Au supported defect free TS-1 for enhanced performance of gas phase propylene epoxidation with H<sub>2</sub> and O<sub>2</sub>

Li, Wenqian; Qiu, Minghuang; Li, Wanting; Ge, Lixia; Zhang, Kun; Chen, Xinqing

doi:10.1039/d2se00365a

Cited by 6 publications

(6 citation statements)

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“…At 200 °C, the PO selectivity of 76.8% was obtained with a propylene conversion of 6.8%, giving a PO formation rate of 151.9 g/(h·kg cat ). According to our previous work, at the same temperature, the Au/TS-1 catalyst exhibited a PO selectivity of 93.32%, propylene conversion of 4.81%, H 2 efficiency of 32.5%, and PO formation rate of 73.44 g/(h·Kg cat ). The PO formation rate on Ni/TS-1 was much higher than that of the Au/TS-1 catalyst under the same condition (Figure a).…”

Section: Resultsmentioning

confidence: 61%

Section: Resultsmentioning

confidence: 99%

“…The TS-1 zeolite was synthesized by the hydrothermal method with TPAOH as the template and urea as the additive according to our previous research . As-prepared TS-1 zeolite was calcined at 550 °C for 6 h to remove the templating agent.…”

Section: Methodsmentioning

confidence: 99%

“…Before the catalytic evaluation, the catalysts were pretreated with 5 vol % H 2 in Ar for 6 h at up to 500 °C (10 °C/min). In contrast, the Au/TS-1 catalyst was synthesized reported in our previous work …”

Section: Methodsmentioning

confidence: 99%

“…The TS-1 zeolite was synthesized by the hydrothermal method with TPAOH as the template and urea as the additive according to our previous research. 46 As-prepared TS-1 zeolite was calcined at 550 °C for 6 h to remove the templating agent. The TS-1-supported Ni NP catalysts were prepared using the deposition precipitation method (DP) with NaOH as the precipitator.…”

Section: Methodsmentioning

confidence: 99%

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Highly Efficient Epoxidation of Propylene with In Situ-Generated H₂O₂ over a Hierarchical TS-1 Zeolite-Supported Non-Noble Nickel Catalyst

Qiu

et al. 2023

ACS Catal.

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Propylene epoxidation with H 2 and O 2 to propylene oxide (PO) is a very valuable reaction. Considering the precious gold catalysts commonly used in the current research, the design of highly active non-noble metal catalysts is a huge challenge. Herein, we report a non-noble Ni/TS-1 catalyst, supported Ni nanoparticles on a hierarchical titanium silicate-1 (TS-1) zeolite by the deposition precipitation method, which exhibits desirable catalytic performance in the gas-phase epoxidation of propylene due to the strong metal−support interaction between Ni NPs and TS-1. Significantly, the prepared 2%Ni/TS-1 exhibited high PO selectivity of 76.8%, PO formation rate of 151.9 g PO /(h•Kg cat ), and long-term stability at 200 °C. Notably, the catalytic performance of Ni/TS-1 is higher than that of the goldbased catalyst in the same condition. Furthermore, the reaction mechanism was investigated by various characterizations, including high-resolution transmission electron microscopy (HR-TEM), extended X-ray absorption fine structure (EXAFS), in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), and in situ electron paramagnetic resonance (EPR), proving that metallic Ni was the dominant nickel species, and the presence of nickel species was found to catalyze the reaction between hydrogen and oxygen, which could induce the formation of active radicals ( • O 2 − , and • OOH) to achieve the in situ synthesis of H 2 O 2 and subsequently oxidize propylene to PO. In addition, density functional theory (DFT) calculations indicated that the passivation layer on the Ni surface facilitates the production of H 2 O 2 . This work provides a promising way for the highly efficient catalyst on the selective oxidation with non-noble metals.

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Section: Resultsmentioning

confidence: 61%

Section: Resultsmentioning

confidence: 99%

Section: Methodsmentioning

confidence: 99%

Section: Methodsmentioning

confidence: 99%

Section: Methodsmentioning

confidence: 99%

See 3 more Smart Citations

Highly Efficient Epoxidation of Propylene with In Situ-Generated H₂O₂ over a Hierarchical TS-1 Zeolite-Supported Non-Noble Nickel Catalyst

Qiu

et al. 2023

ACS Catal.

