Mesoporous silica stabilized MOF nanoreactor for highly selective semi-hydrogenation of phenylacetylene via synergistic effect of Pd and Ru single site
Abstract Selective semi-hydrogenation of phenylacetylene to styrene is a crucial step in the polystyrene industry. Although Pd-based catalysts are widely used in this reaction due to their excellent hydrogenation activity, the selectivity for styrene remains a great challenge. Herein, we designed a...
Ausführliche Beschreibung
Autor*in: |
Li, Zhenxing [verfasserIn] |
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Format: |
E-Artikel |
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Sprache: |
Englisch |
Erschienen: |
2021 |
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Schlagwörter: |
metal-organic frameworks (MOF) |
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Anmerkung: |
© Tsinghua University Press and Springer-Verlag GmbH Germany, part of Springer Nature 2021 |
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Übergeordnetes Werk: |
Enthalten in: Nano research - [S.l.] : Tsinghua Press, 2008, 15(2021), 3 vom: 30. Sept., Seite 1983-1992 |
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Übergeordnetes Werk: |
volume:15 ; year:2021 ; number:3 ; day:30 ; month:09 ; pages:1983-1992 |
Links: |
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DOI / URN: |
10.1007/s12274-021-3849-2 |
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Katalog-ID: |
SPR050487582 |
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520 | |a Abstract Selective semi-hydrogenation of phenylacetylene to styrene is a crucial step in the polystyrene industry. Although Pd-based catalysts are widely used in this reaction due to their excellent hydrogenation activity, the selectivity for styrene remains a great challenge. Herein, we designed a mesoporous silica stabilized Pd-RuZIF-8 (MS Pd-Ru@ZIF-8) nanoreactor with novel Pd and Ru single site synergistic catalytical system for semi-hydrogenation of phenylacetylene. The nanoreactor exhibited a superior performance, achieving 98% conversion of phenylacetylene and 96% selectivity to styrene. Turnover frequency (TOF) of nanoreactor was up to as high as 2,188 $ h^{−1} $, which was 25 times and 5 times more than the single metal species catalysts, mesoporous silica stabilized Pd@ZIF-8 nanoreactor (MS Pd@ZIF-8), and mesoporous silica stabilized Ru@ZIF-8 nanoreactor (MS Ru@ZIF-8). This catalytic activity was attributed to the synergistic effect of Pd and Ru single site anchored strongly into the framework of ZIF-8, which reduced the desorption energy of styrene and increased the hydrogenation energy barrier of styrene. Importantly, since the ordered mesoporous silica was introduced into the nanoreactor shell to stabilize ZIF-8, MS Pd-Ru@ZIF-8 showed excellent reusability and stability. After the five cycles, the catalytical activity and selectivity still remained. This work provides insights for a synergistic catalytic system based on single-site active sites for selective hydrogenation reactions. | ||
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650 | 4 | |a semi-hydrogenation of phenylacetylene |7 (dpeaa)DE-He213 | |
650 | 4 | |a synergistic effect |7 (dpeaa)DE-He213 | |
650 | 4 | |a single site |7 (dpeaa)DE-He213 | |
700 | 1 | |a Hu, Mingliang |4 aut | |
700 | 1 | |a Liu, Jiahao |4 aut | |
700 | 1 | |a Wang, Weiwei |4 aut | |
700 | 1 | |a Li, Yanjie |4 aut | |
700 | 1 | |a Fan, Wenbin |4 aut | |
700 | 1 | |a Gong, Yixuan |4 aut | |
700 | 1 | |a Yao, Jiasai |4 aut | |
700 | 1 | |a Wang, Ping |4 aut | |
700 | 1 | |a He, Miao |4 aut | |
700 | 1 | |a Li, Yongle |4 aut | |
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10.1007/s12274-021-3849-2 doi (DE-627)SPR050487582 (SPR)s12274-021-3849-2-e DE-627 ger DE-627 rakwb eng Li, Zhenxing verfasserin aut Mesoporous silica stabilized MOF nanoreactor for highly selective semi-hydrogenation of phenylacetylene via synergistic effect of Pd and Ru single site 2021 Text txt rdacontent Computermedien c rdamedia Online-Ressource cr rdacarrier © Tsinghua University Press and Springer-Verlag GmbH Germany, part of Springer Nature 2021 Abstract Selective semi-hydrogenation of phenylacetylene to styrene is a crucial step in the polystyrene industry. Although Pd-based catalysts are widely used in this reaction due to their excellent hydrogenation activity, the selectivity for styrene remains a great challenge. Herein, we