PL220511B1 - Method for photocatalytic reduction of carbon dioxide to methanol - Google Patents
Method for photocatalytic reduction of carbon dioxide to methanolInfo
- Publication number
- PL220511B1 PL220511B1 PL400037A PL40003712A PL220511B1 PL 220511 B1 PL220511 B1 PL 220511B1 PL 400037 A PL400037 A PL 400037A PL 40003712 A PL40003712 A PL 40003712A PL 220511 B1 PL220511 B1 PL 220511B1
- Authority
- PL
- Poland
- Prior art keywords
- methanol
- carbon dioxide
- photocatalytic reduction
- reduction
- tio2
- Prior art date
Links
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 title claims description 48
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 title claims description 24
- 238000000034 method Methods 0.000 title claims description 18
- 229910002092 carbon dioxide Inorganic materials 0.000 title claims description 12
- 239000001569 carbon dioxide Substances 0.000 title claims description 11
- 230000001699 photocatalysis Effects 0.000 title claims description 8
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 claims description 34
- 239000011941 photocatalyst Substances 0.000 claims description 9
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 7
- 239000004408 titanium dioxide Substances 0.000 claims description 4
- 239000000725 suspension Substances 0.000 claims description 3
- 239000002071 nanotube Substances 0.000 claims description 2
- 230000005855 radiation Effects 0.000 claims description 2
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 description 15
- 239000003054 catalyst Substances 0.000 description 8
- 238000006555 catalytic reaction Methods 0.000 description 8
- 238000006722 reduction reaction Methods 0.000 description 8
- 238000001027 hydrothermal synthesis Methods 0.000 description 6
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 4
- 150000002894 organic compounds Chemical class 0.000 description 4
- WSFSSNUMVMOOMR-UHFFFAOYSA-N Formaldehyde Chemical compound O=C WSFSSNUMVMOOMR-UHFFFAOYSA-N 0.000 description 3
- 229910010413 TiO 2 Inorganic materials 0.000 description 2
- 239000012153 distilled water Substances 0.000 description 2
- 229910052751 metal Inorganic materials 0.000 description 2
- 239000002184 metal Substances 0.000 description 2
- 150000002739 metals Chemical class 0.000 description 2
- 238000007540 photo-reduction reaction Methods 0.000 description 2
- 239000010457 zeolite Substances 0.000 description 2
- NLXLAEXVIDQMFP-UHFFFAOYSA-N Ammonium chloride Substances [NH4+].[Cl-] NLXLAEXVIDQMFP-UHFFFAOYSA-N 0.000 description 1
- VHUUQVKOLVNVRT-UHFFFAOYSA-N Ammonium hydroxide Chemical compound [NH4+].[OH-] VHUUQVKOLVNVRT-UHFFFAOYSA-N 0.000 description 1
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 1
- OTMSDBZUPAUEDD-UHFFFAOYSA-N Ethane Chemical compound CC OTMSDBZUPAUEDD-UHFFFAOYSA-N 0.000 description 1
- VGGSQFUCUMXWEO-UHFFFAOYSA-N Ethene Chemical compound C=C VGGSQFUCUMXWEO-UHFFFAOYSA-N 0.000 description 1
- 239000005977 Ethylene Substances 0.000 description 1
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 1
- 229910021536 Zeolite Inorganic materials 0.000 description 1
- 235000011114 ammonium hydroxide Nutrition 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 230000005587 bubbling Effects 0.000 description 1
- 230000003197 catalytic effect Effects 0.000 description 1
- 238000006243 chemical reaction Methods 0.000 description 1
- 229910052802 copper Inorganic materials 0.000 description 1
- 239000010949 copper Substances 0.000 description 1
