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Open Access Publications from the University of California

Tuning Internal Strain in Metal-Organic Frameworks via Vapor Phase Infiltration for CO2 Reduction.

  • Author(s): Yang, Fan;
  • Hu, Wenhui;
  • Yang, Chongqing;
  • Patrick, Margaret;
  • Cooksy, Andrew L;
  • Zhang, Jian;
  • Aguiar, Jeffery A;
  • Fang, Chengcheng;
  • Zhou, Yinghua;
  • Meng, Ying Shirley;
  • Huang, Jier;
  • Gu, Jing
  • et al.

A gas-phase approach to form Zn coordination sites on metal-organic frameworks (MOFs) by vapor-phase infiltration (VPI) was developed. Compared to Zn sites synthesized by the solution-phase method, VPI samples revealed approximately 2.8 % internal strain. Faradaic efficiency towards conversion of CO2 to CO was enhanced by up to a factor of four, and the initial potential was positively shifted by 200-300 mV. Using element-specific X-ray absorption spectroscopy, the local coordination environment of the Zn center was determined to have square-pyramidal geometry with four Zn-N bonds in the equatorial plane and one Zn-OH2 bond in the axial plane. The fine-tuned internal strain was further supported by monitoring changes in XRD and UV/Visible absorption spectra across a range of infiltration cycles. The ability to use internal strain to increase catalytic activity of MOFs suggests that applying this strategy will enhance intrinsic catalytic capabilities of a variety of porous materials.

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