C1气体环境下Ga改性ZSM-5催化剂上塑料废弃物热解制芳烃的性能优化

doi:10.1016/S1872-2067(25)64683-3

催化学报 ›› 2025, Vol. 73: 368-383.DOI: 10.1016/S1872-2067(25)64683-3

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C1气体环境下Ga改性ZSM-5催化剂上塑料废弃物热解制芳烃的性能优化

Haneul Shim^a^,¹, Sumin Pyo^b^,¹, Avnish Kumar^a, Yasin Khani^a, Siyoung Q. Choi^b, Kanghee Cho^c, Jechan Lee^d, Young-Kwon Park^a()

^a首尔大学环境工程学院, 首尔, 韩国
^b韩国科学技术院(KAIST)化学与生物分子工程系, 大田, 韩国
^c仁荷大学化学与化学工程系, 仁川, 韩国
^d成均馆大学土木建筑工程与景观设计学院, 全球智慧城市系, 水原, 韩国

收稿日期:2025-01-07 接受日期:2025-03-21 出版日期:2025-06-18 发布日期:2025-06-12
通讯作者: *电子信箱: catalica@uos.ac.kr (Y.-K. Park).
作者简介:¹共同第一作者.

Improvement in the production of aromatics from pyrolysis of plastic waste over Ga-modified ZSM-5 catalyst under C1-gas environment

Haneul Shim^a^,¹, Sumin Pyo^b^,¹, Avnish Kumar^a, Yasin Khani^a, Siyoung Q. Choi^b, Kanghee Cho^c, Jechan Lee^d, Young-Kwon Park^a()

^aSchool of Environmental Engineering, University of Seoul, Seoul 02504, Republic of Korea
^bDepartment of Chemical and Biomolecular Engineering, Korea Advanced Institute of Science and Technology (KAIST), Daejeon 34141, Republic of Korea
^cDepartment of Chemistry and Chemical Engineering, Inha University, 100 Inha-ro, Michuhol-gu, Incheon 22212, Republic of Korea
^dDepartment of Global Smart City & School of Civil, Architectural Engineering, and Landscape Architecture, Sungkyunkwan University, Suwon 16419, Republic of Korea

Received:2025-01-07 Accepted:2025-03-21 Online:2025-06-18 Published:2025-06-12
Contact: *E-mail: catalica@uos.ac.kr (Y.-K. Park).
About author:¹ Contributed equally to this work.

摘要/Abstract

摘要： 本文系统研究了甲烷(CH₄)、二氧化碳(CO₂)和沼气(CH₄+CO₂)等C1气体对镓(Ga)改性ZSM-5催化剂催化热解聚塑料废弃物(聚丙烯)生成芳香烃的影响. 通过浸渍结合还原-氧化工艺制备了不同Ga负载量(0.5 wt%, 1 wt%, 3 wt%和5 wt%)的RO-GHZ催化剂, 结果表明: 在CH₄气氛下, RO-GHZ(1)催化剂的BTEX(苯、甲苯、二甲苯和乙苯)产率最高(39.5 wt%). 相较于GHZ(1), 还原-氧化处理使Ga颗粒尺寸显著减小并扩散至ZSM-5孔道内, 形成高活性GaO⁺离子物种, 平衡了Lewis/Brönsted酸比例, 从而加速了芳构化反应. 进一步研究发现, RO-GHZ催化剂中Ga负载量增加会降低活性GaO⁺浓度, 导致BTEX产率下降. 值得注意的是, CO₂对RO-GHZ(1)的抑制作用使其在沼气及纯CO₂条件下的BTEX产率降低, 而GHZ(1)在CO₂条件下则表现出最高产率. 同时, CO₂与沼气体系通过焦炭部分氧化显著减少催化剂积碳. 该研究证实CH₄与CO₂等可持续C1气体可协同实现废塑料高效热解制备高值BTEX, 为绿色资源化提供了新思路.

关键词: 聚丙烯, 热解, Ga负载HZSM-5, 甲烷, 还原-氧化

Abstract:

This study explores, for the first time, the influence of various C1 gases, such as methane (CH₄), carbon dioxide (CO₂), and biogas (CH₄ + CO₂), on catalytic pyrolysis of plastic waste (polypropylene) to evaluate their potential in producing aromatic hydrocarbons. Also, this study used the 0.5 wt%, 1 wt%, 3 wt%, and 5 wt% Ga-modified ZSM-5 catalyst and its reduction-oxidation processed catalysts owing to their promising catalytic properties. According to the results, the highest yield (39.5 wt%) of BTEX (benzene, toluene, xylene, and ethylbenzene) was achieved under CH₄ over RO-GHZ(1) catalyst among all tested conditions. The reduction-oxidation process not only promotes a significant reduction of the Ga-size but also induces its diffusion inside the pore, compared to GHZ(1). This leads to the formation of highly active GaO⁺ ionic species, balancing the Lewis/Brönsted ratio, thereby accelerating the aromatization reaction. The effect of Ga loading on the RO-GHZ catalyst was also evaluated systematically, which showed a negative impact on the BTEX yield owing to the lowering in the concentration of active GaO⁺ species. A detailed catalyst characterization supports the experimental results well.

