Substitution of Cetyltrimethylammonium for OSDA Cations During B-SSZ-70 Zeotype Synthesis and Its Influence on Delamination
We investigated the substitution of structure-directing agent diisobutylimidazolium hydroxide with cetyltrimethylammonium hydroxide (CTA+OH−) surfactant in the synthesis gel of layered-zeotype-precursor B-SSZ-70(P). At low substitution levels, CTA+ interacts with the external-zeotype surface, where...
Ausführliche Beschreibung
Gespeichert in:
| Autor*in: |
Ramamurthy, Maya [verfasserIn] |
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| Format: |
E-Artikel |
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| Sprache: |
Englisch |
| Erschienen: |
2021transfer abstract |
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| Schlagwörter: |
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| Übergeordnetes Werk: |
Enthalten in: Impact of North Atlantic-East Asian teleconnections on extremely high January PM - Kim, Jeong-Hun ELSEVIER, 2021, the official journal of the International Zeolite Association, Amsterdam [u.a.] |
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| Übergeordnetes Werk: |
volume:319 ; year:2021 ; pages:0 |
| Links: |
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| DOI / URN: |
10.1016/j.micromeso.2021.111042 |
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ELV053781880 |
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| 245 | 1 | 0 | |a Substitution of Cetyltrimethylammonium for OSDA Cations During B-SSZ-70 Zeotype Synthesis and Its Influence on Delamination |
| 264 | 1 | |c 2021transfer abstract | |
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| 520 | |a We investigated the substitution of structure-directing agent diisobutylimidazolium hydroxide with cetyltrimethylammonium hydroxide (CTA+OH−) surfactant in the synthesis gel of layered-zeotype-precursor B-SSZ-70(P). At low substitution levels, CTA+ interacts with the external-zeotype surface, where it assembles. At higher surfactant amounts, CTA+ intercalation occurs, leading to swelling of the precursor material, as evidenced by powder X-ray diffraction. Characterization of adsorbed CTA+ cations by 13C MAS NMR spectroscopy demonstrates unique broad resonances in the intercalated layers, which represent a more rigid environment than in the external-surface assemblies. At still higher CTA+ substitution levels in the synthesis gel, we observe the formation of amorphous mesoporous silica. We attempted to delaminate materials synthesized with varying CTA+ substitution levels using mild conditions, in which the conventional sonication step is replaced with an easy-to-scale high-shear mixing, and in which the use of halide reagents, which are corrosive and have been required in the past, is also avoided. Our data demonstrate that synthesis of a swollen material per se is not essential as an intermediate for delamination, and that layered zeolite precursor swelling can actually undermine zeolite delamination. Our results instead point to the CTA+ external-surface assemblies as facilitating ease of SSZ-70 delamination under these mild conditions. When calcined and functionalized with grafted titanium centers, the delaminated materials are highly active and selective olefin epoxidation catalysts with organic hydroperoxides, showing a 40% higher epoxide conversion than a catalyst prepared from conventional B-SSZ-70. | ||
| 520 | |a We investigated the substitution of structure-directing agent diisobutylimidazolium hydroxide with cetyltrimethylammonium hydroxide (CTA+OH−) surfactant in the synthesis gel of layered-zeotype-precursor B-SSZ-70(P). At low substitution levels, CTA+ interacts with the external-zeotype surface, where it assembles. At higher surfactant amounts, CTA+ intercalation occurs, leading to swelling of the precursor material, as evidenced by powder X-ray diffraction. Characterization of adsorbed CTA+ cations by 13C MAS NMR spectroscopy demonstrates unique broad resonances in the intercalated layers, which represent a more rigid environment than in the external-surface assemblies. At still higher CTA+ substitution levels in the synthesis gel, we observe the formation of amorphous mesoporous silica. We attempted to delaminate materials synthesized with varying CTA+ substitution levels using mild conditions, in which the conventional sonication step is replaced with an easy-to-scale high-shear mixing, and in which the use of halide reagents, which are corrosive and have been required in the past, is also avoided. Our data demonstrate that synthesis of a swollen material per se is not essential as an intermediate for delamination, and that layered zeolite precursor swelling can actually undermine zeolite delamination. Our results instead point to the CTA+ external-surface assemblies as facilitating ease of SSZ-70 delamination under these mild conditions. When calcined and functionalized with grafted titanium centers, the delaminated materials are highly active and selective olefin epoxidation catalysts with organic hydroperoxides, showing a 40% higher epoxide conversion than a catalyst prepared from conventional B-SSZ-70. | ||
