2A review of research progress on CO capture,storage,and utilization in 34Q156789111213141516171819202122232425262728293031323334353637383940414243444546474849505152535455565758596061626364656667686970717273747576with 58%of the sources being located within the east and south 77central regions.The contributions of large point sources in each 78sector to total CO 2emissions in China are listed in Fig.2[13].With 79rapid development of energy technologies in the 21st century,fos-80sil fuels,especially coal,will still remain the dominant energy0016-2361/$-see front matter Ó2011Elsevier Ltd.All rights reserved.doi:10.1016/j.fuel.2011.08.022⇑Corresponding authors.Q2Address:State Key Laboratory of Coal Conversion,Institute of Coal Chemistry,Chinese Academy of Sciences,Taiyuan 030001,China (Y.Sun).Tel.:+863514049612;fax:+863514041153.E-mail addresses:zhaoning@ (N.Zhao),weiwei@ (W.Wei),yhsun@ (Y.Sun).Please cite this article in press as:L Q1i L et al.A review of research progress on CO 2capture,storage,and utilization in Chinese Academy of Sciences.Fuel(2011),doi:10.1016/j.fuel.2011.08.022source in China for decades to come.Chinese government recognized the huge challenge of CO 2abatement while satisfying ever-increasing energy demand.In the light of this situation,November 26,2009,China officially announced action to control emissions per unit of GDP by 40–45%by 2020,based on 86levels [14].To address this,China is undertaking a range of techni-87cal research and development projects on CCSU,including the na-88tional fundamental research and high-tech programs,as well as a 89large number of international programs.The CCS projects,fun-90dings,and research institutes in China is shown in Table 1.91Since 1990,China had carried out a series of climate change 92projects under framework of national programs,such as China’s 93National Climate Change Program (CNCCP),National Hi-tech R&D949596979899100101102103104105106107108109110111112113114115116117118119120121cooperation with international on CCSU.On the basis of the finical 122support of both Chinese government and CAS,a lot of progresses 123were obtained in several academic institutes in CAS including 124CO 2capture;enhanced oil recovery (EOR)and enhanced coal bed 125methane (ECBM)projects as well as CO 2chemical utilizations.This 126brief review has covered the research progress in CO 2capture,stor-127age,and utilization in CAS.2.The contributions of large point sources in each sector to overall total emissions in China [12].Please cite this article in press as:L Q1i L et al.A review of research progress on CO 2capture,storage,and utilization in Chinese Academy of Sciences.Fuel(2011),doi:10.1016/j.fuel.2011.08.022128129130131132133134135136137aration,and cryogenic fractionation.138 2.1.Amine-based scrubbing solvent139Amine scrubbing is a well known technology for capturing CO 2140from flue gas,which has been widely deployed on a large scale 141across several industries [25–28].The industrially most important142143144145146147148149150151152the environment [30].1532.2.Ionic liquids154Therefore,a nonvolatile solvent that could facilitate CO 2capture 155without the loss of solvent into the gas stream would be advanta-156geous.Ionic liquids (ILs)are commonly defined as liquids whichTable 1CCS projects,fundings,and research institutes in China.China and international cooperation on CCS projects and fundingsResearch institutes aBNLMS–CAS IET–CAS RCEES–CAS ICC–CAS IPE–CAS LICP–CAS CIAC–CAS National High Technology Research and Development Program of China (863)SIC–CAS National Key Basic Research and Development Program of China (973)IGG–CAS China’s National Climate Change Program (CNCCP)IAP–CAS L.L Q1i et al./Fuel xxx (2011)xxx–xxx3Please cite this article in press as:L Q1i L et al.A review of research progress on CO 2capture,storage,and utilization in Chinese Academy of Sciences.Fuel(2011),doi:10.1016/j.fuel.2011.08.022157are composed entirely of ions with a melting point of less than 158100°C.ILs have many unique properties in comparison to other 159solvents as extremely low volatility,broad range of liquid temper-160ature,high thermal and chemical stability,and tunable physico-161chemical characteristics and as a result,ILs have been considered 162as a potential substitute of