Sunlight-Driven Fixation of CO2 to Cyclic Carbonates Using Carbon Dots as a Photothermal Catalyst

Ruijia Wang , Hongda Guo , Tao Zhang , Xiaoxia Chen , Min Ge , Shujun Li , Jian Li , Bing Tian , Bernd Strehmel , Shouxin Liu , Andrey L. Rogach , Tony D. James , Zhijun Chen

Exploration ›› 2026, Vol. 6 ›› Issue (1) : 20250043

PDF (2505KB)
Exploration ›› 2026, Vol. 6 ›› Issue (1) :20250043 DOI: 10.1002/EXP.20250043
RESEARCH ARTICLE
Sunlight-Driven Fixation of CO2 to Cyclic Carbonates Using Carbon Dots as a Photothermal Catalyst
Author information +
History +
PDF (2505KB)

Abstract

Fixation of CO2 through photocatalytic cycloaddition with epoxides to synthesize cyclic carbonates is an important but challenging process. In this work, carbon dots (CDs) synthesized from gallic acid and polyethylenimine are used for the efficient catalytic cycloaddition of CO2 with epoxides in the absence of any solvent, additives, and halides, and importantly upon irradiation by natural sunlight. Specifically, carbon dots generated thermal energy and electrons upon solar irradiation, which together with their surface N-sites activated the inert CO2. Meanwhile, epoxides were activated by the surface hydroxyl and carboxylic groups of the carbon dots, which reacted with activated CO2 at solar thermal-induced high temperatures. The CDs shows excellent stability and recyclability during the catalysis. A 1000 mmol scale reaction for cyclic carbonate synthesis performed well upon irradiation with natural sunlight in the presence of CDs, showing great potential for the industrial application due to the simple, mild, and energy-saving process.

Keywords

carbon dioxide / carbon dots / cyclic carbonate / photothermal catalysis / sunlight utilization

Cite this article

Download citation ▾
Ruijia Wang, Hongda Guo, Tao Zhang, Xiaoxia Chen, Min Ge, Shujun Li, Jian Li, Bing Tian, Bernd Strehmel, Shouxin Liu, Andrey L. Rogach, Tony D. James, Zhijun Chen. Sunlight-Driven Fixation of CO2 to Cyclic Carbonates Using Carbon Dots as a Photothermal Catalyst. Exploration, 2026, 6 (1) : 20250043 DOI:10.1002/EXP.20250043

登录浏览全文

4963

注册一个新账户 忘记密码

References

[1]

A. J. Kamphuis, F. Picchioni, and P. P. Pescarmona, “CO2 -Fixation Into Cyclic and Polymeric Carbonates: Principles and Applications,” Green Chemistry 21 (2019): 406–448, https://doi.org/10.1039/C8GC03086C.

[2]

B. Schafner, F. Schafner, S. P. Verevkin, and A. Borner, “Organic Carbonates as Solvents in Synthesis and Catalysis,” Chemical Reviews 110 (2010): 4554–4581, https://doi.org/10.1021/cr900393d.

[3]

W. Guo, J. E. Gómez, À. Cristòfol, J. Xie, and A. W. Kleij, “Catalytic Transformations of Functionalized Cyclic Organic Carbonates,” Angewandte Chemie International Edition 57 (2018): 13735–13747, https://doi.org/10.1002/anie.201805009.

[4]

Q. Liu, L. Wu, R. Jackstell, and M. Beller, “Using Carbon Dioxide as a Building Block in Organic Synthesis,” Nature Communications 6 (2015): 5933, https://doi.org/10.1038/ncomms6933.

[5]

W.-H. Wang, Y. Himeda, J. T. Muckerman, G. F. Manbeck, and E. Fujita, “CO2 Hydrogenation to Formate and Methanol as an Alternative to Photo- and Electrochemical CO2 Reduction,” Chemical Reviews 115 (2015): 12936–12973, https://doi.org/10.1021/acs.chemrev.5b00197.

[6]

W. Wang, S. Wang, X. Ma, and J. Gong, “Recent Advances in Catalytic Hydrogenation of Carbon Dioxide,” Chemical Society Reviews 40 (2011): 3703, https://doi.org/10.1039/c1cs15008a.

[7]

J. Artz, T. E. Muller, K. Thenert, et al., “Sustainable Conversion of Carbon Dioxide: An Integrated Review of Catalysis and Life Cycle Assessment,” Chemical Reviews 118 (2018): 434–504, https://doi.org/10.1021/acs.chemrev.7b00435.

