合理设计双功能催化剂用于聚乙烯废塑料加氢裂解制备较窄碳数分布的液体燃料

doi:10.1016/S1872-2067(25)64916-3

催化学报 ›› 2026, Vol. 82: 42-60.DOI: 10.1016/S1872-2067(25)64916-3

合理设计双功能催化剂用于聚乙烯废塑料加氢裂解制备较窄碳数分布的液体燃料

马哲^a, 王晨朝^a, 许朋^a, 周鑫^b^,^*(), 冯翔^a^,^*(), 陈德^a^,^c^,^*()

^a中国石油大学(华东)化学化工学院, 重质油全国重点实验室, 山东青岛 266580, 中国
^b中国海洋大学化学化工学院, 山东青岛 266100, 中国
^c挪威科技大学化学工程系, 特隆赫姆, 挪威

收稿日期:2025-10-03 接受日期:2025-11-24 出版日期:2026-03-18 发布日期:2026-03-05
通讯作者: * 电子信箱: xinzhou@ouc.edu.cn (周鑫),xiangfeng@upc.edu.cn (冯翔),de.chen@ntnu.no (陈德).
基金资助:
国家自然科学基金(22322814);国家自然科学基金(22405293)

Rational design of bifunctional catalysts for hydrocracking of polyethylene waste plastics to narrow-distributed liquid fuels

Zhe Ma^a, Chenzhao Wang^a, Peng Xu^a, Xin Zhou^b^,^*(), Xiang Feng^a^,^*(), De Chen^a^,^c^,^*()

^aState Key Laboratory of Heavy Oil Processing, China University of Petroleum, Qingdao 266580, Shandong, China
^bCollege of Chemistry and Chemical Engineering, Ocean University of China, Qingdao 266100, Shandong, China
^cDepartment of Chemical Engineering, Norwegian University of Science and Technology, Trondheim 7591, Norway

Received:2025-10-03 Accepted:2025-11-24 Online:2026-03-18 Published:2026-03-05
Contact: * E-mail: xinzhou@ouc.edu.cn (X. Zhou),xiangfeng@upc.edu.cn (X. Feng),de.chen@ntnu.no (D. Chen).
About author:Xin Zhou (Department of Chemical Engineering, Ocean University of China) received his Ph.D. in 2020 from China University of Petroleum (East China). He is currently an associate professor in the Department of Chemical Engineering at the College of Chemistry and Chemical Engineering, Ocean University of China. His research focuses on the intersection of AI and chemical engineering, as well as the digitalization and intellectualization of chemical processes. His main areas of interest include: machine learning-assisted development of catalytic new materials for chemical processes, machine learning-assisted optimization of chemical processes, and machine learning-accelerated DFT and computational fluid dynamics calculations.
Xiang Feng (State Key Laboratory of Heavy Oil Processing, China University of Petroleum) received his bachelor's degree and doctoral degree from East China University of Science and Technology, and studied as a postdoctoral fellow in China University of Petroleum (East China) and Norwegian University of Science and Technology. With heterogeneous catalytic reaction engineering as the research direction, he is committed to the study of regulating the active site and enhancing stability of industrial metal/zeolite catalysts in the field of high value-added olefin derivatization.
De Chen (Department of Chemical Engineering, Norwegian University of Science and Technology) received his Ph.D. in industrial catalysis at NTNU, Norway, in 1998. He is a professor in catalysis at the Department of Chemical Engineering, Norwegian University of Science and Technology (NTNU) since 2001 (associate professor 1998-2001). His research is mainly on a multiscale approach at the interface between catalysis science and industrial chemical processes. He is a member of the Norwegian Academy of Technological Science and the Royal Norwegian Academy of Sciences and Letters, as well as the Academy of Europe. He is the director of the innovation hub for the upcycling of wastes, a member of the leader group at the National Innovation Center (iCSI), and FME Center of biomass for fuels (Bio4Fuels).
Supported by:
National Natural Science Foundation of China-Outstanding Youth Foundation of China(22322814);National Natural Science Foundation of China(22405293)

摘要/Abstract

摘要：

将废弃聚乙烯升级转化为液体燃料, 对推动循环经济发展具有重要潜力. 与热裂解及催化裂解相比, 双功能催化剂催化的加氢裂解技术因其反应温度较低、产物饱和度高、CO₂排放量少以及高效脱除杂原子等优势, 成为塑料废弃物资源化极具前景的化学途径. 然而, 该过程复杂的反应机制导致目前对“结构-性能”关系缺乏清晰认知, 产物碳数分布较宽, 因而如何定向设计合成面向目标产物的高效催化剂仍是关键挑战.