Key words: Polypropylene, Pyrolysis, Ga-loaded HZSM-5, Methane, Reduction-oxidation

Haneul Shim, Sumin Pyo, Avnish Kumar, Yasin Khani, Siyoung Q. Choi, Kanghee Cho, Jechan Lee, Young-Kwon Park. C1气体环境下Ga改性ZSM-5催化剂上塑料废弃物热解制芳烃的性能优化[J]. 催化学报, 2025, 73: 368-383.

Haneul Shim, Sumin Pyo, Avnish Kumar, Yasin Khani, Siyoung Q. Choi, Kanghee Cho, Jechan Lee, Young-Kwon Park. Improvement in the production of aromatics from pyrolysis of plastic waste over Ga-modified ZSM-5 catalyst under C1-gas environment[J]. Chinese Journal of Catalysis, 2025, 73: 368-383.

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Sample	S_BET (m²/g)	S_Micro (m²/g)	S_External (m²/g)	Pore volume (cm³/g)	Micropore volume (cm³/g)
HZ	410	375	35	0.32	0.177
GHZ(1)	389	350	39	0.31	0.165
RO-GHZ(1)	406	371	35	0.32	0.176
RO-GHZ(3)	403	363	40	0.34	0.171
RO-GHZ(5)	383	350	33	0.31	0.161

Sample	S_BET (m²/g)	S_Micro (m²/g)	S_External (m²/g)	Pore volume (cm³/g)	Micropore volume (cm³/g)
HZ	410	375	35	0.32	0.177
GHZ(1)	389	350	39	0.31	0.165
RO-GHZ(1)	406	371	35	0.32	0.176
RO-GHZ(3)	403	363	40	0.34	0.171
RO-GHZ(5)	383	350	33	0.31	0.161

Catalyst	Acidity (mmol/g)
Catalyst	Weak and medium	Strong	Total
HZ	0.67	0.308	0.978
GHZ(1)	0.673	0.23	0.903
RO-GHZ(1)	0.692	0.269	0.961
RO-GHZ(3)	0.707	0.241	0.948
RO-GHZ(5)	0.72	0.209	0.929

Catalyst	Acidity (mmol/g)
Catalyst	Weak and medium	Strong	Total
HZ	0.67	0.308	0.978
GHZ(1)	0.673	0.23	0.903
RO-GHZ(1)	0.692	0.269	0.961
RO-GHZ(3)	0.707	0.241	0.948
RO-GHZ(5)	0.72	0.209	0.929

Catalysts	N₂	CH₄	Biogas	CO₂
HZ	0.443	0.547	0.383	-
GHZ(1)	0.415	0.455	0.375	0.414
RO-GHZ(1)	0.439	0.576	0.383	0.381

C1气体环境下Ga改性ZSM-5催化剂上塑料废弃物热解制芳烃的性能优化

Improvement in the production of aromatics from pyrolysis of plastic waste over Ga-modified ZSM-5 catalyst under C1-gas environment

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Metrics

Catalyst	HZ			GHZ(1)			RO-GHZ(1)
Atmosphere	N₂	CH₄	Biogas	N₂	CH₄	Biogas	N₂	CH₄	Biogas
C₂H₄/C₂H₆	1.99	1.61	1.98	2.09	2.64	1.80	1.96	1.80	1.85
C₃H₆/C₃H₈	0.76	0.60	0.62	1.20	1.26	0.75	0.97	0.91	0.90

