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ELECTROCHEMICAL REDUCTION OF CARBON DIOXIDE NEW

外国特許コード F170008971
整理番号 AF39-01WO
掲載日 2017年3月13日
出願国 世界知的所有権機関(WIPO)
国際出願番号 2016JP053558
国際公開番号 WO 2016136433
国際出願日 平成28年2月5日(2016.2.5)
国際公開日 平成28年9月1日(2016.9.1)
優先権データ
  • 特願2015-037839 (2015.2.27) JP
  • 特願2015-160768 (2015.8.18) JP
発明の名称 (英語) ELECTROCHEMICAL REDUCTION OF CARBON DIOXIDE NEW
発明の概要(英語) Provided are: a method for selectively reducing CO2 to carbon monoxide or formic acid using electrical energy; a catalyst used therefor; and an electrochemical reduction system. A method for manufacturing carbon monoxide or formic acid from carbon dioxide by electrochemical reduction characterized in comprising steps (a) and (b). (a) A step for reacting carbon dioxide with a metal complex represented by general formula (1) (in the formula, M represents rhenium, manganese, ruthenium or iron; X represents OR1, SR1, NR2R3R4 or PX1X2X3; Y represents CO, OR1, SR1, NR2R3R4 or PX1X2X3; ring A and ring B are the same or different and represent nitrogen atom-containing heterocyclic rings that may have a substituent; R1 represents a hydrocarbon group that may have a substituent; one to three of R2, R3 and R4 can be the same or different and represent hydrocarbon groups that may have a substituent, the remainder representing a hydrogen atom; one to three of X1, X2 and X3 can be the same or different and represent hydrocarbon groups that may have a substituent or a hydrocarbon oxy group that may have a substituent, the remainder representing a hydrogen atom or hydroxyl group.) (b) A step for applying voltage on the reaction product of carbon dioxide with the metal complex represented by general formula (1).
特許請求の範囲(英語) [claim1]
1. The following process (a) and (b) the production method from carbon dioxide which feature that it possesses due to the electrochemistry restoration of carbon monoxide.
(A) Carbon dioxide and general system (1)
(In formula, as for X, OR (1), SR (1), NR (2) R (3) R (4) or PX (1) X (2) X (3) showing,
As for Y, CO and OR (1), SR (1), NR (2) R (3) R (4) or PX (1) X (2) X (3) showing,
As for A ring and B ring, equality or differing, showing the nitrogen atomic content complex ring which is possible to have possessed the substituent,
As for R (1), showing the hydrocarbon radical which is possible to have possessed the substituent,
R (2), R (3) and R (4) the 1-3 to show the hydrocarbon radical which equality or differs and is possible to have possessed the substituent, as for the remainder showing the hydrogen atom,
X (1) and X (2) and X (3) 1-3, equality or differing, shows the hydrocarbon oxy basis which is possible to have possessed the hydrocarbon radical or the substituent which is possible to have possessed the substituent, the remainder shows the hydrogen atom or the hydroxy basis.)
So the process which reacts with the metal complex which is displayed,
(B) Carbon dioxide and general system the process which impresses voltage in the reactant of the metal complex which is displayed with (1).
[claim2]
2. Production method of the claim 1 statement where the aforementioned process (a) and (b) action extremely and is the method of being done inside the electrochemistry cell which possesses the counter electrode process (a1) and (b1) is something which is included.
(A1) Carbon dioxide the process which is introduced in the solution which includes the aforementioned metal complex inside the electrochemistry cell,
(B1) Action of the electrochemistry cell extremely and the process which impresses negative voltage and correct voltage respectively in the counter electrode.
[claim3]
3. Introduction of carbon dioxide, production method of the claim 2 statement which introduces carbon dioxide content gases in the solution which contains the aforementioned metal complex.
[claim4]
4. Carbon dioxide which are used for the reaction, either of the claim 1-3 which is the gas which carbon dioxide the 0.03-100% is contained production method of 1 section statements.
[claim5]
5. The nitrogen atomic content complex ring which includes A ring and B ring, 2,2 where it is possible to have possessed the substituent' - either of the claim 1-4 which is the complex ring which possesses bibyridine structure production method of 1 section statements.
[claim6]
6. R (1), R (2), R (3), R (4) and X (1) and X (2) and X the hydrocarbon radical which is possible to have possessed the substituent which is shown with (3), the alkyl group and the [arukeniru] basis, [shikuroarukiru] , the [shikuroarukeniru] basis or the aromatic hydrocarbon radical (as for these bases, one class, two classes or three class amino groups, the hydroxy basis, alkoxy group and the aryl oxy basis, the halogen atom, the 1-3 which is chosen from the nitro group, the cyano basis, the formyl basis, the [arukanoiru] basis and the aryl carbonyl group the substituent had could have had either of the claim 1-5 which) is production method of 1 section statements.