[8]

L. Guo, K. J. Lamb, and M. North, “Recent Developments in Organocatalysed Transformations of Epoxides and Carbon Dioxide into Cyclic Carbonates,” Green Chemistry 23 (2021): 77–118, https://doi.org/10.1039/D0GC03465G.

[9]

B.-H. Xu, J.-Q. Wang, J. Sun, et al., “Fixation of CO2 into Cyclic Carbonates Catalyzed by Ionic Liquids: A Multi-Scale Approach,” Green Chemistry 17 (2015): 108–122, https://doi.org/10.1039/C4GC01754D.

[10]

A. Decortes, A. M. Castilla, and A. W. Kleij, “Salen-Complex-Mediated Formation of Cyclic Carbonates by Cycloaddition of CO2 to Epoxides,” Angewandte Chemie International Edition 49 (2010): 9822–9837, https://doi.org/10.1002/anie.201002087.

[11]

R. Huang, J. Rintjema, J. González-Fabra, et al., “Deciphering Key Intermediates in the Transformation of Carbon Dioxide into Heterocyclic Products,” Nature Catalysis 2 (2019): 62–70, https://doi.org/10.1038/s41929-018-0189-z.

[12]

J. O. Kroll, J. Kothandaraman, K. Grubel, and D. J. Heldebrant, “Integrated Approach to CO2 Capture and Conversion to Cyclic Carbonates Under Solvent- and Additive-Free Conditions Utilizing the CO2 Capture Solvent EEMPA,” Energy & Fuels 38 (2024): 7959–7965, https://doi.org/10.1021/acs.energyfuels.3c04993.

[13]

W. Zhou, Q. W. Deng, G. Q. Ren, et al., “Enhanced Carbon Dioxide Conversion at Ambient Conditions via a Pore Enrichment Effect,” Nature Communications 11 (2020): 4481, https://doi.org/10.1038/s41467-020-18154-9.

[14]

Y. Zhi, P. Shao, X. Feng, et al., “Covalent Organic Frameworks: Efficient, Metal-Free, Heterogeneous Organocatalysts for Chemical Fixation of CO2 Under Mild Conditions,” Journal of Materials Chemistry A 6 (2018): 374–382, https://doi.org/10.1039/C7TA08629F.

[15]

T. K. Pal, D. De, and P. K. Bharadwaj, “Metal–Organic Frameworks for the Chemical Fixation of CO2 Into Cyclic Carbonates,” Coordination Chemistry Reviews 408 (2020): 213173, https://doi.org/10.1016/j.ccr.2019.213173.

[16]

J. W. Maina, C. Pozo-Gonzalo, L. Kong, J. Schütz, M. Hill, and L. F. Dumée, “Metal Organic Framework Based Catalysts for CO2 Conversion,” Materials Horizons 4 (2017): 345.

[17]

M. Zhu and M. A. Carreon, “Porous Crystals as Active Catalysts for the Synthesis of Cyclic Carbonates,” Journal of Applied Polymer Science 131 (2014): 39738, https://doi.org/10.1002/app.39738.

[18]

Y. Xie, T.-T. Wang, X.-H. Liu, K. Zou, and W.-Q. Deng, “Capture and Conversion of CO2 at Ambient Conditions by a Conjugated Microporous Polymer,” Nature Communications 4 (2013): 1960, https://doi.org/10.1038/ncomms2960.

[19]

K. S. Song, P. W. Fritz, and A. Coskun, “Porous Organic Polymers for CO2 Capture, Separation and Conversion,” Chemical Society Reviews 51 (2022): 9831–9852, https://doi.org/10.1039/D2CS00727D.

[20]

A. Helal, M. Fettouhi, S. M. Alqahtani, Y. Umar, S. Khan, and M. A. Sanhoob, “Nitrogen-Rich Barium–Organic Framework for Capture and Cocatalysts Free Chemical Fixation of CO2 via Cyclic Carbonates and Oxazolidinones,” ACS Applied Materials & Interfaces 17 (2025): 6271–6281, https://doi.org/10.1021/acsami.4c18062.

[21]

P. Mikšovsky, K. Rauchenwald, S. Naghdi, et al., “Silicon Oxycarbide (SiOC)-Supported Ionic Liquids: Heterogeneous Catalysts for Cyclic Carbonate Formation,” ACS Sustainable Chemistry & Engineering 12 (2024): 1455–1467, https://doi.org/10.1021/acssuschemeng.3c05569.

[22]

M. H. Alenazi, A. Helal, M. Y. Khan, et al., “Covalent Organic Frameworks (COFs) for CO2 Utilizations,” Carbon Capture Science & Technology 14 (2025): 100365.

