Acta Phys. -Chim. Sin. ›› 2025, Vol. 41 ›› Issue (7): 100073.doi: 10.1016/j.actphy.2025.100073
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Recent advances in synergistic catalytic valorization of CO2 and hydrocarbons by heterogeneous catalysis
Honghong Zhang1, Zhen Wei1,*(
), Derek Hao2, Lin Jing1, Yuxi Liu1, Hongxing Dai1, Weiqin Wei3,*(), Jiguang Deng1,*()
- 1 Beijing Key Laboratory for Green Catalysis and Separation, College of Materials Science and Engineering, Beijing University of Technology, Beijing 100124, China
2 Centre for Atomaterials and Nanomanufacturing (CAN), School of Science, RMIT University, Melbourne 3000, Australia
3 Beijing National Laboratory for Molecular Engineering, College of Chemistry and Molecular Engineering, Peking University, Beijing 100871, China
-
Received:2025-01-08Revised:2025-02-05Accepted:2025-02-25Published:2025-05-22 -
Contact:Email: xfwz522@126.com (Zhen Wei)2306388562@pku.edu.cn (Weiqin Wei)jgdeng@bjut.edu.cn (Jiguang Deng) -
Supported by:the National Natural Science Foundation of China(22406009); the National Natural Science Foundation of China(U23A20120); Natural Science Foundation of Hebei Province(B2021208033); R & D Program of Beijing Municipal Education Commission(KZ202210005011)
Cite this article
Honghong Zhang, Zhen Wei, Derek Hao, Lin Jing, Yuxi Liu, Hongxing Dai, Weiqin Wei, Jiguang Deng. Recent advances in synergistic catalytic valorization of CO2 and hydrocarbons by heterogeneous catalysis[J]. Acta Phys. -Chim. Sin. 2025, 41(7), 100073. doi: 10.1016/j.actphy.2025.100073
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Fig 1
(a) Molecular structure and related parameters and properties of CO2. Possible CO2 adsorption models: (b) monodentate and (c) bidentate coordination adsorption."
Fig 1
"
| Reactants | Catalyst | Reaction condition | Products | Reference |
| CO2 and Methane | Rh/InGaN1−xOx nanoarchitecture | Light-driven reforming; CH4 : CO2 : Ar = 1 : 1 : 2 (volume ratio); Reactor volume was 440 mL | Syngas (CO and H2) | [ |
| 0.6% Ir/CeO2−x | Thermal catalysis; CH4 : CO2 : N2 = 20 : 20 : 5 mL∙min−1; Space Velocity (SV) = 240000 mL∙g−1∙h−1 | [ | ||
| HZSM-5 zeolites | Plasma catalysis; CH4 : CO2 = 1 : 1 (molar ratio); Total flow = 40 mL∙min−1 | Acetic acid | [ | |
| 13X zeolite | Methanol | |||
| CO2 and Ethane | Zn3Cr1/SSZ-13 | Thermal catalysis; C2H6 : CO2 = 5% : 5%, equilibrated with Ar flow; Total flow = 25 sccm | Ethylene and CO | [ |
| Fe/Al2O3 Co/Al2O3 Ni/Al2O3 | Thermal catalysis; CO2 : C2H6 = 0 : 1 – 2 : 1, equilibrated with Ar flow | Carbon nanotubes and syngas (byproducts) | [ | |
| PdCox/CeO2 | Thermal catalysis; CO2 : C2H6 : Ar = 10 : 10 : 20 mL∙min−1 | CO and H2 | [ | |
| PdInx/CeO2 | C2H4, CO and H2O | |||
| CO2 and Propane | Cu/Ga-MFI zeolite | Thermal catalysis; C3H8 : CO2 : N2 = 3 : 3 : 4 mL∙min−1; SV = 2000 mL∙g−1·h−1 | Aromatics | [ |
| ZnFe2Ox/S-1 | Thermal catalysis; 0.1 MPa, N2 : CO2 : C3H8 = 4 : 1 : 1; SV = 7200 mL∙g−1·h−1 | C3H6, CO and H2 | [ | |
| CO2 and n-Butane/n-Pentane/n-Hexane | HZSM-5(17), Si/Al ratio = 17 | Thermal catalysis; Pn-alkane = 21 kPa, PCO2 = 2355 kPa and PAr = 124 kPa; Total flow = 30 mL∙min−1 | Aromatics | [ |
| CO2 and Alkene | Defective BCN | Light-driven fixation of CO2; visible light irradiation (λ = 420 nm); 1 atm of CO2 | Carboxylic acids | [ |
| CO2 and Toluene | NiFe/(Mg, Al)Ox | Plasma catalysis; CO2 : toluene : Ar = 7 : 1 : 63 | CO and H2 | [ |
| CO2 and Polyolefin | Pt/MnOx-ZSM-5 | Thermal catalysis; 1.0 MPa CO2, 100 mL batch reactor | Benzene, toluene and xylene | [ |
| CO2 and Polyethylene | HZSM-5 + CuZnZrOx | Thermal catalysis; 5 bar CO2 | Aromatics and CO | [ |
Fig 2
The hydrocarbon molecules involved in the synergistic conversion with CO2 in this article."
