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That the Ultimate THAT THEUS009764283B2 ULTIMATE (12 ) United States Patent ( 10 ) Patent No. : US 9 ,764 , 283 B2 Fischer et al. (45 ) Date of Patent: Sep . 19 , 2017 (54 ) SCRUBBING SOLUTION FOR ABSORPTION ( 52) U . S . CI. OF CARBON DIOXIDE AND METHOD FOR CPC .. .. BOID 53 /8671 (2013 . 01 ) ; B01D 53 / 1475 ACCELERATING THE ABSORPTION BY ( 2013 .01 ) ; B01D 53 / 1493 ( 2013 .01 ) ; GERMANIUM DIOXIDE (Continued ) ( 58 ) Field of Classification Search (71 ) Applicant : Siemens Aktiengesellschaft , Munich None (DE ) See application file for complete search history. References Cited (72 ) Inventors : Bjorn Fischer , Dusseldorf ( DE ) ; Ralph (56 ) Joh , Seligenstadt (DE ) ; Markus Kinzl , U . S . PATENT DOCUMENTS Dietzenbach (DE ) ; Diego Andres 3 ,790 ,503 A 2 / 1974 McCartney Kuettel, Kassel ( DE ) ; Rudiger 5 , 556 ,603 A 9 / 1996 Succi et al. Schneider , Eppstein (DE ) (Continued ) ( 73 ) Assignee : Siemens Aktiengesellschaft , Munich FOREIGN PATENT DOCUMENTS (DE ) CN 1094377 A 11/ 1994 ( * ) Notice : Subject to any disclaimer , the term of this CN 1636863 A 7 / 2005 patent is extended or adjusted under 35 ( Continued ) U . S . C . 154 ( b ) by 126 days . ( 21 ) Appl. No. : 14 /414 , 110 OTHER PUBLICATIONS Database WPI; “ Database WPI, Week 200618 ” ; Thomson Scien ( 22 ) PCT Filed : Jul. 8 , 2013 tific ; pp . 1 - 3 ; XP002714413 ; 2006 ; GB ; Feb . 16 , 2006 . (Continued ) ( 86 ) PCT No. : PCT/ EP2013 / 064345 Primary Examiner — Daniel Berns $ 371 ( C ) ( 1 ) , (74 ) Attorney , Agent, or Firm — Beusse Wolter Sanks & ( 2 ) Date : Jan . 11 , 2015 Maire (57 ) ABSTRACT (87 ) PCT Pub . No .: WO2014 /012808 A scrubbing solution is provided having an absorbent for PCT Pub . Date : Jan . 23 , 2014 carbon dioxide based on amines , or ethanolamines , or amino acid salts , or potash , or a combination thereof , and an (65 ) Prior Publication Data additive activating the absorption rate , wherein the activat ing additive is a germanium dioxide . A corresponding US 2015 /0165375 A1 Jun . 18 , 2015 method for accelerating the absorption of carbon dioxide is also provided , wherein a carbon dioxide - containing gas is ( 30 ) Foreign Application Priority Data contacted with such a scrubbing solution , wherein the car bon dioxide is physically dissolved in the scrubbing solution Jul . 17, 2012 (DE ) .. 10 2012 212 482 and is chemically absorbed with the participation of the ( 51 ) Int. Ci. absorbent, and wherein the germanium dioxide acts cata BOID 53 / 62 ( 2006 .01 ) lytically for at least one reaction step of the chemical BOID 53 / 14 ( 2006 . 01 ) absorption of the carbon dioxide . (Continued ) 16 Claims, 4 Drawing Sheets CO2( g ) 24 T 1111. , 1919 ,. + Rp CO2 (10aq )] +19 2 RB Ro JURISM- N Le to RANGEja N O 0SM ++ REja Room0 21 11, 19 , B ] > 20 R2 Ñ O + Re- NH2O + HO_ TOM * 4, 182 bao " 12ya ni Sam to US 9 ,764 ,283 B2 Page 2 (51 ) Int. Cl. 2004 / 0123735 A1 7 /2004 Watanabe et al. 2005 / 0106090 A1 5 / 2005 Agarwal et al . B01D 53 / 78 ( 2006 . 01) 2011 /0059845 Al 3 / 2011 Fryxell B01D 53 / 86 ( 2006 .01 ) 2011 /0182799 AL 7 / 2011 Li (52 ) U . S . CI. 2015 / 0011523 A1* 1 / 2015 Isaev CO7F 7 / 30 CPC . .. .. .. B01D 53/ 62 (2013 .01 ) ; B01D 53 /78 317 514 / 188 ( 2013 .01 ) ; BOID 2251 / 306 ( 2013 .01 ) ; BOLD 2251 /606 ( 2013 .01 ) ; B01D 2252 / 10 ( 2013 .01 ) ; FOREIGN PATENT DOCUMENTS B01D 2252 / 204 ( 2013 .01 ) ; B01D 2252 / 20484 JP 2006045456 A 2 / 2006 ( 2013 . 