Authors
Chengsheng Yang, Bo Wu, Huimin Xu, Doudou Hu, Xiwen Song, Ziang Liu, Yifeng Zhu, Sai Chen, Chunlei Pei, Jinlong Gong
Published in
Science advances. Volume 12. Issue 34. Pages eaeg1076. Aug 21, 2026. Epub Aug 19, 2026.
Abstract
Direct hydrogenation of carbon dioxide (CO2 ) to acetic acid, a key commodity chemical, offers a sustainable route to valorize greenhouse gases but is plagued by CO2 inertness, thermodynamic barriers, and poor selectivity for C-C coupling over competing overhydrogenation. This paper describes the design and synthesis of ultrathin cobalt(II) oxide nanosheets (<4 nm thick) that achieve direct one-step CO2 hydrogenation to acetic acid with over 90% selectivity, minimal C1 by-products and the highest reported yield under mild conditions, surpassing traditional multistep routes (such as CO2 to CO/methanol followed by carbonylation) in cost, efficiency, and atom economy. These two-dimensional structures feature extended terraces that undergo in situ reconstruction in CO2/H2 mixtures to a cobalt(II) carbonate hydroxide-like phase, stabilizing Co2+ and generating abundant hydroxyl groups to optimize CO2 activation and selective C-C coupling while suppressing over-reduction. In situ characterizations, including electron energy-loss near-edge structure, spatially resolved infrared spectroscopy, and kinetic/isotopic analyses, reveal the reconstructed phase's role in modulating electron density for superior yields and confirm a formate-coupling mechanism unattainable with conventional catalysts. This study introduces a paradigm for CO2 upgrading: harnessing dynamic surface reconstructions and nanoscale morphology to access elusive multicarbon pathways, with implications for sustainable chemical synthesis.
PMID:
42616894
Bibliographic data and abstract were imported from PubMed on 20 Aug 2026.
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