Ultraviolet light-induced decomposition of benzothiophene and dibenzothiophene derivatives for efficient sulfur removal without additives and catalysts
When producing liquid fuels from petroleum, hydrodesulfurization methods reduce the concentration of sulfur to ≤10 mg(S)/L (weight/volume concentration of sulfur), namely, ≤ 0.31 mmol/L. Dibenzothiophene derivatives (DBTs), which are known as particularly difficult desulfurizing substances, have bee...
Ausführliche Beschreibung
Gespeichert in:
| Autor*in: |
Shinozaki, Taka-Aki [verfasserIn] |
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| Format: |
E-Artikel |
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| Sprache: |
Englisch |
| Erschienen: |
2022transfer abstract |
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| Schlagwörter: |
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| Übergeordnetes Werk: |
Enthalten in: Self-assembled 3D hierarchical MnCO - Rajendiran, Rajmohan ELSEVIER, 2020, Amsterdam [u.a.] |
|---|---|
| Übergeordnetes Werk: |
volume:370 ; year:2022 ; day:10 ; month:10 ; pages:0 |
| Links: |
|---|
| DOI / URN: |
10.1016/j.jclepro.2022.133402 |
|---|
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ELV058949941 |
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| 245 | 1 | 0 | |a Ultraviolet light-induced decomposition of benzothiophene and dibenzothiophene derivatives for efficient sulfur removal without additives and catalysts |
| 264 | 1 | |c 2022transfer abstract | |
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| 520 | |a When producing liquid fuels from petroleum, hydrodesulfurization methods reduce the concentration of sulfur to ≤10 mg(S)/L (weight/volume concentration of sulfur), namely, ≤ 0.31 mmol/L. Dibenzothiophene derivatives (DBTs), which are known as particularly difficult desulfurizing substances, have been decomposed reductively in severe conditions of high temperatures (270–372 °C) and high pressure (50–102 atm of H2). In this study, we developed a UV light irradiation-based desulfurization method for aromatic sulfur compounds such as benzothiophene derivatives (BTs) and DBTs under room temperature and atmospheric pressure without the use of catalysts or additives. This method is simple, location-independent, and low-cost, and has low environmental impact. BTs and DBTs completely decomposed in approximately 8 h and 16 h, respectively, under ultraviolet (UV) light irradiation (λ = 254 nm) from a 8 W lamp. The yellow precipitates that were produced upon decomposition were confirmed to be sulfur allotropes (S n ). The residual hydrocarbon portion of DBT after sulfur removal was determined to be benzene. The decomposition reaction was determined to exhibit pseudo-first-order reaction. DFT calculations confirmed the degradation mechanism as follows: UV light irradiation induces a photochemically excited triplet state of DBTs. The excited DBTs reacts with O2 to form a π-complex, which isomerizes to a more stable σ-complex. The DBTs-O2 (σ-complex) then reacts with free DBTs to afford two molecules of dibenzothiophene-5-oxide derivatives (DBTOs), which are excited to singlet states on photoirradiation. The excited DBTOs isomerize through a minimum energy intersection eventually to dibenzofuran episulfides from which sulfur extrusion occurs. | ||
| 520 | |a When producing liquid fuels from petroleum, hydrodesulfurization methods reduce the concentration of sulfur to ≤10 mg(S)/L (weight/volume concentration of sulfur), namely, ≤ 0.31 mmol/L. Dibenzothiophene derivatives (DBTs), which are known as particularly difficult desulfurizing substances, have been decomposed reductively in severe conditions of high temperatures (270–372 °C) and high pressure (50–102 atm of H2). In this study, we developed a UV light irradiation-based desulfurization method for aromatic sulfur compounds such as benzothiophene derivatives (BTs) and DBTs under room temperature and atmospheric pressure without the use of catalysts or additives. This method is simple, location-independent, and low-cost, and has low environmental impact. BTs and DBTs completely decomposed in approximately 8 h and 16 h, respectively, under ultraviolet (UV) light irradiation (λ = 254 nm) from a 8 W lamp. The yellow precipitates that were produced upon decomposition were confirmed to be sulfur allotropes (S n ). The residual hydrocarbon portion of DBT after sulfur removal was determined to be benzene. The decomposition reaction was determined to exhibit pseudo-first-order reaction. DFT calculations confirmed the degradation mechanism as follows: UV light irradiation induces a photochemically excited triplet state of DBTs. The excited DBTs reacts with O2 to form a π-complex, which isomerizes to a more stable σ-complex. The DBTs-O2 (σ-complex) then reacts with free DBTs to afford two molecules of dibenzothiophene-5-oxide derivatives (DBTOs), which are excited to singlet states on photoirradiation. The excited DBTOs isomerize through a minimum energy intersection eventually to dibenzofuran episulfides from which sulfur extrusion occurs. | ||