designed a mesoporous silica stabilized Pd-RuZIF-8 (MS Pd-Ru@ZIF-8) nanoreactor with novel Pd and Ru single site synergistic catalytical system for semi-hydrogenation of phenylacetylene. The nanoreactor exhibited a superior performance, achieving 98% conversion of phenylacetylene and 96% selectivity to styrene. Turnover frequency (TOF) of nanoreactor was up to as high as 2,188 $ h^{−1} $, which was 25 times and 5 times more than the single metal species catalysts, mesoporous silica stabilized Pd@ZIF-8 nanoreactor (MS Pd@ZIF-8), and mesoporous silica stabilized Ru@ZIF-8 nanoreactor (MS Ru@ZIF-8). This catalytic activity was attributed to the synergistic effect of Pd and Ru single site anchored strongly into the framework of ZIF-8, which reduced the desorption energy of styrene and increased the hydrogenation energy barrier of styrene. Importantly, since the ordered mesoporous silica was introduced into the nanoreactor shell to stabilize ZIF-8, MS Pd-Ru@ZIF-8 showed excellent reusability and stability. After the five cycles, the catalytical activity and selectivity still remained. This work provides insights for a synergistic catalytic system based on single-site active sites for selective hydrogenation reactions. mesoporous silica (dpeaa)DE-He213 metal-organic frameworks (MOF) (dpeaa)DE-He213 semi-hydrogenation of phenylacetylene (dpeaa)DE-He213 synergistic effect (dpeaa)DE-He213 single site (dpeaa)DE-He213 Hu, Mingliang aut Liu, Jiahao aut Wang, Weiwei aut Li, Yanjie aut Fan, Wenbin aut Gong, Yixuan aut Yao, Jiasai aut Wang, Ping aut He, Miao aut Li, Yongle aut Enthalten in Nano research [S.l.] : Tsinghua Press, 2008 15(2021), 3 vom: 30. Sept., Seite 1983-1992 (DE-627)57375361X (DE-600)2442216-2 1998-0000 nnns volume:15 year:2021 number:3 day:30 month:09 pages:1983-1992 https://dx.doi.org/10.1007/s12274-021-3849-2 lizenzpflichtig Volltext GBV_USEFLAG_A SYSFLAG_A GBV_SPRINGER GBV_ILN_11 GBV_ILN_20 GBV_ILN_22 GBV_ILN_23 GBV_ILN_24 GBV_ILN_31 GBV_ILN_32 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_74 GBV_ILN_90 GBV_ILN_95 GBV_ILN_100 GBV_ILN_101 GBV_ILN_105 GBV_ILN_110 GBV_ILN_120 GBV_ILN_138 GBV_ILN_150 GBV_ILN_151 GBV_ILN_152 GBV_ILN_161 GBV_ILN_170 GBV_ILN_171 GBV_ILN_187 GBV_ILN_213 GBV_ILN_224 GBV_ILN_230 GBV_ILN_250 GBV_ILN_281 GBV_ILN_285 GBV_ILN_293 GBV_ILN_370 GBV_ILN_602 GBV_ILN_636 GBV_ILN_702 GBV_ILN_2001 GBV_ILN_2003 GBV_ILN_2004 GBV_ILN_2005 GBV_ILN_2006 GBV_ILN_2007 GBV_ILN_2008 GBV_ILN_2009 GBV_ILN_2010 GBV_ILN_2011 GBV_ILN_2014 GBV_ILN_2015 GBV_ILN_2020 GBV_ILN_2021 GBV_ILN_2025 GBV_ILN_2026 GBV_ILN_2027 GBV_ILN_2031 GBV_ILN_2034 GBV_ILN_2037 GBV_ILN_2038 GBV_ILN_2039 GBV_ILN_2044 GBV_ILN_2048 GBV_ILN_2049 GBV_ILN_2050 GBV_ILN_2055 GBV_ILN_2056 GBV_ILN_2057 GBV_ILN_2059 GBV_ILN_2061 GBV_ILN_2064 GBV_ILN_2065 GBV_ILN_2068 GBV_ILN_2088 GBV_ILN_2093 GBV_ILN_2106 GBV_ILN_2107 GBV_ILN_2108 GBV_ILN_2110 GBV_ILN_2111 GBV_ILN_2112 GBV_ILN_2113 GBV_ILN_2118 GBV_ILN_2122 GBV_ILN_2129 GBV_ILN_2143 GBV_ILN_2144 GBV_ILN_2147 GBV_ILN_2148 GBV_ILN_2152 GBV_ILN_2153 GBV_ILN_2188 GBV_ILN_2190 GBV_ILN_2232 GBV_ILN_2336 GBV_ILN_2446 GBV_ILN_2470 GBV_ILN_2472 GBV_ILN_2507 GBV_ILN_2522 GBV_ILN_2548 GBV_ILN_4035 GBV_ILN_4037 GBV_ILN_4046 GBV_ILN_4112 GBV_ILN_4125 GBV_ILN_4126 GBV_ILN_4242 GBV_ILN_4246 GBV_ILN_4249 GBV_ILN_4251 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_4326 GBV_ILN_4328 GBV_ILN_4333 GBV_ILN_4334 GBV_ILN_4335 GBV_ILN_4336 GBV_ILN_4338 GBV_ILN_4393 GBV_ILN_4700 AR 15 2021 3 30 09 1983-1992 |
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10.1007/s12274-021-3849-2 doi (DE-627)SPR050487582 (SPR)s12274-021-3849-2-e DE-627 ger DE-627 rakwb eng Li, Zhenxing verfasserin aut Mesoporous silica stabilized MOF nanoreactor for highly selective semi-hydrogenation of phenylacetylene via synergistic effect of Pd and Ru single site 2021 Text txt rdacontent Computermedien c rdamedia Online-Ressource cr rdacarrier © Tsinghua University Press and Springer-Verlag GmbH Germany, part of Springer Nature 2021 Abstract Selective semi-hydrogenation of phenylacetylene to styrene is a crucial step in the polystyrene industry. Although Pd-based catalysts are widely used in this reaction due to their excellent hydrogenation activity, the selectivity for styrene remains a great challenge. Herein, we designed a mesoporous silica stabilized Pd-RuZIF-8 (MS Pd-Ru@ZIF-8) nanoreactor with novel Pd and Ru single site synergistic catalytical system for semi-hydrogenation