Mechanism and engineering technology development of hydrocarbons pyrolysis to produce carbon black

doi:10.16085/j.issn.1000-6613.2023-2295

Abstract

Abstract:

Introduction to the history of human manufacturing and utilization of carbon black (CB) as well as the characteristics of CB, this paper simulated and calculated a series of parameters related to the formation of quasi graphite microcrystals (GMCs) and the final formation of CB particles during the process of hydrocarbon pyrolysis, where carbon atoms formed a six carbon ring and undergo one-dimensional (1D), two-dimensional (2D) and three-dimensional (3D) growth. The latest achievements for the growth mechanism of quasi graphite microcrystals in CB and basic research on particle structure as well as its relationship with properties such as particle hardness and conductivity were introduced. Based on the research results of carbon atomic structure and basic physicochemical properties in CB, the molecular formula of CB was proposed. The structural reasons why CB had a hardness of up to 30GPa, the activity of reinforcing rubber and unique conductivity were interpreted based on testing data. This article also calculated the chemical reaction heat of several typical hydrocarbons used to produce CB through thermal cracking from the perspective of bond energy changes. It explained the reason why the yield of coal-based feedstock oil was 10% higher than that of petroleum based-feedstock oil during CB production. The article focused on introducing the engineering technology of modern hydrocarbons pyrolysis to produce CB in terms of raw materials, reactors, refractory materials, large-scale equipment, comprehensive resource utilization technology with equipment achieved and the development process of China becoming the largest country in CB manufacturing. This article summarized the latest requirements for energy conservation and environmental protection in the CB industry, looked forward to the future of the industry, and put forward suggestions for the key directions and research content of its technological progress.

Key words: hydrocarbons, pyrolysis, carbon black, particle, aggregation, microscopic structure

摘要：

简介人类制造和利用炭黑（CB）的历史和炭黑特性，对烃热解过程中碳原子组成六碳环并历经一维（1D）、二维（2D）和三维（3D）增长形成准石墨微晶（GMC）和最终形成CB粒子的系列参数进行了模拟计算，总结有关CB准石墨微晶结构增长机理、粒子结构及其与粒子硬度和导电性等性能间的关系等方面基础研究的最新成果。基于CB中碳原子结构研究成果和基本理化性能，建议了CB的分子式。结合检测数据解读CB拥有高达30GPa硬度、补强橡胶的活性和独特导电性的结构原因。本文还从键能变化角度计算了用于制造CB的几种典型烃热裂解生成CB的化学反应热，解释CB生产时煤系原料油比石油系原料油收率高10%的原因，重点介绍现代热裂解烃制造CB的工程化技术在原料、反应器、耐火材料、装置大型化、资源综合利用技术与装备等方面取得突破并促成我国成为炭黑制造第一大国的发展历程。对炭黑行业节能环保的最新要求进行了归纳，展望了行业未来，并对其技术进步重点方向和研究内容提出建议。

关键词: 烃类化合物, 热解, 炭黑, 粒子, 聚集, 显微结构

CLC Number:

TQ-9

WANG Dingyou, CHEN Jian, FAN Ruxin, LI Dashun. Mechanism and engineering technology development of hydrocarbons pyrolysis to produce carbon black[J]. Chemical Industry and Engineering Progress, 2024, 43(7): 3551-3566.

王定友, 陈建, 范汝新, 李大舜. 热裂解烃制炭黑的机理及工程化技术发展历程[J]. 化工进展, 2024, 43(7): 3551-3566.

Figures/Tables 20

项目	炭黑品种
项目	N115	N330	N550	N660
表面硬度/GPa
1	23.74	53.98	33.96	26.23
2	18.65	27.54	16.16	52.1
3	13.84	14.98	45.15	19.73
4	32.77	16.29	42.44	51.87
5	37.98	39.74	11.39	61.42
6	15.42	34.48	54.4	44.15
7	45.56	15.99	45.99	42.16
8	13.61	41.34	19.48	40.62
均值	25.2	30.5	33.6	42.3
粒径/nm	10~19	26~30	40~48	49~60