| 650 | 7 | |a DFT calculation |2 Elsevier | |
| 650 | 7 | |a Additive-free |2 Elsevier | |
| 650 | 7 | |a Catalyst-free |2 Elsevier | |
| 650 | 7 | |a Deep-desulfurization |2 Elsevier | |
| 650 | 7 | |a Organic sulfur |2 Elsevier | |
| 650 | 7 | |a UV irradiation |2 Elsevier | |
| 700 | 1 | |a Suenaga, Masahiko |4 oth | |
| 700 | 1 | |a Ko, Yohan |4 oth | |
| 700 | 1 | |a Yamamoto, Eiji |4 oth | |
| 700 | 1 | |a Murayama, Haruno |4 oth | |
| 700 | 1 | |a Tokunaga, Makoto |4 oth | |
| 773 | 0 | 8 | |i Enthalten in |n Elsevier Science |a Rajendiran, Rajmohan ELSEVIER |t Self-assembled 3D hierarchical MnCO |d 2020 |g Amsterdam [u.a.] |w (DE-627)ELV003750353 |
| 773 | 1 | 8 | |g volume:370 |g year:2022 |g day:10 |g month:10 |g pages:0 |
| 856 | 4 | 0 | |u https://doi.org/10.1016/j.jclepro.2022.133402 |3 Volltext |
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10.1016/j.jclepro.2022.133402 doi /cbs_pica/cbs_olc/import_discovery/elsevier/einzuspielen/GBV00000000001996.pica (DE-627)ELV058949941 (ELSEVIER)S0959-6526(22)02985-7 DE-627 ger DE-627 rakwb eng 540 VZ 35.18 bkl Shinozaki, Taka-Aki verfasserin aut Ultraviolet light-induced decomposition of benzothiophene and dibenzothiophene derivatives for efficient sulfur removal without additives and catalysts 2022transfer abstract nicht spezifiziert zzz rdacontent nicht spezifiziert z rdamedia nicht spezifiziert zu rdacarrier When producing liquid fuels from petroleum, hydrodesulfurization methods reduce the concentration of sulfur to ≤10 mg(S)/L (weight/volume concentration of sulfur), namely, ≤ 0.31 mmol/L. Dibenzothiophene derivatives (DBTs), which are known as particularly difficult desulfurizing substances, have been decomposed reductively in severe conditions of high temperatures (270–372 °C) and high pressure (50–102 atm of H2). In this study, we developed a UV light irradiation-based desulfurization method for aromatic sulfur compounds such as benzothiophene derivatives (BTs) and DBTs under room temperature and atmospheric pressure without the use of catalysts or additives. This method is simple, location-independent, and low-cost, and has low environmental impact. BTs and DBTs completely decomposed in approximately 8 h and 16 h, respectively, under ultraviolet (UV) light irradiation (λ = 254 nm) from a 8 W lamp. The yellow precipitates that were produced upon decomposition were confirmed to be sulfur allotropes (S n ). The residual hydrocarbon portion of DBT after sulfur removal was determined to be benzene. The decomposition reaction was determined to exhibit pseudo-first-order reaction. DFT calculations confirmed the degradation mechanism as follows: UV light irradiation induces a photochemically excited triplet state of DBTs. The excited DBTs reacts with O2 to form a π-complex, which isomerizes to a more stable σ-complex. The DBTs-O2 (σ-complex) then reacts with free DBTs to afford two molecules of dibenzothiophene-5-oxide derivatives (DBTOs), which are excited to singlet states on photoirradiation. The excited DBTOs isomerize through a minimum energy intersection eventually to dibenzofuran episulfides from which sulfur extrusion occurs. When producing liquid fuels from petroleum, hydrodesulfurization methods reduce the concentration of sulfur to ≤10 mg(S)/L (weight/volume concentration of sulfur), namely, ≤ 0.31 mmol/L. Dibenzothiophene derivatives (DBTs), which are known as particularly difficult desulfurizing substances, have been decomposed reductively in severe conditions of high temperatures (270–372 °C) and high pressure (50–102 atm of H2). In this study, we developed a UV light irradiation-based desulfurization method for aromatic sulfur compounds such as benzothiophene derivatives (BTs) and DBTs under room temperature and atmospheric pressure without the use of catalysts or additives. This method is simple, location-independent, and low-cost, and has low environmental impact. BTs and DBTs completely decomposed in approximately 8 h and 16 h, respectively, under ultraviolet (UV) light irradiation (λ = 254 nm) from a 8 W lamp. The yellow precipitates that were produced upon decomposition were confirmed to be sulfur allotropes (S n ). The residual hydrocarbon portion of DBT after sulfur removal was determined to be benzene. The decomposition reaction was determined to exhibit pseudo-first-order reaction. DFT calculations confirmed the degradation mechanism as follows: UV light irradiation induces a photochemically excited triplet state of DBTs. The excited DBTs reacts with O2 to form a π-complex, which isomerizes to a more stable σ-complex. The DBTs-O2 (σ-complex) then reacts with free DBTs to afford two molecules of dibenzothiophene-5-oxide derivatives (DBTOs), which