Direct Synthesis of Hydrogen Peroxide under Semi-Batch Conditions over Un-Promoted Palladium Catalysts Supported by Ion-Exchange Sulfonated Resins: Effects of the Support Morphology

Palladium catalysts supported by a mesoporous form of sulfonated poly-divinylbenzene, Pd/µS-pDVB10 (1%, <i<w</i</<i<w</i<) and Pd/µS-pDVB35 (3.6% <i<w</i</<i<w</i<), were applied to the direct synthesis of hydrogen peroxide from dihydrogen and dioxygen. The reaction was carried for 4 h out in a semibatch reactor with continuous feed of the gas mixture (H<sub<2</sub</O<sub<2</sub< = 1/24, <i<v</i</<i<v</i<; total flow rate 25 mL·min<sup<−1</sup<), at 25 °C and 101 kPa. The catalytic performances were compared with those of a commercial egg-shell Pd/C catalyst (1%, <i<w</i</<i<w</i<) and of a palladium catalyst supported by a macroreticular sulfonated ion-exchange resin, Pd/mS-pSDVB10 (1%, <i<w</i</<i<w</i<). Pd/µS-pDVB10 and Pd/C showed the highest specific activity (H<sub<2</sub< consumption rate of about 75⁻80 h<sup<−1</sup<), but the resin supported catalyst was much more selective (ca 50% with no promoters). The nanoparticles (NP) size was somewhat larger in Pd/µS-pDVB10, showing that either the reaction was structure insensitive or diffusion limited to some extent over Pd/C, in which the support is microporous. The open pore structure of Pd/µS-pDVB10, possibly ensuring the fast removal of H<sub<2</sub<O<sub<2</sub< from the catalyst, could also be the cause of the relatively high selectivity of this catalyst. In summary, Pd/µS-pDVB10 was the most productive catalyst, forming ca 375 mol<sub<H<sub<2</sub<O<sub<2</sub<</sub<·kg<sub<Pd</sub<<sup<−1</sup<·h<sup<−1</sup<, also because it retained a constant selectivity, while the other ones underwent a more or less pronounced loss of selectivity after 80⁻90 min. Ageing experiments showed that for a palladium catalyst supported on sulfonated mesoporous poly-divinylbenzene storage under oxidative conditions implied some deactivation, but a lower drop in the selectivity; regeneration upon a reductive treatment or storage under strictly anaerobic conditions (dry-box) lead to an increase of the activity but to both a lower initial selectivity and a higher drop of selectivity with time. Ausführliche Beschreibung

Gespeichert in:

Autor*in:	Francesco Frison [verfasserIn] Chiara Dalla Valle [verfasserIn] Claudio Evangelisti [verfasserIn] Paolo Centomo [verfasserIn] Marco Zecca [verfasserIn]

Format:	E-Artikel
Sprache:	Englisch

Erschienen:	2019

Schlagwörter:	hydrogen peroxide support morphology mesoporous poly-divinylbenzene palladium ageing

Übergeordnetes Werk:	In: Catalysts - MDPI AG, 2012, 9(2019), 2, p 124
Übergeordnetes Werk:	volume:9 ; year:2019 ; number:2, p 124

Links:	Link aufrufen Link aufrufen Link aufrufen Journal toc

DOI / URN:	10.3390/catal9020124

Katalog-ID:	DOAJ031878628

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520			\|a Palladium catalysts supported by a mesoporous form of sulfonated poly-divinylbenzene, Pd/µS-pDVB10 (1%, <i<w</i</<i<w</i<) and Pd/µS-pDVB35 (3.6% <i<w</i</<i<w</i<), were applied to the direct synthesis of hydrogen peroxide from dihydrogen and dioxygen. The reaction was carried for 4 h out in a semibatch reactor with continuous feed of the gas mixture (H<sub<2</sub</O<sub<2</sub< = 1/24, <i<v</i</<i<v</i<; total flow rate 25 mL·min<sup<−1</sup<), at 25 °C and 101 kPa. The catalytic performances were compared with those of a commercial egg-shell Pd/C catalyst (1%, <i<w</i</<i<w</i<) and of a palladium catalyst supported by a macroreticular sulfonated ion-exchange resin, Pd/mS-pSDVB10 (1%, <i<w</i</<i<w</i<). Pd/µS-pDVB10 and Pd/C showed the highest specific activity (H<sub<2</sub< consumption rate of about 75⁻80 h<sup<−1</sup<), but the resin supported catalyst was much more selective (ca 50% with no promoters). The nanoparticles (NP) size was somewhat larger in Pd/µS-pDVB10, showing that either the reaction was structure insensitive or diffusion limited to some extent over Pd/C, in which the support is microporous. The open pore structure of Pd/µS-pDVB10, possibly ensuring the fast removal of H<sub<2</sub<O<sub<2</sub< from the catalyst, could also be the cause of the relatively high selectivity of this catalyst. In summary, Pd/µS-pDVB10 was the most productive catalyst, forming ca 375 mol<sub<H<sub<2</sub<O<sub<2</sub<</sub<·kg<sub<Pd</sub<<sup<−1</sup<·h<sup<−1</sup<, also because it retained a constant selectivity, while the other ones underwent a more or less pronounced loss of selectivity after 80⁻90 min. Ageing experiments showed that for a palladium catalyst supported on sulfonated mesoporous poly-divinylbenzene storage under oxidative conditions implied some deactivation, but a lower drop in the selectivity; regeneration upon a reductive treatment or storage under strictly anaerobic conditions (dry-box) lead to an increase of the activity but to both a lower initial selectivity and a higher drop of selectivity with time.