本综述聚焦聚乙烯加氢裂解中双功能催化剂微观结构(金属分散度、金属活性、酸活性及金属-酸间距离)的精准调控, 深入阐明催化剂结构与产物选择性之间的构效关系. 首先, 阐述了双功能催化剂中的聚乙烯加氢裂解反应机制; 随后, 总结了双功能催化剂金属位点与酸性位点的研究进展; 通过分析聚乙烯加氢裂解反应活性, 揭示了双功能催化剂中金属-酸位点协同平衡规律; 最后, 探讨了当前双功能催化剂在聚乙烯加氢裂解体系中的优化策略、精准设计及实际应用面临的挑战与未来发展方向: (1)增强金属分散度方面, 通过使用二维金属氧化物或添加第二金属的策略, 可以为金属位点提供丰富的吸附空位, 提升加氢裂解过程中的脱氢/加氢反应效率. (2)提升金属位点活性方面, 加氢裂解活性位可以来自于贵金属(如Pt, Ru)或非贵金属(如Ni, Co, Mo等), 其中负载金属Pt催化剂具有较强的催化活性, 近期研究聚焦于抑制Ru基催化剂产物中甲烷生成, 以及引入第二金属增强非贵金属催化剂加氢裂解性能. (3)优化酸性位分布及强度, 调控C-H键极化和氢化物萃取, 从而影响加氢裂解速率和反应中间体电子分布, 最终影响产物碳数分布宽度. (4)通过控制金属落位、利用串联催化, 调控金属位与酸性位点间邻近性, 控制裂解深度及异构化程度, 最终调控反应路径及产物选择性.

在未来, 可以继续开发非贵金属双功能催化剂, 在降低催化剂体系总成本的同时窄化产物碳数分布, 在此基础上, 深入探索聚乙烯废塑料自身性质、反应工艺条件对加氢裂解反应性能的影响, 并将双功能催化剂的设计原理拓展应用到其他聚烯烃废塑料转化中; 开发无需外加氢气条件下的自供氢聚乙烯催化转化体系; 建立聚乙烯废塑料与其他物质(如生物质、废润滑油、CO₂等)新型共转化工艺. 希望本文能够为构建高效实用的双功能催化剂聚乙烯加氢裂解体系提供借鉴.

关键词: 聚乙烯废塑料, 加氢裂解, 双功能催化剂, 合理设计, 液体燃料

Abstract:

Upcycling of waste polyethylene into liquid fuels with a narrow molecular-weight distribution presents significant potential for advancing the circular economy. Compared to pyrolysis and catalytic cracking, hydrocracking using bifunctional catalysts offers distinct advantages such as lower reaction temperatures, higher product saturation, reduced CO₂ emissions, and effective heteroatom removal. These benefits position it as a highly promising route for plastic waste valorization. Nevertheless, the intricate reaction mechanisms have hindered the clear understanding on structure-performance relationship. Therefore, the rational design and synthesis of catalysts optimized for specific target products remain a critical challenge. This review focuses on the precise regulation of bifunctional catalyst microstructures (including metal dispersion, metal activity, acid activity, and metal-acid distance) in polyethylene hydrocracking, and further elucidates the structure-performance relationship between catalyst and product selectivity. To better understand the catalyst design strategies, hydrocracking mechanism over bifunctional catalysts is firstly introduced. Next, progress in research to understand the metal sites and acid sites of bifunctional catalysts will be presented. The hydrocracking activities of bifunctional catalysts will also be investigated to demonstrate the metal-acid balance. Finally, the current challenges and future perspectives on optimization, precise design, and practical application of the bifunctional catalysts in polyethylene hydrocracking system will be proposed.

Key words: Polyethylene waste plastic, Hydrocracking, Bifunctional catalyst, Rational design, Liquid fuels

马哲, 王晨朝, 许朋, 周鑫, 冯翔, 陈德. 合理设计双功能催化剂用于聚乙烯废塑料加氢裂解制备较窄碳数分布的液体燃料[J]. 催化学报, 2026, 82: 42-60.