n	r_1ec
1	0.80
2	0.71
3	0.67
4	0.64
5	0.62
6	0.60
7	0.59
8	0.58
9	0.57
10	0.57

n	L_n /nm	r_2ec/%	n	L_n /nm	r_2ec/%
1	0.50	66.9	11	3.0	14.6
2	0.74	49.3	12	3.2	13.6
3	1.0	39.0	13	3.5	12.6
4	1.2	32.3	14	3.7	11.8
5	1.5	27.5	15	4.0	11.1
6	1.7	24.0	16	4.2	10.5
7	2.0	21.3	17	4.5	9.9
8	2.2	19.1	18	4.7	9.4
9	2.5	17.3	19	5.0	9.0
10	2.7	15.9	20	5.2	8.6

n	p	t	L_n /nm	N_3c/个	V₃/nm³	N_3cu/个·nm^-3
1	0	1	0.50	22	0.117	187
2	1	2	0.74	64	0.368	174
3	2	3	0.99	141	0.868	162
4	2	4	1.24	262	1.71	153
5	3	4	1.49	438	2.98	147
6	3	5	1.73	679	4.78	142
7	4	6	1.98	996	7.18	139
8	5	7	2.23	1398	10.3	136
9	5	7	2.48	1896	14.2	133
10	6	8	2.72	2500	19.0	132
11	6	9	2.97	3221	24.8	130
12	7	10	3.22	4068	31.6	129
13	7	10	3.47	5052	39.7	127
14	8	11	3.72	6183	48.9	126
15	9	12	3.96	7471	59.5	126
16	9	13	4.21	8927	71.5	125
17	10	13	4.46	10561	85.1	124
18	10	14	4.71	12383	100	124
19	11	15	4.95	14403	117	123
20	11	16	5.20	16632	136	122

n	N_GMC	n	N_GMC
1	35802	11	169
2	11383	12	133
3	4826	13	106
4	2450	14	86
5	1406	15	70
6	876	16	59
7	583	17	49
8	407	18	42
9	295	19	36
10	220	20	31

R_b/nm	$r R b e c$ /%
5	52.0
10	25.2
20	12.4
30	8.2
40	6.1
50	4.9
60	4.1
70	3.5
80	3.1
90	2.7
100	2.4

R_b/nm	$r R b e c$ /%
5	52.0
10	25.2
20	12.4
30	8.2
40	6.1
50	4.9
60	4.1
70	3.5
80	3.1
90	2.7
100	2.4

项目	沥青	蒽	萘	乙炔	煤焦油	乙烯焦油	催化裂化油浆	乙烯	乙烷	甲烷
C/%	83~87	94.38	93.75	92.31	91.86	91.6	—	85.7	80.0	75
H/C	1.41	0.71	0.80	1.00	0.71	0.88	1.22	2.00	3.00	4.00

化学键	键能/kJ·mol^-1
C—C	332
C $̿$ C	611
C≡≡ C	837
C—H	414
H—H	436

化学键	键能/kJ·mol^-1
C—C	332
C $̿$ C	611
C≡≡ C	837
C—H	414
H—H	436

序号	烃品种	化学反应式	键能/kJ			反应热（以C计）/kJ·mol^-1
序号	烃品种	化学反应式	反应物	产物	E_△	反应热（以C计）/kJ·mol^-1
1	甲烷	6CH₄→C₆+12H₂	9936	9057	-879	-146.5
2	乙烷	3C₂H₆→C₆+9H₂	8448	7749	-699	-116.5
3	乙烯	3C₂H₄→C₆+6H₂	6801	6441	-360	-60.0
4	萘	C₁₀H₈→C₁₀+4H₂	9687	9447	-240	-24.0
5	蒽油	C₁₄H₁₀→C₁₄+5H₂	13065	12765	-300	-21.4
6	乙炔	3C₂H₂→C₆+3H₂	4995	5133	138	23.0

序号	烃种类	能耗	CB产品
序号	烃种类	能耗	产量占比	性能特点	主要用途
1	天然气	高	1%	粒径80~170nm，结构简单，品种单一	填充橡胶并赋予其高伸长率和低硬度，高纯碳源
2	乙炔	低	1%	粒径35~45nm，品种较单一，吸液量大，电阻率较低	在电池、橡塑制品中广泛使用，作工作液保持剂和导电、抗静电、导热、吸波等材料用
3	矿物油	中	98%	粒径10~300nm，品种丰富	橡胶制品（轮胎及管、板、带等）补强、填充、导电剂，高分子材料（塑料、树脂、纤维）等增强与改性剂（抗紫外线老化）、油漆油墨造纸着色剂、特种陶瓷造孔剂等
4	废旧轮胎	较低	5%	—	橡胶制品（轮胎及管、板、带等）补强、填充剂等

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