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allfields	10.3390/catal9020124 doi (DE-627)DOAJ031878628 (DE-599)DOAJf31e534b8e25426a8f4ec5e180fd72a4 DE-627 ger DE-627 rakwb eng TP1-1185 QD1-999 Francesco Frison verfasserin aut Direct Synthesis of Hydrogen Peroxide under Semi-Batch Conditions over Un-Promoted Palladium Catalysts Supported by Ion-Exchange Sulfonated Resins: Effects of the Support Morphology 2019 Text txt rdacontent Computermedien c rdamedia Online-Ressource cr rdacarrier Palladium catalysts supported by a mesoporous form of sulfonated poly-divinylbenzene, Pd/µS-pDVB10 (1%, <i<w</i</<i<w</i<) and Pd/µS-pDVB35 (3.6% <i<w</i</<i<w</i<), were applied to the direct synthesis of hydrogen peroxide from dihydrogen and dioxygen. The reaction was carried for 4 h out in a semibatch reactor with continuous feed of the gas mixture (H<sub<2</sub</O<sub<2</sub< = 1/24, <i<v</i</<i<v</i<; total flow rate 25 mL·min<sup<−1</sup<), at 25 °C and 101 kPa. The catalytic performances were compared with those of a commercial egg-shell Pd/C catalyst (1%, <i<w</i</<i<w</i<) and of a palladium catalyst supported by a macroreticular sulfonated ion-exchange resin, Pd/mS-pSDVB10 (1%, <i<w</i</<i<w</i<). Pd/µS-pDVB10 and Pd/C showed the highest specific activity (H<sub<2</sub< consumption rate of about 75⁻80 h<sup<−1</sup<), but the resin supported catalyst was much more selective (ca 50% with no promoters). The nanoparticles (NP) size was somewhat larger in Pd/µS-pDVB10, showing that either the reaction was structure insensitive or diffusion limited to some extent over Pd/C, in which the support is microporous. The open pore structure of Pd/µS-pDVB10, possibly ensuring the fast removal of H<sub<2</sub<O<sub<2</sub< from the catalyst, could also be the cause of the relatively high selectivity of this catalyst. In summary, Pd/µS-pDVB10 was the most productive catalyst, forming ca 375 mol<sub<H<sub<2</sub<O<sub<2</sub<</sub<·kg<sub<Pd</sub<<sup<−1</sup<·h<sup<−1</sup<, also because it retained a constant selectivity, while the other ones underwent a more or less pronounced loss of selectivity after 80⁻90 min. Ageing experiments showed that for a palladium catalyst supported on sulfonated mesoporous poly-divinylbenzene storage under oxidative conditions implied some deactivation, but a lower drop in the selectivity; regeneration upon a reductive treatment or storage under strictly anaerobic conditions (dry-box) lead to an increase of the activity but to both a lower initial selectivity and a higher drop of selectivity with time. hydrogen peroxide support morphology mesoporous poly-divinylbenzene palladium ageing Chemical technology Chemistry Chiara Dalla Valle verfasserin aut Claudio Evangelisti verfasserin aut Paolo Centomo verfasserin aut Marco Zecca verfasserin aut In Catalysts MDPI AG, 2012 9(2019), 2, p 124 (DE-627)71862646X (DE-600)2662126-5 20734344 nnns volume:9 year:2019 number:2, p 124 https://doi.org/10.3390/catal9020124 kostenfrei https://doaj.org/article/f31e534b8e25426a8f4ec5e180fd72a4 kostenfrei https://www.mdpi.com/2073-4344/9/2/124 kostenfrei https://doaj.org/toc/2073-4344 Journal toc kostenfrei GBV_USEFLAG_A SYSFLAG_A GBV_DOAJ GBV_ILN_20 GBV_ILN_22 GBV_ILN_23 GBV_ILN_24 GBV_ILN_39 GBV_ILN_40 GBV_ILN_60 GBV_ILN_62 GBV_ILN_63 GBV_ILN_65 GBV_ILN_69 GBV_ILN_70 GBV_ILN_73 GBV_ILN_95 GBV_ILN_105 GBV_ILN_110 GBV_ILN_151 GBV_ILN_161 GBV_ILN_170 GBV_ILN_206 GBV_ILN_213 GBV_ILN_230 GBV_ILN_285 GBV_ILN_293 GBV_ILN_602 GBV_ILN_2005 GBV_ILN_2009 GBV_ILN_2011 GBV_ILN_2014 GBV_ILN_2055 GBV_ILN_2111 GBV_ILN_4012 GBV_ILN_4037 GBV_ILN_4112 GBV_ILN_4125 GBV_ILN_4126 GBV_ILN_4249 GBV_ILN_4305 GBV_ILN_4306 GBV_ILN_4307 GBV_ILN_4313 GBV_ILN_4322 GBV_ILN_4323 GBV_ILN_4324 GBV_ILN_4325 GBV_ILN_4338 GBV_ILN_4367 GBV_ILN_4700 AR 9 2019 2, p 124