aqueous amine solutions for CO 2cap-163ture [31–34].164In Changchun Institute of Applied Chemistry,Chinese Academy 165of Sciences (CIAC–CAS),a novel dissolving process for chitin and 166chitosan was developed by using the ionic liquid 1-butyl-3-167methyl-imidazolium chloride ([Bmim]Cl)as a solvent for capturing 168and releasing CO 2.The results showed that the chitin/IL and chito-169170171172173174175176177178179180181182183184185186187188189190191192193194195196197198199200201tant to consider the maximum mass loading when considering the 202support of ILs on inert substrates –yes,these can enhance the ILs’203ability to take up CO 2,but at the expense of cycling an inert sorbent 204round a thermal cycle.The ILs are also monstrously expensive,the 205complex structure,and high cost for preparation,compared to sim-206pler solvents such as MEA or ammonia.Thus,the potential for 207improving CO 2solubilities and reducing cost of the ILs still needs 208to be studied for future applications.In 2010,in Beijing National 209Laboratory for Molecular,Chinese Academy of Sciences (BNLMS–210CAS),Zhang and co-workers first reported on CO 2capture by 211hydrocarbon surfactant liquids.It also found that CO 2had high sol-212ubility in low-cost hydrocarbon surfactant liquids,and the ab-213and the 214215216such as corrosion,at 217regenerable solid sor-218concept for CO 2recov-219into amine-based and 220221222with various so-223as silica gels,activated 224have been shown to phys-225enhance the sorp-226of many amine-based 227In Dalian Institute of 228(DICP–CAS),Zhang 229silica foam (MCF)materi-230with polyethyl-231The results showed that 232having large window 2333.45mmol CO 2/g sorbent 234In Institute of Coal Chem-235Zhao et al.studied 236materials derived 237sorption capabili-238°C and 1bar.The as-pre-239selectivity for CO 2over 240prepared a series of CO 2241pentamine (TEPA)was 242(PMHS)based mesopor-243The highest absorption 24475°C with the 10vol.%245was higher than most 246Desorption could 247in 1h [46].248of amine-based sorbent 249capacity of solid sorbent.250have poor mechanical 251amine-based sorbents 252and require signifi-253processes.254255sorbents for CO 2capture 256Alkali earth metal,such 257form alkali earth metal-258vapor at high tempera-259and post-combus-260simplified process flow 261the calcium looping 262vessel (the carbonator)4L.L Q1i et al./Fuel xxx (2011)xxx–xxxPlease cite this article in press as:L Q1i L et al.A review of research progress on CO 2capture,storage,and utilization in Chinese Academy of Sciences.Fuel(2011),doi:10.1016/j.fuel.2011.08.022the carbonation reaction between CO 2and solid CaO separates CO from coal-combustion flue gas at a temperature between 600°and 650°C.The CaCO 3formed is then passed to another vessel (the calciner),where it is heated to reverse the reaction (900–950°C),releasing the CO 2suitable for sequestration,and regener-ating the CaO-sorbent which is then return to the carbonator.The carbonation process is exothermic,which is matched with the temperature of a steam cycle,allowing recuperation of the heat.In IPE–CAS,the decomposition conditions of CaCO 3particles for CO 2capture in a steam dilution atmosphere (20–100%steam 307308309310311312313314315316317318319320321322323324325326327328329330332333334335336337338339340341342343344345346347348349350351352353354355Fig.3.The process flow diagram of post-combustion capture using the calcium looping cycle [47,48].Please cite this article in press as:L Q1i L et al.A review of research progress on CO 2capture,storage,and utilization in Chinese Academy of Sciences.Fuel(2011),doi:10.1016/j.fuel.2011.08.022strength (998N/cm 2)and exhibited good stability in multiple cy-cles [74,75].Furthermore,the application of a conceptual CO 2cap-ture process using this sorbent was proposed for an existing coal fired power plant [75].However,to optimize CO 2sorption capacity,understand of the interaction between CO 2and the sorbent need to be studied in the further work.Moreover,much work remains before the technology fluidized bed CO 2capture can be commercialized.Simulta-neously,the numerical simulation based on the computational fluid 365dynamics (CFD)method will become a research focus in the future.366 3.CO 2storage367Following the capture and transport