CN104628508B - A kind of taking coal and natural gas as raw material is through system and the technique of synthesis gas alkene processed - Google Patents
A kind of taking coal and natural gas as raw material is through system and the technique of synthesis gas alkene processed Download PDFInfo
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- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 title claims abstract description 266
- 239000007789 gas Substances 0.000 title claims abstract description 234
- 238000003786 synthesis reaction Methods 0.000 title claims abstract description 159
- 230000015572 biosynthetic process Effects 0.000 title claims abstract description 157
- 150000001336 alkenes Chemical class 0.000 title claims abstract description 66
- 238000000034 method Methods 0.000 title claims abstract description 32
- 239000003345 natural gas Substances 0.000 title claims abstract description 20
- 239000002994 raw material Substances 0.000 title claims abstract description 20
- 239000003034 coal gas Substances 0.000 title claims abstract description 18
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 claims abstract description 151
- 239000003245 coal Substances 0.000 claims abstract description 101
- 229910002092 carbon dioxide Inorganic materials 0.000 claims abstract description 81
- 239000001569 carbon dioxide Substances 0.000 claims abstract description 72
- 238000002309 gasification Methods 0.000 claims abstract description 56
- 238000000926 separation method Methods 0.000 claims abstract description 47
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 34
- 239000003250 coal slurry Substances 0.000 claims abstract description 26
- 238000006243 chemical reaction Methods 0.000 claims abstract description 18
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 claims description 52
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 claims description 29
- 239000000203 mixture Substances 0.000 claims description 28
- 229910052799 carbon Inorganic materials 0.000 claims description 24
- QQONPFPTGQHPMA-UHFFFAOYSA-N propylene Natural products CC=C QQONPFPTGQHPMA-UHFFFAOYSA-N 0.000 claims description 22
- 125000004805 propylene group Chemical group [H]C([H])([H])C([H])([*:1])C([H])([H])[*:2] 0.000 claims description 22
- 238000002407 reforming Methods 0.000 claims description 21
- VGGSQFUCUMXWEO-UHFFFAOYSA-N Ethene Chemical compound C=C VGGSQFUCUMXWEO-UHFFFAOYSA-N 0.000 claims description 17
- 238000001035 drying Methods 0.000 claims description 17
- ATUOYWHBWRKTHZ-UHFFFAOYSA-N Propane Chemical compound CCC ATUOYWHBWRKTHZ-UHFFFAOYSA-N 0.000 claims description 16
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims description 16
- 239000001301 oxygen Substances 0.000 claims description 16
- 229910052760 oxygen Inorganic materials 0.000 claims description 16
- 229910052757 nitrogen Inorganic materials 0.000 claims description 15
- 238000010926 purge Methods 0.000 claims description 15
- 239000007788 liquid Substances 0.000 claims description 14
- 239000005977 Ethylene Substances 0.000 claims description 13
- 230000002194 synthesizing effect Effects 0.000 claims description 11
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 9
- 239000001294 propane Substances 0.000 claims description 9
- 238000000746 purification Methods 0.000 claims description 9
- 238000002156 mixing Methods 0.000 claims description 7
- OTMSDBZUPAUEDD-UHFFFAOYSA-N Ethane Chemical compound CC OTMSDBZUPAUEDD-UHFFFAOYSA-N 0.000 claims description 6
- UCKMPCXJQFINFW-UHFFFAOYSA-N Sulphide Chemical compound [S-2] UCKMPCXJQFINFW-UHFFFAOYSA-N 0.000 claims description 6
- 238000001816 cooling Methods 0.000 claims description 6
- 238000005406 washing Methods 0.000 claims description 5
- 241000628997 Flos Species 0.000 claims description 4
- 238000010438 heat treatment Methods 0.000 claims description 4
- 150000001298 alcohols Chemical class 0.000 claims description 3
- 239000002351 wastewater Substances 0.000 claims description 3
- 230000001186 cumulative effect Effects 0.000 claims description 2
- 239000001273 butane Substances 0.000 claims 1
- IJDNQMDRQITEOD-UHFFFAOYSA-N n-butane Chemical compound CCCC IJDNQMDRQITEOD-UHFFFAOYSA-N 0.000 claims 1
- OFBQJSOFQDEBGM-UHFFFAOYSA-N n-pentane Natural products CCCCC OFBQJSOFQDEBGM-UHFFFAOYSA-N 0.000 claims 1
- 238000006057 reforming reaction Methods 0.000 claims 1
- 239000000126 substance Substances 0.000 abstract description 2
- 230000008569 process Effects 0.000 description 11
- 239000004215 Carbon black (E152) Substances 0.000 description 10
- 229930195733 hydrocarbon Natural products 0.000 description 10
- JRZJOMJEPLMPRA-UHFFFAOYSA-N olefin Natural products CCCCCCCC=C JRZJOMJEPLMPRA-UHFFFAOYSA-N 0.000 description 10
- -1 olefin hydrocarbon Chemical class 0.000 description 10