[23]

A. Helal, M. H. Zahir, A. Albadrani, and M. M. Ekhwan, “Triazole Appended Metal–Organic Framework for CO2 Fixation as Cyclic Carbonates Under Solvent-Free Ambient Conditions,” Catalysis Letters 153 (2023): 2883–2891, https://doi.org/10.1007/s10562-022-04213-x.

[24]

G. Zhai, Y. Liu, Y. Mao, et al., “Improved Photocatalytic CO2 and Epoxides Cycloaddition via the Synergistic Effect of Lewis Acidity and Charge Separation over Zn Modified UiO-bpydc,” Applied Catalysis B: Environment and Energy 301 (2022): 120793, https://doi.org/10.1016/j.apcatb.2021.120793.

[25]

Q. Guo, S. G. Xia, X. B. Li, et al., “Flower-Like Cobalt Carbide for Efficient Carbon Dioxide Conversion,” Chemical Communications 56 (2020): 7849–7852, https://doi.org/10.1039/D0CC01091J.

[26]

Q. Yang, H. Peng, Q. Zhang, et al., “Atomically Dispersed High-Density Al–N4 Sites in Porous Carbon for Efficient Photodriven CO2 Cycloaddition,” Advanced Materials 33 (2021): 2103186, https://doi.org/10.1002/adma.202103186.

[27]

X. Chen, M. Wei, A. Yang, et al., “Near-Infrared Photothermal Catalysis for Enhanced Conversion of Carbon Dioxide under Mild Conditions,” ACS Applied Materials & Interfaces 14 (2022): 5194–5202, https://doi.org/10.1021/acsami.1c18889.

[28]

L. P. Zhang, X. W. Tu, Y. Chen, et al., “Photothermal Catalysis Without Solvent for Fixing CO2 to Cyclic Carbonate,” Molecular Catalysis 538 (2023): 112971.

[29]

L. Gong, J. Sun, Y. Liu, and G. Yang, “Photoinduced Synergistic Catalysis on Zn Single-Atom-Loaded Hierarchical Porous Carbon for Highly Efficient CO2 Cycloaddition Conversion,” Journal of Materials Chemistry A 9 (2021): 21689–21694, https://doi.org/10.1039/D1TA06159C.

[30]

R. Cheng, A. Wang, S. Sang, H. Liang, S. Liu, and P. Tsiakaras, “Photocatalytic CO2 Cycloaddition over Highly Efficient W18O49-Based Composites: An Economic and Ecofriendly Choice,” Chemical Engineering Journal 466 (2023): 142982, https://doi.org/10.1016/j.cej.2023.142982.

[31]

P. K. Prajapati, A. Kumar, and S. L. Jain, “First Photocatalytic Synthesis of Cyclic Carbonates from CO2 and Epoxides Using CoPc/TiO2 Hybrid Under Mild Conditions,” ACS Sustainable Chemistry & Engineering 6 (2018): 7799–7809, https://doi.org/10.1021/acssuschemeng.8b00755.

[32]

N. Das, R. Paul, S. Biswas, et al., “Photo-Responsive Signatures in a Porous Organic Polymer Enable Visible Light-Driven CO2 Photofixation,” ACS Sustainable Chemistry & Engineering 11 (2023): 2066–2078, https://doi.org/10.1021/acssuschemeng.2c04428.

[33]

M. Bakiro, S. Hussein Ahmed, and A. Alzamly, “Efficient Visible-Light Photocatalytic Cycloaddition of CO2 and Propylene Oxide Using Reduced Graphene Oxide Supported BiNbO4,” ACS Sustainable Chemistry & Engineering 8 (2020): 12072–12079, https://doi.org/10.1021/acssuschemeng.0c03363.

[34]

C.-L. Tan, M.-Y. Qi, Z.-R. Tang, and Y.-J. Xu, “Isolated Single-Atom Cobalt in the ZnIn2S4 Monolayer With Exposed Zn Sites for CO2 Photofixation,” ACS Catalysis 13 (2023): 8317–8329, https://doi.org/10.1021/acscatal.3c00992.

[35]

A. Said, G. Zhang, C. Liu, et al., “A Butterfly-Like Lead-Doped Titanium-Oxide Compound With High Performance in Photocatalytic Cycloaddition of CO2 to Epoxide,” Dalton Transactions 52 (2023): 2392–2403, https://doi.org/10.1039/D2DT03990G.

[36]

X. Xu, R. Ray, Y. Gu, et al., “Electrophoretic Analysis and Purification of Fluorescent Single-Walled Carbon Nanotube Fragments,” Journal of the American Chemical Society 126 (2024): 12736–12737, https://doi.org/10.1021/ja040082h.