process,CO 2can be dis-368posed of in natural sites such as deep geological sequestration,369mineral carbonation,or ocean storage [76].There are three geolog-370ical formations that have also been recognized as major potential 371CO 2sinks:deep saline-filled sedimentary (DSFs),depleted oil 372natural gas reservoirs,and unmineable coal-seams.The geology 373also suggests possibilities for CO 2enhanced oil recovery (CO 374EOR),CO 2enhanced gas recovery (CO 2–EGR)and CO 2enhanced 375coal-bed methane recovery (CO 2–ECBM)projects [12].3763.1.Geological sequestration377Geological storage involves injecting CO 2at depths greater than 3781000m into porous sedimentary formations using technologies 379derived from the oil and gas industry [77].CO 2can be stored in 380supercritical state at depth below 800–1000m,which provides 381the potential for efficient utilization of the space,due to the li-382quid-like density of supercritical CO 2.The point at which CO 2Table 2Performance summary of K-based sorbents capturing CO 2.Material Temperature (°C)CO 2partial pressure (bar)e Total capacity (mmol CO 2/g sorbent)Method f Regenerature temperature (°C)Ref.K 2CO 3/AC a 600.01 1.95TCD g 150[62]K 2CO 3/SiO 2600.010.23TCD g –[62]K 2CO 3/USY 600.010.43TCD g –[62]K 2CO 3/CsNaX 600.01 1.35TCD g –[62]K 2CO 3/Al 2O 3600.01 1.93TCD g 350[62]K 2CO 3/CaO 600.01 1.11TCD g –[62]K 2CO 3/MgO 600.01 2.70TCD g 400[62]K 2CO 3/TiO 2600.01 1.89TCD g 150[62]K 2CO 3/Al 2O 3600.01 1.96TCD g >300[63]Re-KAl(I)30b 600.01 1.86TCD g <200[63]g Fig.5.The schematic diagram of experimental apparatus for the fluidized bed [74,75].6L.L Q1i et al./Fuel xxx (2011)xxx–xxxPlease cite this article in press as:L Q1i L et al.A review of research progress on CO 2capture,storage,and utilization in Chinese Academy of Sciences.Fuel(2011),doi:10.1016/j.fuel.2011.08.022383transforms from critical to supercritical point is 31.1°C and 3847.38MPa [78].CO 2is injected usually in the supercritical form into 385the saline aquifer or depleted oil or gas reservoir.Four major clas-386ses of deep geologic reservoirs present within China have been 387identified and evaluated as candidates for the long-term storage 388of anthropogenic CO 2:deep saline-filled sedimentary (DSFs)for-389mations,depleted gas basins,depleted oil basins with potential 390for CO 2–EOR,and deep unmineable coal seams with potential for 391CO 2–ECBM.Fig.6shows the map of the combined location and ex-392tent of candidate geologic CO 2storage formations in China [13].393Because the CO 2industry is not mature,there are few active CO 2394storage projects which can provide site specific information;hence417China are also potential storage candidates.Recently,other re-418search has also focused on estimating the distance between CO 2419sources and potential sinks.Zheng et al.superimposed the loca-420tions of these 27facilities onto maps of sedimentary basins in each 421of the five regions of China (Huabei,Ordos,Dongbei,Yuwan,and 422Xinjiang).The majority of the candidate CO 2sources are found in 423the Ordos,Huabei and Dongbei regions [85].424The China–UK Near Zero Emissions Coal (NZEC)Initiative exam-425ined options for carbon (CO 2)capture,transport and geological 426storage in China,which was developed under the 2005EU–China 427NZEC Agreement that aims to demonstrate CCS in China and the 428EU [16,86–88].The NZEC Initiative has evaluated the potential to 429430431432433434435436437438439440441442443444445446447448449450451L.L Q1i et al./Fuel xxx (2011)xxx–xxx7Please cite this article in press as:L Q1i L et al.A review of research progress on CO 2capture,storage,and utilization in Chinese Academy of Sciences.Fuel(2011),doi:10.1016/j.fuel.2011.08.022452Kailuan mining area (Hebei Province)and deep saline aquifers in 453the Jiyang Depression (Shandong province)[89,90].The results 454show that the Dagang oilfield is not suitable for large-scale storage,455though could be considered for EOR pilots.The Shengli oilfield was 456considered more promising for storage (472Mt in eight selected 457fields).Storage potential in the Kailuan mining area is 504,000458Mt adsorbed onto the coal and 38,100Mt void storage capacity.459However,the coals have low porosity and permeability that will af-460fect future energy resources [90].The