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<p>Photocatalytic reduction of CO<sub>2</sub> to natural gas using water vapor is a promising strategy for carbon recycling and renewable energy storage. However, the selectivity of current catalysts still remains a big challenge. Herein, we construct IrCu alloys on TiO<sub>2</sub> nanosheets to promote photocatalytic CO<sub>2</sub> to methane with 98.6% selectivity and 7.9% quantum efficiency at 365 nm under non-sacrificial ambient conditions. The performance is competitive with most other reported metal-based photocatalysts. Experimental and theoretical calculations demonstrate that the intensive H<sub>2</sub>O adsorption on Ir/TiO<sub>2</sub> hinders *H transfer, inevitably generating the H<sub>2</sub> by-product. Conversely, hydrophobic Cu effectively optimizes the interfacial hydrogen-bond network on IrCu/TiO<sub>2</sub>, predominantly in H-down configurations for H<sub>2</sub>O adsorption on the asymmetric charge-polarized Cu<sup>δ+</sup>-Ir<sup>δ-</sup> structure, which facilitates the kinetic migration of dissociated *H to *CO-Cu sites, resulting in the reduced energy barrier for the key *CHO intermediate. This finding enables high CH<sub>4</sub> selectivity on IrCu/TiO<sub>2</sub>, deepening our understanding of gas-solid interfacial water vapor in the enhanced natural gas synthesis.</p>

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Asymmetric charge-polarization tailoring active hydrogen transfer for selective photoreduction CO2 to CH4

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年4月10日

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  • Chenxu Yin,
  • Zhecheng Sun,
  • Kunlin Tang,
  • Weixin Zou,
  • Haiqin Wan,
  • Zhao-Qing Liu,
  • Lin Dong

摘要

Photocatalytic reduction of CO2 to natural gas using water vapor is a promising strategy for carbon recycling and renewable energy storage. However, the selectivity of current catalysts still remains a big challenge. Herein, we construct IrCu alloys on TiO2 nanosheets to promote photocatalytic CO2 to methane with 98.6% selectivity and 7.9% quantum efficiency at 365 nm under non-sacrificial ambient conditions. The performance is competitive with most other reported metal-based photocatalysts. Experimental and theoretical calculations demonstrate that the intensive H2O adsorption on Ir/TiO2 hinders *H transfer, inevitably generating the H2 by-product. Conversely, hydrophobic Cu effectively optimizes the interfacial hydrogen-bond network on IrCu/TiO2, predominantly in H-down configurations for H2O adsorption on the asymmetric charge-polarized Cuδ+-Irδ- structure, which facilitates the kinetic migration of dissociated *H to *CO-Cu sites, resulting in the reduced energy barrier for the key *CHO intermediate. This finding enables high CH4 selectivity on IrCu/TiO2, deepening our understanding of gas-solid interfacial water vapor in the enhanced natural gas synthesis.