- 238000005516 engineering process Methods 0.000 description 9
- 230000000052 comparative effect Effects 0.000 description 6
- 238000002360 preparation method Methods 0.000 description 5
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 description 4
- 238000010586 diagram Methods 0.000 description 3
- 239000001257 hydrogen Substances 0.000 description 3
- 229910052739 hydrogen Inorganic materials 0.000 description 3
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 2
- 238000013461 design Methods 0.000 description 2
- 150000002430 hydrocarbons Chemical class 0.000 description 2
- 238000011160 research Methods 0.000 description 2
- 230000004044 response Effects 0.000 description 2
- 239000002002 slurry Substances 0.000 description 2
- 239000004408 titanium dioxide Substances 0.000 description 2
- RWSOTUBLDIXVET-UHFFFAOYSA-N Dihydrogen sulfide Chemical compound S RWSOTUBLDIXVET-UHFFFAOYSA-N 0.000 description 1
- 241000790917 Dioxys <bee> Species 0.000 description 1
- LOTCVJJDZFMQGB-UHFFFAOYSA-N [N].[O].[S] Chemical compound [N].[O].[S] LOTCVJJDZFMQGB-UHFFFAOYSA-N 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 239000003054 catalyst Substances 0.000 description 1
- 230000008859 change Effects 0.000 description 1
- 239000012141 concentrate Substances 0.000 description 1
- 239000000470 constituent Substances 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 230000002950 deficient Effects 0.000 description 1
- 238000011161 development Methods 0.000 description 1
- 238000004821 distillation Methods 0.000 description 1
- 150000002431 hydrogen Chemical class 0.000 description 1
- 238000002372 labelling Methods 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 239000000463 material Substances 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 239000003921 oil Substances 0.000 description 1
- 210000000056 organ Anatomy 0.000 description 1
- 230000009467 reduction Effects 0.000 description 1
- 239000010117 shenhua Substances 0.000 description 1
- 238000004904 shortening Methods 0.000 description 1
- 239000007787 solid Substances 0.000 description 1
- 125000000383 tetramethylene group Chemical group [H]C([H])([*:1])C([H])([H])C([H])([H])C([H])([H])[*:2] 0.000 description 1
- 239000002918 waste heat Substances 0.000 description 1
- 239000002699 waste material Substances 0.000 description 1
Classifications
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- 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
- Y02P20/10—Process efficiency
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Abstract
The invention belongs to derived energy chemical technical field, disclose a kind of taking coal and natural gas as raw material is through system and the technique of synthesis gas alkene processed. Described system comprises that water-coal-slurry prepares unit, air gas separation unit, coal gasification unit, Water gas shift/WGS unit, purified synthesis gas unit, Fischer-Tropsch olefin unit processed and the dry reformer unit of methane, between purified synthesis gas unit and Fischer-Tropsch olefin unit processed, synthesis gas blender is set, this synthesizer blender can be integrated into the decontaminating syngas of purified synthesis gas unit and the methane dry weight of the dry reformer unit of methane sends into Fischer-Tropsch olefin unit processed after gas mixes; Methane blended device and carbon dioxide mix device are set before the dry reformer unit of methane, and the carbon dioxide that the methane that dry methane reformer unit can be generated and purified synthesis gas unit generate is sent into the dry reformer unit of methane and is participated in reaction. By system of the present invention and technique, can reach the effect that reduces CO2 emission, improves efficiency and minimizing investment in fixed assets.
Description
Technical field
The invention belongs to derived energy chemical technical field, be specifically related to a kind of taking coal and natural gas as raw material is through syntheticThe system of gas alkene processed and technique.
Background technology
Alkene is produced the plurality of raw materials routes such as oil, natural gas, coal and living beings, accounts for the raw material road of main flowLine is naphtha and natural gas, and wherein naphtha accounts for more than 50%. World oil reserves are fewer and feweri, and alkeneHydrocarbon disparities between supply and demand are particularly outstanding in emerging economy country, and development Non oil-based route alkene production technology is compeled at eyebrowEyelash. China is the country of a rich coal, oil-poor, weak breath, and large-scale olefin hydrocarbon making by coal project becomes that all circles pay close attention toFocus, exploitation has important strategic importance taking coal as raw material alkene processed.