Institute of Geology and Geo-461physics,Chinese Academy of Sciences (IGG–CAS)studied the 462potential for storage in the Jiyang Depression.The results revealed 463that Guantao Formation in the Jiyang Depression has good porosity 464and permeability 465areas was 4662010,in South China 467of Sciences 468storage capacity in 469the Pearl River 470CCS-related 471China [78].There 472saline formations 473tive storage 474including 60Mt in 475large for storaging 476in Guangdong in 477In a word,these 478age of CO 2in deep 479Although this is 480countries,it will 481and there was 482characteristics.483 3.1.2.CO 2–EOR484Although CO 2485oil recovery (EOR)486this process can be 487oil,the cost of CO 2,488the CO 2source [92].489the production of 490be an ideal option 49184commercial or 492tion worldwide [1].493been implemented 494Oil Corporation 495in the Daqing,496ernments of Japan 497out a project to 498plant in China into a 499duced from the 500that between 270501ered by using CO 2502including IGG–CAS 503three large oil fields 504oil reservoirs in the 505were suitable both 506found suitable for 507showed that the 508CO 2storage 509the oil recovery by steam injection has been already applied at Lia-510ohe oil field.Each single well,in average,had conducted 7.6times 511of steam injection-oil recovery processing for EOR propose.The to-512tal recovered oil amounts were 12.06Mt [92].Active oil producing 513fields where CO 2–EOR is technically possible provide credible 514opportunities to initiate CO 2storage demonstration projects.How-515ever,significant further investigations,including detailed site516appraisals would be necessary before such fields can be considered 517as technically and economically suitable for CO 2storage.5183.1.3.CO 2–ECBM519In a similar manner,ECBM recovery can be used to store CO 2520while improving methane recovery.A bright prospect of gas injec-521tion technology for ECBM production has been suggested by Chi-522nese engineers since the late 1990s [94].More recently,a joint 523venture was formed between the China United Coal Bed Methane 524Corporation and the Alberta Research Council of Canada to develop 525a project entitled ‘‘Development of China’s coalbed methane tech-526nology/CO 2sequestration’’[12].This project was initiated in March 527project was performed 528in the anthracitic coals of 529China [95],which is 530in China up to now 531at ICC–CAS in 2005532were investigated based 533An equipment simulated 534middle pressures was 535in coal seam,536behaviors were studied.537coal mine and salt-water 538four coals of various rank 539China were tested for 540one of the most impor-541process.The result 542capacities for methane 543>Bulianta coal >Zhangji 544adsorption isotherms 545lattice model [100].546given to estimate the 547[101],which was 548underground stress is so 5492and CH 4respectively 550the mechanical sta-551of the impact factors of 552stress could be obviously 553of the casing or by using 554and Young’s modulus 555China was also estimated 556prospecting data of coal 557and the replacement ratio 558different ranks,it is esti-559methane resources will 560technology is uti-561in coalbeds is about 562as the total CO 2emission 563also developed 564simulation of the CO 2–565is a lack of knowledge 566due to the complexity 567fluid transport processes.568will be the next 569570571Large amounts of CO 2can also be fixed by a process called min-572eral carbonation,which is natural or artificial fixation of CO 2into 573carbonates.It has been proposed as a promising CO 2sequestration 574technology e.g.the silicate rocks (calcium or magnesium)could be 575turned into carbonates by reacting with CO 2following this mech-576anism [8,105]:577ðMg ;Ca Þx Si y O x þ2y þx CO 2!x ðMg ;Ca ÞCO 3þy SiO 25798L.L Q1i et al./Fuel xxx (2011)xxx–xxxPlease cite this article in press as:L Q1i L et al.A review of research progress on CO 2capture,storage,and utilization in Chinese Academy of Sciences.Fuel(2011),doi:10.1016/j.fuel.2011.08.022580581582583584585586587588589590591592593594595596597598599600601602603604605606607608609610611612613614615616617618619620621622623624625626627628629630631632633634635636637638639hanced by the fact that this method of storage is highly verifiable 640and unquestionably permanent,the grinding energy