- HNPSIPDUKPIQMN-UHFFFAOYSA-N dioxosilane;oxo(oxoalumanyloxy)alumane Chemical compound O=[Si]=O.O=[Al]O[Al]=O HNPSIPDUKPIQMN-UHFFFAOYSA-N 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- PCHJSUWPFVWCPO-UHFFFAOYSA-N gold Chemical compound [Au] PCHJSUWPFVWCPO-UHFFFAOYSA-N 0.000 description 1
- 239000010931 gold Substances 0.000 description 1
- 229910052737 gold Inorganic materials 0.000 description 1
- WSFSSNUMVMOOMR-NJFSPNSNSA-N methanone Chemical compound O=[14CH2] WSFSSNUMVMOOMR-NJFSPNSNSA-N 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- SOQBVABWOPYFQZ-UHFFFAOYSA-N oxygen(2-);titanium(4+) Chemical compound [O-2].[O-2].[Ti+4] SOQBVABWOPYFQZ-UHFFFAOYSA-N 0.000 description 1
- 239000012429 reaction media Substances 0.000 description 1
- 239000011541 reaction mixture Substances 0.000 description 1
- 239000002002 slurry Substances 0.000 description 1
- 230000007704 transition Effects 0.000 description 1
Classifications
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P20/00—Technologies relating to chemical industry
- Y02P20/50—Improvements relating to the production of bulk chemicals
- Y02P20/52—Improvements relating to the production of bulk chemicals using catalysts, e.g. selective catalysts
Landscapes
- Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)
- Catalysts (AREA)
Description
Opis wynalazkuDescription of the invention
Przedmiotem wynalazku jest sposób fotokatalitycznej redukcji ditlenku węgla do metanolu.The present invention relates to a process for the photocatalytic reduction of carbon dioxide to methanol.
Fotokatalityczna redukcja ditlenku węgla w wodzie do związków organicznych jest istotna lecz bardzo trudna do zrealizowania. W literaturze opisano kilka aktywnych fotokatalizatorów pracujące przy ekspozycji na światło UV-Vis. Znana jest z literatury A. Fujishima, K. Honda, Nature 238 (1972) 37 metoda fotokatalitycznej redukcji ditlenku węgla w wodzie do związków organicznych (metan, metanol, formaldehyd) w obecności: WO3, TiO2, ZnO, CdS, GaP i SiC. Wydajność z jaką otrzymuje się pożądane związki organiczne jest bardzo niska, dlatego prowadzone są badania zmierzające do jej podwyższenia. Znane są sposoby fotokatalitycznej redukcji ditlenku węgla do metanolu, w których jako fotokatalizator stosowany jest TiO2 otrzymywany i modyfikowany w różny sposób. Wiadomo z literatury M. Anpo, H. Yamashita, Y. Ichihashi, S. Ehara, Journal of Electroanalytical Chemistry, 396 (1995) 21, że szczególne znaczenie ma odmiana polimorficzna TiO2 (anataz, rutyl) oraz jego powierzchnia właściwa. W ostatnich latach zwraca się uwagę na katalizatory zawierające ditlenek tytanu promowany różnymi metalami. Znane jest z literatury I.-H. Tseng, J.C.S. Wu, H.-Y. Chou, Journal of Catalysis 221 (2004) 432, T. Mizuno, H. Tsutsumi, K. Ohta, A. Sagi, H. Noda, Chemistry Letters 46 (1994) 1553, K. Adachi, K. Ohta, T. Mizuno, Solar Energy 53 (1994) 187, I.-H. Tseng, W.C. Chang, J.C.S. Wu, Applied Catalysis B: Environ 37 (2002) 37, że modyfikowanie TiO2 metalami grup przejściowych wpływa na podwyższenie efektywności redukcji CO2. Z polskiego opisu patentowego P 394081 znany jest sposób fotokatalitycznej redukcji ditlenku węgla do związków organicznych takich jak: metan, etan, etylen, metanol i formaldehyd polegający na tym, że jako fotokatalizator stosuje się ditlenek tytanu promowany złotem. W literaturze I-Hsiang Tseng, Jeffrey C.S. Wu, Hsin-Ying Chou, Journal of Catalysis 221 (2004) 432-440, I-Hsiang Tseng, Wan-Chen Chang, Jeffrey C.S. Wu, Applied Catalysis B: Environmental 37 (2002) 37-48, Slamet, H.W. Nasution, E. Purnama, S. Kosela, J. Gunlazuardi, Catalysis Communications 6 (2005) 313-319 wskazano na korzystny wpływ dodatku NaOH do mieszaniny reakcyjnej, zawiesiny fotokatalizatora w wodzie, jeśli fotokatalizatorem tym jest TiO2 dotowany miedzią. Zgłoszenie patentowe P387702 wprowadza również możliwość zastąpienia NaOH za pomocą roztworu amoniaku. Stosowano też TiO2 osadzony na zeolitach: zeolit Y - Anpo, M., Yamashita, H., Ichihashi, Y., Fujii, Y., Honda, M., The Journal of Physical Chemistry B, 101 (1997) 2632-2636, MCM-41, MCM-48 - Anpo, M. Yamashita, H., Ikeue, K., Fujii, Y., Zhang, S.G., Ichihashi, Y., G., Park, D.R., Suzuki, Y., Koyano, K., Tatsumi, T. Catalysis Today, 44 (1998) 327-332. Pan opisał (Pan, P.