of phenylacetylene. The nanoreactor exhibited a superior performance, achieving 98% conversion of phenylacetylene and 96% selectivity to styrene. Turnover frequency (TOF) of nanoreactor was up to as high as 2,188 $ h^{−1} $, which was 25 times and 5 times more than the single metal species catalysts, mesoporous silica stabilized Pd@ZIF-8 nanoreactor (MS Pd@ZIF-8), and mesoporous silica stabilized Ru@ZIF-8 nanoreactor (MS Ru@ZIF-8). This catalytic activity was attributed to the synergistic effect of Pd and Ru single site anchored strongly into the framework of ZIF-8, which reduced the desorption energy of styrene and increased the hydrogenation energy barrier of styrene. Importantly, since the ordered mesoporous silica was introduced into the nanoreactor shell to stabilize ZIF-8, MS Pd-Ru@ZIF-8 showed excellent reusability and stability. After the five cycles, the catalytical activity and selectivity still remained. This work provides insights for a synergistic catalytic system based on single-site active sites for selective hydrogenation reactions. mesoporous silica (dpeaa)DE-He213 metal-organic frameworks (MOF) (dpeaa)DE-He213 semi-hydrogenation of phenylacetylene (dpeaa)DE-He213 synergistic effect (dpeaa)DE-He213 single site (dpeaa)DE-He213 Hu, Mingliang aut Liu, Jiahao aut Wang, Weiwei aut Li, Yanjie aut Fan, Wenbin aut Gong, Yixuan aut Yao, Jiasai aut Wang, Ping aut He, Miao aut Li, Yongle aut Enthalten in Nano research [S.l.] : Tsinghua Press, 2008 15(2021), 3 vom: 30. Sept., Seite 1983-1992 (DE-627)57375361X (DE-600)2442216-2 1998-0000 nnns volume:15 year:2021 number:3 day:30 month:09 pages:1983-1992 https://dx.doi.org/10.1007/s12274-021-3849-2 lizenzpflichtig Volltext GBV_USEFLAG_A SYSFLAG_A GBV_SPRINGER GBV_ILN_11 GBV_ILN_20 GBV_ILN_22 GBV_ILN_23 GBV_ILN_24 GBV_ILN_31 GBV_ILN_32 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_74 GBV_ILN_90 GBV_ILN_95 GBV_ILN_100 GBV_ILN_101 GBV_ILN_105 GBV_ILN_110 GBV_ILN_120 GBV_ILN_138 GBV_ILN_150 GBV_ILN_151 GBV_ILN_152 GBV_ILN_161 GBV_ILN_170 GBV_ILN_171 GBV_ILN_187 GBV_ILN_213 GBV_ILN_224 GBV_ILN_230 GBV_ILN_250 GBV_ILN_281 GBV_ILN_285 GBV_ILN_293 GBV_ILN_370 GBV_ILN_602 GBV_ILN_636 GBV_ILN_702 GBV_ILN_2001 GBV_ILN_2003 GBV_ILN_2004 GBV_ILN_2005 GBV_ILN_2006 GBV_ILN_2007 GBV_ILN_2008 GBV_ILN_2009 GBV_ILN_2010 GBV_ILN_2011 GBV_ILN_2014 GBV_ILN_2015 GBV_ILN_2020 GBV_ILN_2021 GBV_ILN_2025 GBV_ILN_2026 GBV_ILN_2027 GBV_ILN_2031 GBV_ILN_2034 GBV_ILN_2037 GBV_ILN_2038 GBV_ILN_2039 GBV_ILN_2044 GBV_ILN_2048 GBV_ILN_2049 GBV_ILN_2050 GBV_ILN_2055 GBV_ILN_2056 GBV_ILN_2057 GBV_ILN_2059 GBV_ILN_2061 GBV_ILN_2064 GBV_ILN_2065 GBV_ILN_2068 GBV_ILN_2088 GBV_ILN_2093 GBV_ILN_2106 GBV_ILN_2107 GBV_ILN_2108 GBV_ILN_2110 GBV_ILN_2111 GBV_ILN_2112 GBV_ILN_2113 GBV_ILN_2118 GBV_ILN_2122 GBV_ILN_2129 GBV_ILN_2143 GBV_ILN_2144 GBV_ILN_2147 GBV_ILN_2148 GBV_ILN_2152 GBV_ILN_2153 GBV_ILN_2188 GBV_ILN_2190 GBV_ILN_2232 GBV_ILN_2336 GBV_ILN_2446 GBV_ILN_2470 GBV_ILN_2472 GBV_ILN_2507 GBV_ILN_2522 GBV_ILN_2548 GBV_ILN_4035 GBV_ILN_4037 GBV_ILN_4046 GBV_ILN_4112 GBV_ILN_4125 GBV_ILN_4126 GBV_ILN_4242 GBV_ILN_4246 GBV_ILN_4249 GBV_ILN_4251 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_4326 GBV_ILN_4328 GBV_ILN_4333 GBV_ILN_4334 GBV_ILN_4335 GBV_ILN_4336 GBV_ILN_4338 GBV_ILN_4393 GBV_ILN_4700 AR 15 2021 3 30 09 1983-1992 |
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10.1007/s12274-021-3849-2 doi (DE-627)SPR050487582 (SPR)s12274-021-3849-2-e DE-627 ger DE-627 rakwb eng Li, Zhenxing verfasserin aut Mesoporous silica stabilized MOF nanoreactor for highly selective semi-hydrogenation of phenylacetylene via synergistic effect of Pd and Ru single site 2021 Text txt rdacontent Computermedien c rdamedia Online-Ressource cr rdacarrier © Tsinghua University Press and Springer-Verlag GmbH Germany, part of Springer Nature 2021 Abstract Selective semi-hydrogenation of phenylacetylene to styrene is a crucial step in the polystyrene industry. Although Pd-based catalysts are widely used in this reaction due to their excellent hydrogenation activity, the selectivity for styrene remains a great challenge. Herein, we designed a mesoporous silica stabilized Pd-RuZIF-8 (MS Pd-Ru@ZIF-8) nanoreactor with novel Pd and Ru single site synergistic catalytical system for semi-hydrogenation of phenylacetylene. The nanoreactor exhibited a superior performance, achieving 98% conversion of phenylacetylene and 96% selectivity to styrene. Turnover