| 650 | 7 | |a Zeolite delamination |2 Elsevier | |
| 650 | 7 | |a Co-structure directing agent |2 Elsevier | |
| 650 | 7 | |a Epoxidation catalysis |2 Elsevier | |
| 700 | 1 | |a Grosso-Giordano, Nicolás A. |4 oth | |
| 700 | 1 | |a Hwang, Son-Jong |4 oth | |
| 700 | 1 | |a Xu, Le |4 oth | |
| 700 | 1 | |a Xie, Dan |4 oth | |
| 700 | 1 | |a Mishra, Manish |4 oth | |
| 700 | 1 | |a Okrut, Alexander |4 oth | |
| 700 | 1 | |a Zones, Stacey |4 oth | |
| 700 | 1 | |a Katz, Alexander |4 oth | |
| 773 | 0 | 8 | |i Enthalten in |n Elsevier |a Kim, Jeong-Hun ELSEVIER |t Impact of North Atlantic-East Asian teleconnections on extremely high January PM |d 2021 |d the official journal of the International Zeolite Association |g Amsterdam [u.a.] |w (DE-627)ELV006778283 |
| 773 | 1 | 8 | |g volume:319 |g year:2021 |g pages:0 |
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10.1016/j.micromeso.2021.111042 doi /cbs_pica/cbs_olc/import_discovery/elsevier/einzuspielen/GBV00000000001650.pica (DE-627)ELV053781880 (ELSEVIER)S1387-1811(21)00168-2 DE-627 ger DE-627 rakwb eng 333.7 570 690 VZ BIODIV DE-30 fid 48.00 bkl Ramamurthy, Maya verfasserin aut Substitution of Cetyltrimethylammonium for OSDA Cations During B-SSZ-70 Zeotype Synthesis and Its Influence on Delamination 2021transfer abstract nicht spezifiziert zzz rdacontent nicht spezifiziert z rdamedia nicht spezifiziert zu rdacarrier We investigated the substitution of structure-directing agent diisobutylimidazolium hydroxide with cetyltrimethylammonium hydroxide (CTA+OH−) surfactant in the synthesis gel of layered-zeotype-precursor B-SSZ-70(P). At low substitution levels, CTA+ interacts with the external-zeotype surface, where it assembles. At higher surfactant amounts, CTA+ intercalation occurs, leading to swelling of the precursor material, as evidenced by powder X-ray diffraction. Characterization of adsorbed CTA+ cations by 13C MAS NMR spectroscopy demonstrates unique broad resonances in the intercalated layers, which represent a more rigid environment than in the external-surface assemblies. At still higher CTA+ substitution levels in the synthesis gel, we observe the formation of amorphous mesoporous silica. We attempted to delaminate materials synthesized with varying CTA+ substitution levels using mild conditions, in which the conventional sonication step is replaced with an easy-to-scale high-shear mixing, and in which the use of halide reagents, which are corrosive and have been required in the past, is also avoided. Our data demonstrate that synthesis of a swollen material per se is not essential as an intermediate for delamination, and that layered zeolite precursor swelling can actually undermine zeolite delamination. Our results instead point to the CTA+ external-surface assemblies as facilitating ease of SSZ-70 delamination under these mild conditions. When calcined and functionalized with grafted titanium centers, the delaminated materials are highly active and selective olefin epoxidation catalysts with organic hydroperoxides, showing a 40% higher epoxide conversion than a catalyst prepared from conventional B-SSZ-70. We investigated the substitution of structure-directing agent diisobutylimidazolium hydroxide with cetyltrimethylammonium hydroxide (CTA+OH−) surfactant in the synthesis gel of layered-zeotype-precursor B-SSZ-70(P). At low substitution levels, CTA+ interacts with the external-zeotype surface, where it assembles. At higher surfactant amounts, CTA+ intercalation occurs, leading to swelling of the precursor material, as evidenced by powder X-ray diffraction. Characterization of adsorbed CTA+ cations by 13C MAS NMR spectroscopy demonstrates unique broad resonances in the intercalated layers, which represent a more rigid environment than in the external-surface assemblies. At still higher CTA+ substitution levels in the synthesis gel, we observe the formation of amorphous mesoporous silica. We attempted to delaminate materials synthesized with varying CTA+ substitution levels using mild conditions, in which the conventional sonication step is replaced with an easy-to-scale high-shear mixing, and in which the use of halide reagents, which are corrosive and have been required in the past, is also avoided. Our data demonstrate that synthesis of a swollen material per se is not essential as an intermediate for delamination, and that layered zeolite precursor swelling can actually undermine zeolite delamination. Our results instead point to the CTA+ external-surface assemblies as facilitating ease of SSZ-70 delamination under these mild conditions. When calcined and functionalized with grafted titanium centers, the delaminated materials are highly active and selective olefin epoxidation catalysts with organic hydroperoxides, showing a 40% higher epoxide conversion than a catalyst prepared from conventional B-SSZ-70. Zeolite delamination Elsevier Co-structure directing agent Elsevier Epoxidation catalysis Elsevier Grosso-Giordano, Nicolás A. oth Hwang, Son-Jong oth Xu, Le oth Xie, Dan oth Mishra, Manish oth Okrut, Alexander oth Zones, Stacey oth Katz, Alexander oth Enthalten in Elsevier Kim, Jeong-Hun ELSEVIER Impact of North Atlantic-East Asian teleconnections on extremely high January PM 2021 the official journal of the International Zeolite Association Amsterdam [u.a.] (DE-627)ELV006778283 volume:319 year:2021 pages:0 https://doi.org/10.1016/j.micromeso.2021.111042 Volltext GBV_USEFLAG_U GBV_ELV SYSFLAG_U FID-BIODIV SSG-OLC-PHA SSG-OPC-FOR 48.00 Land- und Forstwirtschaft: Allgemeines VZ AR 319 2021 0 |