spelling	10.3390/catal9020124 doi (DE-627)DOAJ031878628 (DE-599)DOAJf31e534b8e25426a8f4ec5e180fd72a4 DE-627 ger DE-627 rakwb eng TP1-1185 QD1-999 Francesco Frison verfasserin aut Direct Synthesis of Hydrogen Peroxide under Semi-Batch Conditions over Un-Promoted Palladium Catalysts Supported by Ion-Exchange Sulfonated Resins: Effects of the Support Morphology 2019 Text txt rdacontent Computermedien c rdamedia Online-Ressource cr rdacarrier Palladium catalysts supported by a mesoporous form of sulfonated poly-divinylbenzene, Pd/µS-pDVB10 (1%, <i<w</i</<i<w</i<) and Pd/µS-pDVB35 (3.6% <i<w</i</<i<w</i<), were applied to the direct synthesis of hydrogen peroxide from dihydrogen and dioxygen. The reaction was carried for 4 h out in a semibatch reactor with continuous feed of the gas mixture (H<sub<2</sub</O<sub<2</sub< = 1/24, <i<v</i</<i<v</i<; total flow rate 25 mL·min<sup<−1</sup<), at 25 °C and 101 kPa. The catalytic performances were compared with those of a commercial egg-shell Pd/C catalyst (1%, <i<w</i</<i<w</i<) and of a palladium catalyst supported by a macroreticular sulfonated ion-exchange resin, Pd/mS-pSDVB10 (1%, <i<w</i</<i<w</i<). Pd/µS-pDVB10 and Pd/C showed the highest specific activity (H<sub<2</sub< consumption rate of about 75⁻80 h<sup<−1</sup<), but the resin supported catalyst was much more selective (ca 50% with no promoters). The nanoparticles (NP) size was somewhat larger in Pd/µS-pDVB10, showing that either the reaction was structure insensitive or diffusion limited to some extent over Pd/C, in which the support is microporous. The open pore structure of Pd/µS-pDVB10, possibly ensuring the fast removal of H<sub<2</sub<O<sub<2</sub< from the catalyst, could also be the cause of the relatively high selectivity of this catalyst. In summary, Pd/µS-pDVB10 was the most productive catalyst, forming ca 375 mol<sub<H<sub<2</sub<O<sub<2</sub<</sub<·kg<sub<Pd</sub<<sup<−1</sup<·h<sup<−1</sup<, also because it retained a constant selectivity, while the other ones underwent a more or less pronounced loss of selectivity after 80⁻90 min. Ageing experiments showed that for a palladium catalyst supported on sulfonated mesoporous poly-divinylbenzene storage under oxidative conditions implied some deactivation, but a lower drop in the selectivity; regeneration upon a reductive treatment or storage under strictly anaerobic conditions (dry-box) lead to an increase of the activity but to both a lower initial selectivity and a higher drop of selectivity with time. hydrogen peroxide support morphology mesoporous poly-divinylbenzene palladium ageing Chemical technology Chemistry Chiara Dalla Valle verfasserin aut Claudio Evangelisti verfasserin aut Paolo Centomo verfasserin aut Marco Zecca verfasserin aut In Catalysts MDPI AG, 2012 9(2019), 2, p 124 (DE-627)71862646X (DE-600)2662126-5 20734344 nnns volume:9 year:2019 number:2, p 124 https://doi.org/10.3390/catal9020124 kostenfrei https://doaj.org/article/f31e534b8e25426a8f4ec5e180fd72a4 kostenfrei https://www.mdpi.com/2073-4344/9/2/124 kostenfrei https://doaj.org/toc/2073-4344 Journal toc kostenfrei GBV_USEFLAG_A SYSFLAG_A GBV_DOAJ GBV_ILN_20 GBV_ILN_22 GBV_ILN_23 GBV_ILN_24 GBV_ILN_39 GBV_ILN_40 GBV_ILN_60 GBV_ILN_62 GBV_ILN_63 GBV_ILN_65 GBV_ILN_69 GBV_ILN_70 GBV_ILN_73 GBV_ILN_95 GBV_ILN_105 GBV_ILN_110 GBV_ILN_151 GBV_ILN_161 GBV_ILN_170 GBV_ILN_206 GBV_ILN_213 GBV_ILN_230 GBV_ILN_285 GBV_ILN_293 GBV_ILN_602 GBV_ILN_2005 GBV_ILN_2009 GBV_ILN_2011 GBV_ILN_2014 GBV_ILN_2055 GBV_ILN_2111 GBV_ILN_4012 GBV_ILN_4037 GBV_ILN_4112 GBV_ILN_4125 GBV_ILN_4126 GBV_ILN_4249 GBV_ILN_4305 GBV_ILN_4306 GBV_ILN_4307 GBV_ILN_4313 GBV_ILN_4322 GBV_ILN_4323 GBV_ILN_4324 GBV_ILN_4325 GBV_ILN_4338 GBV_ILN_4367 GBV_ILN_4700 AR 9 2019 2, p 124
allfields_unstemmed	10.3390/catal9020124 doi (DE-627)DOAJ031878628 (DE-599)DOAJf31e534b8e25426a8f4ec5e180fd72a4 DE-627 ger DE-627 rakwb eng TP1-1185 QD1-999 Francesco Frison verfasserin aut Direct Synthesis of Hydrogen Peroxide under Semi-Batch Conditions over Un-Promoted Palladium Catalysts Supported by Ion-Exchange Sulfonated Resins: Effects of the Support Morphology 2019 Text txt rdacontent Computermedien c rdamedia Online-Ressource cr rdacarrier Palladium catalysts supported by a mesoporous form of sulfonated poly-divinylbenzene, Pd/µS-pDVB10 (1%, <i<w</i</<i<w</i<) and Pd/µS-pDVB35 (3.6% <i<w</i</<i<w</i<), were applied to the direct synthesis of hydrogen peroxide from dihydrogen and dioxygen. The reaction was carried for 4 h out