frequency (TOF) of nanoreactor was up to as high as 2,188 $ h^{−1} $, which was 25 times and 5 times more than the single metal species catalysts, mesoporous silica stabilized Pd@ZIF-8 nanoreactor (MS Pd@ZIF-8), and mesoporous silica stabilized Ru@ZIF-8 nanoreactor (MS Ru@ZIF-8). This catalytic activity was attributed to the synergistic effect of Pd and Ru single site anchored strongly into the framework of ZIF-8, which reduced the desorption energy of styrene and increased the hydrogenation energy barrier of styrene. Importantly, since the ordered mesoporous silica was introduced into the nanoreactor shell to stabilize ZIF-8, MS Pd-Ru@ZIF-8 showed excellent reusability and stability. After the five cycles, the catalytical activity and selectivity still remained. This work provides insights for a synergistic catalytic system based on single-site active sites for selective hydrogenation reactions. mesoporous silica (dpeaa)DE-He213 metal-organic frameworks (MOF) (dpeaa)DE-He213 semi-hydrogenation of phenylacetylene (dpeaa)DE-He213 synergistic effect (dpeaa)DE-He213 single site (dpeaa)DE-He213 Hu, Mingliang aut Liu, Jiahao aut Wang, Weiwei aut Li, Yanjie aut Fan, Wenbin aut Gong, Yixuan aut Yao, Jiasai aut Wang, Ping aut He, Miao aut Li, Yongle aut Enthalten in Nano research [S.l.] : Tsinghua Press, 2008 15(2021), 3 vom: 30. Sept., Seite 1983-1992 (DE-627)57375361X (DE-600)2442216-2 1998-0000 nnns volume:15 year:2021 number:3 day:30 month:09 pages:1983-1992 https://dx.doi.org/10.1007/s12274-021-3849-2 lizenzpflichtig Volltext GBV_USEFLAG_A SYSFLAG_A GBV_SPRINGER GBV_ILN_11 GBV_ILN_20 GBV_ILN_22 GBV_ILN_23 GBV_ILN_24 GBV_ILN_31 GBV_ILN_32 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_74 GBV_ILN_90 GBV_ILN_95 GBV_ILN_100 GBV_ILN_101 GBV_ILN_105 GBV_ILN_110 GBV_ILN_120 GBV_ILN_138 GBV_ILN_150 GBV_ILN_151 GBV_ILN_152 GBV_ILN_161 GBV_ILN_170 GBV_ILN_171 GBV_ILN_187 GBV_ILN_213 GBV_ILN_224 GBV_ILN_230 GBV_ILN_250 GBV_ILN_281 GBV_ILN_285 GBV_ILN_293 GBV_ILN_370 GBV_ILN_602 GBV_ILN_636 GBV_ILN_702 GBV_ILN_2001 GBV_ILN_2003 GBV_ILN_2004 GBV_ILN_2005 GBV_ILN_2006 GBV_ILN_2007 GBV_ILN_2008 GBV_ILN_2009 GBV_ILN_2010 GBV_ILN_2011 GBV_ILN_2014 GBV_ILN_2015 GBV_ILN_2020 GBV_ILN_2021 GBV_ILN_2025 GBV_ILN_2026 GBV_ILN_2027 GBV_ILN_2031 GBV_ILN_2034 GBV_ILN_2037 GBV_ILN_2038 GBV_ILN_2039 GBV_ILN_2044 GBV_ILN_2048 GBV_ILN_2049 GBV_ILN_2050 GBV_ILN_2055 GBV_ILN_2056 GBV_ILN_2057 GBV_ILN_2059 GBV_ILN_2061 GBV_ILN_2064 GBV_ILN_2065 GBV_ILN_2068 GBV_ILN_2088 GBV_ILN_2093 GBV_ILN_2106 GBV_ILN_2107 GBV_ILN_2108 GBV_ILN_2110 GBV_ILN_2111 GBV_ILN_2112 GBV_ILN_2113 GBV_ILN_2118 GBV_ILN_2122 GBV_ILN_2129 GBV_ILN_2143 GBV_ILN_2144 GBV_ILN_2147 GBV_ILN_2148 GBV_ILN_2152 GBV_ILN_2153 GBV_ILN_2188 GBV_ILN_2190 GBV_ILN_2232 GBV_ILN_2336 GBV_ILN_2446 GBV_ILN_2470 GBV_ILN_2472 GBV_ILN_2507 GBV_ILN_2522 GBV_ILN_2548 GBV_ILN_4035 GBV_ILN_4037 GBV_ILN_4046 GBV_ILN_4112 GBV_ILN_4125 GBV_ILN_4126 GBV_ILN_4242 GBV_ILN_4246 GBV_ILN_4249 GBV_ILN_4251 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_4326 GBV_ILN_4328 GBV_ILN_4333 GBV_ILN_4334 GBV_ILN_4335 GBV_ILN_4336 GBV_ILN_4338 GBV_ILN_4393 GBV_ILN_4700 AR 15 2021 3 30 09 1983-1992 |
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10.1007/s12274-021-3849-2 doi (DE-627)SPR050487582 (SPR)s12274-021-3849-2-e DE-627 ger DE-627 rakwb eng Li, Zhenxing verfasserin aut Mesoporous silica stabilized MOF nanoreactor for highly selective semi-hydrogenation of phenylacetylene via synergistic effect of Pd and Ru single site 2021 Text txt rdacontent Computermedien c rdamedia Online-Ressource cr rdacarrier © Tsinghua University Press and Springer-Verlag GmbH Germany, part of Springer Nature 2021 Abstract Selective semi-hydrogenation of phenylacetylene to styrene is a crucial step in the polystyrene industry. Although Pd-based catalysts are widely used in this reaction due to their excellent hydrogenation activity, the selectivity for styrene remains a great challenge. Herein, we designed a mesoporous silica stabilized Pd-RuZIF-8 (MS Pd-Ru@ZIF-8) nanoreactor with novel Pd and Ru single site synergistic catalytical system for semi-hydrogenation of phenylacetylene. The nanoreactor exhibited a superior performance, achieving 98% conversion of phenylacetylene and 96% selectivity to styrene. Turnover frequency (TOF) of nanoreactor was up to as high as 2,188 $ h^{−1} $, which was 25 times and 5 times more than the single metal species catalysts, mesoporous silica