Zhe Ma, Chenzhao Wang, Peng Xu, Xin Zhou, Xiang Feng, De Chen. Rational design of bifunctional catalysts for hydrocracking of polyethylene waste plastics to narrow-distributed liquid fuels[J]. Chinese Journal of Catalysis, 2026, 82: 42-60.

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图/表 21

Table 1 Summary of the representative catalysts and their performance in hydrocracking.

Feed	Catalyst	Feed/ catalyst	Metal loading (wt%)	Reaction condition			Liquid fuels	Yield (%)	Ref.
Feed	Catalyst	Feed/ catalyst	Metal loading (wt%)	Temperature (°C)	Time (h)	Pressure (MPa)	Liquid fuels	Yield (%)	Ref.
HDPE	mSiO₂/Pt/SiO₂	—	0.3	250	6	1.38	C₉-C₁₈	74	[74]
HDPE	Pt-WZr+HY	10	0.5	250	2	3	fuel	85	[43]
LDPE	Pt/W/Beta	40	2	250	1	3	C₅-C₁₂	65	[37]
HDPE	Pt/WO₃	10	0.2	250	3	3	fuel	89	[53]
LDPE	Pt@S-1+Beta	10	0.3	250	2	3	naptha	89	[79]
HDPE	PtSnCe/SiAl	10	1/1.8/3	270	2	3	gasoline	77	[54]
LDPE	Pt/Ce-HY	10	5/5	300	2	3	fuel	81	[68]
LDPE	Pt/Ce-HY	10	0.5/3	280	2	2	C₅-C₁₂	85	[35]
HDPE	Pt/Al₂O₃+HY	28	1	280	3	3	fuel	88	[29]
LDPE	Co/Ni/CeO₂	6.8	—	240	8	2	fuel	—	[46]
LDPE	Ni/SiO₂	5	5	280	4	3	n-alkanes	81	[52]
Mixed waste	MoS_x-Hbeta	10	3	250	6-12	2-3	alkanes	—	[76]
LDPE	NiCo-LDH	20	1/50	280	2-5	2	fuel	74	[65]
LDPE	Ni/WZr	10	10	260	1.5	3	naptha	77	[64]
LDPE	Ni@Beta	20	10	250	3	2	naptha	87	[36]
LDPE	Ni/NbO_x	20	1	240	3	5	C₅-C₂₀	95	[71]
PE film	Ni-Ca/ZrO₂+Beta	10	12.5	250	3	1.5	naptha	87	[67]
LDPE	NiMoS_x/HY	20	2.3	300	—	2	naptha	~81	[66]
LDPE	Ru/CeO₂	34	5	280	12	2	fuel	79	[46]
LDPE	Ru-WZr	40	5	250	2	5	fuel	~63	[60]
PP	Ru/CeO₂	—	0.25	260	18	3	fuel	~69	[47]
PE/PP	Ru/FAU	14	5	200	16	3	alkanes	67	[40]
LDPE	Ru-SBA-15	—	3	230	5	2	diesel	59	[75]
HDPE	Ru-ZSM-5	—	1	210	12	2	fuel	~63	[61]
PE	Ru/γ-Al₂O₃	1	3	240	2	12	C₅-C₂₁	~70	[69]

Fig. 1. (a) Reaction pathway of polyolefin hydrocracking over metal/zeolite bifunctional catalyst. (b) Influence of metal and acid balance on polyolefin hydrocracking. Reproduced with permission from Ref. [13]. Copyright 2022, American Chemical Society.

Fig. 2. Classical carbon-carbon bond cleavage mechanisms in hydrocracking of polyethylene.

Fig. 3. (a) SEM micrograph. (b) TEM micrograph. (c) HAADF-STEM image (inset, FFT image). (d) AFM image and thickness distributions of WO3. (e) HAADF-STEM image of WO3. (f) EPR spectra of Pt/WO3 and WO3. (g) HAADF-STEM image of Pt/WO3. (h) XRD patterns of Pt/WO3 and WO3 catalysts. (i) Product distributions (wt%) and reusability of 2D Pt/WO3 catalyst. (j) HDPE hydrocracking performance of 2D Pt/WO3 in comparison to catalysts in the literature. (k) Schematic diagram of HDPE hydrocracking over 2D Pt/WO3 catalyst. Reproduced with permission from Ref. [53]. Copyright 2023, John Wiley and Sons.

