Photochemical H <sub>2</sub> dissociation for nearly quantitative CO <sub>2</sub> reduction to ethylene

Producing olefins by carbon dioxide (CO<sub>2</sub>) hydrogenation is a long-standing goal. The usual products are multicarbon mixtures because the critical step of heterolytic hydrogen (H<sub>2</sub>) dissociation at high temperatures complicates selectivity control. In this study, we report that irradiating gold-titanium dioxide at 365 nanometers induces heterolytic H<sub>2</sub> dissociation at ambient temperature. This process likely relies on interfacial electric dipoles from photogenerated electrons and holes situated on the metallic gold nanoparticles and interfacial gold-oxygen-titanium scaffolds. The heterolytic H<sub>2</sub> dissociation is further promoted by light-induced coating of gold nanoparticles with a titanium oxide layer. The resulting nucleophilic hydrogen species reduce CO<sub>2</sub> to ethane in >99% yield under light irradiation in a flow apparatus. Furthermore, cascading with a subsequent photocatalytic ethane dehydrogenation generates ethylene in >99% yield over 1500 hours of irradiation.

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Publication Details

Journal
Science
Published
2025-09-04
DOI
https://doi.org/10.1126/science.adq3445
Citations
27
Primary Topic
CO2 Reduction Techniques and Catalysts
Type
article
Field-Weighted Citation Impact
9.81
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article

Photochemical H 2 dissociation for nearly quantitative CO 2 reduction to ethylene

Ruotian Chen, Jianping Xiao, Pu Guo, Chenwei Ni et al.
27 citations
Science
CO2 Reduction Techniques and Catalysts
9.81
article

Photochemical H 2 dissociation for nearly quantitative CO 2 reduction to ethylene

Ruotian Chen, Jianping Xiao, Pu Guo, Chenwei Ni, Guoxiong Wang, Nengchao Luo, Fuxiang Zhang, Feng Wang, Paolo Fornasiero, Ping Jin, Rengui Li, Hui Zhang, Wei Liu
article en
27 citations

Abstract

Producing olefins by carbon dioxide (CO<sub>2</sub>) hydrogenation is a long-standing goal. The usual products are multicarbon mixtures because the critical step of heterolytic hydrogen (H<sub>2</sub>) dissociation at high temperatures complicates selectivity control. In this study, we report that irradiating gold-titanium dioxide at 365 nanometers induces heterolytic H<sub>2</sub> dissociation at ambient temperature. This process likely relies on interfacial electric dipoles from photogenerated electrons and holes situated on the metallic gold nanoparticles and interfacial gold-oxygen-titanium scaffolds. The heterolytic H<sub>2</sub> dissociation is further promoted by light-induced coating of gold nanoparticles with a titanium oxide layer. The resulting nucleophilic hydrogen species reduce CO<sub>2</sub> to ethane in >99% yield under light irradiation in a flow apparatus. Furthermore, cascading with a subsequent photocatalytic ethane dehydrogenation generates ethylene in >99% yield over 1500 hours of irradiation.

ScienceVol. 389(6764)
University of Trieste (IT), Dalian Institute of Chemical Physics (CN), Chinese Academy of Sciences (CN), Fudan University (CN), Shanghai Advanced Research Institute (CN), Dalian National Laboratory for Clean Energy (CN), Shanghai Institute of Microsystem and Information Technology (CN), University of Chinese Academy of Sciences (CN)
Openalex Percentile: Top 1%
CO2 Reduction Techniques and Catalysts
9.81
DOIOpen Access PDFOpenAlex
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