stabilized Pd@ZIF-8 nanoreactor (MS Pd@ZIF-8), and mesoporous silica stabilized Ru@ZIF-8 nanoreactor (MS Ru@ZIF-8). This catalytic activity was attributed to the synergistic effect of Pd and Ru single site anchored strongly into the framework of ZIF-8, which reduced the desorption energy of styrene and increased the hydrogenation energy barrier of styrene. Importantly, since the ordered mesoporous silica was introduced into the nanoreactor shell to stabilize ZIF-8, MS Pd-Ru@ZIF-8 showed excellent reusability and stability. After the five cycles, the catalytical activity and selectivity still remained. This work provides insights for a synergistic catalytic system based on single-site active sites for selective hydrogenation reactions. mesoporous silica (dpeaa)DE-He213 metal-organic frameworks (MOF) (dpeaa)DE-He213 semi-hydrogenation of phenylacetylene (dpeaa)DE-He213 synergistic effect (dpeaa)DE-He213 single site (dpeaa)DE-He213 Hu, Mingliang aut Liu, Jiahao aut Wang, Weiwei aut Li, Yanjie aut Fan, Wenbin aut Gong, Yixuan aut Yao, Jiasai aut Wang, Ping aut He, Miao aut Li, Yongle aut Enthalten in Nano research [S.l.] : Tsinghua Press, 2008 15(2021), 3 vom: 30. Sept., Seite 1983-1992 (DE-627)57375361X (DE-600)2442216-2 1998-0000 nnns volume:15 year:2021 number:3 day:30 month:09 pages:1983-1992 https://dx.doi.org/10.1007/s12274-021-3849-2 lizenzpflichtig Volltext GBV_USEFLAG_A SYSFLAG_A GBV_SPRINGER GBV_ILN_11 GBV_ILN_20 GBV_ILN_22 GBV_ILN_23 GBV_ILN_24 GBV_ILN_31 GBV_ILN_32 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_74 GBV_ILN_90 GBV_ILN_95 GBV_ILN_100 GBV_ILN_101 GBV_ILN_105 GBV_ILN_110 GBV_ILN_120 GBV_ILN_138 GBV_ILN_150 GBV_ILN_151 GBV_ILN_152 GBV_ILN_161 GBV_ILN_170 GBV_ILN_171 GBV_ILN_187 GBV_ILN_213 GBV_ILN_224 GBV_ILN_230 GBV_ILN_250 GBV_ILN_281 GBV_ILN_285 GBV_ILN_293 GBV_ILN_370 GBV_ILN_602 GBV_ILN_636 GBV_ILN_702 GBV_ILN_2001 GBV_ILN_2003 GBV_ILN_2004 GBV_ILN_2005 GBV_ILN_2006 GBV_ILN_2007 GBV_ILN_2008 GBV_ILN_2009 GBV_ILN_2010 GBV_ILN_2011 GBV_ILN_2014 GBV_ILN_2015 GBV_ILN_2020 GBV_ILN_2021 GBV_ILN_2025 GBV_ILN_2026 GBV_ILN_2027 GBV_ILN_2031 GBV_ILN_2034 GBV_ILN_2037 GBV_ILN_2038 GBV_ILN_2039 GBV_ILN_2044 GBV_ILN_2048 GBV_ILN_2049 GBV_ILN_2050 GBV_ILN_2055 GBV_ILN_2056 GBV_ILN_2057 GBV_ILN_2059 GBV_ILN_2061 GBV_ILN_2064 GBV_ILN_2065 GBV_ILN_2068 GBV_ILN_2088 GBV_ILN_2093 GBV_ILN_2106 GBV_ILN_2107 GBV_ILN_2108 GBV_ILN_2110 GBV_ILN_2111 GBV_ILN_2112 GBV_ILN_2113 GBV_ILN_2118 GBV_ILN_2122 GBV_ILN_2129 GBV_ILN_2143 GBV_ILN_2144 GBV_ILN_2147 GBV_ILN_2148 GBV_ILN_2152 GBV_ILN_2153 GBV_ILN_2188 GBV_ILN_2190 GBV_ILN_2232 GBV_ILN_2336 GBV_ILN_2446 GBV_ILN_2470 GBV_ILN_2472 GBV_ILN_2507 GBV_ILN_2522 GBV_ILN_2548 GBV_ILN_4035 GBV_ILN_4037 GBV_ILN_4046 GBV_ILN_4112 GBV_ILN_4125 GBV_ILN_4126 GBV_ILN_4242 GBV_ILN_4246 GBV_ILN_4249 GBV_ILN_4251 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_4326 GBV_ILN_4328 GBV_ILN_4333 GBV_ILN_4334 GBV_ILN_4335 GBV_ILN_4336 GBV_ILN_4338 GBV_ILN_4393 GBV_ILN_4700 AR 15 2021 3 30 09 1983-1992 |
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10.1007/s12274-021-3849-2 doi (DE-627)SPR050487582 (SPR)s12274-021-3849-2-e DE-627 ger DE-627 rakwb eng Li, Zhenxing verfasserin aut Mesoporous silica stabilized MOF nanoreactor for highly selective semi-hydrogenation of phenylacetylene via synergistic effect of Pd and Ru single site 2021 Text txt rdacontent Computermedien c rdamedia Online-Ressource cr rdacarrier © Tsinghua University Press and Springer-Verlag GmbH Germany, part of Springer Nature 2021 Abstract Selective semi-hydrogenation of phenylacetylene to styrene is a crucial step in the polystyrene industry. Although Pd-based catalysts are widely used in this reaction due to their excellent hydrogenation activity, the selectivity for styrene remains a great challenge. Herein, we designed a mesoporous silica stabilized Pd-RuZIF-8 (MS Pd-Ru@ZIF-8) nanoreactor with novel Pd and Ru single site synergistic catalytical system for semi-hydrogenation of phenylacetylene. The nanoreactor exhibited a superior performance, achieving 98% conversion of phenylacetylene and 96% selectivity to styrene. Turnover frequency (TOF) of nanoreactor was up to as high as 2,188 $ h^{−1} $, which was 25 times and 5 times more than the single metal species catalysts, mesoporous silica stabilized Pd@ZIF-8 nanoreactor (MS Pd@ZIF-8), and mesoporous silica stabilized Ru@ZIF-8 nanoreactor (MS Ru@ZIF-8). This catalytic activity was attributed to the