-W., & Chen, Y.-W. (2007). Catalysis Communications, 8, 1546-1549) proces katalitycznej fotoredukcji CO2 przy ekspozycji na światło widzialne przy zastosowaniu NiO/InTaO4.The photocatalytic reduction of carbon dioxide in water to organic compounds is important but very difficult to achieve. Several active photocatalysts operating under UV-Vis light exposure have been described in the literature. A method of photocatalytic reduction of carbon dioxide in water to organic compounds (methane, methanol, formaldehyde) in the presence of: WO3, TiO2, ZnO, CdS, GaP and SiC is known from the literature of A. Fujishima, K. Honda, Nature 238 (1972) 37. The efficiency with which the desired organic compounds are obtained is very low, therefore research is being carried out to increase it. There are known methods of photocatalytic reduction of carbon dioxide to methanol, in which TiO2 obtained and modified in various ways is used as a photocatalyst. It is known from the literature of M. Anpo, H. Yamashita, Y. Ichihashi, S. Ehara, Journal of Electroanalytical Chemistry, 396 (1995) 21 that the polymorphic form of TiO2 (anatase, rutile) and its specific surface are of particular importance. In recent years, attention has been paid to catalysts containing titanium dioxide promoted with various metals. It is known from the literature of I.-H. Tseng, JCS Wu, H.-Y. Chou, Journal of Catalysis 221 (2004) 432, T. Mizuno, H. Tsutsumi, K. Ohta, A. Sagi, H. Noda, Chemistry Letters 46 (1994) 1553, K. Adachi, K. Ohta, T. Mizuno , Solar Energy 53 (1994) 187, I.-H. Tseng, WC Chang, JCS Wu, Applied Catalysis B: Environ 37 (2002) 37 that the modification of TiO2 with transition group metals increases the efficiency of CO2 reduction. The Polish patent P 394081 describes a method of photocatalytic reduction of carbon dioxide to organic compounds such as: methane, ethane, ethylene, methanol and formaldehyde, whereby titanium dioxide promoted with gold is used as a photocatalyst. In the literature I-Hsiang Tseng, Jeffrey CS Wu, Hsin-Ying Chou, Journal of Catalysis 221 (2004) 432-440, I-Hsiang Tseng, Wan-Chen Chang, Jeffrey CS Wu, Applied Catalysis B: Environmental 37 (2002) 37-48, Slamet, HW Nasution, E. Purnama, S. Kosela, J. Gunlazuardi, Catalysis Communications 6 (2005) 313-319 shows the beneficial effect of adding NaOH to the reaction mixture, the photocatalyst suspension in water, if the photocatalyst is TiO2 subsidized with copper. Patent application P387702 also introduces the possibility of replacing NaOH with an ammonia solution. TiO 2 deposited on zeolites was also used: zeolite Y - Anpo, M., Yamashita, H., Ichihashi, Y., Fujii, Y., Honda, M., The Journal of Physical Chemistry B, 101 (1997) 2632-2636 , MCM-41, MCM-48 - Anpo, M. Yamashita, H., Ikeue, K., Fujii, Y., Zhang, SG, Ichihashi, Y., G., Park, DR, Suzuki, Y., Koyano , K., Tatsumi, T. Catalysis Today, 44 (1998) 327-332. You have described (Pan, P.-W., & Chen, Y.-W. (2007). Catalysis Communications, 8, 1546-1549) the process of catalytic CO 2 photo reduction when exposed to visible light using NiO / InTaO 4 .
