = 1 n y i M i T 0 p 22.4 L / m o l × T p 0$ , $p = ρ g, m i x R T M g, m i x$ ， $M g, m i x = ∑ i ρ i ρ g, m i x M i - 1$
多孔基体的渗透率κ^[19]	$κ = κ 0 η η 0 3.55$
质量传递控制方程^[20]	$∂ η ρ g, m i x ω i ∂ t ︸ a c c u m u l a t i o n t e r m + ρ (u ⋅ ∇) ω i ︸ c o n v e c t i v e t e r m + ∇ ⋅ J i ︸ d i f f u s i v e t e r m = R i ︸ s o u r c e t e r m$
扩散通量J_i^[21]	$J i = - ρ g, m i x D i j ∇ ω i$
二元扩散系数D_ij^[22]	$D i j = 0.0101 T 1.75 1 M i + 1 M j 12 p ∑ v i 13 + ∑ v j 13 2$
床层压降∆p^[23]	$Δ p = f L u 02 ρ 1 - η d s η 3$
摩擦系数f	$f = 150 R e + 1.75$
雷诺数Re^[24]	$R e = d ρ g, m i x u μ g, m i x × 1 1 - η$

方程类别	方程
能量守恒方程^[14]	$ρ c p e f f ∂ T ∂ t ︸ a c c u m u l a t i o n t e r m + ρ c p g, m i x u ⋅ ∇ T ︸ c o n v e c t i v e t e r m + ∇ ⋅ - k e f f ∇ T ︸ c o n d u c t i v e t e r m = Q t o t ︸ s o u r c e t e r m$
热源Q_tot	$Q t o t = - ∑ i = 1 7 r i Δ H i$
有效比热容(ρc_p )_eff	$ρ c p e f f = 1 - η c p, C ρ C + η ρ c p g, m i x$
热导率k_eff	$k e f f = 1 - η k C + η k g, m i x$
反应器内的动量传递守恒方程^[15]	$1 η × ρ × ∂ u ∂ t + 1 η × ρ u ⋅ ∇ u × 1 η =$ $∇ ⋅ - p I + K - μ κ - 1 + β ρ u + Q m η 2 u$
催化剂床层内的动量传递守恒方程	$∂ ε ρ g, m i x ∂ t + ∇ ⋅ ρ g, m i x u = Q m$
黏性应力张量K^[16]	$K = μ × 1 η ∇ u + ∇ u T - 23 μ × 1 η ∇ ⋅ u I$
气体流速u^[17-18]	$u = - κ μ g, m i x$
理想气体状态方程^[18]	$ρ g, m i x = ∑ i = 1 n y i M i T 0 p 22.4 L / m o l × T p 0$ , $p = ρ g, m i x R T M g, m i x$ ， $M g, m i x = ∑ i ρ i ρ g, m i x M i - 1$
多孔基体的渗透率κ^[19]	$κ = κ 0 η η 0 3.55$
质量传递控制方程^[20]	$∂ η ρ g, m i x ω i ∂ t ︸ a c c u m u l a t i o n t e r m + ρ (u ⋅ ∇) ω i ︸ c o n v e c t i v e t e r m + ∇ ⋅ J i ︸ d i f f u s i v e t e r m = R i ︸ s o u r c e t e r m$
扩散通量J_i^[21]	$J i = - ρ g, m i x D i j ∇ ω i$
二元扩散系数D_ij^[22]	$D i j = 0.0101 T 1.75 1 M i + 1 M j 12 p ∑ v i 13 + ∑ v j 13 2$
床层压降∆p^[23]	$Δ p = f L u 02 ρ 1 - η d s η 3$
摩擦系数f	$f = 150 R e + 1.75$
雷诺数Re^[24]	$R e = d ρ g, m i x u μ g, m i x × 1 1 - η$

原料	比表面积/m²·g^-1	总孔容/cm³·g^-1
WS-CB-Cat	196.4	0.145
CC-CB-Cat	90.3	0.038
RS-CB-Cat	108.1	0.046

催化剂

比表面积

/m²·g^-1

总孔容

/cm³·g^-1

中孔孔容

/cm³·g^-1

微孔孔容

/cm³·g^-1

比表面积

/m²·g^-1

中孔比表面积

/m²·g^-1

微孔孔容

/cm³·g^-1

中孔孔容

/cm³·g^-1

总孔孔容

/cm³·g^-1

WS-H₂O

样品名称	I_D/I_G	I(_Gr+Vl+Vr)/I_D	L_a	L_c	d₀₀₂
WS-RAW	0.7513	0.3441	3.5361	1.5469	0.3892
WS-KOH	0.9524	0.3375	3.9676	1.1225	0.3731
WS-H₂O	0.8190	0.3883	5.2651	1.6774	0.3749

样品名称	EDS分析（质量分数）/%			元素分析（daf）/%
样品名称	C	O	O/C摩尔比	C	O	O/C
WS-RAW	85.74	13.33	0.16	92.16	6.13	0.07
WS-KOH	88.56	11.10	0.13	87.70	10.52	0.12
WS-H₂O	78.41	14.50	0.18	83.35	14.66	0.18