01 ) ; BOID 2252 / 20494 ( 2013 .01 ) ; BOID KR 20110073284 A1 6 / 2011 2252/ 602 ( 2013 .01 ) ; BOID 2255 / 209 RU 2244587 C2 1 / 2005 ( 2013 .01 ) ; B01D 2257/ 504 (2013 .01 ) ; BOID RU 2275231 C2 4 / 2006 RU 2476436 C1 * 2 /2013 .. .. .. A61K 31/ 28 2258 /0283 ( 2013 .01 ) ; YO2C 10 /04 ( 2013 .01 ) ; WO 9904885 AL 2 / 1999 YO2C 10 / 06 ( 2013 .01 ) WO 2004045767 A2 6 / 2004 ( 56 ) References Cited OTHER PUBLICATIONS U . S . PATENT DOCUMENTS RU Office Action dated Apr. 24 , 2017 , for RU patent application No . 5 , 738 ,956 A * 4 / 1998 Komoda .. .. HO1M 10 /08 2015105182 429 /205 someone6 ,267 ,939 B1 is not7 / 2001 recomendas Gemes et al . me st* cited by examiner U . S . Patent Sep. 19 , 2017 Sheet 1 of 4 US 9 , 764, 283 B2 FIG 1 kJ/ kg CO2 - 14 , 19 FIG 2 p - - - - - - - U . S . Patent Sep. 19 , 2017 Sheet 2 of 4 US 9 , 764, 283 B2 FIG 3 CO2( g ) 10 11, 19, CO2( aq ) + 2 Rx- N O to R - NH2 + R2 N 4, 18 /* I OM 13 MI OM JER SM 11, 19 , ?H Ra N 0 , R - NH2 0 , HO . 4. 18 OM OM OF atent Sep . 19 , 2017 Sheet 3 of 4 US 9 , 764, 283 B2 FIG 4 CO2 (g ) ? 11, 19 O . C02 ( aq ) + 2 R2 - HN 0 - R2 - NH: 0 + R ) - N 0 4, 18 o om 12 / ÒM AA A Com > 21 RaN + NYXlY6171 ön * O o 4, 18 Om 12 RohoOM 11, 19, 20 U . S . Patent Sep . 19, 2017 Sheet 4 of 4 US 9 , 764, 283 B2 FIG 5 OOKO = OK - 16, 18 FIG 6 R2N 7 , 18 RTOM US 9 , 764 , 283 B2 SCRUBBING SOLUTION FOR ABSORPTION secondary and tertiary amines have a higher loading capac OF CARBON DIOXIDE AND METHOD FOR ity for carbon dioxide than primary amines. ACCELERATING THE ABSORPTION BY However, the primary amine compounds do have the GERMANIUM DIOXIDE advantage of distinctly faster absorption kinetics . So , com 5 pared with secondary amines or amino acid salts , the CROSS REFERENCE TO RELATED absorber columns or reactors , in which the carbon dioxide is APPLICATIONS absorbed , can be designed smaller, which leads to lower capital costs . Sterically hindered , secondary or tertiary amines or amino acid salts have slower reaction kinetics This application is the US National Stage of Internationaland 10 because they form unstable carbamate products , if any at all . Application No . PCT/ EP2013 / 064345 filed Jul. 8 , 2013 , and b The advantage of amino acid salts over heterocyclic claims the benefit thereof. The International Application amines or alkanolamines is in turn that amino acid salts have claims the benefit of German Application No . DE no noticeable vapor pressure and thus do not evaporate and 102012212482. 9 filed Jul . 17 , 2012 . All of the applications can be dragged out into the environment during the separa are incorporated by reference herein in their entirety . 15 tion process . Heterocyclic amines and alkanolamines are volatile and are dragged out by the cleaned flue gas as it FIELD OF INVENTION passes into the environment, leading to adverse environmen The invention relates to a scrubbing solution having an tal impacts . absorbent for carbon dioxide and an additive activating the 20 SUMMARY OF INVENTION absorption rate . The invention further relates to a corre sponding method for accelerating the absorption of carbon It is an object of the present invention to