Xi Chen,Wei Zhou,Xu Fang,Cheng Li,Die Cong,Tie Yu,Wei-Qiao Deng,Chengcheng Liu
Photocatalytic CO2 reduction to syngas has recently garnered substantial interest due to its mild reaction conditions, high safety, and environmental sustainability. However, the efficiency of syngas production remains relatively low. In this study, we have developed metallosalen-based poly(ionic liquid)s (PILs) to enhance syngas production, achieving one of the highest production rates recorded to date. The Co(Salen)-PIL demonstrates a syngas production rate of 168.1 mmol g−1 h−1, including a CO production rate of 69.3 mmol g−1 h−1, which is more than eight times higher than that of the best previously reported organic materials. Mechanistic investigations reveal that pyridine ions facilitate electron transfer from the heptazine light-harvester to the Co(Salen) active site. This study lays the groundwork for developing high-performance catalysts for photocatalytic syngas production.
A series of effective heterogeneous catalysts, Cu or Ni salen with various loadings encapsulated in amino functionalized MOFs, were synthesized successfully for the first time via a one-pot method and denoted as metal salen@NH2-MIL-101(Cr). On the basis of detailed characterization of the catalysts, the varying coordination abilities between the Cu or Ni salen and NH2-MIL-101(Cr) provided the as-prepared Cu or Ni salen@NH2-MIL-101(Cr) with distinct activities toward styrene oxidation. The catalytic results showed that the introduction of Cu or Ni salen can significantly promote the selectivity to epoxide. However, Cu salen@NH2-MIL-101(Cr) showed preferable activity for styrene oxidation, and phenylacetaldehyde was generated with increasing Cu salen content. The optimal conditions for the reaction were also discussed, including the types of oxidants present, molar ratios of styrene and TBHP, and temperature. In particular, the mechanism of the styrene oxidation in 70% TBHP over Cu salen@NH2-MIL-101(Cr) was proposed in this work.
Metal-Salen (M = Fe, Co, Ni, Cu, Zn) complexes were synthesized to catalyze the oxidation of benzoin to benzil with air as the “green” oxidizing reagent. The effects of temperature, base and solvent on M-Salen catalyzed oxidation of benzoin had been examined and optimized. The catalysis results showed that Co-Salen and Fe-Salen complexes were efficient to catalyze the oxidation reaction with yields over 80% while the catalytic activities of other three M-Salen complexes were poor. Moreover, the Co-Salen catalysis system could be reused three times with satisfied yield.
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