基于社区发现算法的复杂网络关键反应路线提取

doi:10.16085/j.issn.1000-6613.2022-1409

摘要/Abstract

摘要：

在分子自由基尺寸上对化工过程建立准确的机理过程模型，是目前世界“分子炼油”发展的重要方向。分子炼油过程体系的复杂性主要来源于化学反应网络的耦合性和多尺度性，这对深入了解化工生产过程提出了挑战。对复杂化学反应网络进行关键信息挖掘与表达，有助于工程师深入理解化学反应过程机理，实现机理透明化。由于炼油炼化过程的复杂反应网络存在以关键反应物质为中心的模块化、社区化特征，本文采用Leiden社区发现算法，从介尺度上对蒸汽热裂解制乙烯的反应网络进行反应社区划分，并基于分子自由基尺度从简化后的反应社区提取出对应的关键反应路线，为宏观反应网络到微观物质的相互作用提供一种可解释性的桥梁，助力揭示物质转化过程的知识传递机制。

关键词: 反应, 网络, 算法, 介尺度, 社区发现, 反应路线

Abstract:

The development of accurate mechanistic process models of processes at the molecular radical scale is an important direction in the development of "molecular refining" in the world. The complexity of molecular refining process systems is mainly due to the coupling and multiscale of chemical reaction networks, which poses a challenge to the in-depth understanding of chemical production processes. The key information mining and representation of the complex reaction network can help engineers to understand the process mechanism in depth and realize the transparency of the mechanism. Since the complex reaction networks of oil refining processes have modular and community-based characteristics centered on key reaction substances, this paper adopted the Leiden community detection algorithm to divide the reaction networks of steam cracking into reaction communities at mesoscale. The corresponding key reaction pathways were extracted from the reduced reaction communities at the molecular free radical scale. It provided an interpretable bridge from macroscopic reaction networks to microscopic substance interactions and helped to reveal the knowledge transfer mechanism of the substance transformation process.

Key words: reaction, network, algorithm, mesoscale, community detection, reaction pathway

中图分类号:

TQ037

陈土杰, 毕可鑫, 邱彤, 吉旭, 戴一阳. 基于社区发现算法的复杂网络关键反应路线提取[J]. 化工进展, 2023, 42(2): 684-691.

CHEN Tujie, BI Kexin, QIU Tong, JI Xu, DAI Yiyang. Extraction of important reaction pathways for complex reaction network based on community detection algorithm[J]. Chemical Industry and Engineering Progress, 2023, 42(2): 684-691.

图/表 8

参考文献 32

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类别	示例反应	数量	指前因子/s^-1	活化能/kcal·mol^-1
0	H•+NC₃H₇•→C₃H₈	2189	—	—
1	NC₆H₁₄→2 NC₃H₇	110	2×10¹¹	11.2
2	C₂H₅CYC₆H₁₁→CYC₆CH₂•+CH₃•	28	5×10¹⁶	81
3	CH₂CHCH₂•+NC₅H₁₀→C₃H₆+C₄H₆+CH₃•	10	2×10¹¹	11
4	CH₃•+NC₅H₁₀→CH₄+C₄H₆+CH₃•	10	1×10¹¹	9.5
5	H•+C₂H₅CYC₆H₁₁→H₂+C₂H₄+CYC₆H₁₁•	98	3×10⁸	13.5
6	H•+IC₅H₁₂→H₂+C₂H₄+IC₃H₇•	154	2×10⁸	12.2
7	H•+IC₅H₁₂→H₂+IC₄H₈+CH₃•	154	1×10⁸	9
8	H•+NC₅H₁₀→H₂+C₄H₆+CH₃•	10	4.47×10⁶	5.2
9	H•+NC₅H₁₂→H₂+C₃H₆+C₂H₅•	574	4×10⁸	12.2
10	H•+NC₅H₁₂→H₂+C₄H₈+CH₃•	378	2×10⁸	12.2
11	IC₃H₇•+C₂H₅CYC₆H₁₁→C₃H₈+C₂H₄+CYC₆H₁₁•	56	3×10⁸	14.5
12	IC₃H₇•+IC₅H₁₂→C₃H₈+C₂H₄+IC₃H₇•	88	2×10⁸	12.2
13	IC₃H₇•+NC₅H₁₀→C₃H₈+C₄H₆+CH₃•	80	2×10¹¹	12.2
14	IC₃H₇•+NC₅H₁₂→C₃H₈+C₃H₆+C₂H₅•	328	4×10⁸	12.2
15	IC₃H₇•+NC₅H₁₂→C₃H₈+NC₄H₈+CH₃•	216	2×10⁸	12.2
16	IC₅H₁₂+IC₃H₇•→C₃H₈+IC₄H₈+CH₃•	88	1×10⁸	10
17	IC₅H₁₂→IC₃H₇•+C₂H₅•	41	5×10¹⁶	80
18	NC₅H₁₀→C₃H₆+C₂H₄	11	9.12×10¹²	15
19	NC₅H₁₀→CH₄+C₄H₆	8	9.12×10¹³	13
20	NC₆H₁₄→2C₃H₇•	5	5×10¹⁶	81
21	NC₅H₇ +NC₅H₁₀→C₅H₈+C₄H₆+ CH₃•	36	1×10¹⁷	81
22	NC₅H₁₀+C₁₀H₇•→CH₃•+C₁₀H₈+C₄H₆	22	1×10¹⁷	83.5