synergistic effect of Pd and Ru single site anchored strongly into the framework of ZIF-8, which reduced the desorption energy of styrene and increased the hydrogenation energy barrier of styrene. Importantly, since the ordered mesoporous silica was introduced into the nanoreactor shell to stabilize ZIF-8, MS Pd-Ru@ZIF-8 showed excellent reusability and stability. After the five cycles, the catalytical activity and selectivity still remained. This work provides insights for a synergistic catalytic system based on single-site active sites for selective hydrogenation reactions. mesoporous silica (dpeaa)DE-He213 metal-organic frameworks (MOF) (dpeaa)DE-He213 semi-hydrogenation of phenylacetylene (dpeaa)DE-He213 synergistic effect (dpeaa)DE-He213 single site (dpeaa)DE-He213 Hu, Mingliang aut Liu, Jiahao aut Wang, Weiwei aut Li, Yanjie aut Fan, Wenbin aut Gong, Yixuan aut Yao, Jiasai aut Wang, Ping aut He, Miao aut Li, Yongle aut Enthalten in Nano research [S.l.] : Tsinghua Press, 2008 15(2021), 3 vom: 30. Sept., Seite 1983-1992 (DE-627)57375361X (DE-600)2442216-2 1998-0000 nnns volume:15 year:2021 number:3 day:30 month:09 pages:1983-1992 https://dx.doi.org/10.1007/s12274-021-3849-2 lizenzpflichtig Volltext GBV_USEFLAG_A SYSFLAG_A GBV_SPRINGER GBV_ILN_11 GBV_ILN_20 GBV_ILN_22 GBV_ILN_23 GBV_ILN_24 GBV_ILN_31 GBV_ILN_32 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_74 GBV_ILN_90 GBV_ILN_95 GBV_ILN_100 GBV_ILN_101 GBV_ILN_105 GBV_ILN_110 GBV_ILN_120 GBV_ILN_138 GBV_ILN_150 GBV_ILN_151 GBV_ILN_152 GBV_ILN_161 GBV_ILN_170 GBV_ILN_171 GBV_ILN_187 GBV_ILN_213 GBV_ILN_224 GBV_ILN_230 GBV_ILN_250 GBV_ILN_281 GBV_ILN_285 GBV_ILN_293 GBV_ILN_370 GBV_ILN_602 GBV_ILN_636 GBV_ILN_702 GBV_ILN_2001 GBV_ILN_2003 GBV_ILN_2004 GBV_ILN_2005 GBV_ILN_2006 GBV_ILN_2007 GBV_ILN_2008 GBV_ILN_2009 GBV_ILN_2010 GBV_ILN_2011 GBV_ILN_2014 GBV_ILN_2015 GBV_ILN_2020 GBV_ILN_2021 GBV_ILN_2025 GBV_ILN_2026 GBV_ILN_2027 GBV_ILN_2031 GBV_ILN_2034 GBV_ILN_2037 GBV_ILN_2038 GBV_ILN_2039 GBV_ILN_2044 GBV_ILN_2048 GBV_ILN_2049 GBV_ILN_2050 GBV_ILN_2055 GBV_ILN_2056 GBV_ILN_2057 GBV_ILN_2059 GBV_ILN_2061 GBV_ILN_2064 GBV_ILN_2065 GBV_ILN_2068 GBV_ILN_2088 GBV_ILN_2093 GBV_ILN_2106 GBV_ILN_2107 GBV_ILN_2108 GBV_ILN_2110 GBV_ILN_2111 GBV_ILN_2112 GBV_ILN_2113 GBV_ILN_2118 GBV_ILN_2122 GBV_ILN_2129 GBV_ILN_2143 GBV_ILN_2144 GBV_ILN_2147 GBV_ILN_2148 GBV_ILN_2152 GBV_ILN_2153 GBV_ILN_2188 GBV_ILN_2190 GBV_ILN_2232 GBV_ILN_2336 GBV_ILN_2446 GBV_ILN_2470 GBV_ILN_2472 GBV_ILN_2507 GBV_ILN_2522 GBV_ILN_2548 GBV_ILN_4035 GBV_ILN_4037 GBV_ILN_4046 GBV_ILN_4112 GBV_ILN_4125 GBV_ILN_4126 GBV_ILN_4242 GBV_ILN_4246 GBV_ILN_4249 GBV_ILN_4251 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_4326 GBV_ILN_4328 GBV_ILN_4333 GBV_ILN_4334 GBV_ILN_4335 GBV_ILN_4336 GBV_ILN_4338 GBV_ILN_4393 GBV_ILN_4700 AR 15 2021 3 30 09 1983-1992 |
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Enthalten in Nano research 15(2021), 3 vom: 30. Sept., Seite 1983-1992 volume:15 year:2021 number:3 day:30 month:09 pages:1983-1992 |
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Enthalten in Nano research 15(2021), 3 vom: 30. Sept., Seite 1983-1992 volume:15 year:2021 number:3 day:30 month:09 pages:1983-1992 |
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Li, Zhenxing @@aut@@ Hu, Mingliang @@aut@@ Liu, Jiahao @@aut@@ Wang, Weiwei @@aut@@ Li, Yanjie @@aut@@ Fan, Wenbin @@aut@@ Gong, Yixuan @@aut@@ Yao, Jiasai @@aut@@ Wang, Ping @@aut@@ He, Miao @@aut@@ Li, Yongle @@aut@@ |
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Although Pd-based catalysts are widely used in this reaction due to their excellent hydrogenation activity, the selectivity for styrene remains a great challenge. Herein, we designed a mesoporous silica stabilized Pd-RuZIF-8 (MS Pd-Ru@ZIF-8) nanoreactor with novel Pd and Ru single site synergistic catalytical system for semi-hydrogenation of phenylacetylene. The nanoreactor exhibited a superior performance, achieving 98% conversion of phenylacetylene and 96% selectivity to styrene. Turnover frequency (TOF) of nanoreactor was up to as high as 2,188 $ h^{−1} $, which was 25 times and 5 times more than the single metal species catalysts, mesoporous silica stabilized Pd@ZIF-8 nanoreactor (MS Pd@ZIF-8), and mesoporous silica stabilized Ru@ZIF-8 nanoreactor (MS Ru@ZIF-8). This catalytic activity was attributed to the synergistic effect of Pd and Ru single site anchored strongly into the framework of ZIF-8, which reduced the desorption energy of styrene and increased the hydrogenation energy barrier of styrene. Importantly, since the ordered mesoporous silica was introduced into the nanoreactor shell to stabilize ZIF-8, MS Pd-Ru@ZIF-8 showed excellent reusability and stability. After the five cycles, the catalytical activity and selectivity still remained. 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|