are excited to singlet states on photoirradiation. The excited DBTOs isomerize through a minimum energy intersection eventually to dibenzofuran episulfides from which sulfur extrusion occurs. DFT calculation Elsevier Additive-free Elsevier Catalyst-free Elsevier Deep-desulfurization Elsevier Organic sulfur Elsevier UV irradiation Elsevier Suenaga, Masahiko oth Ko, Yohan oth Yamamoto, Eiji oth Murayama, Haruno oth Tokunaga, Makoto oth Enthalten in Elsevier Science Rajendiran, Rajmohan ELSEVIER Self-assembled 3D hierarchical MnCO 2020 Amsterdam [u.a.] (DE-627)ELV003750353 volume:370 year:2022 day:10 month:10 pages:0 https://doi.org/10.1016/j.jclepro.2022.133402 Volltext GBV_USEFLAG_U GBV_ELV SYSFLAG_U 35.18 Kolloidchemie Grenzflächenchemie VZ AR 370 2022 10 1010 0 |
| spelling |
10.1016/j.jclepro.2022.133402 doi /cbs_pica/cbs_olc/import_discovery/elsevier/einzuspielen/GBV00000000001996.pica (DE-627)ELV058949941 (ELSEVIER)S0959-6526(22)02985-7 DE-627 ger DE-627 rakwb eng 540 VZ 35.18 bkl Shinozaki, Taka-Aki verfasserin aut Ultraviolet light-induced decomposition of benzothiophene and dibenzothiophene derivatives for efficient sulfur removal without additives and catalysts 2022transfer abstract nicht spezifiziert zzz rdacontent nicht spezifiziert z rdamedia nicht spezifiziert zu rdacarrier When producing liquid fuels from petroleum, hydrodesulfurization methods reduce the concentration of sulfur to ≤10 mg(S)/L (weight/volume concentration of sulfur), namely, ≤ 0.31 mmol/L. Dibenzothiophene derivatives (DBTs), which are known as particularly difficult desulfurizing substances, have been decomposed reductively in severe conditions of high temperatures (270–372 °C) and high pressure (50–102 atm of H2). In this study, we developed a UV light irradiation-based desulfurization method for aromatic sulfur compounds such as benzothiophene derivatives (BTs) and DBTs under room temperature and atmospheric pressure without the use of catalysts or additives. This method is simple, location-independent, and low-cost, and has low environmental impact. BTs and DBTs completely decomposed in approximately 8 h and 16 h, respectively, under ultraviolet (UV) light irradiation (λ = 254 nm) from a 8 W lamp. The yellow precipitates that were produced upon decomposition were confirmed to be sulfur allotropes (S n ). The residual hydrocarbon portion of DBT after sulfur removal was determined to be benzene. The decomposition reaction was determined to exhibit pseudo-first-order reaction. DFT calculations confirmed the degradation mechanism as follows: UV light irradiation induces a photochemically excited triplet state of DBTs. The excited DBTs reacts with O2 to form a π-complex, which isomerizes to a more stable σ-complex. The DBTs-O2 (σ-complex) then reacts with free DBTs to afford two molecules of dibenzothiophene-5-oxide derivatives (DBTOs), which are excited to singlet states on photoirradiation. The excited DBTOs isomerize through a minimum energy intersection eventually to dibenzofuran episulfides from which sulfur extrusion occurs. When producing liquid fuels from petroleum, hydrodesulfurization methods reduce the concentration of sulfur to ≤10 mg(S)/L (weight/volume concentration of sulfur), namely, ≤ 0.31 mmol/L. Dibenzothiophene derivatives (DBTs), which are known as particularly difficult desulfurizing substances, have been decomposed reductively in severe conditions of high temperatures (270–372 °C) and high pressure (50–102 atm of H2). In this study, we developed a UV light irradiation-based desulfurization method for aromatic sulfur compounds such as benzothiophene derivatives (BTs) and DBTs under room temperature and atmospheric pressure without the use of catalysts or additives. This method is simple, location-independent, and low-cost, and has low environmental impact. BTs and DBTs completely decomposed in approximately 8 h and 16 h, respectively, under ultraviolet (UV) light irradiation (λ = 254 nm) from a 8 W lamp. The yellow precipitates that were produced upon decomposition were confirmed to be sulfur allotropes (S n ). The residual hydrocarbon portion of DBT after sulfur removal was determined to be benzene. The decomposition reaction was determined to exhibit pseudo-first-order reaction. DFT calculations confirmed the degradation mechanism as follows: UV light irradiation induces a photochemically excited triplet state of DBTs. The excited DBTs reacts with O2 to form a π-complex, which isomerizes to a more stable σ-complex. The DBTs-O2 (σ-complex) then reacts with free DBTs to afford two molecules of dibenzothiophene-5-oxide derivatives (DBTOs), which are excited to singlet states on photoirradiation. The excited DBTOs isomerize through a minimum energy intersection eventually to dibenzofuran episulfides from which sulfur extrusion occurs. DFT calculation Elsevier Additive-free Elsevier Catalyst-free Elsevier Deep-desulfurization Elsevier Organic sulfur Elsevier UV irradiation Elsevier Suenaga, Masahiko oth Ko, Yohan oth Yamamoto, Eiji oth Murayama, Haruno oth Tokunaga, Makoto oth Enthalten in Elsevier Science Rajendiran, Rajmohan ELSEVIER Self-assembled 3D hierarchical MnCO 2020 Amsterdam [u.a.] (DE-627)ELV003750353 volume:370 year:2022 day:10 month:10 pages:0 https://doi.org/10.1016/j.jclepro.2022.133402 Volltext GBV_USEFLAG_U GBV_ELV SYSFLAG_U 35.18 Kolloidchemie Grenzflächenchemie VZ AR 370 2022 10 1010 0 |