Fig 2
Fig 3
Possible reaction processes that involve (a) carbenium ions and (b) free radicals in the catalytic transformation of CO2 and alkanes on oxygen-vacancy-containing MOx loaded with active components."
Fig 3
Fig 4
(a) The catalytic cycle of Zn-doped CeO2 catalyzed C―C coupling to generate CH3COOH from CH4 and CO2. Reproduced with permission from Ref. [105]. Copyright 2016, American Chemical Society. (b) Reaction mechanism of coupling CH4 and CO2 to ethanol over Zn―Ce/ZSM-5 catalyst. Reproduced with permission from Ref. [55]. Copyright 2024, American Chemical Society. (c) Formation rates of liquid-phase and gas-phase products on ZnO, CeO2, and ZnO doped with different ratios of Ce. (d) Schematic diagram of different pathways for the co-photo reaction of CH4 and CO2 on Ce-ZnO catalyst. Reproduced with permission from Ref. [53]. Copyright 2023, Wiley-VCH GmbH. (e) The selectivity of oxygen-containing compounds in the conversion of CO2 and CH4 by plasma catalysis. (f) Possible reaction pathways, including the E-R and L-H mechanism for the plasma-catalytic conversion of CO2 and CH4 to CH3COOH [106]."
Fig 4
Fig 5
(a) Trends in product yields in C2H6-CO2 reaction over various 1% PdM3/CeO2 catalysts. Reproduced with permission from Ref. [57]. Copyright 2022, American Chemical Society. (b) Normalized operando Cr K-edge XANES spectra of Cr/Si-MFI during the C2H6 dehydrogenation (with/without CO2) reaction at 650 ℃. (c) Comparison of the average coordination number of Cr―O scattering paths based on the EXAFS spectra recorded during the reactions with different reactant feed ratios [109]. (d) Electron transfer from Zn to H after the 2nd C―H bond scission in C2H6, where electron accumulation and depletion are represented by yellow and cyan, respectively. (e) Oxidation of Cr in Zn―O―Cr during the decomposition of COOH* intermediates [69]."
Fig 5
Fig 6
(a) Design concept for HEI catalyst. The Pt and Sn sites in the intermetallic compound PtSn are partially replaced by Co/Ni and In/Ga, respectively, to form the PtSn-type HEI. (b) The atomic arrangement of the most stable (110) face of PtSn (left) and HEI (right). (c) Role of individual metals and effect of polymetallization on CO2-ODHP catalysis [122]. (d) Schematic diagram of the effect of CrOx/silica zeolite on the activity and selectivity of CO2-ODHP. Reproduced with permission from Ref. [124]. Copyright 2021, Elsevier, B.V."
Fig 6
Fig 7
(a) Catalytic performance of coupled conversion of CO2 and n-butane over metal-modified ZSM-5. (b) Conversion, and product and CO selectivity in the CO2/n-butane reaction over Zn/ZSM-5. (c) CH4, C2H6, C3H8, BTX, and A9+ aromatics selectivity. (d) The proposed mechanism for the coupling reaction between CO2 and n-butane over the Zn/ZSM-5 catalyst (1. cracking, 2. carbonylation, 3. cyclization, 4. isomerization, 5. dehydration, 6. dehydroxylation). Reproduced with permission from Ref. [126]. Copyright 2023, American Chemical Society."
Fig 7
Fig 8
In situ DRIFTS recorded during n-butane conversion in (a) Ar and (b) CO2 atmosphere. Reproduced with permission from Ref. [127]. Copyright 2023, Dalian Institute of Chemical Physics, Chinese Academy of Sciences."
Fig 8
Fig 9
(a) Under visible light irradiation, the β-hydroxycarboxylation reaction of alkenes with CO2 on d-BCN. Reproduced with permission from Ref. [65]. Copyright 2023, Wiley-VCH GmbH. (b) Proposed reaction pathway of plasma-catalytic CRT reaction over Ni-Fe/(Mg, Al)Ox [134]. (c) TOFEB of VOx-Al2O3 catalysts in CO2-ODEB before and after NH3·H2O treatment. (d) Catalytic stability of s-3VA-pH 13 and s-28CZA-pH 13 [66]."
Fig 9
Fig 10
(a) Schematic diagram of the reactor and product fractions. (b) Distribution of detectable hydrocarbons in volatile and low-boiling liquid products. (c) The proposed coupling reaction mechanism between CO2 and PE over a tandem catalyst [58]."
Fig 10
Fig 11
(a) Schematic representation of the reaction system and structure of the HZSM-5 + CuZnZrOx catalyst. (b) Apparent H2 evolution, (c) CO2 consumption, and (d) aromatic yield over HZSM-5 + CuZnZrOx or HZSM-5 catalyst [59]. (e) Reaction pathways for CO2-promoted polyolefins conversion to BTX over bifunctional Pt/MnOx-ZSM-5 catalyst [56]."
Fig 11
Fig 12
Summary of progress and prospects in the conversion of CO2 and hydrocarbons"
Fig 12
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