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Recent Advances in the Synthesis and Application of TS‐1 Zeolite for Green Catalytic Oxidation

Wang,

Duan,

et al. 2024

Advanced Sustainable Systems

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TS‐1 has a unique structure, and TS‐1/H2O2 oxidation system for composition shows excellent catalytic performance in the oxidation of a variety of organic matter. The response conditions of the reaction system are mild, and the ultimate oxidation product is water. It is a typical “green catalytic” system and has received widespread attention from researchers. Here, the synthesis progress of TS‐1 to improve the accessibility and activity of active sites by doping mesoporous and microporous structures into traditional TS‐1 zeolite in recent five years are reviewed, including hydrothermal synthesis, dry gel conversion synthesis, solvent‐free synthesis, microwave assisted synthesis, and isomorphous substitution. Meanwhile, the application of TS‐1/H2O2 system in oxidative desulfurization, ketone ammonia oxidation, olefin epoxidation, and hydroxylation of aromatic hydrocarbons reactions are summarized and discussed. What's more, the reaction mechanism based on TS‐1/H2O2 system is proposed on regarding the isolated skeleton Ti site in titanium‐silicon zeolite as the active central site. Finally, the challenges and future development prospects of TS‐1 zeolite in synthesis and catalytic applications are predicted.

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Au/TS-1 catalyst for propylene epoxidation with H2 and O2: Effect of surface property and morphology of TS-1 zeolite

Zhang

et al. 2023

Nano Res.

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Au supported defect free TS-1 for enhanced performance of gas phase propylene epoxidation with H₂ and O₂

Abstract: The traditional TS-1 zeolite synthesis method inevitably produces extraframework titanium species, which reduces the reaction performance. Optimizing the coordination environments of Ti active sites in TS-1 zeolite is a big...

Cited by 6 publications

References 62 publications

Highly Efficient Epoxidation of Propylene with In Situ-Generated H₂O₂ over a Hierarchical TS-1 Zeolite-Supported Non-Noble Nickel Catalyst

Highly Efficient Epoxidation of Propylene with In Situ-Generated H₂O₂ over a Hierarchical TS-1 Zeolite-Supported Non-Noble Nickel Catalyst

Recent Advances in the Synthesis and Application of TS‐1 Zeolite for Green Catalytic Oxidation

Au/TS-1 catalyst for propylene epoxidation with H2 and O2: Effect of surface property and morphology of TS-1 zeolite

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Au supported defect free TS-1 for enhanced performance of gas phase propylene epoxidation with H2 and O2

Abstract: The traditional TS-1 zeolite synthesis method inevitably produces extraframework titanium species, which reduces the reaction performance. Optimizing the coordination environments of Ti active sites in TS-1 zeolite is a big...

Cited by 6 publications

References 62 publications

Highly Efficient Epoxidation of Propylene with In Situ-Generated H2O2 over a Hierarchical TS-1 Zeolite-Supported Non-Noble Nickel Catalyst

Highly Efficient Epoxidation of Propylene with In Situ-Generated H2O2 over a Hierarchical TS-1 Zeolite-Supported Non-Noble Nickel Catalyst

Recent Advances in the Synthesis and Application of TS‐1 Zeolite for Green Catalytic Oxidation

Au/TS-1 catalyst for propylene epoxidation with H2 and O2: Effect of surface property and morphology of TS-1 zeolite

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Product

Resources

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Au supported defect free TS-1 for enhanced performance of gas phase propylene epoxidation with H₂ and O₂

Highly Efficient Epoxidation of Propylene with In Situ-Generated H₂O₂ over a Hierarchical TS-1 Zeolite-Supported Non-Noble Nickel Catalyst

Highly Efficient Epoxidation of Propylene with In Situ-Generated H₂O₂ over a Hierarchical TS-1 Zeolite-Supported Non-Noble Nickel Catalyst