Fig. 4. (a) Time-dependent reaction results from 0.5 to 3 h at 270 °C, 30 bar H2, 2 g of HDPE, 0.2 g of the PtSn-0.5Ce/SiAl catalyst. (b) Reaction network according to a time-dependent reaction. (c) The reaction mechanism study for hydrocracking at 270 °C, 2 h, 30 bar H2, 2 g of octadecane, 0.1 g of Pt/SiAl or PtSn/SiAl or PtSn-0.5Ce/SiAl catalyst. (d) Reaction mechanism for hydrocracking where n-octane is used as a reactant mode. Reproduced with permission from Ref. [54]. Copyright 2023, American Chemical Society.

Fig. 5. Strategies for enhancing metal dispersion: (a) Creating oxygen vacancies on two-dimensional metal oxides; (b) Adding second-metal to stabilize metal sites.

Fig. 6. The selection of metal sites and enhancement of dehydrogenation-hydrogenation activity.

Fig. 7. (a) Proposed reaction mechanism of LDPE hydrogenolysis on Ru-based catalysts. R1, R2 = CnH2n+1 (n ≥ 0) alkyl groups. (b) Selective pathway on Ru-WZr catalysts induced by ～1 nm, slightly reduced (WOx)n clusters. Reproduced with permission from Ref. [60]. Copyright 2021, American Chemical Society.

Fig. 8. Role of Bifunctional Ru/Acid Catalysts in the Selective Hydrocracking of Polyethylene and Polypropylene Waste to Liquid Hydrocarbons. Reproduced with permission from ref 40. Copyright 2022, American Chemical Society.

Fig. 9. (a) Turnover rates of C?C cleavage on various metals calculated by DFT prediction. (b) Schematic diagram depicting the structural evolution of CoAl-LDH during the high-temperature reduction process. (c) Hydrogenolysis performance of LDPE over CoAlOx, NiCoAlOx and NiAlOx catalysts. (d) In-situ DRIFTS of n-butane hydrogenolysis on CoAlOx-H650; (e) In situ DRIFTS of n-butane hydrogenolysis on 6NiCoAlOx. (f) Energy barriers of *C2H4 hydrogenation/desorption over Co?Co site on Co (111) facet, Ni-Co/Co-Co sites on Ni1/Co (111) facet. (g) H2-TPD curves of CoAlOx, NiCoAlOx and NiAlOx catalysts. Reproduced with permission from Ref. [65]. Copyright 2024, American Chemical Society.

Fig. 10. The regulation of acidity for PE hydrocracking: (a) The influence of acid types on the product distribution; (b) The influence of acid distribution on the product distribution.

Fig. 11. β-scission mechanism of PO hydrocracking over Ru1-ZrO2. (a) Reaction pathways and DFT calculated energy profiles of PP hydrocracking to gas products via β-scission mechanism with carbonium ions (energy unit: eV). The molecule structures in red or blue color are the same type of carbonium circularizing in the hydrocracking loop. (b) Schematic catalytic cycle of PO (PE or PP) hydrocracking on Ru1-ZrO2. Reproduced with permission from Ref. [70]. Copyright 2025, Springer Nature.

Fig. 12. (a) Operando DRIFT spectra of 1Ni/NbOx-Ax with and without PE under H2 or Ar pressure. (b) The liquid formation rate as a function of the in situ generated Br?nsted acidity over 1Ni/NbOx-Ax catalysts. (c) Snapshots of formation of Br?nsted acid site and the NH3 adsorption on Nb-OH site (110). (d) The proton affinity (Epa) of Nb-O site and NH3 adsorption energy (Ead) of Nb-OH sites. (e) The potential energy corrugation of the hydrocracking of butene on NbOx surfaces. (f) Snapshots of the C-C bond cleavage steps over Nb-OH sites using butene as a model molecule. (g) The mechanistic illustration of the formation of hydrogen spillover-induced Br?nsted acid and PE hydrocracking pathways over Ni/NbOx catalyst. Reproduced with permission from Ref. [71]. Copyright 2025, John Wiley and Sons.