| allfields_unstemmed |
10.1016/j.jclepro.2022.133402 doi /cbs_pica/cbs_olc/import_discovery/elsevier/einzuspielen/GBV00000000001996.pica (DE-627)ELV058949941 (ELSEVIER)S0959-6526(22)02985-7 DE-627 ger DE-627 rakwb eng 540 VZ 35.18 bkl Shinozaki, Taka-Aki verfasserin aut Ultraviolet light-induced decomposition of benzothiophene and dibenzothiophene derivatives for efficient sulfur removal without additives and catalysts 2022transfer abstract nicht spezifiziert zzz rdacontent nicht spezifiziert z rdamedia nicht spezifiziert zu rdacarrier When producing liquid fuels from petroleum, hydrodesulfurization methods reduce the concentration of sulfur to ≤10 mg(S)/L (weight/volume concentration of sulfur), namely, ≤ 0.31 mmol/L. Dibenzothiophene derivatives (DBTs), which are known as particularly difficult desulfurizing substances, have been decomposed reductively in severe conditions of high temperatures (270–372 °C) and high pressure (50–102 atm of H2). In this study, we developed a UV light irradiation-based desulfurization method for aromatic sulfur compounds such as benzothiophene derivatives (BTs) and DBTs under room temperature and atmospheric pressure without the use of catalysts or additives. This method is simple, location-independent, and low-cost, and has low environmental impact. BTs and DBTs completely decomposed in approximately 8 h and 16 h, respectively, under ultraviolet (UV) light irradiation (λ = 254 nm) from a 8 W lamp. The yellow precipitates that were produced upon decomposition were confirmed to be sulfur allotropes (S n ). The residual hydrocarbon portion of DBT after sulfur removal was determined to be benzene. The decomposition reaction was determined to exhibit pseudo-first-order reaction. DFT calculations confirmed the degradation mechanism as follows: UV light irradiation induces a photochemically excited triplet state of DBTs. The excited DBTs reacts with O2 to form a π-complex, which isomerizes to a more stable σ-complex. The DBTs-O2 (σ-complex) then reacts with free DBTs to afford two molecules of dibenzothiophene-5-oxide derivatives (DBTOs), which are excited to singlet states on photoirradiation. The excited DBTOs isomerize through a minimum energy intersection eventually to dibenzofuran episulfides from which sulfur extrusion occurs. When producing liquid fuels from petroleum, hydrodesulfurization methods reduce the concentration of sulfur to ≤10 mg(S)/L (weight/volume concentration of sulfur), namely, ≤ 0.31 mmol/L. Dibenzothiophene derivatives (DBTs), which are known as particularly difficult desulfurizing substances, have been decomposed reductively in severe conditions of high temperatures (270–372 °C) and high pressure (50–102 atm of H2). In this study, we developed a UV light irradiation-based desulfurization method for aromatic sulfur compounds such as benzothiophene derivatives (BTs) and DBTs under room temperature and atmospheric pressure without the use of catalysts or additives. This method is simple, location-independent, and low-cost, and has low environmental impact. BTs and DBTs completely decomposed in approximately 8 h and 16 h, respectively, under ultraviolet (UV) light irradiation (λ = 254 nm) from a 8 W lamp. The yellow precipitates that were produced upon decomposition were confirmed to be sulfur allotropes (S n ). The residual hydrocarbon portion of DBT after sulfur removal was determined to be benzene. The decomposition reaction was determined to exhibit pseudo-first-order reaction. DFT calculations confirmed the degradation mechanism as follows: UV light irradiation induces a photochemically excited triplet state of DBTs. The excited DBTs reacts with O2 to form a π-complex, which isomerizes to a more stable σ-complex. The DBTs-O2 (σ-complex) then reacts with free DBTs to afford two molecules of dibenzothiophene-5-oxide derivatives (DBTOs), which are excited to singlet states on photoirradiation. The excited DBTOs isomerize through a minimum energy intersection eventually to dibenzofuran episulfides from which sulfur extrusion occurs. DFT calculation Elsevier Additive-free Elsevier Catalyst-free Elsevier Deep-desulfurization Elsevier Organic sulfur Elsevier UV irradiation Elsevier Suenaga, Masahiko oth Ko, Yohan oth Yamamoto, Eiji oth Murayama, Haruno oth Tokunaga, Makoto oth Enthalten in Elsevier Science Rajendiran, Rajmohan ELSEVIER Self-assembled 3D hierarchical MnCO 2020 Amsterdam [u.a.] (DE-627)ELV003750353 volume:370 year:2022 day:10 month:10 pages:0 https://doi.org/10.1016/j.jclepro.2022.133402 Volltext GBV_USEFLAG_U GBV_ELV SYSFLAG_U 35.18 Kolloidchemie Grenzflächenchemie VZ AR 370 2022 10 1010 0 |