Nieoczekiwanie okazało się, że nanorurki TiO2 mogą być katalizatorami fotoredukcji ditlenku węgla do metanolu.Surprisingly, it turned out that TiO2 nanotubes can be catalysts for the photo reduction of carbon dioxide to methanol.
Sposób fotokatalitycznej redukcji ditlenku węgla do metanolu, według wynalazku, polegający na jego redukcji w wodzie w obecności fotokatalizatora, w temperaturze 20 - 30°C, pod ciśnieniem od 0,1 do 15 MPa, charakteryzuje się tym, że jako fotokatalizator stosuje się zawiesinę nanorurek ditlenku tytanu o stężeniu 0,01 - 10% masowych. Proces prowadzi się stosując promieniowanie z zakresu UV-Vis.The method of photocatalytic reduction of carbon dioxide to methanol, according to the invention, consisting in its reduction in water in the presence of a photocatalyst, at a temperature of 20-30 ° C, under a pressure of 0.1 to 15 MPa, is characterized in that a nanotube suspension is used as the photocatalyst titanium dioxide with a concentration of 0.01 - 10% by mass. The process is carried out using radiation in the UV-Vis range.
Sposób według wynalazku przedstawiony Jest bliżej w przykładach wykonania.The method according to the invention is presented in more detail in the working examples.
P r z y k ł a d IP r z k ł a d I
Do reaktora półprzepływowego wyposażonego w lampę emitującą światło UV-Vis o długości fal 300-600 nm doprowadzano ditlenek węgla króćcem wlotowym umieszczonym blisko dna reaktora, tak aby zapewnić jego powolny barbotaż przez medium reakcyjne, czyli wodę destylowaną oraz kataliza3 tor w postaci nierozpuszczalnej w medium reakcyjnym zawiesiny. Do reaktora wlano 600 cm3 wody destylowanej i wsypano 0,5 g rurek TiO2 otrzymanych metodą hydrotermalną z P25 i NaOH. Włączo3 no lampę UV-Vis. Ditlenek węgla doprowadzano z szybkością 100 cm3/min. W reaktorze utrzymywano temperaturę 30°C i ciśnienie 0,1 MPa. Po dwóch godzinach pobierano próbki do analizy. Zawartość metanolu oznaczano wykorzystując chromatograf gazowy. Stwierdzono, że metanol był otrzymywany z wydajnością 0,07 μmol/(g·h).Półprzepływowego to the reactor equipped with a lamp emitting UV-Vis wavelength of 300-600 nm was fed carbon dioxide inlet port located near the bottom of the reactor so as to ensure its slow bubbling through the reaction medium, the catalysis and distilled water three track-insoluble form of medium slurry reaction. 600 cm 3 of distilled water are poured into the reactor and 0.5 g of TiO2 tubes obtained with the hydrothermal method with P25 and NaOH are poured in. The UV-Vis lamp is turned on. Carbon dioxide was fed at a rate of 100 cm 3 / min. The temperature of the reactor was 30 ° C and the pressure was 0.1 MPa. Two hours later, samples were taken for analysis. The methanol content was determined using a gas chromatograph. It was found that methanol was obtained with a yield of 0.07 µmol / (g · h).