[claim7]
7. From carbon dioxide which feature that you use the carbon monoxide which is obtained either of the claim 1-6 by the production method of 1 section statements as the reducing agent production method of carbon monoxide.
[claim8]
8. Production method of the hydrocarbon type chemical compound which designates the carbon monoxide which is obtained either of the claim 1-6 by the production method of 1 section statements as the raw materials.
[claim9]
9. General system (1)
(In formula, as for X, OR (1), SR (1), NR (2) R (3) R (4) or PX (1) X (2) X (3) showing,
As for Y, CO and OR (1), SR (1), NR (2) R (3) R (4) or PX (1) X (2) X (3) showing,
As for A ring and B ring, equality or differing, showing the nitrogen atomic content complex ring which is possible to have possessed the substituent,
As for R (1), showing the hydrocarbon radical which is possible to have possessed the substituent,
R (2), R (3) and R (4) the 1-3 to show the hydrocarbon radical which equality or differs and is possible to have possessed the substituent, as for the remainder showing the hydrogen atom,
X (1) and X (2) and X (3) 1-3, equality or differing, shows the hydrocarbon oxy basis which is possible to have possessed the hydrocarbon radical or the substituent which is possible to have possessed the substituent, the remainder shows the hydrogen atom or the hydroxy basis.)
So from carbon dioxide which are displayed the catalyst for electrochemistry restoration to carbon monoxide.
[claim10]
10. The nitrogen atomic content complex ring which includes A ring and B ring, 2,2 where it is possible to have possessed the substituent' - the catalyst of the claim 9 statement which is the complex ring which possesses bibyridine structure.
[claim11]
11. R (1), R (2), R (3), R (4) and X (1) and X (2) and X the hydrocarbon radical which is possible to have possessed the substituent which is shown with (3), the alkyl group and the [arukeniru] basis, [shikuroarukiru] , the [shikuroarukeniru] basis or the aromatic hydrocarbon radical (as for these bases, one class, two classes or three class amino groups, the hydroxy basis, alkoxy group and the aryl oxy basis, the halogen atom, the 1-3 which is chosen from the nitro group, the cyano basis, the formyl basis, the [arukanoiru] basis and the aryl carbonyl group the substituent had could have had the claim the catalyst of 9 which) is or 10 statements.
[claim12]
12. The following process (a) and (b) the production method from carbon dioxide which feature that it possesses due to the electrochemistry restoration of formic acid.
(A) Carbon dioxide and general system (2)
(In formula, as for M [1], showing manganese, ruthenium or iron,
As for X, OR (1), SR (1), NR (2) R (3) R (4) or PX (1) X (2) X (3) showing,
As for Y, CO and OR (1), SR (1), NR (2) R (3) R (4) or PX (1) X (2) X (3) showing,
As for A ring and B ring, equality or differing, showing the nitrogen atomic content complex ring which is possible to have possessed the substituent,
As for R (1), showing the hydrocarbon radical which is possible to have possessed the substituent,
R (2), R (3) and R (4) the 1-3 to show the hydrocarbon radical which equality or differs and is possible to have possessed the substituent, as for the remainder showing the hydrogen atom,
X (1) and X (2) and X (3) 1-3, equality or differing, shows the hydrocarbon oxy basis which is possible to have possessed the hydrocarbon radical or the substituent which is possible to have possessed the substituent, the remainder shows the hydrogen atom or the hydroxy basis.)
So the process which reacts with the metal complex which is displayed,
(B) Carbon dioxide and general system the process which impresses voltage in the reactant of the metal complex which is displayed with (2).
[claim13]
13. Production method of the claim 12 statement where the aforementioned process (a) and (b) action extremely and is the method of being done inside the electrochemistry cell which possesses the counter electrode process (a1) and (b1) is something which is included.
(A1) Carbon dioxide the process which is introduced in the solution which includes the aforementioned metal complex inside the electrochemistry cell,
(B1) Action of the electrochemistry cell extremely and the process which impresses negative voltage and correct voltage respectively in the counter electrode.
[claim14]
14. Introduction of carbon dioxide, production method of the claim 13 statement which introduces carbon dioxide content gases in the solution which contains the aforementioned metal complex.
[claim15]
15. Carbon dioxide which are used for the reaction, either of the claim 12-14 which is the gas which carbon dioxide the 0.03-100% is contained production method of 1 section statements.
[claim16]
16. The nitrogen atomic content complex ring which includes A ring and B ring, 2,2 where it is possible to have possessed the substituent' - either of the claim 12-15 which is the complex ring which possesses bibyridine structure production method of 1 section statements.
