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

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

Chinese Journal of Catalysis ›› 2026, Vol. 82: 42-60.DOI: 10.1016/S1872-2067(25)64916-3

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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)

Abstract

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

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

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