in a semibatch reactor with continuous feed of the gas mixture (H<sub<2</sub</O<sub<2</sub< = 1/24, <i<v</i</<i<v</i<; total flow rate 25 mL·min<sup<−1</sup<), at 25 °C and 101 kPa. The catalytic performances were compared with those of a commercial egg-shell Pd/C catalyst (1%, <i<w</i</<i<w</i<) and of a palladium catalyst supported by a macroreticular sulfonated ion-exchange resin, Pd/mS-pSDVB10 (1%, <i<w</i</<i<w</i<). Pd/µS-pDVB10 and Pd/C showed the highest specific activity (H<sub<2</sub< consumption rate of about 75⁻80 h<sup<−1</sup<), but the resin supported catalyst was much more selective (ca 50% with no promoters). The nanoparticles (NP) size was somewhat larger in Pd/µS-pDVB10, showing that either the reaction was structure insensitive or diffusion limited to some extent over Pd/C, in which the support is microporous. The open pore structure of Pd/µS-pDVB10, possibly ensuring the fast removal of H<sub<2</sub<O<sub<2</sub< from the catalyst, could also be the cause of the relatively high selectivity of this catalyst. In summary, Pd/µS-pDVB10 was the most productive catalyst, forming ca 375 mol<sub<H<sub<2</sub<O<sub<2</sub<</sub<·kg<sub<Pd</sub<<sup<−1</sup<·h<sup<−1</sup<, also because it retained a constant selectivity, while the other ones underwent a more or less pronounced loss of selectivity after 80⁻90 min. Ageing experiments showed that for a palladium catalyst supported on sulfonated mesoporous poly-divinylbenzene storage under oxidative conditions implied some deactivation, but a lower drop in the selectivity; regeneration upon a reductive treatment or storage under strictly anaerobic conditions (dry-box) lead to an increase of the activity but to both a lower initial selectivity and a higher drop of selectivity with time. hydrogen peroxide support morphology mesoporous poly-divinylbenzene palladium ageing Chemical technology Chemistry Chiara Dalla Valle verfasserin aut Claudio Evangelisti verfasserin aut Paolo Centomo verfasserin aut Marco Zecca verfasserin aut In Catalysts MDPI AG, 2012 9(2019), 2, p 124 (DE-627)71862646X (DE-600)2662126-5 20734344 nnns volume:9 year:2019 number:2, p 124 https://doi.org/10.3390/catal9020124 kostenfrei https://doaj.org/article/f31e534b8e25426a8f4ec5e180fd72a4 kostenfrei https://www.mdpi.com/2073-4344/9/2/124 kostenfrei https://doaj.org/toc/2073-4344 Journal toc kostenfrei GBV_USEFLAG_A SYSFLAG_A GBV_DOAJ GBV_ILN_20 GBV_ILN_22 GBV_ILN_23 GBV_ILN_24 GBV_ILN_39 GBV_ILN_40 GBV_ILN_60 GBV_ILN_62 GBV_ILN_63 GBV_ILN_65 GBV_ILN_69 GBV_ILN_70 GBV_ILN_73 GBV_ILN_95 GBV_ILN_105 GBV_ILN_110 GBV_ILN_151 GBV_ILN_161 GBV_ILN_170 GBV_ILN_206 GBV_ILN_213 GBV_ILN_230 GBV_ILN_285 GBV_ILN_293 GBV_ILN_602 GBV_ILN_2005 GBV_ILN_2009 GBV_ILN_2011 GBV_ILN_2014 GBV_ILN_2055 GBV_ILN_2111 GBV_ILN_4012 GBV_ILN_4037 GBV_ILN_4112 GBV_ILN_4125 GBV_ILN_4126 GBV_ILN_4249 GBV_ILN_4305 GBV_ILN_4306 GBV_ILN_4307 GBV_ILN_4313 GBV_ILN_4322 GBV_ILN_4323 GBV_ILN_4324 GBV_ILN_4325 GBV_ILN_4338 GBV_ILN_4367 GBV_ILN_4700 AR 9 2019 2, p 124
allfieldsGer	10.3390/catal9020124 doi (DE-627)DOAJ031878628 (DE-599)DOAJf31e534b8e25426a8f4ec5e180fd72a4 DE-627 ger DE-627 rakwb eng TP1-1185 QD1-999 Francesco Frison verfasserin aut Direct Synthesis of Hydrogen Peroxide under Semi-Batch Conditions over Un-Promoted Palladium Catalysts Supported by Ion-Exchange Sulfonated Resins: Effects of the Support Morphology 2019 Text txt rdacontent Computermedien c rdamedia Online-Ressource cr rdacarrier Palladium catalysts supported by a mesoporous form of sulfonated poly-divinylbenzene, Pd/µS-pDVB10 (1%, <i<w</i</<i<w</i<) and Pd/µS-pDVB35 (3.6% <i<w</i</<i<w</i<), were applied to the direct synthesis of hydrogen peroxide from dihydrogen and dioxygen. The reaction was carried for 4 h out in a semibatch reactor with continuous feed of the gas mixture (H<sub<2</sub</O<sub<2</sub< = 1/24, <i<v</i</<i<v</i<; total flow rate 25 mL·min<sup<−1</sup<), at 25 °C and 101 kPa. The catalytic performances were compared with those of a commercial egg-shell Pd/C catalyst (1%, <i<w</i</<i<w</i<) and of a palladium catalyst supported by a macroreticular sulfonated ion-exchange resin, Pd/mS-pSDVB10 (1%, <i<w</i</<i<w</i<). Pd/µS-pDVB10 and Pd/C showed the highest specific activity (H<sub<2</sub< consumption rate of about 75⁻80 h<sup<−1</sup<), but the resin supported catalyst was much more selective (ca 50% with no promoters). The nanoparticles (NP) size was somewhat larger in Pd/µS-pDVB10, showing that either the reaction was structure insensitive or diffusion limited to some extent over Pd/C, in which the support is microporous. The open pore structure of Pd/µS-pDVB10, possibly ensuring the fast removal of H<sub<2</sub<O<sub<2</sub< from the catalyst, could also be the cause of the relatively high selectivity of this catalyst. In summary, Pd/µS-pDVB10 was the most productive catalyst, forming ca 375 mol<sub<H<sub<2</sub<O<sub<2</sub<</sub<·kg<sub<Pd</sub<<sup<−1</sup<·h<sup<−1</sup<, also because it retained a constant selectivity, while the other ones underwent a more or less pronounced loss of selectivity after 80⁻90 min. Ageing experiments showed that for a palladium catalyst supported on sulfonated mesoporous poly-divinylbenzene storage under oxidative conditions implied some deactivation, but a lower drop in the selectivity; regeneration upon a reductive treatment or storage under strictly anaerobic conditions (dry-box) lead to an increase of the activity but to both a lower initial selectivity and a higher drop of selectivity with time. hydrogen peroxide support morphology mesoporous poly-divinylbenzene palladium ageing Chemical technology Chemistry Chiara Dalla Valle verfasserin aut Claudio Evangelisti verfasserin aut Paolo Centomo verfasserin aut Marco Zecca verfasserin aut In Catalysts MDPI AG, 2012 9(2019), 2, p 124 (DE-627)71862646X (DE-600)2662126-5 20734344 nnns volume:9 year:2019 number:2, p 124 https://doi.org/10.3390/catal9020124 kostenfrei https://doaj.org/article/f31e534b8e25426a8f4ec5e180fd72a4 kostenfrei https://www.mdpi.com/2073-4344/9/2/124 kostenfrei https://doaj.org/toc/2073-4344 Journal toc kostenfrei GBV_USEFLAG_A SYSFLAG_A GBV_DOAJ GBV_ILN_20 GBV_ILN_22 GBV_ILN_23 GBV_ILN_24 GBV_ILN_39 GBV_ILN_40 GBV_ILN_60 GBV_ILN_62 GBV_ILN_63 GBV_ILN_65 GBV_ILN_69 GBV_ILN_70 GBV_ILN_73 GBV_ILN_95 GBV_ILN_105 GBV_ILN_110 GBV_ILN_151 GBV_ILN_161 GBV_ILN_170 GBV_ILN_206 GBV_ILN_213 GBV_ILN_230 GBV_ILN_285 GBV_ILN_293 GBV_ILN_602 GBV_ILN_2005 GBV_ILN_2009 GBV_ILN_2011 GBV_ILN_2014 GBV_ILN_2055 GBV_ILN_2111 GBV_ILN_4012 GBV_ILN_4037 GBV_ILN_4112 GBV_ILN_4125 GBV_ILN_4126 GBV_ILN_4249 GBV_ILN_4305 GBV_ILN_4306 GBV_ILN_4307 GBV_ILN_4313 GBV_ILN_4322 GBV_ILN_4323 GBV_ILN_4324 GBV_ILN_4325 GBV_ILN_4338 GBV_ILN_4367 GBV_ILN_4700 AR 9 2019 2, p 124
allfieldsSound	10.3390/catal9020124 doi (DE-627)DOAJ031878628 (DE-599)DOAJf31e534b8e25426a8f4ec5e180fd72a4 DE-627 ger DE-627 rakwb eng TP1-1185 QD1-999 Francesco Frison verfasserin aut Direct Synthesis of Hydrogen Peroxide under Semi-Batch Conditions over Un-Promoted Palladium Catalysts Supported by Ion-Exchange Sulfonated Resins: Effects of the Support Morphology 2019 Text txt rdacontent Computermedien c rdamedia Online-Ressource cr rdacarrier Palladium catalysts supported by a mesoporous form of sulfonated poly-divinylbenzene, Pd/µS-pDVB10 (1%, <i<w</i</<i<w</i<) and Pd/µS-pDVB35 (3.6% <i<w</i</<i<w</i<), were applied to the direct synthesis of hydrogen peroxide from dihydrogen and dioxygen. The reaction was carried for 4 h out in a semibatch reactor with continuous feed of the gas mixture (H<sub<2</sub</O<sub<2</sub< = 1/24, <i<v</i</<i<v</i<; total flow rate 25 mL·min<sup<−1</sup<), at 25 °C and 101 kPa. The catalytic performances were compared with those of a commercial egg-shell Pd/C catalyst (1%, <i<w</i</<i<w</i<) and of a palladium catalyst supported by a macroreticular sulfonated ion-exchange resin, Pd/mS-pSDVB10 (1%, <i<w</i</<i<w</i<). Pd/µS-pDVB10 and Pd/C showed the highest specific activity (H<sub<2</sub< consumption rate of about 75⁻80 h<sup<−1</sup<), but the resin supported catalyst was much more selective (ca 50% with no promoters). The nanoparticles (NP) size was somewhat larger in Pd/µS-pDVB10, showing that either the reaction was structure insensitive or diffusion limited to some