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<p>Chemical looping hydrogen production (CLHP) is a highly efficient and low-carbon technology that enables continuous hydrogen production. It is based on the transfer of oxygen atoms between two or three reactors using an oxygen carrier as an intermediate medium to produce high-value-added syngas and high-purity hydrogen. This study begins with a brief overview of the technical principles and key advantages of methane chemical looping reforming for hydrogen production. Based on the Web of Science Core Collection database, bibliometric keyword clustering analysis was employed to identify trends in oxygen carrier materials within the chemical looping hydrogen production field, with a particular focus on progress in the modification and design of Fe-, Ni-, and Cu-based, and composite mineral oxygen carriers. Furthermore, by systematically collating previously reported density functional theory (DFT) calculation data, a comparative analysis of the differences in key thermodynamic and kinetic parameters among various oxygen carriers, including the reaction activation energy, oxygen vacancy formation energy, and adsorption energies of reactants and intermediates, was performed. Finally, the review systematically summarizes the mechanisms by which preparation methods regulate the microstructure and redox properties of oxygen carriers, aiming to provide a reference for the rational design and controlled synthesis of high-performance oxygen carriers, fill gaps in existing reviews, and offer cutting-edge systematic reference material for future research into chemical looping hydrogen production technology.</p> Graphical Abstract <p>This illustrated summary builds upon the core technical principles to explore strategies for oxygen carrier modification, mainstream hydrogen production methods, and the preparation techniques for high-performance oxygen carriers. Within this framework, this study first systematically reviews the technical principles and core advantages of methane-based chemical looping hydrogen production. Subsequently, focusing on the design and modification of oxygen carriers, three major strategies are introduced: inert carrier doping, addition of active components, and microstructural regulation. Furthermore, it conducts a comparative analysis of the key parameters of different oxygen carriers using DFT calculation data. Finally, this study summarizes the preparation methods and characteristics of high-performance oxygen carriers, including the sol–gel (SG) method, impregnation method (IM), spray drying (SD), mechanical mixing (MM), freeze granulation (FG), and coprecipitation (CP). Particular emphasis is placed on multiscale regulation methods for oxygen carriers, providing a reference for the rational design and controlled synthesis of high-performance oxygen carriers in the future.</p>

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Progress and Challenges in Chemical Looping Hydrogen Production Technology and Oxygen Carrier Development: A Review

  • 期刊论文

  • 发表日期：

    2026年6月20日

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  • Chunhuan Deng,
  • Zisheng Ding,
  • Hao Ma,
  • Liangnuo Yang,
  • Yifeng Cheng,
  • Dingyuan Feng,
  • Danyang Li,
  • Ming Li,
  • Zhenhua Gu

摘要

Chemical looping hydrogen production (CLHP) is a highly efficient and low-carbon technology that enables continuous hydrogen production. It is based on the transfer of oxygen atoms between two or three reactors using an oxygen carrier as an intermediate medium to produce high-value-added syngas and high-purity hydrogen. This study begins with a brief overview of the technical principles and key advantages of methane chemical looping reforming for hydrogen production. Based on the Web of Science Core Collection database, bibliometric keyword clustering analysis was employed to identify trends in oxygen carrier materials within the chemical looping hydrogen production field, with a particular focus on progress in the modification and design of Fe-, Ni-, and Cu-based, and composite mineral oxygen carriers. Furthermore, by systematically collating previously reported density functional theory (DFT) calculation data, a comparative analysis of the differences in key thermodynamic and kinetic parameters among various oxygen carriers, including the reaction activation energy, oxygen vacancy formation energy, and adsorption energies of reactants and intermediates, was performed. Finally, the review systematically summarizes the mechanisms by which preparation methods regulate the microstructure and redox properties of oxygen carriers, aiming to provide a reference for the rational design and controlled synthesis of high-performance oxygen carriers, fill gaps in existing reviews, and offer cutting-edge systematic reference material for future research into chemical looping hydrogen production technology.

Graphical Abstract

This illustrated summary builds upon the core technical principles to explore strategies for oxygen carrier modification, mainstream hydrogen production methods, and the preparation techniques for high-performance oxygen carriers. Within this framework, this study first systematically reviews the technical principles and core advantages of methane-based chemical looping hydrogen production. Subsequently, focusing on the design and modification of oxygen carriers, three major strategies are introduced: inert carrier doping, addition of active components, and microstructural regulation. Furthermore, it conducts a comparative analysis of the key parameters of different oxygen carriers using DFT calculation data. Finally, this study summarizes the preparation methods and characteristics of high-performance oxygen carriers, including the sol–gel (SG) method, impregnation method (IM), spray drying (SD), mechanical mixing (MM), freeze granulation (FG), and coprecipitation (CP). Particular emphasis is placed on multiscale regulation methods for oxygen carriers, providing a reference for the rational design and controlled synthesis of high-performance oxygen carriers in the future.