author |
Li, Zhenxing |
spellingShingle |
Li, Zhenxing misc mesoporous silica misc metal-organic frameworks (MOF) misc semi-hydrogenation of phenylacetylene misc synergistic effect misc single site Mesoporous silica stabilized MOF nanoreactor for highly selective semi-hydrogenation of phenylacetylene via synergistic effect of Pd and Ru single site |
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1998-0000 |
topic_title |
Mesoporous silica stabilized MOF nanoreactor for highly selective semi-hydrogenation of phenylacetylene via synergistic effect of Pd and Ru single site mesoporous silica (dpeaa)DE-He213 metal-organic frameworks (MOF) (dpeaa)DE-He213 semi-hydrogenation of phenylacetylene (dpeaa)DE-He213 synergistic effect (dpeaa)DE-He213 single site (dpeaa)DE-He213 |
topic |
misc mesoporous silica misc metal-organic frameworks (MOF) misc semi-hydrogenation of phenylacetylene misc synergistic effect misc single site |
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misc mesoporous silica misc metal-organic frameworks (MOF) misc semi-hydrogenation of phenylacetylene misc synergistic effect misc single site |
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misc mesoporous silica misc metal-organic frameworks (MOF) misc semi-hydrogenation of phenylacetylene misc synergistic effect misc single site |
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Mesoporous silica stabilized MOF nanoreactor for highly selective semi-hydrogenation of phenylacetylene via synergistic effect of Pd and Ru single site |
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(DE-627)SPR050487582 (SPR)s12274-021-3849-2-e |
title_full |
Mesoporous silica stabilized MOF nanoreactor for highly selective semi-hydrogenation of phenylacetylene via synergistic effect of Pd and Ru single site |
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Li, Zhenxing |
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1983 |
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Li, Zhenxing Hu, Mingliang Liu, Jiahao Wang, Weiwei Li, Yanjie Fan, Wenbin Gong, Yixuan Yao, Jiasai Wang, Ping He, Miao Li, Yongle |
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15 |
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Elektronische Aufsätze |
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Li, Zhenxing |
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10.1007/s12274-021-3849-2 |
title_sort |
mesoporous silica stabilized mof nanoreactor for highly selective semi-hydrogenation of phenylacetylene via synergistic effect of pd and ru single site |
title_auth |
Mesoporous silica stabilized MOF nanoreactor for highly selective semi-hydrogenation of phenylacetylene via synergistic effect of Pd and Ru single site |
abstract |
Abstract Selective semi-hydrogenation of phenylacetylene to styrene is a crucial step in the polystyrene industry. Although Pd-based catalysts are widely used in this reaction due to their excellent hydrogenation activity, the selectivity for styrene remains a great challenge. Herein, we designed a mesoporous silica stabilized Pd-RuZIF-8 (MS Pd-Ru@ZIF-8) nanoreactor with novel Pd and Ru single site synergistic catalytical system for semi-hydrogenation of phenylacetylene. The nanoreactor exhibited a superior performance, achieving 98% conversion of phenylacetylene and 96% selectivity to styrene. Turnover frequency (TOF) of nanoreactor was up to as high as 2,188 $ h^{−1} $, which was 25 times and 5 times more than the single metal species catalysts, mesoporous silica stabilized Pd@ZIF-8 nanoreactor (MS Pd@ZIF-8), and mesoporous silica stabilized Ru@ZIF-8 nanoreactor (MS Ru@ZIF-8). This catalytic activity was attributed to the synergistic effect of Pd and Ru single site anchored strongly into the framework of ZIF-8, which reduced the desorption energy of styrene and increased the hydrogenation energy barrier of styrene. Importantly, since the ordered mesoporous silica was introduced into the nanoreactor shell to stabilize ZIF-8, MS Pd-Ru@ZIF-8 showed excellent reusability and stability. After the five cycles, the catalytical activity and selectivity still remained. This work provides insights for a synergistic catalytic system based on single-site active sites for selective hydrogenation reactions. © Tsinghua University Press and Springer-Verlag GmbH Germany, part of Springer Nature 2021 |