| allfieldsGer |
10.1016/j.jclepro.2022.133402 doi /cbs_pica/cbs_olc/import_discovery/elsevier/einzuspielen/GBV00000000001996.pica (DE-627)ELV058949941 (ELSEVIER)S0959-6526(22)02985-7 DE-627 ger DE-627 rakwb eng 540 VZ 35.18 bkl Shinozaki, Taka-Aki verfasserin aut Ultraviolet light-induced decomposition of benzothiophene and dibenzothiophene derivatives for efficient sulfur removal without additives and catalysts 2022transfer abstract nicht spezifiziert zzz rdacontent nicht spezifiziert z rdamedia nicht spezifiziert zu rdacarrier When producing liquid fuels from petroleum, hydrodesulfurization methods reduce the concentration of sulfur to ≤10 mg(S)/L (weight/volume concentration of sulfur), namely, ≤ 0.31 mmol/L. Dibenzothiophene derivatives (DBTs), which are known as particularly difficult desulfurizing substances, have been decomposed reductively in severe conditions of high temperatures (270–372 °C) and high pressure (50–102 atm of H2). In this study, we developed a UV light irradiation-based desulfurization method for aromatic sulfur compounds such as benzothiophene derivatives (BTs) and DBTs under room temperature and atmospheric pressure without the use of catalysts or additives. This method is simple, location-independent, and low-cost, and has low environmental impact. BTs and DBTs completely decomposed in approximately 8 h and 16 h, respectively, under ultraviolet (UV) light irradiation (λ = 254 nm) from a 8 W lamp. The yellow precipitates that were produced upon decomposition were confirmed to be sulfur allotropes (S n ). The residual hydrocarbon portion of DBT after sulfur removal was determined to be benzene. The decomposition reaction was determined to exhibit pseudo-first-order reaction. DFT calculations confirmed the degradation mechanism as follows: UV light irradiation induces a photochemically excited triplet state of DBTs. The excited DBTs reacts with O2 to form a π-complex, which isomerizes to a more stable σ-complex. The DBTs-O2 (σ-complex) then reacts with free DBTs to afford two molecules of dibenzothiophene-5-oxide derivatives (DBTOs), which are excited to singlet states on photoirradiation. The excited DBTOs isomerize through a minimum energy intersection eventually to dibenzofuran episulfides from which sulfur extrusion occurs. When producing liquid fuels from petroleum, hydrodesulfurization methods reduce the concentration of sulfur to ≤10 mg(S)/L (weight/volume concentration of sulfur), namely, ≤ 0.31 mmol/L. Dibenzothiophene derivatives (DBTs), which are known as particularly difficult desulfurizing substances, have been decomposed reductively in severe conditions of high temperatures (270–372 °C) and high pressure (50–102 atm of H2). In this study, we developed a UV light irradiation-based desulfurization method for aromatic sulfur compounds such as benzothiophene derivatives (BTs) and DBTs under room temperature and atmospheric pressure without the use of catalysts or additives. This method is simple, location-independent, and low-cost, and has low environmental impact. BTs and DBTs completely decomposed in approximately 8 h and 16 h, respectively, under ultraviolet (UV) light irradiation (λ = 254 nm) from a 8 W lamp. The yellow precipitates that were produced upon decomposition were confirmed to be sulfur allotropes (S n ). The residual hydrocarbon portion of DBT after sulfur removal was determined to be benzene. The decomposition reaction was determined to exhibit pseudo-first-order reaction. DFT calculations confirmed the degradation mechanism as follows: UV light irradiation induces a photochemically excited triplet state of DBTs. The excited DBTs reacts with O2 to form a π-complex, which isomerizes to a more stable σ-complex. The DBTs-O2 (σ-complex) then reacts with free DBTs to afford two molecules of dibenzothiophene-5-oxide derivatives (DBTOs), which are excited to singlet states on photoirradiation. The excited DBTOs isomerize through a minimum energy intersection eventually to dibenzofuran episulfides from which sulfur extrusion occurs. DFT calculation Elsevier Additive-free Elsevier Catalyst-free Elsevier Deep-desulfurization Elsevier Organic sulfur Elsevier UV irradiation Elsevier Suenaga, Masahiko oth Ko, Yohan oth Yamamoto, Eiji oth Murayama, Haruno oth Tokunaga, Makoto oth Enthalten in Elsevier Science Rajendiran, Rajmohan ELSEVIER Self-assembled 3D hierarchical MnCO 2020 Amsterdam [u.a.] (DE-627)ELV003750353 volume:370 year:2022 day:10 month:10 pages:0 https://doi.org/10.1016/j.jclepro.2022.133402 Volltext GBV_USEFLAG_U GBV_ELV SYSFLAG_U 35.18 Kolloidchemie Grenzflächenchemie VZ AR 370 2022 10 1010 0 |
| allfieldsSound |