extent over Pd/C, in which the support is microporous. The open pore structure of Pd/µS-pDVB10, possibly ensuring the fast removal of H<sub<2</sub<O<sub<2</sub< from the catalyst, could also be the cause of the relatively high selectivity of this catalyst. In summary, Pd/µS-pDVB10 was the most productive catalyst, forming ca 375 mol<sub<H<sub<2</sub<O<sub<2</sub<</sub<·kg<sub<Pd</sub<<sup<−1</sup<·h<sup<−1</sup<, also because it retained a constant selectivity, while the other ones underwent a more or less pronounced loss of selectivity after 80⁻90 min. Ageing experiments showed that for a palladium catalyst supported on sulfonated mesoporous poly-divinylbenzene storage under oxidative conditions implied some deactivation, but a lower drop in the selectivity; regeneration upon a reductive treatment or storage under strictly anaerobic conditions (dry-box) lead to an increase of the activity but to both a lower initial selectivity and a higher drop of selectivity with time. hydrogen peroxide support morphology mesoporous poly-divinylbenzene palladium ageing Chemical technology Chemistry Chiara Dalla Valle verfasserin aut Claudio Evangelisti verfasserin aut Paolo Centomo verfasserin aut Marco Zecca verfasserin aut In Catalysts MDPI AG, 2012 9(2019), 2, p 124 (DE-627)71862646X (DE-600)2662126-5 20734344 nnns volume:9 year:2019 number:2, p 124 https://doi.org/10.3390/catal9020124 kostenfrei https://doaj.org/article/f31e534b8e25426a8f4ec5e180fd72a4 kostenfrei https://www.mdpi.com/2073-4344/9/2/124 kostenfrei https://doaj.org/toc/2073-4344 Journal toc kostenfrei GBV_USEFLAG_A SYSFLAG_A GBV_DOAJ GBV_ILN_20 GBV_ILN_22 GBV_ILN_23 GBV_ILN_24 GBV_ILN_39 GBV_ILN_40 GBV_ILN_60 GBV_ILN_62 GBV_ILN_63 GBV_ILN_65 GBV_ILN_69 GBV_ILN_70 GBV_ILN_73 GBV_ILN_95 GBV_ILN_105 GBV_ILN_110 GBV_ILN_151 GBV_ILN_161 GBV_ILN_170 GBV_ILN_206 GBV_ILN_213 GBV_ILN_230 GBV_ILN_285 GBV_ILN_293 GBV_ILN_602 GBV_ILN_2005 GBV_ILN_2009 GBV_ILN_2011 GBV_ILN_2014 GBV_ILN_2055 GBV_ILN_2111 GBV_ILN_4012 GBV_ILN_4037 GBV_ILN_4112 GBV_ILN_4125 GBV_ILN_4126 GBV_ILN_4249 GBV_ILN_4305 GBV_ILN_4306 GBV_ILN_4307 GBV_ILN_4313 GBV_ILN_4322 GBV_ILN_4323 GBV_ILN_4324 GBV_ILN_4325 GBV_ILN_4338 GBV_ILN_4367 GBV_ILN_4700 AR 9 2019 2, p 124
language	English
source	In Catalysts 9(2019), 2, p 124 volume:9 year:2019 number:2, p 124
sourceStr	In Catalysts 9(2019), 2, p 124 volume:9 year:2019 number:2, p 124
format_phy_str_mv	Article
institution	findex.gbv.de
topic_facet	hydrogen peroxide support morphology mesoporous poly-divinylbenzene palladium ageing Chemical technology Chemistry
isfreeaccess_bool	true
container_title	Catalysts
authorswithroles_txt_mv	Francesco Frison @@aut@@ Chiara Dalla Valle @@aut@@ Claudio Evangelisti @@aut@@ Paolo Centomo @@aut@@ Marco Zecca @@aut@@
publishDateDaySort_date	2019-01-01T00:00:00Z
hierarchy_top_id	71862646X
id	DOAJ031878628
language_de	englisch
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The reaction was carried for 4 h out in a semibatch reactor with continuous feed of the gas mixture (H<sub<2</sub</O<sub<2</sub< = 1/24, <i<v</i</<i<v</i<; total flow rate 25 mL·min<sup<−1</sup<), at 25 °C and 101 kPa. The catalytic performances were compared with those of a commercial egg-shell Pd/C catalyst (1%, <i<w</i</<i<w</i<) and of a palladium catalyst supported by a macroreticular sulfonated ion-exchange resin, Pd/mS-pSDVB10 (1%, <i<w</i</<i<w</i<). Pd/µS-pDVB10 and Pd/C showed the highest specific activity (H<sub<2</sub< consumption rate of about 75⁻80 h<sup<−1</sup<), but the resin supported catalyst was much more selective (ca 50% with no promoters). The nanoparticles (NP) size was somewhat larger in Pd/µS-pDVB10, showing that either the reaction was structure insensitive or diffusion limited to some extent over Pd/C, in which the support is microporous. 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callnumber-first	T - Technology
author	Francesco Frison
spellingShingle	Francesco Frison misc TP1-1185 misc QD1-999 misc hydrogen peroxide misc support morphology misc mesoporous poly-divinylbenzene misc palladium misc ageing misc Chemical technology misc Chemistry Direct Synthesis of Hydrogen Peroxide under Semi-Batch Conditions over Un-Promoted Palladium Catalysts Supported by Ion-Exchange Sulfonated Resins: Effects of the Support Morphology