abstractGer |
Abstract Selective semi-hydrogenation of phenylacetylene to styrene is a crucial step in the polystyrene industry. Although Pd-based catalysts are widely used in this reaction due to their excellent hydrogenation activity, the selectivity for styrene remains a great challenge. Herein, we designed a mesoporous silica stabilized Pd-RuZIF-8 (MS Pd-Ru@ZIF-8) nanoreactor with novel Pd and Ru single site synergistic catalytical system for semi-hydrogenation of phenylacetylene. The nanoreactor exhibited a superior performance, achieving 98% conversion of phenylacetylene and 96% selectivity to styrene. Turnover frequency (TOF) of nanoreactor was up to as high as 2,188 $ h^{−1} $, which was 25 times and 5 times more than the single metal species catalysts, mesoporous silica stabilized Pd@ZIF-8 nanoreactor (MS Pd@ZIF-8), and mesoporous silica stabilized Ru@ZIF-8 nanoreactor (MS Ru@ZIF-8). This catalytic activity was attributed to the synergistic effect of Pd and Ru single site anchored strongly into the framework of ZIF-8, which reduced the desorption energy of styrene and increased the hydrogenation energy barrier of styrene. Importantly, since the ordered mesoporous silica was introduced into the nanoreactor shell to stabilize ZIF-8, MS Pd-Ru@ZIF-8 showed excellent reusability and stability. After the five cycles, the catalytical activity and selectivity still remained. This work provides insights for a synergistic catalytic system based on single-site active sites for selective hydrogenation reactions. © Tsinghua University Press and Springer-Verlag GmbH Germany, part of Springer Nature 2021 |
abstract_unstemmed |
Abstract Selective semi-hydrogenation of phenylacetylene to styrene is a crucial step in the polystyrene industry. Although Pd-based catalysts are widely used in this reaction due to their excellent hydrogenation activity, the selectivity for styrene remains a great challenge. Herein, we designed a mesoporous silica stabilized Pd-RuZIF-8 (MS Pd-Ru@ZIF-8) nanoreactor with novel Pd and Ru single site synergistic catalytical system for semi-hydrogenation of phenylacetylene. The nanoreactor exhibited a superior performance, achieving 98% conversion of phenylacetylene and 96% selectivity to styrene. Turnover frequency (TOF) of nanoreactor was up to as high as 2,188 $ h^{−1} $, which was 25 times and 5 times more than the single metal species catalysts, mesoporous silica stabilized Pd@ZIF-8 nanoreactor (MS Pd@ZIF-8), and mesoporous silica stabilized Ru@ZIF-8 nanoreactor (MS Ru@ZIF-8). This catalytic activity was attributed to the synergistic effect of Pd and Ru single site anchored strongly into the framework of ZIF-8, which reduced the desorption energy of styrene and increased the hydrogenation energy barrier of styrene. Importantly, since the ordered mesoporous silica was introduced into the nanoreactor shell to stabilize ZIF-8, MS Pd-Ru@ZIF-8 showed excellent reusability and stability. After the five cycles, the catalytical activity and selectivity still remained. This work provides insights for a synergistic catalytic system based on single-site active sites for selective hydrogenation reactions. © Tsinghua University Press and Springer-Verlag GmbH Germany, part of Springer Nature 2021 |
collection_details |
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container_issue |
3 |
title_short |
Mesoporous silica stabilized MOF nanoreactor for highly selective semi-hydrogenation of phenylacetylene via synergistic effect of Pd and Ru single site |
url |
https://dx.doi.org/10.1007/s12274-021-3849-2 |
remote_bool |
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author2 |
Hu, Mingliang Liu, Jiahao Wang, Weiwei Li, Yanjie Fan, Wenbin Gong, Yixuan Yao, Jiasai Wang, Ping He, Miao Li, Yongle |
author2Str |
Hu, Mingliang Liu, Jiahao Wang, Weiwei Li, Yanjie Fan, Wenbin Gong, Yixuan Yao, Jiasai Wang, Ping He, Miao Li, Yongle |
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doi_str |
10.1007/s12274-021-3849-2 |
up_date |
2024-07-03T15:51:29.957Z |
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|
score |
7.400728 |