provide a carbon dioxide . dioxide absorption scrubbing solution which combines a high rate of absorption with low regeneration energy BACKGROUND OF INVENTION 25 requirements and is very environmentally compatible . It is a further object of the present invention to devise a method for A fossil - fuel power plant for generating electric energy accelerating the absorption of carbon dioxide, wherein a gas produces a flue gas comprising carbon dioxide in particular comprising carbon dioxide is contacted with a scrubbing by the combustion of a fossil fuel . To reduce the emission of solution comprising an absorbentwith absorption of carbon carbon dioxide (CO ) , a known secondary measure is to 30 dioxide . remove the carbon dioxide from the flue gas by means of a That object of the invention which is directed to a flue gas scrub . The absorption - desorption procedure is cus - scrubbing solution is achieved by a scrubbing solution tomary in particular. On a large industrial scale this involves comprising an absorbent on the basis of amines , or ethano the flue gas being contacted in an absorber with a scrubbing lamines, or amino acid salts , or potash , or a combination solution comprising an absorbent , scrubbing the carbon 35 thereof, and an activator additive , wherein the activator dioxide out of the flue gas into the scrubbing solution ( CO , additive is a germanium dioxide . capture process ). The carbon dioxide is initially dissolved The invention here proceeds in a first step from the physically in the scrubbing solution and then chemically consideration that the chemical absorption of carbon dioxide absorbed by the adsorbent. The scrubbing solution laden takes place straight away in the scrubbing solution ' s bound with carbon dioxide is subsequently sent into a desorber 40 ary layer with the gas, where the carbon dioxide is initially where , by raising the temperature , the carbon dioxide can be dissolved physically . Hence the reaction involved in absorb desorbed and , for example, sent into suitable storage . The ing the carbon dioxide has an effect on the concentration absorbent is regenerated in the process , so it can be rein profile in the boundary layer. The absorption kinetics as a troduced into the absorber for renewed absorption . whole , i. e ., including the physically dissolving step , which Commonly used absorbents are based in particular on 45 precedes the actual absorption , is accordingly influenced as primary , secondary or tertiary amines or a mixture thereof, such by the reaction rate of the chemical absorption in and display good selectivity and high capacity for the particular. An increase in the reaction rate accordingly leads absorption of carbon dioxide . The chemical industry to an increase in the pickup rate for carbon dioxide from the employs mainly the primary amine MEA (monoetha - gas to be cleaned . nolamine ) for its fast absorption kinetics . However, the 50 The admixture of an activator or a hydration catalyst to a energy efficiency of primary amines in an absorption -des - relatively slow - reacting absorbent, for example the afore orption process is poor, since the regeneration energy mentioned secondary or tertiary amines , amino acid salts or requirements are comparatively high .
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