| spelling |
10.1016/j.micromeso.2021.111042 doi /cbs_pica/cbs_olc/import_discovery/elsevier/einzuspielen/GBV00000000001650.pica (DE-627)ELV053781880 (ELSEVIER)S1387-1811(21)00168-2 DE-627 ger DE-627 rakwb eng 333.7 570 690 VZ BIODIV DE-30 fid 48.00 bkl Ramamurthy, Maya verfasserin aut Substitution of Cetyltrimethylammonium for OSDA Cations During B-SSZ-70 Zeotype Synthesis and Its Influence on Delamination 2021transfer abstract nicht spezifiziert zzz rdacontent nicht spezifiziert z rdamedia nicht spezifiziert zu rdacarrier We investigated the substitution of structure-directing agent diisobutylimidazolium hydroxide with cetyltrimethylammonium hydroxide (CTA+OH−) surfactant in the synthesis gel of layered-zeotype-precursor B-SSZ-70(P). At low substitution levels, CTA+ interacts with the external-zeotype surface, where it assembles. At higher surfactant amounts, CTA+ intercalation occurs, leading to swelling of the precursor material, as evidenced by powder X-ray diffraction. Characterization of adsorbed CTA+ cations by 13C MAS NMR spectroscopy demonstrates unique broad resonances in the intercalated layers, which represent a more rigid environment than in the external-surface assemblies. At still higher CTA+ substitution levels in the synthesis gel, we observe the formation of amorphous mesoporous silica. We attempted to delaminate materials synthesized with varying CTA+ substitution levels using mild conditions, in which the conventional sonication step is replaced with an easy-to-scale high-shear mixing, and in which the use of halide reagents, which are corrosive and have been required in the past, is also avoided. Our data demonstrate that synthesis of a swollen material per se is not essential as an intermediate for delamination, and that layered zeolite precursor swelling can actually undermine zeolite delamination. Our results instead point to the CTA+ external-surface assemblies as facilitating ease of SSZ-70 delamination under these mild conditions. When calcined and functionalized with grafted titanium centers, the delaminated materials are highly active and selective olefin epoxidation catalysts with organic hydroperoxides, showing a 40% higher epoxide conversion than a catalyst prepared from conventional B-SSZ-70. We investigated the substitution of structure-directing agent diisobutylimidazolium hydroxide with cetyltrimethylammonium hydroxide (CTA+OH−) surfactant in the synthesis gel of layered-zeotype-precursor B-SSZ-70(P). At low substitution levels, CTA+ interacts with the external-zeotype surface, where it assembles. At higher surfactant amounts, CTA+ intercalation occurs, leading to swelling of the precursor material, as evidenced by powder X-ray diffraction. Characterization of adsorbed CTA+ cations by 13C MAS NMR spectroscopy demonstrates unique broad resonances in the intercalated layers, which represent a more rigid environment than in the external-surface assemblies. At still higher CTA+ substitution levels in the synthesis gel, we observe the formation of amorphous mesoporous silica. We attempted to delaminate materials synthesized with varying CTA+ substitution levels using mild conditions, in which the conventional sonication step is replaced with an easy-to-scale high-shear mixing, and in which the use of halide reagents, which are corrosive and have been required in the past, is also avoided. Our data demonstrate that synthesis of a swollen material per se is not essential as an intermediate for delamination, and that layered zeolite precursor swelling can actually undermine zeolite delamination. Our results instead point to the CTA+ external-surface assemblies as facilitating ease of SSZ-70 delamination under these mild conditions. When calcined and functionalized with grafted titanium centers, the delaminated materials are highly active and selective olefin epoxidation catalysts with organic hydroperoxides, showing a 40% higher epoxide conversion than a catalyst prepared from conventional B-SSZ-70. Zeolite delamination Elsevier Co-structure directing agent Elsevier Epoxidation catalysis Elsevier Grosso-Giordano, Nicolás A. oth Hwang, Son-Jong oth Xu, Le oth Xie, Dan oth Mishra, Manish oth Okrut, Alexander oth Zones, Stacey oth Katz, Alexander oth Enthalten in Elsevier Kim, Jeong-Hun ELSEVIER Impact of North Atlantic-East Asian teleconnections on extremely high January PM 2021 the official journal of the International Zeolite Association Amsterdam [u.a.] (DE-627)ELV006778283 volume:319 year:2021 pages:0 https://doi.org/10.1016/j.micromeso.2021.111042 Volltext GBV_USEFLAG_U GBV_ELV SYSFLAG_U FID-BIODIV SSG-OLC-PHA SSG-OPC-FOR 48.00 Land- und Forstwirtschaft: Allgemeines VZ AR 319 2021 0 |