Coal-based alkene mainly contains two kinds of paths, and the one, coal is through methanol-to-olefins; The 2nd, coal is through synthesis gas alkene processed.The former is industrial implementation, and Shenhua packet header olefin hydrocarbon making by coal has adopted DMTO technology, is the first cover in the whole world and successThe coal of commercial operation is through methanol-to-olefins industrialized unit. Coal is through existing 2,760,000 tons of methanol-to-olefins at presentOlefin hydrocarbon apparatus drops into commercialized running. For further shortening response path, reducing cost of investment, coal is through syntheticGas alkene processed becomes study hotspot in recent years. Research mainly concentrates on the exploitation of effective catalyst, in techniqueThe research of the aspect such as flow scheme design, design of new processes is relatively deficient.
Coal through methanol-to-olefins system mainly by water-coal-slurry prepare unit, air gas separation unit, coal gasification unit,Water coal converter unit, purified synthesis gas unit, methyl alcohol synthesis unit and methanol-to-olefins unit composition. FormerMaterial coal is mixed and made into water-coal-slurry with water after washing is ground, and water-coal-slurry enters coal gasification unit, with air separationThe oxygen that unit obtains is made synthesis gas through high-temperature gasification stove, and crude synthesis gas enters the adjustment of Water gas shift/WGS unitHydrogen-carbon ratio, enters afterwards purified synthesis gas unit and removes the sour gas such as sulfide and carbon dioxide in synthesis gasBody, clean synthesis gas through methanol synthesis unit synthesizing methanol, then through methanol-to-olefins unit synthesizing ethylene,Propylene and butylene. But there are two subject matters through methanol-to-olefins process in existing coal: the first, and olefin hydrocarbon making by coalProcess route length and flow process complexity; The second, the direct CO2 emission of olefin hydrocarbon making by coal process is up to 5-6t/t alkeneHydrocarbon. With coal compared with the methanol-to-olefins, although coal of the prior art has reduced methyl alcohol through synthesis gas alkene processedSynthesizer, has reduced investment, but its CO2 emission is still higher and efficiency is low, and its reason is coalThe hydrogen-carbon ratio of the crude synthesis gas that gasification produces is only 0.7:1 left and right, and the synthetic required hydrogen of alkene of Fischer-TropschCarbon ratio is 1:1～2:1, and therefore crude synthesis gas need enter water coal converter unit, and the CO in synthesis gas is converted into H2And CO2, secondly the synthetic olefin hydrocarbon of Fischer-Tropsch produces approximately 30% carbon dioxide product, has so just caused a large amount ofCO2Waste and the olefin yield of discharge and carbon are low.
In order to reduce olefin hydrocarbon making by coal CO2 emission and to improve efficiency, rich carbon resource and rich hydrogen resource alliance mistakeJourney is a feasible path. For example, coal and natural gas alliance methanol process processed, Energy Efficiency Ratio coal is produced separatelyMethanol process has improved five percentage points, and the net profit of process improves 1.4 times. Should in gas repositoryDevelopment of Coal and coal bed gas, casing-head gas or oven gas alliance alkene processed. But still there is no at present coal and natural gas allianceSynthesis gas is produced the related invention of alkene.
Summary of the invention
In order to solve the shortcoming and defect part of above prior art, primary and foremost purpose of the present invention is to provide oneKind taking coal and natural gas as raw material is through the system of synthesis gas alkene processed.
Another object of the present invention is to provide a kind of technique that adopts said system to prepare alkene.
