Properties of palladium-phosphorus catalysts supported on HZSM-5 zeolite in the direct synthesis of hydrogen peroxide

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Abstract

The properties of Pd/HZSM-5 and Pd–nP/HZSM-5 catalysts in direct synthesis and side processes of decomposition and hydrogenation of H2O2 under mild conditions in ethanol and aqueous-ethanol medium in the presence of an acid inhibitor were studied. Using HR-TEM, XRD and ICP MS methods, it was shown that as a result of modification with phosphorus, X-ray amorphous highly dispersed systems are formed, which represent structurally disordered solid solutions of phosphorus in palladium. The main reasons for the promoting effect of phosphorus on the yield of H2O2 are considered. It has been established that, along with phosphorus and acid modifiers, the use of a zeolite support in the H-form favors the inhibition of the side process of H2O2 decomposition.

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About the authors

L. B. Belykh

Irkutsk State University

Author for correspondence.
Email: belykh@chem.isu.ru
Russian Federation, K. Marx, 1, Irkutsk, 664003

N. I. Skripov

Irkutsk State University

Email: belykh@chem.isu.ru
Russian Federation, K. Marx, 1, Irkutsk, 664003

E. A. Milenkaya

Irkutsk State University

Email: belykh@chem.isu.ru
Russian Federation, K. Marx, 1, Irkutsk, 664003

T. A. Kornaukhova

Irkutsk State University

Email: belykh@chem.isu.ru
Russian Federation, K. Marx, 1, Irkutsk, 664003

T. P. Sterenchuk

Irkutsk State University

Email: belykh@chem.isu.ru
Russian Federation, K. Marx, 1, Irkutsk, 664003

Yu. K. Stepanova

Irkutsk State University

Email: belykh@chem.isu.ru
Russian Federation, K. Marx, 1, Irkutsk, 664003

F. K. Schmidt

Irkutsk State University

Email: belykh@chem.isu.ru
Russian Federation, K. Marx, 1, Irkutsk, 664003

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Supplementary files

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2. Fig. 1. Kinetic curves of H2O2 accumulation (a), change in H2O2 selectivity (b) and H2 conversion (c) under mild conditions in the presence of Pd–1.0P/НZSM-5(toluene) (1), Pd–0.3P/НZSM-5(DMF) (2), Pd–0.3P/НZSM-5(toluene) (3), Pd/НZSM-5(toluene) (4), Pd/НZSM-5(DMF) (5) catalysts. Process conditions: ν(Pd) = 5 × 10–6 mol, T = 10°C, P = 1 atm, solvent – ​​ethanol (50 ml). Selectivity in the presence of Pd/НZSM-5(DMF) catalyst was not calculated due to low hydrogen conversion.

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3. Fig. 2. Activities of Pd and Pd–P catalysts (a) and turnover frequencies of H2O2 accumulation (b) in direct synthesis under mild conditions in ethanol (green) and in the presence of HCl solution (red).

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4. Fig. 3. PEM images of Pd/HZSM-5(toluene) catalysts (a), Pd–0.3P/HZSM-5(toluene) (b), Pd–1.0P/HZSM-5(toluene) (c), Pd– 0.3P/HZSM-5(DMFA) (d) and Pd–0.3P/HZSM-5(DMFA) (e).

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5. Fig. 4. High-resolution PEM images of Pd–0.3P/HZSM5(toluene) (a), Pd–1.0P/HZSM-5(toluene) (b), Pd–0.3P/HZSM-5(DMFA) (c) catalysts .

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6. Fig. 5. Kinetic curves of H2O2 accumulation (a), change in H2O2 selectivity (b) and H2 conversion (c) under mild conditions in the presence of Pd–1.0P/НZSM-5(toluene) (1), Pd–0.3P/НZSM-5(toluene) (2), Pd–0.3P/НZSM-5(DMF) (3), Pd/НZSM-5(toluene) (4), Pd/НZSM-5(DMF) (5) catalysts. Process conditions: ν(Pd) = 5 × 10–6 mol, T = 10°C, P = 1 atm, solvent – ​​ethanol (40 ml) : HCl solution (10 ml). Selectivity in the presence of Pd/НZSM-5(DMF) catalyst was not calculated due to low hydrogen conversion.

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