[37]

K. Hola, Y. Zhang, Y. Wang, E. P. Giannelis, R. Zboril, and A. L. Rogach, “Carbon Dots—Emerging Light Emitters for Bioimaging, Cancer Therapy and Optoelectronics,” Nano Today 9 (2014): 590–603, https://doi.org/10.1016/j.nantod.2014.09.004.

[38]

L. Ðorđević, F. Arcudi, M. Cacioppo, and M. Prato, “multifunctional Chemical Toolbox to Engineer Carbon Dots for Biomedical and Energy Applications,” Nature Nanotechnology 17 (2022): 112–130.

[39]

G. Ragazzon, A. Cadranel, E. V. Ushakova, et al., “Optical Processes in Carbon Nanocolloids,” Chemistry 7 (2021): 606–628, https://doi.org/10.1016/j.chempr.2020.11.012.

[40]

C. Rosso, G. Filippini, and M. Prato, “Carbon Dots as Nano-Organocatalysts for Synthetic Applications,” ACS Catalysis 10 (2020): 8090–8105, https://doi.org/10.1021/acscatal.0c01989.

[41]

B. Jana, Y. Reva, T. Scharl, V. Strauss, A. Cadranel, and D. M. Guldi, “Carbon Nanodots for All-in-One Photocatalytic Hydrogen Generation,” Journal of the American Chemical Society 143 (2021): 20122–20132, https://doi.org/10.1021/jacs.1c07049.

[42]

J. Lu, Y. Shi, Z. Chen, et al., “Photothermal Effect of Carbon Dots for Boosted Photothermal-Assisted Photocatalytic Water/Seawater Splitting into Hydrogen,” Chemical Engineering Journal 453 (2023): 139834, https://doi.org/10.1016/j.cej.2022.139834.

[43]

K. Wang, R. Jiang, T. Peng, X. Chen, W. Dai, and X. Fu, “Modeling the Effect of Cu Doped TiO2 with Carbon Dots on CO2 Methanation by H2O in a Photo-Thermal System,” Applied Catalysis B: Environment and Energy 256 (2019): 117780, https://doi.org/10.1016/j.apcatb.2019.117780.

[44]

J. H. Zhang, J. C. Liu, X. Y. Wang, et al., “Construction of Z-Scheme Tungsten Trioxide Nanosheets-Nitrogen-Doped Carbon Dots Composites for the Enhanced Photothermal Synergistic Catalytic Oxidation of Cyclohexane,” Applied Catalysis B: Environment and Energy 259 (2019): 118063.

[45]

Q. Cheng, Z. Wang, X. Wang, J. Li, Y. Li, and G. Zhang, “A Novel Cu1.5Mn1.5O4 Photothermal Catalyst With Boosted Surface Lattice Oxygen Activation for Efficiently Photothermal Mineralization of Toluene,” Nano Research 16 (2023): 2133–2141, https://doi.org/10.1007/s12274-022-4946-6.

[46]

X. Wang, X. Feng, J. Liu, et al., “Photo-Thermo Catalytic Selective Oxidation of Cyclohexane by In-Situ Prepared Nonstoichiometric Molybdenum Oxide and Silver-Palladium Alloy Composite,” Journal of Colloid and Interface Science 607 (2022): 954–966, https://doi.org/10.1016/j.jcis.2021.09.058.

[47]

L. H. Kugelmass, C. Tagnon, and E. E. Stache, “Photothermal Mediated Chemical Recycling to Monomers via Carbon Quantum Dots,” Journal of the American Chemical Society 145 (2023): 16090–16097, https://doi.org/10.1021/jacs.3c04448.

[48]

D. S. Achilleos, W. Yang, H. Kasap, et al., “Solar Reforming of Biomass With Homogeneous Carbon Dots,” Angewandte Chemie, International Edition 59 (2020): 18184–18188, https://doi.org/10.1002/anie.202008217.

[49]

Z. Li, H. Lei, A. Kan, H. Xie, and W. Yu, “Photothermal Applications Based on Graphene and Its Derivatives: A State-of-the-Art Review,” Energy 216 (2021): 119262, https://doi.org/10.1016/j.energy.2020.119262.

[50]

S. Balou, P. Shandilya, and A. Priye, “Carbon Dots for Photothermal Applications,” Frontiers in Chemistry 10 (2022): 1023602, https://doi.org/10.3389/fchem.2022.1023602.

[51]

C. Claver, M. B. Yeamin, M. Reguero, and A. M. Masdeu-Bulto, “Recent Advances in the Use of Catalysts Based on Natural Products for the Conversion of CO2 Into Cyclic Carbonates,” Green Chemistry 22 (2020): 7665–7706, https://doi.org/10.1039/D0GC01870H.