The object of the invention is achieved through the following technical solutions:
Taking coal and natural gas as raw material is through a system for synthesis gas alkene processed, comprise water-coal-slurry prepare unit,Air gas separation unit, coal gasification unit, Water gas shift/WGS unit, purified synthesis gas unit, Fischer-Tropsch alkene processedThe dry reformer unit of unit and methane, arranges synthesis gas mixed between purified synthesis gas unit and Fischer-Tropsch olefin unit processedClose device, methane blended device and carbon dioxide mix device are set before the dry reformer unit of methane, water-coal-slurry is prepared unitFeed coal entrance and raw water entrance are set; Air gas separation unit arrange the outlet of air intake, nitrogen purge gas andPurified oxygen outlet, nitrogen purge gas outlet is connected to purified synthesis gas unit, and purified oxygen outlet is connected to coalGasification unit; Coal gasification unit arranges water-coal-slurry entrance and water-coal-slurry and prepares unit outlet and be connected; Water-gas becomesChanging unit arranges steam entry and exports with coal gasification unit the synthesis gas from coal gasification entrance being connected; Synthesis gasClean unit arranges conversion synthesis gas entrance, purification of carbon dioxide outlet, sulfide outlet and decontaminating syngasOutlet, conversion synthesis gas entrance is connected with the outlet of Water gas shift/WGS unit; Fischer-Tropsch olefin unit processed arranges mixingThe synthetic carbon dioxide outlet of synthesis gas entrance, unreacted synthesis gas outlet, the outlet of Fischer-Tropsch synthesizing methane and Fischer-Tropsch;The dry reformer unit of methane arranges mixing methane entrance, carbon dioxide entrance and methane dry weight and is integrated into gas outlet;Synthesis gas mixer entrance and decontaminating syngas outlet, methane dry weight are integrated into gas outlet and unreacted synthesis gasOutlet is connected, and its outlet is connected with mixed synthesis gas entrance; Methane blended device entrance and additional methane entrance andThe outlet of Fischer-Tropsch synthesizing methane is connected, and its outlet is connected with mixing methane entrance; Carbon dioxide mix device entrance withSynthetic carbon dioxide outlet is connected with Fischer-Tropsch in purification of carbon dioxide outlet, its outlet and carbon dioxide entrance and twoCarbonoxide evacuation port is connected.
Described Fischer-Tropsch olefin unit processed comprise First Heat Exchanger, Fischer-Tropsch synthesis device, carbon dioxide eliminating tower,Analytic Tower, drying tower, the first compressor, methane separation tower, gas-liquid separation tower, gasoline separation tower, de-fourthAlkane tower, the second compressor, domethanizing column, dethanizer, ethylene rectifying column and propylene rectification tower; First changesHot organ pipe journey entrance is connected with synthesis gas mixer outlet, and tube side outlet is connected with Fischer-Tropsch synthesis device entrance,Its shell side entrance is connected with the outlet of Fischer-Tropsch synthesis device, and shell side outlet is connected with gas-liquid separation tower entrance; GasLiquid knockout tower tower top outlet is connected with carbon dioxide eliminating tower entrance, tower reactor outlet and gasoline separation tower entrance phaseConnect, gasoline separation tower tower top arranges oil product outlet, and tower reactor arranges alcohols outlet; Carbon dioxide eliminating column overheadOutlet is connected with drying tower entrance, and tower reactor outlet is connected with Analytic Tower entrance; Analytic Tower tower top arranges Fischer-Tropsch and closesBecome carbon dioxide outlet to be connected with carbon dioxide mix device entrance, tower reactor arranges low-temp methanol outlet; Drying towerTower top outlet is connected with the first suction port of compressor, and tower reactor arranges wastewater outlet; The first compressor outlet and de-fourthAlkane tower entrance is connected, and debutanizing tower tower top outlet is connected with the second suction port of compressor, and tower reactor arranges carbon four mixingThing floss hole; The second compressor outlet is connected with domethanizing column entrance, and demethanizer column overhead outlet divides with methaneBe connected from tower entrance, tower reactor outlet is connected with dethanizer entrance; The synthetic first of Fischer-Tropsch of methane separation column overheadAlkane outlet is connected with methane blended device entrance, unreacted synthesis gas outlet and the synthesis gas mixer entrance of tower reactorBe connected; Deethanizer overhead outlet is connected with ethylene rectifying column entrance, tower reactor outlet and propylene rectification tower entranceBe connected; Ethylene distillation column overhead arranges ethene outlet, and tower reactor arranges ethane outlet, and propylene rectification tower tower top is establishedPut propylene outlet, tower reactor arranges propane outlet.
The dry reformer unit of described methane comprises the dry reforming reactor of methane, and the dry reforming reactor of methane arranges heat supplyChuck, this is connected for the entrance of thermal jacket and the outlet of coal gasification unit, for outlet and the coal gasification of thermal jacketSynthesis gas entrance connects.