P r z y k ł a d IIP r z x l a d II
Postępowano jak w przykładzie I z tym, że masa katalizatora wynosiła 0,1 g, a ciśnienie 15 MPa. Stwierdzono, że metanol był otrzymywany z wydajnością 0,01 μmol/(g·h).The procedure was as in Example 1, except that the weight of the catalyst was 0.1 g and the pressure was 15 MPa. It was found that methanol was obtained with a yield of 0.01 µmol / (g · h).
PL 220 511 B1PL 220 511 B1
P r z y k ł a d IIIP r x l a d III
Postępowano analogicznie jak w przykładzie I z tym, że jako katalizator zastosowano rurki TiO2 otrzymane metodą hydrotermalną z anatazu i NaOH. Stwierdzono, że metanol był otrzymywany z wydajnością 0,02 pmol/(g-h).The procedure was analogous to that in Example 1, except that the catalyst was TiO 2 tubes obtained by hydrothermal method from anatase and NaOH. It was found that methanol was obtained in a yield of 0.02 pmol / (gh).
P r z y k ł a d IVP r x l a d IV
Postępowano analogicznie jak w przykładzie I z tym, że jako katalizator zastosowano 2 g rurek TiO2 otrzymanych metodą hydrotermalną z rutylu i NaOH. Stwierdzono, że metanol był otrzymywany z wydajnością 0,001 pmol/(g-h).The procedure was analogous to that in Example 1, except that 2 g of TiO2 tubes obtained by hydrothermal method from rutile and NaOH were used as the catalyst. It was found that methanol was obtained in a yield of 0.001 pmol / (g-h).
P r z y k ł a d VP r z k ł a d V
Postępowano analogicznie jak w przykładzie I z tym, że jako katalizator zastosowano 6 g rurek TiO2 otrzymanych metodą hydrotermalną z rutylu i KOH. Stwierdzono, że metanol był otrzymywany z wydajnością 0,001 pmol/(g-h).The procedure was analogous to that in Example 1, except that the catalyst used was 6 g of TiO2 tubes obtained by hydrothermal method from rutile and KOH. It was found that methanol was obtained in a yield of 0.001 pmol / (g-h).
P r z y k ł a d VIP r x l a d VI
Postępowano analogicznie jak w przykładzie I z tym, że jako katalizator zastosowano 70 g rurek TiO2 otrzymanych metodą hydrotermalną z P25 i KOH. Stwierdzono, że metanol był otrzymywany z wydajnością 0,09 pmol/(g-h).The procedure was analogous to that in Example 1, except that the catalyst used was 70 g of TiO2 tubes obtained by hydrothermal method with P25 and KOH. It was found that methanol was obtained with a yield of 0.09 pmol / (g-h).
P r z y k ł a d VIIP r o x l a d VII
Postępowano analogicznie jak w przykładzie I z tym, że jako katalizator zastosowano 4 g rurek TiO2 otrzymanych metodą hydrotermalną z anatazu i KOH. Stwierdzono, że metanol był otrzymywany z wydajnością 0,08 pmol/(g-h).The procedure was analogous to that in Example 1, except that 4 g of TiO2 tubes obtained by hydrothermal method from anatase and KOH were used as the catalyst. It was found that methanol was obtained with a yield of 0.08 pmol / (g-h).
Claims (2)
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| PL400037A PL220511B1 (en) | 2012-07-19 | 2012-07-19 | Method for photocatalytic reduction of carbon dioxide to methanol |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| PL400037A PL220511B1 (en) | 2012-07-19 | 2012-07-19 | Method for photocatalytic reduction of carbon dioxide to methanol |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| PL400037A1 PL400037A1 (en) | 2014-01-20 |
| PL220511B1 true PL220511B1 (en) | 2015-11-30 |
Family
ID=49920862
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| PL400037A PL220511B1 (en) | 2012-07-19 | 2012-07-19 | Method for photocatalytic reduction of carbon dioxide to methanol |
Country Status (1)
| Country | Link |
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| PL (1) | PL220511B1 (en) |
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2012
- 2012-07-19 PL PL400037A patent/PL220511B1/en unknown
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| Publication number | Publication date |
|---|---|
| PL400037A1 (en) | 2014-01-20 |
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