10.1016/j.jclepro.2022.133402 doi /cbs_pica/cbs_olc/import_discovery/elsevier/einzuspielen/GBV00000000001996.pica (DE-627)ELV058949941 (ELSEVIER)S0959-6526(22)02985-7 DE-627 ger DE-627 rakwb eng 540 VZ 35.18 bkl Shinozaki, Taka-Aki verfasserin aut Ultraviolet light-induced decomposition of benzothiophene and dibenzothiophene derivatives for efficient sulfur removal without additives and catalysts 2022transfer abstract nicht spezifiziert zzz rdacontent nicht spezifiziert z rdamedia nicht spezifiziert zu rdacarrier When producing liquid fuels from petroleum, hydrodesulfurization methods reduce the concentration of sulfur to ≤10 mg(S)/L (weight/volume concentration of sulfur), namely, ≤ 0.31 mmol/L. Dibenzothiophene derivatives (DBTs), which are known as particularly difficult desulfurizing substances, have been decomposed reductively in severe conditions of high temperatures (270–372 °C) and high pressure (50–102 atm of H2). In this study, we developed a UV light irradiation-based desulfurization method for aromatic sulfur compounds such as benzothiophene derivatives (BTs) and DBTs under room temperature and atmospheric pressure without the use of catalysts or additives. This method is simple, location-independent, and low-cost, and has low environmental impact. BTs and DBTs completely decomposed in approximately 8 h and 16 h, respectively, under ultraviolet (UV) light irradiation (λ = 254 nm) from a 8 W lamp. The yellow precipitates that were produced upon decomposition were confirmed to be sulfur allotropes (S n ). The residual hydrocarbon portion of DBT after sulfur removal was determined to be benzene. The decomposition reaction was determined to exhibit pseudo-first-order reaction. DFT calculations confirmed the degradation mechanism as follows: UV light irradiation induces a photochemically excited triplet state of DBTs. The excited DBTs reacts with O2 to form a π-complex, which isomerizes to a more stable σ-complex. The DBTs-O2 (σ-complex) then reacts with free DBTs to afford two molecules of dibenzothiophene-5-oxide derivatives (DBTOs), which are excited to singlet states on photoirradiation. The excited DBTOs isomerize through a minimum energy intersection eventually to dibenzofuran episulfides from which sulfur extrusion occurs. When producing liquid fuels from petroleum, hydrodesulfurization methods reduce the concentration of sulfur to ≤10 mg(S)/L (weight/volume concentration of sulfur), namely, ≤ 0.31 mmol/L. Dibenzothiophene derivatives (DBTs), which are known as particularly difficult desulfurizing substances, have been decomposed reductively in severe conditions of high temperatures (270–372 °C) and high pressure (50–102 atm of H2). In this study, we developed a UV light irradiation-based desulfurization method for aromatic sulfur compounds such as benzothiophene derivatives (BTs) and DBTs under room temperature and atmospheric pressure without the use of catalysts or additives. This method is simple, location-independent, and low-cost, and has low environmental impact. BTs and DBTs completely decomposed in approximately 8 h and 16 h, respectively, under ultraviolet (UV) light irradiation (λ = 254 nm) from a 8 W lamp. The yellow precipitates that were produced upon decomposition were confirmed to be sulfur allotropes (S n ). The residual hydrocarbon portion of DBT after sulfur removal was determined to be benzene. The decomposition reaction was determined to exhibit pseudo-first-order reaction. DFT calculations confirmed the degradation mechanism as follows: UV light irradiation induces a photochemically excited triplet state of DBTs. The excited DBTs reacts with O2 to form a π-complex, which isomerizes to a more stable σ-complex. The DBTs-O2 (σ-complex) then reacts with free DBTs to afford two molecules of dibenzothiophene-5-oxide derivatives (DBTOs), which are excited to singlet states on photoirradiation. The excited DBTOs isomerize through a minimum energy intersection eventually to dibenzofuran episulfides from which sulfur extrusion occurs. DFT calculation Elsevier Additive-free Elsevier Catalyst-free Elsevier Deep-desulfurization Elsevier Organic sulfur Elsevier UV irradiation Elsevier Suenaga, Masahiko oth Ko, Yohan oth Yamamoto, Eiji oth Murayama, Haruno oth Tokunaga, Makoto oth Enthalten in Elsevier Science Rajendiran, Rajmohan ELSEVIER Self-assembled 3D hierarchical MnCO 2020 Amsterdam [u.a.] (DE-627)ELV003750353 volume:370 year:2022 day:10 month:10 pages:0 https://doi.org/10.1016/j.jclepro.2022.133402 Volltext GBV_USEFLAG_U GBV_ELV SYSFLAG_U 35.18 Kolloidchemie Grenzflächenchemie VZ AR 370 2022 10 1010 0 |
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Enthalten in Self-assembled 3D hierarchical MnCO Amsterdam [u.a.] volume:370 year:2022 day:10 month:10 pages:0 |
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Ultraviolet light-induced decomposition of benzothiophene and dibenzothiophene derivatives for efficient sulfur removal without additives and catalysts |