[claim17]
17. R (1), R (2), R (3), R (4) and X (1) and X (2) and X the hydrocarbon radical which is possible to have possessed the substituent which is shown with (3), the alkyl group and the [arukeniru] basis, [shikuroarukiru] , the [shikuroarukeniru] basis or the aromatic hydrocarbon radical (as for these bases, one class, two classes or three class amino groups, the hydroxy basis, alkoxy group and the aryl oxy basis, the halogen atom, the 1-3 which is chosen from the nitro group, the cyano basis, the formyl basis, the [arukanoiru] basis and the aryl carbonyl group the substituent had could have had either of the claim 12-16 which) is production method of 1 section statements.
[claim18]
18. General system (2)
(In formula, as for M [1], showing manganese, ruthenium or iron,
As for X, OR (1), SR (1), NR (2) R (3) R (4) or PX (1) X (2) X (3) showing,
As for Y, CO and OR (1), SR (1), NR (2) R (3) R (4) or PX (1) X (2) X (3) showing,
As for A ring and B ring, equality or differing, showing the nitrogen atomic content complex ring which is possible to have possessed the substituent,
As for R (1), showing the hydrocarbon radical which is possible to have possessed the substituent,
R (2), R (3) and R (4) the 1-3 to show the hydrocarbon radical which equality or differs and is possible to have possessed the substituent, as for the remainder showing the hydrogen atom,
X (1) and X (2) and X (3) 1-3, equality or differing, shows the hydrocarbon oxy basis which is possible to have possessed the hydrocarbon radical or the substituent which is possible to have possessed the substituent, the remainder shows the hydrogen atom or the hydroxy basis.)
So from carbon dioxide which are displayed the catalyst for electrochemistry restoration to formic acid.
[claim19]
19. The nitrogen atomic content complex ring which includes A ring and B ring, 2,2 where it is possible to have possessed the substituent' - the catalyst of the claim 18 statement which is the complex ring which possesses bibyridine structure.
[claim20]
20. R (1), R (2), R (3), R (4) and X (1) and X (2) and X the hydrocarbon radical which is possible to have possessed the substituent which is shown with (3), the alkyl group and the [arukeniru] basis, [shikuroarukiru] , the [shikuroarukeniru] basis or the aromatic hydrocarbon radical (as for these bases, one class, two classes or three class amino groups, the hydroxy basis, alkoxy group and the aryl oxy basis, the halogen atom, the 1-3 which is chosen from the nitro group, the cyano basis, the formyl basis, the [arukanoiru] basis and the aryl carbonyl group the substituent had could have had the claim the catalyst of 18 which) is or 19 statements.
[claim21]
21. General system (2a)
(In formula, as for M [1], showing manganese, ruthenium or iron,
As for X, O (CH [2]) [n] NR (5) R (6), NR (5) R (6) or PX (1) X (2) X (3) showing,
As for Y, CO and C (CH [2]) [n] NR (5) R (6), NR (5) R (6) or PX (1) X (2) X (3) showing,
As for A ring and B ring, equality or differing, showing the nitrogen atomic content complex ring which is possible to have possessed the substituent,
X (1) and X (2) and X (3) 1-3 to show the hydrocarbon oxy basis which is possible to have possessed the hydrocarbon radical or the substituent which equality or differs and is possible to have possessed the substituent, as for the remainder showing the hydrogen atom or the hydroxy basis,
R (5) and R as for (6), equality or differing, showing the alkyl group, the hydroxy alkyl group or the hydrogen atom,
n shows the quantity of 2-8.)
So the metal complex which is displayed.
[claim22]
22. The nitrogen atomic content complex ring which includes A ring and B ring, 2,2 where it is possible to have possessed the substituent' - the metal complex of the claim 21 statement which is the complex ring which possesses bibyridine structure.
[claim23]
23. X (1) and X (2) and X the hydrocarbon radical which is possible to have possessed the substituent which is shown with (3), the alkyl group and the [arukeniru] basis, [shikuroarukiru] , the [shikuroarukeniru] basis or the aromatic hydrocarbon radical (as for these bases, one class, two classes or three class amino groups, the hydroxy basis, alkoxy group and the aryl oxy basis, the halogen atom, the 1-3 which is chosen from the nitro group, the cyano basis, the formyl basis, the [arukanoiru] basis and the aryl carbonyl group the substituent had could have had the claim the metal complex of 21 which) is or 22 statements.