[52]

K. R. Roshan, B. M. Kim, A. C. Kathalikkattil, J. Tharun, Y. S. Won, and D. W. Park, “The Unprecedented Catalytic Activity of Alkanolamine CO2 Scrubbers in the Cycloaddition of CO2 and Oxiranes: A DFT Endorsed Study,” Chemical Communications 50 (2014): 13664–13667, https://doi.org/10.1039/C4CC04195J.

[53]

M. Alves, B. Grignard, R. Méreau, C. Jerome, T. Tassaing, and C. Detrembleur, “Organocatalyzed Coupling of Carbon Dioxide with Epoxides for the Synthesis of Cyclic Carbonates: Catalyst Design and Mechanistic Studies,” Catalysis Science & Technology 7 (2017): 2651–2684, https://doi.org/10.1039/C7CY00438A.

[54]

J. Sheng, Y. He, J. Li, et al., “Identification of Halogen-Associated Active Sites on Bismuth-Based Perovskite Quantum Dots for Efficient and Selective CO2-to-CO Photoreduction,” ACS Nano 14 (2020): 13103–13114, https://doi.org/10.1021/acsnano.0c04659.

[55]

I. M. Garazade, R. K. Gupta, K. Singh, et al., “Insights Into the Catalytic Application of Coordinated Metal Complexes in CO2 Conversion via Cycloaddition,” Journal of Molecular Structure 1337 (2025): 142200, https://doi.org/10.1016/j.molstruc.2025.142200.

[56]

Y. Wang, H. Liu, Q. Shi, et al., “Single-Atom Titanium on Mesoporous Nitrogen, Oxygen-Doped Carbon for Efficient Photo-Thermal Catalytic CO2 Cycloaddition by a Radical Mechanism,” Angewandte Chemie, International Edition 63 (2024): e202404911, https://doi.org/10.1002/anie.202404911.

[57]

F. A. Villamena, E. J. Locigno, A. Rockenbauer, C. M. Hadad, and J. L. Zweier, “Theoretical and Experimental Studies of the Spin Trapping of Inorganic Radicals by 5,5-Dimethyl-1-Pyrroline N-Oxide (DMPO). 1. Carbon Dioxide Radical Anion,” Journal of Physical Chemistry A 110 (2006): 13253–13258, https://doi.org/10.1021/jp064892m.

[58]

L.-G. Ding, B.-J. Yao, W.-X. Wu, et al., “Metalloporphyrin and Ionic Liquid-Functionalized Covalent Organic Frameworks for Catalytic CO2 Cycloaddition via Visible-Light-Induced Photothermal Conversion,” Inorganic Chemistry 60 (2021): 12591–12601, https://doi.org/10.1021/acs.inorgchem.1c01975.

[59]

Z. Wang, T. Wang, Y. Zhao, Q. Ye, and P. He, “Photothermal CO2 Conversion to Cyclic Carbonate Over Titanium-Substituted Polyoxometalate Within Covalent Organic Frameworks,” Journal of Catalysis 442 (2025): 115908, https://doi.org/10.1016/j.jcat.2024.115908.

[60]

H. Zhang, G. Zhai, L. Lei, et al., “Photo-Induced Photo-Thermal Synergy Effect Leading to Efficient CO2 Cycloaddition with Epoxide over a Fe-Based Metal Organic Framework,” Journal of Colloid & Interface Science 625 (2022): 33–40, https://doi.org/10.1016/j.jcis.2022.05.146.

[61]

Y. Liu, Y. Chen, Y. Liu, et al., “Zn and N Co-Doped Porous Carbon Nanosheets for Photothermally-Driven CO2 Cycloaddition,” Journal of Catalysis 407 (2022): 65–76, https://doi.org/10.1016/j.jcat.2022.01.016.

[62]

L. P. Zhang, X. W. Tu, Y. T. Chen, et al., “Photothermal Catalysis Without Solvent for Fixing CO2 to Cyclic Carbonate,” Molecular Catalysis 538 (2023): 112971–112979.

[63]

W. Rong, M. Ding, Y. Wang, S. Kong, and J. Yao, “Porous Biochar with a Tubular Structure for Photothermal CO2 Cycloaddition: One-Step Doping Versus Two-Step Doping,” Separation and Purification Technology 353 (2025): 128427, https://doi.org/10.1016/j.seppur.2024.128427.

RIGHTS & PERMISSIONS

2026 The Author(s). Exploration published by Henan University and John Wiley & Sons Australia, Ltd.

PDF (2505KB)

2

Accesses

0

Citation

Detail

Sections
Recommended

/