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topic_title	TP1-1185 QD1-999 Direct Synthesis of Hydrogen Peroxide under Semi-Batch Conditions over Un-Promoted Palladium Catalysts Supported by Ion-Exchange Sulfonated Resins: Effects of the Support Morphology hydrogen peroxide support morphology mesoporous poly-divinylbenzene palladium ageing
topic	misc TP1-1185 misc QD1-999 misc hydrogen peroxide misc support morphology misc mesoporous poly-divinylbenzene misc palladium misc ageing misc Chemical technology misc Chemistry
topic_unstemmed	misc TP1-1185 misc QD1-999 misc hydrogen peroxide misc support morphology misc mesoporous poly-divinylbenzene misc palladium misc ageing misc Chemical technology misc Chemistry
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title	Direct Synthesis of Hydrogen Peroxide under Semi-Batch Conditions over Un-Promoted Palladium Catalysts Supported by Ion-Exchange Sulfonated Resins: Effects of the Support Morphology
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title_full	Direct Synthesis of Hydrogen Peroxide under Semi-Batch Conditions over Un-Promoted Palladium Catalysts Supported by Ion-Exchange Sulfonated Resins: Effects of the Support Morphology
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author_browse	Francesco Frison Chiara Dalla Valle Claudio Evangelisti Paolo Centomo Marco Zecca
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author-letter	Francesco Frison
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title_sort	direct synthesis of hydrogen peroxide under semi-batch conditions over un-promoted palladium catalysts supported by ion-exchange sulfonated resins: effects of the support morphology
callnumber	TP1-1185
title_auth	Direct Synthesis of Hydrogen Peroxide under Semi-Batch Conditions over Un-Promoted Palladium Catalysts Supported by Ion-Exchange Sulfonated Resins: Effects of the Support Morphology
abstract	Palladium catalysts supported by a mesoporous form of sulfonated poly-divinylbenzene, Pd/µS-pDVB10 (1%, <i<w</i</<i<w</i<) and Pd/µS-pDVB35 (3.6% <i<w</i</<i<w</i<), were applied to the direct synthesis of hydrogen peroxide from dihydrogen and dioxygen. The reaction was carried for 4 h out in a semibatch reactor with continuous feed of the gas mixture (H<sub<2</sub</O<sub<2</sub< = 1/24, <i<v</i</<i<v</i<; total flow rate 25 mL·min<sup<−1</sup<), at 25 °C and 101 kPa. The catalytic performances were compared with those of a commercial egg-shell Pd/C catalyst (1%, <i<w</i</<i<w</i<) and of a palladium catalyst supported by a macroreticular sulfonated ion-exchange resin, Pd/mS-pSDVB10 (1%, <i<w</i</<i<w</i<). Pd/µS-pDVB10 and Pd/C showed the highest specific activity (H<sub<2</sub< consumption rate of about 75⁻80 h<sup<−1</sup<), but the resin supported catalyst was much more selective (ca 50% with no promoters). The nanoparticles (NP) size was somewhat larger in Pd/µS-pDVB10, showing that either the reaction was structure insensitive or diffusion limited to some extent over Pd/C, in which the support is microporous. The open pore structure of Pd/µS-pDVB10, possibly ensuring the fast removal of H<sub<2</sub<O<sub<2</sub< from the catalyst, could also be the cause of the relatively high selectivity of this catalyst. In summary, Pd/µS-pDVB10 was the most productive catalyst, forming ca 375 mol<sub<H<sub<2</sub<O<sub<2</sub<</sub<·kg<sub<Pd</sub<<sup<−1</sup<·h<sup<−1</sup<, also because it retained a constant selectivity, while the other ones underwent a more or less pronounced loss of selectivity after 80⁻90 min. Ageing experiments showed that for a palladium catalyst supported on sulfonated mesoporous poly-divinylbenzene storage under oxidative conditions implied some deactivation, but a lower drop in the selectivity; regeneration upon a reductive treatment or storage under strictly anaerobic conditions (dry-box) lead to an increase of the activity but to both a lower initial selectivity and a higher drop of selectivity with time.
