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 Ni3InC0.5 nanoparticles, leading to the formation of defective In2O3-x overlayers and inverse In2O3-x/Ni interfaces, driven by CO2-induced selective surface oxidation during CO2 hydrogenation. The synergy between In2O3-x overlayers and inverse In2O3-x/Ni interfaces facilitates CO2 adsorption and activation, as well as the following hydrogenation of HCOO and CHxO intermediates, enabling efficient methanol synthesis from CO2. Accordingly, the optimized LDH-NiInCAl catalyst achieves an impressive CO2 conversion of 19% with 65% methanol selectivity and 508.4 <InlineEquation ID="IEq1"> <EquationSource Format="TEX">${{\rm{mg}}}{{{\rm{g}}}}_{{{\rm{cat}}}}^{-1}{{{\rm{h}}}}^{-1}$</EquationSource> <EquationSource Format="MATHML"><math> <mi mathvariant="normal">mg</mi> <msubsup> <mrow> <mi mathvariant="normal">g</mi> </mrow> <mrow> <mi mathvariant="normal">cat</mi> </mrow> <mrow> <mo>−</mo> <mn>1</mn> </mrow> </msubsup> <msup> <mrow> <mi mathvariant="normal">h</mi> </mrow> <mrow> <mo>−</mo> <mn>1</mn> </mrow> </msup> </math></EquationSource> </InlineEquation> methanol space-time yield at 260 °C, 5 MPa, and 12000 <InlineEquation ID="IEq2"> <EquationSource Format="TEX">${{\rm{mL}}}{{{\rm{g}}}}_{{{\rm{cat}}}}^{-1}{{{\rm{h}}}}^{-1}$</EquationSource> <EquationSource Format="MATHML"><math> <mi mathvariant="normal">mL</mi> <msubsup> <mrow> <mi mathvariant="normal">g</mi> </mrow> <mrow> <mi mathvariant="normal">cat</mi> </mrow> <mrow> <mo>−</mo> <mn>1</mn> </mrow> </msubsup> <msup> <mrow> <mi mathvariant="normal">h</mi> </mrow> <mrow> <mo>−</mo> <mn>1</mn> </mrow> </msup> </math></EquationSource> </InlineEquation>, outperforming commercial Cu/ZnO/Al2O3 catalysts. This work showcases how structural evolution and surface reconstruction enhance catalytic performance, providing new insights into the dynamic structure-activity relationship.

Inverse In₂O_3-x/Ni interfaces via Ni₃InC_0.5 surface reconstruction for efficient CO₂ hydrogenation to methanol

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2025年12月8日

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Jiyi Chen,
Tiantian Xiao,
Bingqing Yao,
Maoshuai Li,
Heng Zhang,
Mingwu Tan,
Shibo Xi,
Shixiong Tang,
Wenyan Jia,
Qi Yang,
Ziwen Hao,
Zhenmei Zhang,
Kang Hui Lim,
Xiaoyu Han,
Xiaohui Zi,
Yue Wang,
Jing Lv,
Qian He,
Yong Wang,
Sibudjing Kawi,
Xinbin Ma

摘要

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 Ni₃InC_0.5 nanoparticles, leading to the formation of defective In₂O_3-x overlayers and inverse In₂O_3-x/Ni interfaces, driven by CO₂-induced selective surface oxidation during CO₂ hydrogenation. The synergy between In₂O_3-x overlayers and inverse In₂O_3-x/Ni interfaces facilitates CO₂ adsorption and activation, as well as the following hydrogenation of HCOO^* and CH_xO^* intermediates, enabling efficient methanol synthesis from CO₂. Accordingly, the optimized LDH-NiInCAl catalyst achieves an impressive CO₂ conversion of 19% with 65% methanol selectivity and 508.4 ${{\rm{mg}}}{{{\rm{g}}}}_{{{\rm{cat}}}}^{-1}{{{\rm{h}}}}^{-1}$ $mg g_{cat}^{- 1} h^{- 1}$ methanol space-time yield at 260 °C, 5 MPa, and 12000 ${{\rm{mL}}}{{{\rm{g}}}}_{{{\rm{cat}}}}^{-1}{{{\rm{h}}}}^{-1}$ $mL g_{cat}^{- 1} h^{- 1}$ , outperforming commercial Cu/ZnO/Al₂O₃ catalysts. This work showcases how structural evolution and surface reconstruction enhance catalytic performance, providing new insights into the dynamic structure-activity relationship.

Inverse In2O3-x/Ni interfaces via Ni3InC0.5 surface reconstruction for efficient CO2 hydrogenation to methanol

摘要

Inverse In₂O_3-x/Ni interfaces via Ni₃InC_0.5 surface reconstruction for efficient CO₂ hydrogenation to methanol