| allfields_unstemmed |
10.1016/j.micromeso.2021.111042 doi /cbs_pica/cbs_olc/import_discovery/elsevier/einzuspielen/GBV00000000001650.pica (DE-627)ELV053781880 (ELSEVIER)S1387-1811(21)00168-2 DE-627 ger DE-627 rakwb eng 333.7 570 690 VZ BIODIV DE-30 fid 48.00 bkl Ramamurthy, Maya verfasserin aut Substitution of Cetyltrimethylammonium for OSDA Cations During B-SSZ-70 Zeotype Synthesis and Its Influence on Delamination 2021transfer abstract nicht spezifiziert zzz rdacontent nicht spezifiziert z rdamedia nicht spezifiziert zu rdacarrier We investigated the substitution of structure-directing agent diisobutylimidazolium hydroxide with cetyltrimethylammonium hydroxide (CTA+OH−) surfactant in the synthesis gel of layered-zeotype-precursor B-SSZ-70(P). At low substitution levels, CTA+ interacts with the external-zeotype surface, where it assembles. At higher surfactant amounts, CTA+ intercalation occurs, leading to swelling of the precursor material, as evidenced by powder X-ray diffraction. Characterization of adsorbed CTA+ cations by 13C MAS NMR spectroscopy demonstrates unique broad resonances in the intercalated layers, which represent a more rigid environment than in the external-surface assemblies. At still higher CTA+ substitution levels in the synthesis gel, we observe the formation of amorphous mesoporous silica. We attempted to delaminate materials synthesized with varying CTA+ substitution levels using mild conditions, in which the conventional sonication step is replaced with an easy-to-scale high-shear mixing, and in which the use of halide reagents, which are corrosive and have been required in the past, is also avoided. Our data demonstrate that synthesis of a swollen material per se is not essential as an intermediate for delamination, and that layered zeolite precursor swelling can actually undermine zeolite delamination. Our results instead point to the CTA+ external-surface assemblies as facilitating ease of SSZ-70 delamination under these mild conditions. When calcined and functionalized with grafted titanium centers, the delaminated materials are highly active and selective olefin epoxidation catalysts with organic hydroperoxides, showing a 40% higher epoxide conversion than a catalyst prepared from conventional B-SSZ-70. We investigated the substitution of structure-directing agent diisobutylimidazolium hydroxide with cetyltrimethylammonium hydroxide (CTA+OH−) surfactant in the synthesis gel of layered-zeotype-precursor B-SSZ-70(P). At low substitution levels, CTA+ interacts with the external-zeotype surface, where it assembles. At higher surfactant amounts, CTA+ intercalation occurs, leading to swelling of the precursor material, as evidenced by powder X-ray diffraction. Characterization of adsorbed CTA+ cations by 13C MAS NMR spectroscopy demonstrates unique broad resonances in the intercalated layers, which represent a more rigid environment than in the external-surface assemblies. At still higher CTA+ substitution levels in the synthesis gel, we observe the formation of amorphous mesoporous silica. We attempted to delaminate materials synthesized with varying CTA+ substitution levels using mild conditions, in which the conventional sonication step is replaced with an easy-to-scale high-shear mixing, and in which the use of halide reagents, which are corrosive and have been required in the past, is also avoided. Our data demonstrate that synthesis of a swollen material per se is not essential as an intermediate for delamination, and that layered zeolite precursor swelling can actually undermine zeolite delamination. Our results instead point to the CTA+ external-surface assemblies as facilitating ease of SSZ-70 delamination under these mild conditions. When calcined and functionalized with grafted titanium centers, the delaminated materials are highly active and selective olefin epoxidation catalysts with organic hydroperoxides, showing a 40% higher epoxide conversion than a catalyst prepared from conventional B-SSZ-70. Zeolite delamination Elsevier Co-structure directing agent Elsevier Epoxidation catalysis Elsevier Grosso-Giordano, Nicolás A. oth Hwang, Son-Jong oth Xu, Le oth Xie, Dan oth Mishra, Manish oth Okrut, Alexander oth Zones, Stacey oth Katz, Alexander oth Enthalten in Elsevier Kim, Jeong-Hun ELSEVIER Impact of North Atlantic-East Asian teleconnections on extremely high January PM 2021 the official journal of the International Zeolite Association Amsterdam [u.a.] (DE-627)ELV006778283 volume:319 year:2021 pages:0 https://doi.org/10.1016/j.micromeso.2021.111042 Volltext GBV_USEFLAG_U GBV_ELV SYSFLAG_U FID-BIODIV SSG-OLC-PHA SSG-OPC-FOR 48.00 Land- und Forstwirtschaft: Allgemeines VZ AR 319 2021 0 |
| allfieldsGer |