[claim24]
24. Being the system which produces carbon monoxide from carbon dioxide with electrochemistry restoration,
The solution and the action which include the metal complex extremely, and the electrochemical cell which possesses the counter electrode and,
The fill section which fills carbon dioxide to the solution which includes the aforementioned metal complex of the aforementioned electrochemical cell circles, and,
The aforementioned action of the aforementioned electrochemical cell circles extremely and between the counter electrodes, the righteousness or negative voltage the voltage source which is made applicable and,
The discharge section which discharges the carbon monoxide which is formed inside the solution which includes the aforementioned metal complex and,
Possessing,
In the aforementioned metal complex reactant which is formed by the solution and carbon dioxide which include the aforementioned metal complex, the righteousness or by impressing negative voltage, the carbon monoxide manufacturing system which formation obtains carbon monoxide.
[claim25]
25. The aforementioned metal complex general system (1)
(In formula, as for X, OR (1), SR (1), NR (2) R (3) R (4) or PX (1) X (2) X (3) showing,
As for Y, CO and OR (1), SR (1), NR (2) R (3) R (4) or PX (1) X (2) X (3) showing,
As for A ring and B ring, equality or differing, showing the nitrogen atomic content complex ring which is possible to have possessed the substituent,
As for R (1), showing the hydrocarbon radical which is possible to have possessed the substituent,
R (2), R (3) and R (4) the 1-3 to show the hydrocarbon radical which equality or differs and is possible to have possessed the substituent, as for the remainder showing the hydrogen atom,
X (1) and X (2) and X (3) 1-3, equality or differing, shows the hydrocarbon oxy basis which is possible to have possessed the hydrocarbon radical or the substituent which is possible to have possessed the substituent, the remainder shows the hydrogen atom or the hydroxy basis.)
So the carbon monoxide manufacturing system of the claim 24 statement which is the metal complex which is displayed.
[claim26]
26. In the forwarding section which forwards the aforementioned carbon dioxide, as for the aforementioned carbon dioxide the claim the carbon monoxide manufacturing system of 24 which is forwarded without concentrating or 25 statements.
[claim27]
27. From the solution which includes the aforementioned metal complex, either of the claim 24-26 which furthermore includes the carbon monoxide sensing station which detects the density of the carbon monoxide which is discharged the carbon monoxide manufacturing system of 1 section statements.
[claim28]
28. The aforementioned carbon monoxide sensing station, the carbon monoxide manufacturing system of the claim 27 statement which is the gas chromatography.
[claim29]
29. The nitrogen atomic content complex ring which includes A ring and B ring, 2,2 where it is possible to have possessed the substituent' - either of the claim 24-28 which is the complex ring which possesses bibyridine structure the carbon monoxide manufacturing system of 1 section statements.
[claim30]
30. R (1), R (2), R (3), R (4) and X (1) and X (2) and X the hydrocarbon radical which is possible to have possessed the substituent which is shown with (3), the alkyl group and the [arukeniru] basis, [shikuroarukiru] , the [shikuroarukeniru] basis or the aromatic hydrocarbon radical (as for these bases, one class, two classes or three class amino groups, the hydroxy basis, alkoxy group and the aryl oxy basis, the halogen atom, the 1-3 which is chosen from the nitro group, the cyano basis, the formyl basis, the [arukanoiru] basis and the aryl carbonyl group the substituent had could have had either of the claim 24-29 which) is the carbon monoxide manufacturing system of 1 section statements.
  • 出願人(英語)
  • ※2012年7月以前掲載分については米国以外のすべての指定国
  • JAPAN SCIENCE AND TECHNOLOGY AGENCY
  • 発明者(英語)
  • ISHITANI OSAMU
国際特許分類(IPC)
指定国 (WO2016136433)
National States: AE AG AL AM AO AT AU AZ BA BB BG BH BN BR BW BY BZ CA CH CL CN CO CR CU CZ DE DK DM DO DZ EC EE EG ES FI GB GD GE GH GM GT HN HR HU ID IL IN IR IS JP KE KG KN KP KR KZ LA LC LK LR LS LU LY MA MD ME MG MK MN MW MX MY MZ NA NG NI NO NZ OM PA PE PG PH PL PT QA RO RS RU RW SA SC SD SE SG SK SL SM ST SV SY TH TJ TM TN TR TT TZ UA UG US UZ VC VN ZA ZM ZW
ARIPO: BW GH GM KE LR LS MW MZ NA RW SD SL SZ TZ UG ZM ZW
EAPO: AM AZ BY KG KZ RU TJ TM
EPO: AL AT BE BG CH CY CZ DE DK EE ES FI FR GB GR HR HU IE IS IT LT LU LV MC MK MT NL NO PL PT RO RS SE SI SK SM TR
OAPI: BF BJ CF CG CI CM GA GN GQ GW KM ML MR NE SN ST TD TG
参考情報 (研究プロジェクト等) CREST Establishment of molecular technology towards the Creation of New Functions AREA
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