required to 641produce particles of the size required to react rapidly with the 642acids is large,and the residence times on the order of hours re-643quired to allow carbonation of the solids,via either route,is so long 644that immense reactors would be required,associating environmen-645tal concerns.Furthermore,mineral carbonation will always be646expensive than most applications of geological storage 647important gap in mineral carbonation is the lack of 648onstration plant.649Ocean storage650Captured CO 2also could help reduce the atmospheric 6516526536546556566576586596606616626636646656666676686696706716726736746756766776786796806816826836842685carbonic acid,which would be likely harmful to ocean organisms 686and ecosystems [17].Additionally,it is not known whether the 687public will accept the deliberate storage of CO 2in the ocean as part 688of a climate change mitigation strategy.The development of ocean 689storage technology is generally at a conceptual stage;thus,further 690research and development would be needed to make technologies 691available.3.Reaction mechanism for enhanced carbonation crystallization Q1Please cite this article in press as:L Q1i L et al.A review of research progress on CO 2capture,storage,and utilization in Chinese Academy of Sciences.Fuel(2011),doi:10.1016/j.fuel.2011.08.022692693694695696697698699700701702703704705706707708709710711712713714715716717718719721722723the reaction [131–135],such as in ICC–CAS,Zhao et al.had reported 724a catalyst system composed of KI supported on metal oxides for 725cycloaddition of propylene oxide with CO 2.It was found that the 726activity of KI for cycloaddition was greatly enhanced by ZnO as both 727support and promoter,resulting in a high yield of propylene 728carbonate within a short reaction time.The mechanism is also pro-729posed (Scheme 4)[133].Recently,a large number of catalytic730systems,such as metal oxides,transition metal,ammonium 731well as main group complexes,were reported to be active 732reactions [136–139].In ICC–CAS,the efficient ultrasonic tech-733nique was used for the preparation of amine-functionalized porous 734catalysts for CO 2coupling with epoxide.According to 735study by Zhang and co-workers [140],the reaction conditions 736great influence on the performance and the silanols on the surface 737played an important role in the chemical fixation of CO 2.In addi-738they also proposed the possible reaction mechanism for 739coupling with epoxide over such type of catalysts (Scheme 5).740In recent years,ionic liquids as environmentally benign media 741organic synthesis and catalytic reaction significant progress 7427437447457467477487492750catalyst system without using additional organic solvents was 751achieved in excellent selectivity and TOF (5410h À1)[144].In 752IPE–CAS,an efficient Lewis acid/base catalyst composed of ZnCl 2/753PPh 3C 6H 13Br was developed and showed high activity and selectiv-754ity for the coupling reaction of CO 2and epoxide under the mild 755conditions [145].Sun et al.prepared a series of hydroxyl-function-756alized ionic liquids (HFILs)which showed efficient reactivity andScheme 4.The proposed diagram of reaction mechanism [133].Q1Please cite this article in press as:L Q1i L et al.A review of research progress on CO 2capture,storage,and utilization in Chinese Academy of Sciences.Fuel(2011),doi:10.1016/j.fuel.2011.08.022780781782783784785786787788789790791792793794795796797798799800802803804805806807Please cite this article in press as:L Q1i L et al.A review of research progress on CO 2capture,storage,and utilization in Chinese Academy of Sciences.Fuel(2011),doi:10.1016/j.fuel.2011.08.022CO 2þCH 4¼2CO þ2H 2841842In the past decade,a lot of researches have been devoted to the 843catalytic performance of noble metals,including Pt,Ru,Rh,Pd,844and Ir for this reaction [165–169].It showed that Rh and Ru845exhibited both high activity and stability in CH 4dry reforming,846while Pd,Pt and Ir were less active and prone to deactivation.847Nevertheless,considering the aspects of high cost and limitedPlease cite this article in press as:L Q1i L et al.A review of research progress on CO 2capture,storage,and utilization in Chinese Academy of Sciences.Fuel(2011),doi:10.1016/j.fuel.2011.08.022848availability of