10.1016/j.micromeso.2021.111042 doi /cbs_pica/cbs_olc/import_discovery/elsevier/einzuspielen/GBV00000000001650.pica (DE-627)ELV053781880 (ELSEVIER)S1387-1811(21)00168-2 DE-627 ger DE-627 rakwb eng 333.7 570 690 VZ BIODIV DE-30 fid 48.00 bkl Ramamurthy, Maya verfasserin aut Substitution of Cetyltrimethylammonium for OSDA Cations During B-SSZ-70 Zeotype Synthesis and Its Influence on Delamination 2021transfer abstract nicht spezifiziert zzz rdacontent nicht spezifiziert z rdamedia nicht spezifiziert zu rdacarrier We investigated the substitution of structure-directing agent diisobutylimidazolium hydroxide with cetyltrimethylammonium hydroxide (CTA+OH−) surfactant in the synthesis gel of layered-zeotype-precursor B-SSZ-70(P). At low substitution levels, CTA+ interacts with the external-zeotype surface, where it assembles. At higher surfactant amounts, CTA+ intercalation occurs, leading to swelling of the precursor material, as evidenced by powder X-ray diffraction. Characterization of adsorbed CTA+ cations by 13C MAS NMR spectroscopy demonstrates unique broad resonances in the intercalated layers, which represent a more rigid environment than in the external-surface assemblies. At still higher CTA+ substitution levels in the synthesis gel, we observe the formation of amorphous mesoporous silica. We attempted to delaminate materials synthesized with varying CTA+ substitution levels using mild conditions, in which the conventional sonication step is replaced with an easy-to-scale high-shear mixing, and in which the use of halide reagents, which are corrosive and have been required in the past, is also avoided. Our data demonstrate that synthesis of a swollen material per se is not essential as an intermediate for delamination, and that layered zeolite precursor swelling can actually undermine zeolite delamination. Our results instead point to the CTA+ external-surface assemblies as facilitating ease of SSZ-70 delamination under these mild conditions. When calcined and functionalized with grafted titanium centers, the delaminated materials are highly active and selective olefin epoxidation catalysts with organic hydroperoxides, showing a 40% higher epoxide conversion than a catalyst prepared from conventional B-SSZ-70. We investigated the substitution of structure-directing agent diisobutylimidazolium hydroxide with cetyltrimethylammonium hydroxide (CTA+OH−) surfactant in the synthesis gel of layered-zeotype-precursor B-SSZ-70(P). At low substitution levels, CTA+ interacts with the external-zeotype surface, where it assembles. At higher surfactant amounts, CTA+ intercalation occurs, leading to swelling of the precursor material, as evidenced by powder X-ray diffraction. Characterization of adsorbed CTA+ cations by 13C MAS NMR spectroscopy demonstrates unique broad resonances in the intercalated layers, which represent a more rigid environment than in the external-surface assemblies. At still higher CTA+ substitution levels in the synthesis gel, we observe the formation of amorphous mesoporous silica. We attempted to delaminate materials synthesized with varying CTA+ substitution levels using mild conditions, in which the conventional sonication step is replaced with an easy-to-scale high-shear mixing, and in which the use of halide reagents, which are corrosive and have been required in the past, is also avoided. Our data demonstrate that synthesis of a swollen material per se is not essential as an intermediate for delamination, and that layered zeolite precursor swelling can actually undermine zeolite delamination. Our results instead point to the CTA+ external-surface assemblies as facilitating ease of SSZ-70 delamination under these mild conditions. When calcined and functionalized with grafted titanium centers, the delaminated materials are highly active and selective olefin epoxidation catalysts with organic hydroperoxides, showing a 40% higher epoxide conversion than a catalyst prepared from conventional B-SSZ-70. Zeolite delamination Elsevier Co-structure directing agent Elsevier Epoxidation catalysis Elsevier Grosso-Giordano, Nicolás A. oth Hwang, Son-Jong oth Xu, Le oth Xie, Dan oth Mishra, Manish oth Okrut, Alexander oth Zones, Stacey oth Katz, Alexander oth Enthalten in Elsevier Kim, Jeong-Hun ELSEVIER Impact of North Atlantic-East Asian teleconnections on extremely high January PM 2021 the official journal of the International Zeolite Association Amsterdam [u.a.] (DE-627)ELV006778283 volume:319 year:2021 pages:0 https://doi.org/10.1016/j.micromeso.2021.111042 Volltext GBV_USEFLAG_U GBV_ELV SYSFLAG_U FID-BIODIV SSG-OLC-PHA SSG-OPC-FOR 48.00 Land- und Forstwirtschaft: Allgemeines VZ AR 319 2021 0 |
| allfieldsSound |