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When producing liquid fuels from petroleum, hydrodesulfurization methods reduce the concentration of sulfur to ≤10 mg(S)/L (weight/volume concentration of sulfur), namely, ≤ 0.31 mmol/L. Dibenzothiophene derivatives (DBTs), which are known as particularly difficult desulfurizing substances, have been decomposed reductively in severe conditions of high temperatures (270–372 °C) and high pressure (50–102 atm of H2). In this study, we developed a UV light irradiation-based desulfurization method for aromatic sulfur compounds such as benzothiophene derivatives (BTs) and DBTs under room temperature and atmospheric pressure without the use of catalysts or additives. This method is simple, location-independent, and low-cost, and has low environmental impact. BTs and DBTs completely decomposed in approximately 8 h and 16 h, respectively, under ultraviolet (UV) light irradiation (λ = 254 nm) from a 8 W lamp. The yellow precipitates that were produced upon decomposition were confirmed to be sulfur allotropes (S n ). The residual hydrocarbon portion of DBT after sulfur removal was determined to be benzene. The decomposition reaction was determined to exhibit pseudo-first-order reaction. DFT calculations confirmed the degradation mechanism as follows: UV light irradiation induces a photochemically excited triplet state of DBTs. The excited DBTs reacts with O2 to form a π-complex, which isomerizes to a more stable σ-complex. The DBTs-O2 (σ-complex) then reacts with free DBTs to afford two molecules of dibenzothiophene-5-oxide derivatives (DBTOs), which are excited to singlet states on photoirradiation. The excited DBTOs isomerize through a minimum energy intersection eventually to dibenzofuran episulfides from which sulfur extrusion occurs. |
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When producing liquid fuels from petroleum, hydrodesulfurization methods reduce the concentration of sulfur to ≤10 mg(S)/L (weight/volume concentration of sulfur), namely, ≤ 0.31 mmol/L. Dibenzothiophene derivatives (DBTs), which are known as particularly difficult desulfurizing substances, have been decomposed reductively in severe conditions of high temperatures (270–372 °C) and high pressure (50–102 atm of H2). In this study, we developed a UV light irradiation-based desulfurization method for aromatic sulfur compounds such as benzothiophene derivatives (BTs) and DBTs under room temperature and atmospheric pressure without the use of catalysts or additives. This method is simple, location-independent, and low-cost, and has low environmental impact. BTs and DBTs completely decomposed in approximately 8 h and 16 h, respectively, under ultraviolet (UV) light irradiation (λ = 254 nm) from a 8 W lamp. The yellow precipitates that were produced upon decomposition were confirmed to be sulfur allotropes (S n ). The residual hydrocarbon portion of DBT after sulfur removal was determined to be benzene. The decomposition reaction was determined to exhibit pseudo-first-order reaction. DFT calculations confirmed the degradation mechanism as follows: UV light irradiation induces a photochemically excited triplet state of DBTs. The excited DBTs reacts with O2 to form a π-complex, which isomerizes to a more stable σ-complex. The DBTs-O2 (σ-complex) then reacts with free DBTs to afford two molecules of dibenzothiophene-5-oxide derivatives (DBTOs), which are excited to singlet states on photoirradiation. The excited DBTOs isomerize through a minimum energy intersection eventually to dibenzofuran episulfides from which sulfur extrusion occurs. |
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When producing liquid fuels from petroleum, hydrodesulfurization methods reduce the concentration of sulfur to ≤10 mg(S)/L (weight/volume concentration of sulfur), namely, ≤ 0.31 mmol/L. Dibenzothiophene derivatives (DBTs), which are known as particularly difficult desulfurizing substances, have been decomposed reductively in severe conditions of high temperatures (270–372 °C) and high pressure (50–102 atm of H2). In this study, we developed a UV light irradiation-based desulfurization method for aromatic sulfur compounds such as benzothiophene derivatives (BTs) and DBTs under room temperature and atmospheric pressure without the use of catalysts or additives. This method is simple, location-independent, and low-cost, and has low environmental impact. BTs and DBTs completely decomposed in approximately 8 h and 16 h, respectively, under ultraviolet (UV) light irradiation (λ = 254 nm) from a 8 W lamp. The yellow precipitates that were produced upon decomposition were confirmed to be sulfur allotropes (S n ). The residual hydrocarbon portion of DBT after sulfur removal was determined to be benzene. The decomposition reaction was determined to exhibit pseudo-first-order reaction. DFT calculations confirmed the degradation mechanism as follows: UV light irradiation induces a photochemically excited triplet state of DBTs. The excited DBTs reacts with O2 to form a π-complex, which isomerizes to a more stable σ-complex. The DBTs-O2 (σ-complex) then reacts with free DBTs to afford two molecules of dibenzothiophene-5-oxide derivatives (DBTOs), which are excited to singlet states on photoirradiation. The excited DBTOs isomerize through a minimum energy intersection eventually to dibenzofuran episulfides from which sulfur extrusion occurs. |