abstractGer	Palladium catalysts supported by a mesoporous form of sulfonated poly-divinylbenzene, Pd/µS-pDVB10 (1%, <i<w</i</<i<w</i<) and Pd/µS-pDVB35 (3.6% <i<w</i</<i<w</i<), were applied to the direct synthesis of hydrogen peroxide from dihydrogen and dioxygen. The reaction was carried for 4 h out in a semibatch reactor with continuous feed of the gas mixture (H<sub<2</sub</O<sub<2</sub< = 1/24, <i<v</i</<i<v</i<; total flow rate 25 mL·min<sup<−1</sup<), at 25 °C and 101 kPa. The catalytic performances were compared with those of a commercial egg-shell Pd/C catalyst (1%, <i<w</i</<i<w</i<) and of a palladium catalyst supported by a macroreticular sulfonated ion-exchange resin, Pd/mS-pSDVB10 (1%, <i<w</i</<i<w</i<). Pd/µS-pDVB10 and Pd/C showed the highest specific activity (H<sub<2</sub< consumption rate of about 75⁻80 h<sup<−1</sup<), but the resin supported catalyst was much more selective (ca 50% with no promoters). The nanoparticles (NP) size was somewhat larger in Pd/µS-pDVB10, showing that either the reaction was structure insensitive or diffusion limited to some extent over Pd/C, in which the support is microporous. The open pore structure of Pd/µS-pDVB10, possibly ensuring the fast removal of H<sub<2</sub<O<sub<2</sub< from the catalyst, could also be the cause of the relatively high selectivity of this catalyst. In summary, Pd/µS-pDVB10 was the most productive catalyst, forming ca 375 mol<sub<H<sub<2</sub<O<sub<2</sub<</sub<·kg<sub<Pd</sub<<sup<−1</sup<·h<sup<−1</sup<, also because it retained a constant selectivity, while the other ones underwent a more or less pronounced loss of selectivity after 80⁻90 min. Ageing experiments showed that for a palladium catalyst supported on sulfonated mesoporous poly-divinylbenzene storage under oxidative conditions implied some deactivation, but a lower drop in the selectivity; regeneration upon a reductive treatment or storage under strictly anaerobic conditions (dry-box) lead to an increase of the activity but to both a lower initial selectivity and a higher drop of selectivity with time.
abstract_unstemmed	Palladium catalysts supported by a mesoporous form of sulfonated poly-divinylbenzene, Pd/µS-pDVB10 (1%, <i<w</i</<i<w</i<) and Pd/µS-pDVB35 (3.6% <i<w</i</<i<w</i<), were applied to the direct synthesis of hydrogen peroxide from dihydrogen and dioxygen. The reaction was carried for 4 h out in a semibatch reactor with continuous feed of the gas mixture (H<sub<2</sub</O<sub<2</sub< = 1/24, <i<v</i</<i<v</i<; total flow rate 25 mL·min<sup<−1</sup<), at 25 °C and 101 kPa. The catalytic performances were compared with those of a commercial egg-shell Pd/C catalyst (1%, <i<w</i</<i<w</i<) and of a palladium catalyst supported by a macroreticular sulfonated ion-exchange resin, Pd/mS-pSDVB10 (1%, <i<w</i</<i<w</i<). Pd/µS-pDVB10 and Pd/C showed the highest specific activity (H<sub<2</sub< consumption rate of about 75⁻80 h<sup<−1</sup<), but the resin supported catalyst was much more selective (ca 50% with no promoters). The nanoparticles (NP) size was somewhat larger in Pd/µS-pDVB10, showing that either the reaction was structure insensitive or diffusion limited to some extent over Pd/C, in which the support is microporous. The open pore structure of Pd/µS-pDVB10, possibly ensuring the fast removal of H<sub<2</sub<O<sub<2</sub< from the catalyst, could also be the cause of the relatively high selectivity of this catalyst. In summary, Pd/µS-pDVB10 was the most productive catalyst, forming ca 375 mol<sub<H<sub<2</sub<O<sub<2</sub<</sub<·kg<sub<Pd</sub<<sup<−1</sup<·h<sup<−1</sup<, also because it retained a constant selectivity, while the other ones underwent a more or less pronounced loss of selectivity after 80⁻90 min. Ageing experiments showed that for a palladium catalyst supported on sulfonated mesoporous poly-divinylbenzene storage under oxidative conditions implied some deactivation, but a lower drop in the selectivity; regeneration upon a reductive treatment or storage under strictly anaerobic conditions (dry-box) lead to an increase of the activity but to both a lower initial selectivity and a higher drop of selectivity with time.
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title_short	Direct Synthesis of Hydrogen Peroxide under Semi-Batch Conditions over Un-Promoted Palladium Catalysts Supported by Ion-Exchange Sulfonated Resins: Effects of the Support Morphology
url	https://doi.org/10.3390/catal9020124 https://doaj.org/article/f31e534b8e25426a8f4ec5e180fd72a4 https://www.mdpi.com/2073-4344/9/2/124 https://doaj.org/toc/2073-4344
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author2	Chiara Dalla Valle Claudio Evangelisti Paolo Centomo Marco Zecca
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Direct Synthesis of Hydrogen Peroxide under Semi-Batch Conditions over Un-Promoted Palladium Catalysts Supported by Ion-Exchange Sulfonated Resins: Effects of the Support Morphology

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