10.1016/j.micromeso.2021.111042 doi /cbs_pica/cbs_olc/import_discovery/elsevier/einzuspielen/GBV00000000001650.pica (DE-627)ELV053781880 (ELSEVIER)S1387-1811(21)00168-2 DE-627 ger DE-627 rakwb eng 333.7 570 690 VZ BIODIV DE-30 fid 48.00 bkl Ramamurthy, Maya verfasserin aut Substitution of Cetyltrimethylammonium for OSDA Cations During B-SSZ-70 Zeotype Synthesis and Its Influence on Delamination 2021transfer abstract nicht spezifiziert zzz rdacontent nicht spezifiziert z rdamedia nicht spezifiziert zu rdacarrier We investigated the substitution of structure-directing agent diisobutylimidazolium hydroxide with cetyltrimethylammonium hydroxide (CTA+OH−) surfactant in the synthesis gel of layered-zeotype-precursor B-SSZ-70(P). At low substitution levels, CTA+ interacts with the external-zeotype surface, where it assembles. At higher surfactant amounts, CTA+ intercalation occurs, leading to swelling of the precursor material, as evidenced by powder X-ray diffraction. Characterization of adsorbed CTA+ cations by 13C MAS NMR spectroscopy demonstrates unique broad resonances in the intercalated layers, which represent a more rigid environment than in the external-surface assemblies. At still higher CTA+ substitution levels in the synthesis gel, we observe the formation of amorphous mesoporous silica. We attempted to delaminate materials synthesized with varying CTA+ substitution levels using mild conditions, in which the conventional sonication step is replaced with an easy-to-scale high-shear mixing, and in which the use of halide reagents, which are corrosive and have been required in the past, is also avoided. Our data demonstrate that synthesis of a swollen material per se is not essential as an intermediate for delamination, and that layered zeolite precursor swelling can actually undermine zeolite delamination. Our results instead point to the CTA+ external-surface assemblies as facilitating ease of SSZ-70 delamination under these mild conditions. When calcined and functionalized with grafted titanium centers, the delaminated materials are highly active and selective olefin epoxidation catalysts with organic hydroperoxides, showing a 40% higher epoxide conversion than a catalyst prepared from conventional B-SSZ-70. We investigated the substitution of structure-directing agent diisobutylimidazolium hydroxide with cetyltrimethylammonium hydroxide (CTA+OH−) surfactant in the synthesis gel of layered-zeotype-precursor B-SSZ-70(P). At low substitution levels, CTA+ interacts with the external-zeotype surface, where it assembles. At higher surfactant amounts, CTA+ intercalation occurs, leading to swelling of the precursor material, as evidenced by powder X-ray diffraction. Characterization of adsorbed CTA+ cations by 13C MAS NMR spectroscopy demonstrates unique broad resonances in the intercalated layers, which represent a more rigid environment than in the external-surface assemblies. At still higher CTA+ substitution levels in the synthesis gel, we observe the formation of amorphous mesoporous silica. We attempted to delaminate materials synthesized with varying CTA+ substitution levels using mild conditions, in which the conventional sonication step is replaced with an easy-to-scale high-shear mixing, and in which the use of halide reagents, which are corrosive and have been required in the past, is also avoided. Our data demonstrate that synthesis of a swollen material per se is not essential as an intermediate for delamination, and that layered zeolite precursor swelling can actually undermine zeolite delamination. Our results instead point to the CTA+ external-surface assemblies as facilitating ease of SSZ-70 delamination under these mild conditions. When calcined and functionalized with grafted titanium centers, the delaminated materials are highly active and selective olefin epoxidation catalysts with organic hydroperoxides, showing a 40% higher epoxide conversion than a catalyst prepared from conventional B-SSZ-70. Zeolite delamination Elsevier Co-structure directing agent Elsevier Epoxidation catalysis Elsevier Grosso-Giordano, Nicolás A. oth Hwang, Son-Jong oth Xu, Le oth Xie, Dan oth Mishra, Manish oth Okrut, Alexander oth Zones, Stacey oth Katz, Alexander oth Enthalten in Elsevier Kim, Jeong-Hun ELSEVIER Impact of North Atlantic-East Asian teleconnections on extremely high January PM 2021 the official journal of the International Zeolite Association Amsterdam [u.a.] (DE-627)ELV006778283 volume:319 year:2021 pages:0 https://doi.org/10.1016/j.micromeso.2021.111042 Volltext GBV_USEFLAG_U GBV_ELV SYSFLAG_U FID-BIODIV SSG-OLC-PHA SSG-OPC-FOR 48.00 Land- und Forstwirtschaft: Allgemeines VZ AR 319 2021 0 |
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Enthalten in Impact of North Atlantic-East Asian teleconnections on extremely high January PM Amsterdam [u.a.] volume:319 year:2021 pages:0 |
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Enthalten in Impact of North Atlantic-East Asian teleconnections on extremely high January PM Amsterdam [u.a.] volume:319 year:2021 pages:0 |
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Substitution of Cetyltrimethylammonium for OSDA Cations During B-SSZ-70 Zeotype Synthesis and Its Influence on Delamination |