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	HZ (Vol%)			GHZ(1) (Vol%)				RO-GHZ(1) ( Vol%)				RO-GHZ(3) ( Vol%)		RO-GHZ(5) ( Vol%)
	N₂	CH₄	BG	N₂	CH₄	BG	CO₂	N₂	CH₄	BG	CO₂	CH₄	BG	CH₄	BG
H₂	8.0	8.0	4.7	26.4	15.0	17.2	22.5	21.8	30.7	21.9	14.9	25.9	21.0	26.9	20.1
CO	0.0	0.0	0.4	0.0	0.0	0.8	1.7	0.0	0.7	1.7	1.2	0.4	1.7	0.2	1.2
CH₄	8.6	22.7	19.2	7.4	20.7	18.2	7.6	6.8	20.9	19.5	4.5	23.4	19.6	23.2	20.4
CO₂	0.0	0.0	9.1	0.0	0.0	7.4	22.6	0.0	0.0	7.5	31.2	0.0	8.7	0.0	9.7
Ethane	7.3	6.8	4.5	4.9	3.3	4.1	4.3	4.4	4.6	3.7	2.5	4.0	3.0	3.6	2.9
Ethene	14.6	11.0	8.9	10.3	8.7	7.3	7.4	8.7	8.3	6.9	5.8	7.8	6.2	7.5	6.3
Propane	23.3	21.3	20.1	13.2	12.1	14.7	11.1	15.6	11.1	11.2	9.9	8.3	8.0	8.1	6.6
Propene	17.7	12.8	12.4	15.8	15.3	11.1	9.6	15.2	10.1	10.1	11.0	12.6	11.9	11.9	12.8
Isobutane	5.6	4.9	7.0	5.5	7.4	6.4	3.5	9.1	3.6	5.0	5.8	4.1	5.0	5.1	4.7
Butane	3.5	3.0	3.6	3.0	3.4	3.3	2.1	4.0	2.2	2.6	2.6	2.1	2.3	2.4	2.0
t-2-butene	1.7	1.3	1.4	1.8	2.0	1.3	1.0	2.0	0.9	1.2	1.4	1.6	1.8	1.5	1.9
1-butene	1.4	1.1	1.1	1.5	1.6	1.0	0.8	1.5	0.8	1.0	1.1	1.2	1.3	1.2	1.4
isobutylene	3.2	2.5	2.8	3.6	4.1	2.5	1.9	4.1	1.9	2.7	3.2	3.4	3.8	3.1	4.1
c-2-butene	1.2	0.9	1.0	1.3	1.4	0.9	0.7	1.4	0.7	0.9	1.0	1.1	1.2	1.0	1.3
>C5	3.9	3.7	3.8	5.3	5.0	3.7	3.4	5.5	3.6	4.1	3.8	4.2	4.4	4.3	4.5
Total	100	100	100	100	100	100	100	100	100	100	100	100	100	100	100

	HZ (Vol%)			GHZ(1) (Vol%)				RO-GHZ(1) ( Vol%)				RO-GHZ(3) ( Vol%)		RO-GHZ(5) ( Vol%)
	N₂	CH₄	BG	N₂	CH₄	BG	CO₂	N₂	CH₄	BG	CO₂	CH₄	BG	CH₄	BG
H₂	8.0	8.0	4.7	26.4	15.0	17.2	22.5	21.8	30.7	21.9	14.9	25.9	21.0	26.9	20.1
CO	0.0	0.0	0.4	0.0	0.0	0.8	1.7	0.0	0.7	1.7	1.2	0.4	1.7	0.2	1.2
CH₄	8.6	22.7	19.2	7.4	20.7	18.2	7.6	6.8	20.9	19.5	4.5	23.4	19.6	23.2	20.4
CO₂	0.0	0.0	9.1	0.0	0.0	7.4	22.6	0.0	0.0	7.5	31.2	0.0	8.7	0.0	9.7
Ethane	7.3	6.8	4.5	4.9	3.3	4.1	4.3	4.4	4.6	3.7	2.5	4.0	3.0	3.6	2.9
Ethene	14.6	11.0	8.9	10.3	8.7	7.3	7.4	8.7	8.3	6.9	5.8	7.8	6.2	7.5	6.3
Propane	23.3	21.3	20.1	13.2	12.1	14.7	11.1	15.6	11.1	11.2	9.9	8.3	8.0	8.1	6.6
Propene	17.7	12.8	12.4	15.8	15.3	11.1	9.6	15.2	10.1	10.1	11.0	12.6	11.9	11.9	12.8
Isobutane	5.6	4.9	7.0	5.5	7.4	6.4	3.5	9.1	3.6	5.0	5.8	4.1	5.0	5.1	4.7
Butane	3.5	3.0	3.6	3.0	3.4	3.3	2.1	4.0	2.2	2.6	2.6	2.1	2.3	2.4	2.0
t-2-butene	1.7	1.3	1.4	1.8	2.0	1.3	1.0	2.0	0.9	1.2	1.4	1.6	1.8	1.5	1.9
1-butene	1.4	1.1	1.1	1.5	1.6	1.0	0.8	1.5	0.8	1.0	1.1	1.2	1.3	1.2	1.4
isobutylene	3.2	2.5	2.8	3.6	4.1	2.5	1.9	4.1	1.9	2.7	3.2	3.4	3.8	3.1	4.1
c-2-butene	1.2	0.9	1.0	1.3	1.4	0.9	0.7	1.4	0.7	0.9	1.0	1.1	1.2	1.0	1.3
>C5	3.9	3.7	3.8	5.3	5.0	3.7	3.4	5.5	3.6	4.1	3.8	4.2	4.4	4.3	4.5
Total	100	100	100	100	100	100	100	100	100	100	100	100	100	100	100