Inverse In<sub>2</sub>O<sub>3-x</sub>/Ni interfaces via Ni<sub>3</sub>InC<sub>0.5</sub> surface reconstruction for efficient CO<sub>2</sub> hydrogenation to methanol.
basic_science · Level V
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- Record sourced from PubMed, PMID 41360783.
- Also identified by DOI 10.1038/s41467-025-65929-z and PMC identifier 12686540.
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Abstract
Catalyst surface reconstruction under reaction conditions is ubiquitous and crucial for creating unusual active sites, thereby enhancing catalytic performance. Here, we report the surface reconstruction of supported Ni<sub>3</sub>InC<sub>0.5</sub> nanoparticles, leading to the formation of defective In<sub>2</sub>O<sub>3-x</sub> overlayers and inverse In<sub>2</sub>O<sub>3-x</sub>/Ni interfaces, driven by CO<sub>2</sub>-induced selective surface oxidation during CO<sub>2</sub> hydrogenation. The synergy between In<sub>2</sub>O<sub>3-x</sub> overlayers and inverse In<sub>2</sub>O<sub>3-x</sub>/Ni interfaces facilitates CO<sub>2</sub> adsorption and activation, as well as the following hydrogenation of HCOO<sup>*</sup> and CH<sub>x</sub>O<sup>*</sup> intermediates, enabling efficient methanol synthesis from CO<sub>2</sub>. Accordingly, the optimized LDH-NiInCAl catalyst achieves an impressive CO<sub>2</sub> conversion of 19% with 65% methanol selectivity and 508.4 <math xmlns="http://www.w3.org/1998/Math/MathML"><mi>mg</mi> <msubsup><mrow><mi>g</mi></mrow> <mrow><mi>cat</mi></mrow> <mrow><mo>-</mo> <mn>1</mn></mrow> </msubsup> <msup><mrow><mi>h</mi></mrow> <mrow><mo>-</mo> <mn>1</mn></mrow> </msup> </math> methanol space-time yield at 260 °C, 5 MPa, and 12000 <math xmlns="http://www.w3.org/1998/Math/MathML"><mi>mL</mi> <msubsup><mrow><mi>g</mi></mrow> <mrow><mi>cat</mi></mrow> <mrow><mo>-</mo> <mn>1</mn></mrow> </msubsup> <msup><mrow><mi>h</mi></mrow> <mrow><mo>-</mo> <mn>1</mn></mrow> </msup> </math> , outperforming commercial Cu/ZnO/Al<sub>2</sub>O<sub>3</sub> catalysts. This work showcases how structural evolution and surface reconstruction enhance catalytic performance, providing new insights into the dynamic structure-activity relationship.