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We investigated the substitution of structure-directing agent diisobutylimidazolium hydroxide with cetyltrimethylammonium hydroxide (CTA+OH−) surfactant in the synthesis gel of layered-zeotype-precursor B-SSZ-70(P). At low substitution levels, CTA+ interacts with the external-zeotype surface, where it assembles. At higher surfactant amounts, CTA+ intercalation occurs, leading to swelling of the precursor material, as evidenced by powder X-ray diffraction. Characterization of adsorbed CTA+ cations by 13C MAS NMR spectroscopy demonstrates unique broad resonances in the intercalated layers, which represent a more rigid environment than in the external-surface assemblies. At still higher CTA+ substitution levels in the synthesis gel, we observe the formation of amorphous mesoporous silica. We attempted to delaminate materials synthesized with varying CTA+ substitution levels using mild conditions, in which the conventional sonication step is replaced with an easy-to-scale high-shear mixing, and in which the use of halide reagents, which are corrosive and have been required in the past, is also avoided. Our data demonstrate that synthesis of a swollen material per se is not essential as an intermediate for delamination, and that layered zeolite precursor swelling can actually undermine zeolite delamination. Our results instead point to the CTA+ external-surface assemblies as facilitating ease of SSZ-70 delamination under these mild conditions. When calcined and functionalized with grafted titanium centers, the delaminated materials are highly active and selective olefin epoxidation catalysts with organic hydroperoxides, showing a 40% higher epoxide conversion than a catalyst prepared from conventional B-SSZ-70. |
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We investigated the substitution of structure-directing agent diisobutylimidazolium hydroxide with cetyltrimethylammonium hydroxide (CTA+OH−) surfactant in the synthesis gel of layered-zeotype-precursor B-SSZ-70(P). At low substitution levels, CTA+ interacts with the external-zeotype surface, where it assembles. At higher surfactant amounts, CTA+ intercalation occurs, leading to swelling of the precursor material, as evidenced by powder X-ray diffraction. Characterization of adsorbed CTA+ cations by 13C MAS NMR spectroscopy demonstrates unique broad resonances in the intercalated layers, which represent a more rigid environment than in the external-surface assemblies. At still higher CTA+ substitution levels in the synthesis gel, we observe the formation of amorphous mesoporous silica. We attempted to delaminate materials synthesized with varying CTA+ substitution levels using mild conditions, in which the conventional sonication step is replaced with an easy-to-scale high-shear mixing, and in which the use of halide reagents, which are corrosive and have been required in the past, is also avoided. Our data demonstrate that synthesis of a swollen material per se is not essential as an intermediate for delamination, and that layered zeolite precursor swelling can actually undermine zeolite delamination. Our results instead point to the CTA+ external-surface assemblies as facilitating ease of SSZ-70 delamination under these mild conditions. When calcined and functionalized with grafted titanium centers, the delaminated materials are highly active and selective olefin epoxidation catalysts with organic hydroperoxides, showing a 40% higher epoxide conversion than a catalyst prepared from conventional B-SSZ-70. |
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We investigated the substitution of structure-directing agent diisobutylimidazolium hydroxide with cetyltrimethylammonium hydroxide (CTA+OH−) surfactant in the synthesis gel of layered-zeotype-precursor B-SSZ-70(P). At low substitution levels, CTA+ interacts with the external-zeotype surface, where it assembles. At higher surfactant amounts, CTA+ intercalation occurs, leading to swelling of the precursor material, as evidenced by powder X-ray diffraction. Characterization of adsorbed CTA+ cations by 13C MAS NMR spectroscopy demonstrates unique broad resonances in the intercalated layers, which represent a more rigid environment than in the external-surface assemblies. At still higher CTA+ substitution levels in the synthesis gel, we observe the formation of amorphous mesoporous silica. We attempted to delaminate materials synthesized with varying CTA+ substitution levels using mild conditions, in which the conventional sonication step is replaced with an easy-to-scale high-shear mixing, and in which the use of halide reagents, which are corrosive and have been required in the past, is also avoided. Our data demonstrate that synthesis of a swollen material per se is not essential as an intermediate for delamination, and that layered zeolite precursor swelling can actually undermine zeolite delamination. Our results instead point to the CTA+ external-surface assemblies as facilitating ease of SSZ-70 delamination under these mild conditions. When calcined and functionalized with grafted titanium centers, the delaminated materials are highly active and selective olefin epoxidation catalysts with organic hydroperoxides, showing a 40% higher epoxide conversion than a catalyst prepared from conventional B-SSZ-70. |
