Advancing CO2 Valorization Beyond C2 Products.

Journal: ACS nano
Published Date:

Abstract

The catalytic valorization of carbon dioxide (CO2) has attracted extensive attention as a promising route to mitigate greenhouse gas emissions while producing value-added chemicals. Significant progress has been achieved in the selective reduction of CO2 to C1 and C2 products such as CO, CH4, HCOO-, C2H4, and C2H5OH through precise control of catalysts and reaction environments within single-batch systems. However, the formation of higher-order carbon products (C3+) remains a major challenge because it requires complex multielectron and multiproton transfer steps, typically involving 18-20 electrons and protons for intermediates such as propanol or propylene. These demanding reaction pathways lead to sluggish C-C-C coupling kinetics and limited energy utilization under conventional single-cell configurations. Recent advances have focused on multibatch cascade catalytic systems that integrate thermochemical, photochemical, and electrochemical processes to overcome these intrinsic barriers. By enabling the stepwise conversion of CO2-derived intermediates, such hybrid platforms improve selectivity and efficiency toward C3+ products that are difficult to achieve in single-batch systems. Nevertheless, the integration of distinct reaction environments introduces challenges, including intermediate loss between reactors and reduced overall energy efficiency. This review provides a comprehensive overview of cascade strategies for CO2 conversion, emphasizing mechanistic understanding, reactor design, and operando characterization. The discussion aims to guide the rational design of next-generation catalytic architectures capable of achieving efficient and scalable C3+ production from CO2 through improved control of multistep extended hybrid reaction pathways and interfacial energy management.

Authors

  • Seyoon Kim
    SKKU Advanced Institute of Nanotechnology and Department of Nanoengineering, Sungkyunkwan University, Suwon 16419, Republic of Korea.
  • Hyung Il Lee
    SKKU Advanced Institute of Nanotechnology and Department of Nanoengineering, Sungkyunkwan University, Suwon 16419, Republic of Korea.
  • Soon-Ho Kwon
    Materials and Process Simulation Center (MSC), California Institute of Technology, Pasadena, California 91125, United States.
  • Jin-Wook Lee
    SKKU Advanced Institute of Nanotechnology and Department of Nanoengineering, Sungkyunkwan University, Suwon 16419, Republic of Korea.
  • I I Jeon
    SKKU Advanced Institute of Nanotechnology and Department of Nanoengineering, Sungkyunkwan University, Suwon 16419, Republic of Korea.
  • Hyung-Suk Oh
    Clean Energy Research Center, Korea Institute of Science and Technology (KIST), Seoul 02792, Republic of Korea.
  • Michael Grätzel
    Laboratory of Photonics and Interfaces, Institute of Chemical Sciences and Engineering, École Polytechnique Fédérale deLausanne (EPFL), 1015 Lausanne, Switzerland.
  • William A Goddard
    Materials and Process Simulation Center (MSC), California Institute of Technology, Pasadena, California 91125, United States.
  • Chungseok Choi
    SKKU Advanced Institute of Nanotechnology and Department of Nanoengineering, Sungkyunkwan University, Suwon 16419, Republic of Korea.

Keywords

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