样品名称	C $̿$ C/C—H _x /C—C	C—O	C $̿$ O	O—C $̿$ O
WS-RAW	59.02	23.49	8.56	8.94
WS-KOH	42.66	29.18	14.92	13.25
WS-H₂O	40.92	37.67	12.24	9.16

样品名称	C $̿$ C/C—H _x /C—C	C—O	C $̿$ O	O—C $̿$ O
WS-RAW	59.02	23.49	8.56	8.94
WS-KOH	42.66	29.18	14.92	13.25
WS-H₂O	40.92	37.67	12.24	9.16

样品名称	晶格氧	氧缺陷	吸附氧
WS-RAW	96.22	2.56	1.22
WS-KOH	44.64	27.22	28.14
WS-H₂O	77.98	4.49	17.54

催化剂	ξ	a
WS-RAW	13.08	$a (t) W S - R A W = 1.65 - 1.43 × 1 - e x p - t 1.83 - 0.07 × 1 - e x p - t 33.23$
WS-KOH	210.85	$a (t) W S - K O H = 0.19 + 1.21 1 + e x p t - 13.78 17.33$
WS-H₂O	136.57	$a (t) W S - H 2 O = 1.04 - 0.10 × 1 - e x p - t 80.67 - 0.83 × 1 - e x p - t 6.35$

催化剂	ξ	a
WS-RAW	13.08	$a (t) W S - R A W = 1.65 - 1.43 × 1 - e x p - t 1.83 - 0.07 × 1 - e x p - t 33.23$
WS-KOH	210.85	$a (t) W S - K O H = 0.19 + 1.21 1 + e x p t - 13.78 17.33$
WS-H₂O	136.57	$a (t) W S - H 2 O = 1.04 - 0.10 × 1 - e x p - t 80.67 - 0.83 × 1 - e x p - t 6.35$

物性参数	数值
比热容	(c_p )_g,mix=1390J/(kg·K)；(c_p )_cat=470J/(kg·K)
热导率	k_g,mix=0.08W/(m·K)；k_cat=37.2W/(m·K)
密度	ρ_g,mix=1.05kg/m³；ρ_cat=400kg/m³
黏度	μ_g,mix=1.99×10^-4Pa·s

反应方程式	∆H/kJ·mol^-1	反应速率表达式
C₇H₈ $→$ 7C+4H₂	-50.0	$r 1 = 1.03 × 1013 e x p - 324500 R T C C 7 H 8$
C+2H₂ $→$ CH₄	-74.6	$r 2 = 3.18 × 102 e x p - 237400 R T C H 2$
C₇H₈+10.5H₂O $→$ 3.5CO+3.5CO₂+14.5H₂	725.0	$r 3 = 1.0 × 108 e x p - 100000 R T C C 7 H 8$
CO+H₂O CO₂+H₂	-41.2	$r 4 = k f C C O C H 2 O - k b C C O 2 C H 2$ , $k f = 2.79 × 102 e x p - 12560 R T$ , $k b = 1.26 × 104 e x p - 47290 R T$
CO₂+C $→$ 2CO	-172.4	$r 5 = 1.18 × 107 e x p - 245000 R T C C O 2$
CH₄+H₂O $→$ CO+3H₂	205.9	$r 6 = 3.10 × 103 e x p - 124700 R T C C H 4 C H 2 O$
C+H₂O $→$ CO+H₂	131.3	$r 7 = 3.6 × 1012 e x p - 310000 R T C C C H 2 O$

反应方程式	∆H/kJ·mol^-1	反应速率表达式
C₇H₈ $→$ 7C+4H₂	-50.0	$r 1 = 1.03 × 1013 e x p - 324500 R T C C 7 H 8$
C+2H₂ $→$ CH₄	-74.6	$r 2 = 3.18 × 102 e x p - 237400 R T C H 2$
C₇H₈+10.5H₂O $→$ 3.5CO+3.5CO₂+14.5H₂	725.0	$r 3 = 1.0 × 108 e x p - 100000 R T C C 7 H 8$
CO+H₂O CO₂+H₂	-41.2	$r 4 = k f C C O C H 2 O - k b C C O 2 C H 2$ , $k f = 2.79 × 102 e x p - 12560 R T$ , $k b = 1.26 × 104 e x p - 47290 R T$
CO₂+C $→$ 2CO	-172.4	$r 5 = 1.18 × 107 e x p - 245000 R T C C O 2$
CH₄+H₂O $→$ CO+3H₂	205.9	$r 6 = 3.10 × 103 e x p - 124700 R T C C H 4 C H 2 O$
C+H₂O $→$ CO+H₂	131.3	$r 7 = 3.6 × 1012 e x p - 310000 R T C C C H 2 O$

网格类型	单元数	相同条件下出口焦油浓度为0的时间/s
较细化	723359	11
常规	80855	11
较粗化	16238	11

项目	d₁/m	h₁/m	h₂/m	h₃/m	高径比	停留时间/s
Case1	0.06	0.12	0.18	0.02	5.00	0.67
Case2	0.08	0.03	0.14	0.02	2.10	1
Case3	0.10	0.02	0.09	0.01	1.08	4

项目	d₁/m	h₁/m	催化剂床层压降/Pa	停留时间/s
Case4	0.10	0.02	2301.18	0.67
Case5	0.10	0.08	9204.73	2.67
Case6	0.10	0.11	12656.50	3.60

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