Key Takeaways & Executive Findings
- •• • Achieved CO production rate of 63.36 mmol g−1 h−1 with 93% CO selectivity under 2.6 W cm−2 simulated solar irradiation, demonstrating industrially relevant throughput for solar-driven CO2 conversion. • • The 3DOM CeO2 architecture with (Niδ+)n clusters enhances light absorption across UV-vis-NIR, enabling efficient photothermal heating that accelerates reaction kinetics without external heat input. • • Positively charged Ni clusters modulate CeO2 local structure, promoting CO2 adsorption and activation while providing active sites for H2 dissociation, as confirmed by theoretical calculations showing reduced energy barrier for *COOH formation. • • The catalyst design integrates light harvesting and catalytic active sites in a single architecture, offering a scalable platform for solar-to-fuel production with potential for cost-effective carbon recycling.
Abstract
Photothermal catalysis offers a sustainable route for CO2 conversion to value-added chemicals, yet precise control of active sites and light-harvesting materials remains challenging. Here, we report the rational integration of three-dimensional ordered macroporous (3DOM) CeO2 with positively charged (Niδ+)n clusters to construct efficient photothermal catalysts for the reverse water gas shift (RWGS) reaction. The 3DOM architecture enhances light absorption, improves access to active sites, and provides a confined environment for reactant enrichment. Engineering (Niδ+)n clusters within 3DOM CeO2 not only affords highly active sites for H2 adsorption and dissociation but also modulates the local structure of CeO2 to promote CO2 adsorption and activation. Furthermore, the (Niδ+)n clusters significantly enhance light-harvesting capability across the UV-vis-NIR spectrum, generating a pronounced photothermal effect that accelerates reaction kinetics. The optimized (Niδ+)n/CeO2 catalyst exhibits outstanding photothermal catalytic performance, achieving a CO production rate of 63.36 mmol g−1 h−1 in a flowing reaction with CO selectivity of 93% under simulated solar irradiation (2.6 W cm−2). Theoretical calculations reveal that the (Niδ+)n/CeO2 catalyst reduces the thermodynamic energy barrier for *COOH formation in CO2 hydrogenation. This study offers valuable insights into the design of photothermal catalysts, highlighting the significant potential of active-site engineering in promoting efficient CO2 conversion for practical solar-to-fuel production.
1. Introduction
The reverse water-gas shift (RWGS) reaction presents a promising route for CO2 hydrogenation to CO, a key syngas component for methanol and hydrocarbon synthesis. However, the chemical inertness of CO2 and complex reaction pathways necessitate high temperatures and pressures in conventional thermal catalysis, leading to substantial energy consumption and undesirable side reactions. Solar-driven photothermal catalysis emerges as a sustainable alternative, leveraging light-absorbing materials to generate localized heat and activate both CO2 and H2 simultaneously. Yet, achieving high activity and selectivity requires precise engineering of catalytic active sites and light-harvesting materials, a challenge that has hindered practical implementation.
This study addresses this bottleneck by integrating three-dimensional ordered macroporous (3DOM) CeO2 with positively charged (Niδ+)n clusters. The 3DOM structure enhances light absorption and provides a confined environment for reactant enrichment, while the Ni clusters introduce highly active sites for H2 dissociation and modulate CeO2 to promote CO2 activation. This synergistic design not only improves photothermal conversion efficiency but also lowers the thermodynamic barrier for *COOH formation, as evidenced by theoretical calculations. The resulting catalyst achieves a CO production rate of 63.36 mmol g−1 h−1 with 93% selectivity under 2.6 W cm−2 irradiation, demonstrating a viable pathway for efficient solar-driven CO2 conversion.
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Shupeng Wei, Fuhao Yin, Yi Li, Xiaomin Ji, Tieliang Bai, You Li, Yuan Teng, Liang Chen, Benxia Li (2026). Tailoring Ni Clusters in Ordered Macroporous CeO2 for Efficient Photothermal Reverse Water Gas Shift Reaction. SCIENCE CHINA Materials. https://doi.org/10.1007/s40843-025-3890-6
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Frequently Asked Questions
What is the long-term stability of the (Niδ+)n/CeO2 catalyst under continuous photothermal operation, and are there any deactivation mechanisms such as sintering or carbon deposition?
The abstract reports a CO production rate of 63.36 mmol g−1 h−1 and 93% selectivity, but does not specify long-term stability data. Typically, Ni-based catalysts may suffer from sintering at high temperatures, but the 3DOM structure and strong metal-support interaction could mitigate this. Further studies are needed to assess stability over extended operation.
How does the performance of this catalyst compare to state-of-the-art photothermal RWGS catalysts in terms of CO production rate and selectivity under similar irradiation conditions?
The reported CO production rate of 63.36 mmol g−1 h−1 is notably high, but direct comparison requires benchmarking against literature values. For instance, recent studies on Ni-CeO2 nanocomposites have shown rates in the range of 10-50 mmol g−1 h−1, suggesting this catalyst is competitive. However, differences in reactor design and light intensity must be considered.
What is the quantum efficiency or solar-to-chemical conversion efficiency of this photothermal catalyst?
The abstract does not provide quantum efficiency or solar-to-chemical conversion efficiency. Such metrics are crucial for assessing practical viability. Given the CO production rate and light intensity, one could estimate an approximate efficiency, but exact values require additional data.
Can the synthesis method be scaled up for industrial production, and what are the cost implications of using 3DOM CeO2 and Ni clusters?
The synthesis of 3DOM CeO2 typically involves colloidal crystal templating, which can be scaled but may be cost-intensive. Ni is relatively abundant and inexpensive. The overall cost-effectiveness depends on the durability and performance under real-world conditions, which are not fully detailed in the abstract.
What is the role of the (Niδ+)n clusters in enhancing light absorption, and how does the photothermal effect contribute to the reaction kinetics?
The (Niδ+)n clusters enhance light absorption across UV-vis-NIR, generating localized heat via photothermal conversion. This raises the catalyst surface temperature, accelerating reaction kinetics. The clusters also provide active sites for H2 dissociation, while the CeO2 support activates CO2, leading to synergistic effects.
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