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Dibenzothiophene derivatives (DBTs), which are known as particularly difficult desulfurizing substances, have been decomposed reductively in severe conditions of high temperatures (270–372 °C) and high pressure (50–102 atm of H2). In this study, we developed a UV light irradiation-based desulfurization method for aromatic sulfur compounds such as benzothiophene derivatives (BTs) and DBTs under room temperature and atmospheric pressure without the use of catalysts or additives. This method is simple, location-independent, and low-cost, and has low environmental impact. BTs and DBTs completely decomposed in approximately 8 h and 16 h, respectively, under ultraviolet (UV) light irradiation (λ = 254 nm) from a 8 W lamp. The yellow precipitates that were produced upon decomposition were confirmed to be sulfur allotropes (S n ). The residual hydrocarbon portion of DBT after sulfur removal was determined to be benzene. The decomposition reaction was determined to exhibit pseudo-first-order reaction. DFT calculations confirmed the degradation mechanism as follows: UV light irradiation induces a photochemically excited triplet state of DBTs. The excited DBTs reacts with O2 to form a π-complex, which isomerizes to a more stable σ-complex. The DBTs-O2 (σ-complex) then reacts with free DBTs to afford two molecules of dibenzothiophene-5-oxide derivatives (DBTOs), which are excited to singlet states on photoirradiation. The excited DBTOs isomerize through a minimum energy intersection eventually to dibenzofuran episulfides from which sulfur extrusion occurs.</subfield></datafield><datafield tag="650" ind1=" " ind2="7"><subfield code="a">DFT calculation</subfield><subfield code="2">Elsevier</subfield></datafield><datafield tag="650" ind1=" " ind2="7"><subfield code="a">Additive-free</subfield><subfield code="2">Elsevier</subfield></datafield><datafield tag="650" ind1=" " ind2="7"><subfield code="a">Catalyst-free</subfield><subfield code="2">Elsevier</subfield></datafield><datafield tag="650" ind1=" " ind2="7"><subfield code="a">Deep-desulfurization</subfield><subfield code="2">Elsevier</subfield></datafield><datafield tag="650" ind1=" " ind2="7"><subfield code="a">Organic sulfur</subfield><subfield code="2">Elsevier</subfield></datafield><datafield tag="650" ind1=" " ind2="7"><subfield code="a">UV irradiation</subfield><subfield code="2">Elsevier</subfield></datafield><datafield tag="700" ind1="1" ind2=" "><subfield code="a">Suenaga, Masahiko</subfield><subfield code="4">oth</subfield></datafield><datafield tag="700" ind1="1" ind2=" "><subfield code="a">Ko, Yohan</subfield><subfield code="4">oth</subfield></datafield><datafield tag="700" ind1="1" ind2=" "><subfield code="a">Yamamoto, Eiji</subfield><subfield code="4">oth</subfield></datafield><datafield tag="700" ind1="1" ind2=" "><subfield code="a">Murayama, Haruno</subfield><subfield code="4">oth</subfield></datafield><datafield tag="700" ind1="1" ind2=" "><subfield code="a">Tokunaga, Makoto</subfield><subfield code="4">oth</subfield></datafield><datafield tag="773" ind1="0" ind2="8"><subfield code="i">Enthalten in</subfield><subfield code="n">Elsevier Science</subfield><subfield code="a">Rajendiran, Rajmohan ELSEVIER</subfield><subfield code="t">Self-assembled 3D hierarchical MnCO</subfield><subfield code="d">2020</subfield><subfield code="g">Amsterdam [u.a.]</subfield><subfield code="w">(DE-627)ELV003750353</subfield></datafield><datafield tag="773" ind1="1" ind2="8"><subfield code="g">volume:370</subfield><subfield code="g">year:2022</subfield><subfield code="g">day:10</subfield><subfield code="g">month:10</subfield><subfield code="g">pages:0</subfield></datafield><datafield tag="856" ind1="4" ind2="0"><subfield code="u">https://doi.org/10.1016/j.jclepro.2022.133402</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="936" ind1="b" ind2="k"><subfield code="a">35.18</subfield><subfield code="j">Kolloidchemie</subfield><subfield code="j">Grenzflächenchemie</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">370</subfield><subfield code="j">2022</subfield><subfield code="b">10</subfield><subfield code="c">1010</subfield><subfield code="h">0</subfield></datafield></record></collection>
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