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<p>Adjusting the structure and composition of active sites is a highly effective method for activating linear CO<sub>2</sub> molecules. Nonetheless, precise control of interfacial chemistry within molecular-scale environments presents a significant challenge in heterogeneous catalysis. In our study, we present symmetry-broken Mo-O-Co triple-atom active sites within the hybrid zeolite imidazole framework HZIF-CoMo. These sites disrupt the electronic balance and create a weak built-in electric field, thus promoting photocatalytic CO<sub>2</sub> reduction. The CO yield over HZIF-CoMo is improved to 3.1 mmol g<sup>−1</sup> h<sup>−1</sup>, which is over four times higher than the parent cobalt-imidazole framework MAF-6-Co. Both experimental and theoretical studies indicate that electronic modulation through the symmetry-breaking Mo-O-Co moiety acts as an organizing knob to accelerate charge separation and result in more carriers participating in the catalytic reaction. This work provides important insights into optimizing site-related electronic structures for targeted photocatalytic reactions.</p>

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Breaking the structural symmetry of active sites in zeolite imidazolate framework for enhanced CO2 photoreduction

  • 期刊论文

  • 发表日期：

    2025年1月3日

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  • Yupeng Han,
  • Yayu Yan,
  • Qiaohong Li,
  • Xin Wu,
  • Fei Wang,
  • Jian Zhang

摘要

Adjusting the structure and composition of active sites is a highly effective method for activating linear CO2 molecules. Nonetheless, precise control of interfacial chemistry within molecular-scale environments presents a significant challenge in heterogeneous catalysis. In our study, we present symmetry-broken Mo-O-Co triple-atom active sites within the hybrid zeolite imidazole framework HZIF-CoMo. These sites disrupt the electronic balance and create a weak built-in electric field, thus promoting photocatalytic CO2 reduction. The CO yield over HZIF-CoMo is improved to 3.1 mmol g−1 h−1, which is over four times higher than the parent cobalt-imidazole framework MAF-6-Co. Both experimental and theoretical studies indicate that electronic modulation through the symmetry-breaking Mo-O-Co moiety acts as an organizing knob to accelerate charge separation and result in more carriers participating in the catalytic reaction. This work provides important insights into optimizing site-related electronic structures for targeted photocatalytic reactions.