类别	示例反应	数量	指前因子/s^-1	活化能/kcal·mol^-1
0	H•+NC₃H₇•→C₃H₈	2189	—	—
1	NC₆H₁₄→2 NC₃H₇	110	2×10¹¹	11.2
2	C₂H₅CYC₆H₁₁→CYC₆CH₂•+CH₃•	28	5×10¹⁶	81
3	CH₂CHCH₂•+NC₅H₁₀→C₃H₆+C₄H₆+CH₃•	10	2×10¹¹	11
4	CH₃•+NC₅H₁₀→CH₄+C₄H₆+CH₃•	10	1×10¹¹	9.5
5	H•+C₂H₅CYC₆H₁₁→H₂+C₂H₄+CYC₆H₁₁•	98	3×10⁸	13.5
6	H•+IC₅H₁₂→H₂+C₂H₄+IC₃H₇•	154	2×10⁸	12.2
7	H•+IC₅H₁₂→H₂+IC₄H₈+CH₃•	154	1×10⁸	9
8	H•+NC₅H₁₀→H₂+C₄H₆+CH₃•	10	4.47×10⁶	5.2
9	H•+NC₅H₁₂→H₂+C₃H₆+C₂H₅•	574	4×10⁸	12.2
10	H•+NC₅H₁₂→H₂+C₄H₈+CH₃•	378	2×10⁸	12.2
11	IC₃H₇•+C₂H₅CYC₆H₁₁→C₃H₈+C₂H₄+CYC₆H₁₁•	56	3×10⁸	14.5
12	IC₃H₇•+IC₅H₁₂→C₃H₈+C₂H₄+IC₃H₇•	88	2×10⁸	12.2
13	IC₃H₇•+NC₅H₁₀→C₃H₈+C₄H₆+CH₃•	80	2×10¹¹	12.2
14	IC₃H₇•+NC₅H₁₂→C₃H₈+C₃H₆+C₂H₅•	328	4×10⁸	12.2
15	IC₃H₇•+NC₅H₁₂→C₃H₈+NC₄H₈+CH₃•	216	2×10⁸	12.2
16	IC₅H₁₂+IC₃H₇•→C₃H₈+IC₄H₈+CH₃•	88	1×10⁸	10
17	IC₅H₁₂→IC₃H₇•+C₂H₅•	41	5×10¹⁶	80
18	NC₅H₁₀→C₃H₆+C₂H₄	11	9.12×10¹²	15
19	NC₅H₁₀→CH₄+C₄H₆	8	9.12×10¹³	13
20	NC₆H₁₄→2C₃H₇•	5	5×10¹⁶	81
21	NC₅H₇ +NC₅H₁₀→C₅H₈+C₄H₆+ CH₃•	36	1×10¹⁷	81
22	NC₅H₁₀+C₁₀H₇•→CH₃•+C₁₀H₈+C₄H₆	22	1×10¹⁷	83.5

反应社区	未简化网络		简化网络		关键物质		特征
反应社区	节点	边	节点	边	起点	终点	特征
1	1816	5518	229	594	长链正构烷烃	C₂H₄	正烷烃裂解
2	271	503	47	69	环烷烃的取代物	环烷烃	环烷烃之间的相互转化
3	372	684	70	125	IC₄H₇·	2-C₄H₈	链终止反应1
4	1283	2762	282	626	苯	C₂H₂ C₄H₄	逆Diels-Alder反应；焦炭形成
5	582	1367	202	447	芳烃的取代物	C₇H₈	芳烃之间的相互转化
6	124	235	38	75	CH₃·	CH₄	链终止反应2
7	185	402	69	163	1-C₄H₈	C₄H₆	丁二烯形成
8	203	468	62	125	异构烷烃	C₃H₆	丙烯形成

反应社区	未简化网络		简化网络		关键物质		特征
反应社区	节点	边	节点	边	起点	终点	特征
1	1816	5518	229	594	长链正构烷烃	C₂H₄	正烷烃裂解
2	271	503	47	69	环烷烃的取代物	环烷烃	环烷烃之间的相互转化
3	372	684	70	125	IC₄H₇·	2-C₄H₈	链终止反应1
4	1283	2762	282	626	苯	C₂H₂ C₄H₄	逆Diels-Alder反应；焦炭形成
5	582	1367	202	447	芳烃的取代物	C₇H₈	芳烃之间的相互转化
6	124	235	38	75	CH₃·	CH₄	链终止反应2
7	185	402	69	163	1-C₄H₈	C₄H₆	丁二烯形成
8	203	468	62	125	异构烷烃	C₃H₆	丙烯形成

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