Fig. 13. (a) Schematic diagram of hydrogenolysis mechanism of polyolefin over Ru catalysts. (b) Schematic illustration of the conventional impregnation and precise-impregnation approaches. TEM image (c) and elemental mapping (d) of p-Ru/SBA. (e) Reducing the original entropy of polymer chains by strong localization in the space-confined catalyst. Reproduced with permission from Ref. [75]. Copyright 2023, John Wiley and Sons.

Fig. 14. (a) Catalytic performance of LDPE (left) and n-C16 (right) over Pt/5Ce-HY and Pt@5Ce-HY. (b) Catalytic performance of LDPE over Pt/Ce-SiAlO and Pt/SiAlO (left) and catalytic performance of n-C16 over Pt@5Ce-HY and Pt@HY (right). (c) The potential catalytic route over Pt/5Ce-HY. Reproduced with permission Ref. [68]. Copyright 2024, John Wiley and Sons.

Fig. 15. Plastics recycling routes: (a) Schematic summary of current physical and chemical recycling routes of waste plastics; (b) Illustration of our hydrocracking method. Reproduced with permission from Ref. [76]. Copyright 2023, The American Association for the Advancement of Science.

Fig. 16. (a) Catalytic performance of Pt-USY with different metal-acid proximity and referential catalysts in hydrocracking PE. (b) Product distribution of the corresponding Pt-USY catalysts. 1H-NMR (c) and 13C-NMR (d) spectra profile of typical liquid products. (e) Molecular weight distributions of pristine PE and solid product by HT-GPC. (f) The proposed mechanism of hydrocracking of PE on Pt/USY catalysts with different metal-acid proximity. Reproduced with permission from Ref. [77]. Copyright 2024, Royal Society of Chemistry.

Fig. 17. (A) Schematic diagram of 0.05 wt% Ptn/Hβ-SiO2 by surface silication. Hydrocracking of LDPE (200 mg of 0.05 wt% Ptn/Hβ or Ptn/Hβ-SiO2 catalyst, 2.0 g of LDPE, 2.2 MPa 90%H2/Ar, 240 °C 2 h) (B) and PP (50 mg of catalyst) (C). (D) Schematic diagram of the reaction using alkane and LDPE mixtures. (E) Hydroconversion of n-C18H38 and (F) n-C6H14 with/without adding LDPE (50 mg of 0.05 wt% Ptn/Hβ catalyst, 2.0 g of substrate, 2.0 g of LDPE, 2.2 MPa 90%H2/Ar, 250 °C 2 h). Reproduced with permission from Ref. [78]. Copyright 2025, American Chemical Society.

Fig. 18. (a) Effect of selective poisoning of Pt/WO3/ZrO2 or HY(30) zeolite by pyridine on reaction performance. (b) Depiction of main intermediates diffusing over Pt/WO3/ZrO2 + HY(30) catalyst. (c) Reaction selectivity in case of intimate contact between Pt particles and zeolite acid sites. Reproduced with permission from Ref. [43]. Copyright 2021, The American Association for the Advancement of Science.

Fig. 19. Characterization and catalytic performance of Pt@S-1 and Pt/S-1. TEM images and particle size distribution of Pt@S-1 (a) and Pt/S-1 (b). (c) HAADF-STEM and EDS mappings of Pt@S-1. (d) XRD patterns. (e) Pt 4f XPS spectra. (f) Fourier transform of k3-weighted EXAFS spectra. (g) Relationship between isomer/normal (i/n) and Pt/Br?nsted acid sites (nPt/na) over different catalysts. (h,i) Product distribution and isomerization comparison over Pt@S-1 and Pt/S-1 catalysts. Reproduced with permission from Ref. [79]. Copyright 2023, Royal Society of Chemistry.

Fig. 20. The structure-activity relationship between metal-acid site proximity and PE hydrocracking performance. (a) Metal sites on zeolite outer surface. (b) Metal sites within zeolites channels. (c) Metal-acid proximity increases to the nano-/micro-meter scale

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合理设计双功能催化剂用于聚乙烯废塑料加氢裂解制备较窄碳数分布的液体燃料

Rational design of bifunctional catalysts for hydrocracking of polyethylene waste plastics to narrow-distributed liquid fuels

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