noble metals,it is more practical to develop non-849noble metal catalysts which exhibited both high activity and pared with noble metals,Ni-based catalysts have been 851widely investigated because of their high activity and relatively 852low price [170–172].Nevertheless,application of Ni-based cata-853lysts in a large scale process is not so straightforward due to rapid 854carbon deposition,resulting in the deactivation of the catalyst 855[173].It was found that when Ni is supported on a alkaline earth 856metal oxide such as MgO,CaO,and BaO with strong Lewis basi-857city,carbon deposition can be attenuated or even suppressed 858[174]which is because that the support could promote chemi-859sorption of CO 2and thus,accelerated the reaction of CO 2and C 8608618628638648658668678688698708718728738748758768778788798808818828838848858868878888898908918928938948958968974.4.Reaction of CO 2with ethane and propane898Ethylene and propylene are basic raw material in the petrol-899chemical industry.Thermal cracking of hydrocarbons (such as eth-900ane)in the presence of steam is currently the main source of eth-901ylene [181,182].Nevertheless,steam cracking of ethane to 902ethylene is a highly endothermic process that must be performed 903at high temperatures,which means the consumption of a large 904amount of energy.The introduction of CO 2could reduce the extent 905of deep oxidation which results in many byproducts whereas eth-906ylene selectivity drops when oxygen is used as oxidant [183].907Thermodynamics analysis and experimental results have indi-908909910911912913915916917918919920921922923924925926927928929930931932933934935936938939940941L.L Q1i et al./Fuel xxx (2011)xxx–xxx13Please cite this article in press as:L Q1i L et al.A review of research progress on CO 2capture,storage,and utilization in Chinese Academy of Sciences.Fuel(2011),doi:10.1016/j.fuel.2011.08.022969970971972973974975976977978979980981982983984985986987988990991992993994995996997998999100010011002100310041005100610071008100910101011101210131014Please cite this article in press as:L Q1i L et al.A review of research progress on CO 2capture,storage,and utilization in Chinese Academy of Sciences.Fuel(2011),doi:10.1016/j.fuel.2011.08.0221015DMC in supercritical phase was proposed in Scheme 11.Recently,developed a supported Cu-Ni/V 2O 5-SiO 2heterogeneous because the reaction can be carried out in a fixed-bed the side production of water molecules 10341035103610371038103910401041104210431044and theoretical approaches,which enable the development of 1045CO 2selective sorbents.Besides,the sorbent performance,lifetime,10461047104810491050105110521053105410551056105710581059106010611062106310641065Scheme 11.The proposed catalytic reaction mechanism Please cite this article in press as:L Q1i L et al.A review of research progress on CO 2capture,storage,and utilization in Chinese Academy of Sciences.Fuel(2011),doi:10.1016/j.fuel.2011.08.0221066of component costs,specific Chinese market conditions,and other 1067factors impacting costs of deployment in China will be important 1068to consider in greater detail.To propose the storage mechanism,1069monitoring,simulation,risk assessment,control methods as well 1070as engineering design will be studied in future.1071The utilization of CO 2to chemicals has attracted considerable 1072attention as a possible way to manufacture useful commercial 1073chemicals from CO 2in some specific locations (Scheme 12)[222].1074The utilization of CO 2as a raw material in the synthesis of chemi-1075cals was also conducted by CAS,including synthesis of cyclic car-1076bonate from CO 2and epoxide,reaction of CO 2and propylene 1077glycol (PG),CO 2reforming of CH 4,reaction of CO 2and ethane 1078and propane,CO 21079methyl carbonate 1080amount of CO 2can 1081to the order of 1082ent the typical 1083cations is only 1084laminates are used 1085of the materials can 1086and overall net 1087ation.1088and fundamental 1089lue-added chemicals 1090tive net carbon 1091moderate reaction 1092the energy or 1093clear,wind,1094also important to 1095 6.Uncited 1096[201].Q31097Acknowledgments1098This work was 1099vation Programme 1100323);the Ministry of 1101lic of China 1102Climate Change:1103Academy of 1104the 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