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At low substitution levels, CTA+ interacts with the external-zeotype surface, where it assembles. At higher surfactant amounts, CTA+ intercalation occurs, leading to swelling of the precursor material, as evidenced by powder X-ray diffraction. Characterization of adsorbed CTA+ cations by 13C MAS NMR spectroscopy demonstrates unique broad resonances in the intercalated layers, which represent a more rigid environment than in the external-surface assemblies. At still higher CTA+ substitution levels in the synthesis gel, we observe the formation of amorphous mesoporous silica. We attempted to delaminate materials synthesized with varying CTA+ substitution levels using mild conditions, in which the conventional sonication step is replaced with an easy-to-scale high-shear mixing, and in which the use of halide reagents, which are corrosive and have been required in the past, is also avoided. Our data demonstrate that synthesis of a swollen material per se is not essential as an intermediate for delamination, and that layered zeolite precursor swelling can actually undermine zeolite delamination. Our results instead point to the CTA+ external-surface assemblies as facilitating ease of SSZ-70 delamination under these mild conditions. When calcined and functionalized with grafted titanium centers, the delaminated materials are highly active and selective olefin epoxidation catalysts with organic hydroperoxides, showing a 40% higher epoxide conversion than a catalyst prepared from conventional B-SSZ-70.</subfield></datafield><datafield tag="650" ind1=" " ind2="7"><subfield code="a">Zeolite delamination</subfield><subfield code="2">Elsevier</subfield></datafield><datafield tag="650" ind1=" " ind2="7"><subfield code="a">Co-structure directing agent</subfield><subfield code="2">Elsevier</subfield></datafield><datafield tag="650" ind1=" " ind2="7"><subfield code="a">Epoxidation catalysis</subfield><subfield code="2">Elsevier</subfield></datafield><datafield tag="700" ind1="1" ind2=" "><subfield code="a">Grosso-Giordano, Nicolás A.</subfield><subfield code="4">oth</subfield></datafield><datafield tag="700" ind1="1" ind2=" "><subfield code="a">Hwang, Son-Jong</subfield><subfield code="4">oth</subfield></datafield><datafield tag="700" ind1="1" ind2=" "><subfield code="a">Xu, Le</subfield><subfield code="4">oth</subfield></datafield><datafield tag="700" ind1="1" ind2=" "><subfield code="a">Xie, Dan</subfield><subfield code="4">oth</subfield></datafield><datafield tag="700" ind1="1" ind2=" "><subfield code="a">Mishra, Manish</subfield><subfield code="4">oth</subfield></datafield><datafield tag="700" ind1="1" ind2=" "><subfield code="a">Okrut, Alexander</subfield><subfield code="4">oth</subfield></datafield><datafield tag="700" ind1="1" ind2=" "><subfield code="a">Zones, Stacey</subfield><subfield code="4">oth</subfield></datafield><datafield tag="700" ind1="1" ind2=" "><subfield code="a">Katz, Alexander</subfield><subfield code="4">oth</subfield></datafield><datafield tag="773" ind1="0" ind2="8"><subfield code="i">Enthalten in</subfield><subfield code="n">Elsevier</subfield><subfield code="a">Kim, Jeong-Hun ELSEVIER</subfield><subfield code="t">Impact of North Atlantic-East Asian teleconnections on extremely high January PM</subfield><subfield code="d">2021</subfield><subfield code="d">the official journal of the International Zeolite Association</subfield><subfield code="g">Amsterdam [u.a.]</subfield><subfield code="w">(DE-627)ELV006778283</subfield></datafield><datafield tag="773" ind1="1" ind2="8"><subfield code="g">volume:319</subfield><subfield code="g">year:2021</subfield><subfield code="g">pages:0</subfield></datafield><datafield tag="856" ind1="4" ind2="0"><subfield code="u">https://doi.org/10.1016/j.micromeso.2021.111042</subfield><subfield code="3">Volltext</subfield></datafield><datafield tag="912" ind1=" " ind2=" "><subfield code="a">GBV_USEFLAG_U</subfield></datafield><datafield tag="912" ind1=" " ind2=" "><subfield code="a">GBV_ELV</subfield></datafield><datafield tag="912" ind1=" " ind2=" "><subfield code="a">SYSFLAG_U</subfield></datafield><datafield tag="912" ind1=" " ind2=" "><subfield code="a">FID-BIODIV</subfield></datafield><datafield tag="912" ind1=" " ind2=" "><subfield code="a">SSG-OLC-PHA</subfield></datafield><datafield tag="912" ind1=" " ind2=" "><subfield code="a">SSG-OPC-FOR</subfield></datafield><datafield tag="936" ind1="b" ind2="k"><subfield code="a">48.00</subfield><subfield code="j">Land- und Forstwirtschaft: Allgemeines</subfield><subfield code="q">VZ</subfield></datafield><datafield tag="951" ind1=" " ind2=" "><subfield code="a">AR</subfield></datafield><datafield tag="952" ind1=" " ind2=" "><subfield code="d">319</subfield><subfield code="j">2021</subfield><subfield code="h">0</subfield></datafield></record></collection>
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