Adopt said system to prepare a technique for alkene, comprise the following steps:
Feed coal is prepared and in unit, is mixed and made into water coal in water-coal-slurry with raw water after washing grinds to form coal dustSlurry; Air is divided into nitrogen purge gas and purified oxygen after air gas separation unit, and wherein nitrogen purge gas enters and closesBecome gas clean unit, purified oxygen enters coal gasification unit; Water-coal-slurry directly enters coal gasification unit and oxygenHigh-temperature gasification reaction makes synthesis gas from coal gasification; After described synthesis gas from coal gasification is the whole unit heating of methane dry weightEnter Water gas shift/WGS unit and adjust hydrogen-carbon ratio, the conversion synthesis gas obtaining enters purified synthesis gas unit and removesSulfide is purified the decontaminating syngas that carbon dioxide and hydrogen-carbon ratio are 1:1～2:1, and described decontaminating syngas is logicalPiping enters synthesis gas blender; The methane that additional methane and Fischer-Tropsch olefin unit processed generates is in methane blendedAfter mixing in device, pass into the dry reforming reactor of methane, purification of carbon dioxide and the Fischer-Tropsch system of purified synthesis gas unitThe carbon dioxide that olefin unit generates passes into the dry reforming reactor of methane after carbon dioxide mix device mixes; FirstAlkane and carbon dioxide react and obtain methane dry weight and be integrated into gas in the dry reforming reactor of methane, and methane dry weight is wholeSynthesis gas enters synthesis gas blender by pipeline; Decontaminating syngas, methane dry weight are integrated into gas and unreactedSynthesis gas is mixed to get the mixed synthesis gas that hydrogen-carbon ratio is 1:1～2:1, mixed synthesis gas in synthesis gas blenderPass into Fischer-Tropsch synthesis device and carry out Fischer-Tropsch synthesis, reacted product is through cooling and through gas-liquid separationTower separates the gas product and the oil product that obtain removing after oil product with gasoline separation tower, after gas product is cooled, enter twoCarbonoxide enters drying tower after removing tower and Analytic Tower carbon dioxide removal, removes moisture and obtain in drying towerDry gas product, described dry gas product, after overcompression is cooling, enters debutanizing tower separation and obtains towerThe C 4 mixture of top debutanization gas product and tower reactor, described debutanization gas product enters domethanizing column, tower topFor methane and unreacted synthesis gas, tower reactor is demethanation gas product; Methane and unreacted synthesis gas enter into firstAlkane knockout tower, obtains unreacted synthesis gas and enter Fischer-Tropsch synthesis device after synthesis gas blender mixes, de-Methane product gas enters into dethanizer, and tower top obtains deethanization gas product and enters into ethylene rectifying column and obtain secondAlkene and ethane, tower reactor obtains propane and propylene mixtures and enters into propylene rectification tower and obtain propylene and propane.
In above-mentioned preparation technology, described carbon dioxide mix device passes into the titanium dioxide in the dry reforming reactor of methaneCarbon is to mix 80% of rear carbon dioxide cumulative volume, and residue 20% is emptying.
In above-mentioned preparation technology, described feed coal 10 is (0.5～1) with the charging mass ratio of additional methane 30:1; Preferably 0.68:1.
In above-mentioned preparation technology, in described coal gasification unit, the condition of high-temperature gasification reaction is: temperature is 1200～1500 DEG C, pressure is 2.8～3.2Mpa; Preferably temperature is 1350 DEG C, and pressure is 3.0Mpa.
In above-mentioned preparation technology, the temperature of described Fischer-Tropsch synthesis is 300～450 DEG C, and pressure is 2.0～3.0Mpa; Preferable reaction temperature is 350 DEG C, pressure 2.5Mpa.
In above-mentioned preparation technology, the condition of reacting in described dry reforming reactor is: temperature is 650～900 DEG C, pressure is 0.5～1.5Mpa; Preferably temperature is 750 DEG C, and pressure is 1.0Mpa.
System of the present invention and technique tool have the following advantages and beneficial effect:
(1) the present invention proposes a kind of coal through directly technique and the system of alkene processed of synthesis gas, compared to traditionCoal through methanol-to-olefins process, the present invention has shortened response path, has effectively reduced equipment investment;
(2) system of the present invention and technique can be integrated into the methane dry weight of the dry reformer unit of methane gas with syntheticThe decontaminating syngas that gas clean unit generates mixes, and adjusts the hydrogen-carbon ratio of synthesis gas to meeting the synthetic alkene of Fischer-TropschRequirement, then synthetic alkene in Fischer-Tropsch olefin unit processed, easy and simple to handle, saves the energy;
(3) by the whole effective CO2 emission having reduced in olefin hydrocarbon making by coal process of methane dry weight, the present inventionCan reduce the CO of existing olefin hydrocarbon making by coal process approximately 80%2Discharge capacity;
(4) synthesis gas of the integrated different material of the present invention is prepared unit, the sensible heat that utilizes coal gasification unit to dischargeFor methane reforming unit heating, the efficiency of coal and natural gas alliance synthesis gas olefin hydrocarbon processed can reach 49.3%,Compare coal through methanol-to-olefins process, efficiency has improved approximately 13 percentage points.
Brief description of the drawings
Fig. 1 be embodiment 1 taking coal and natural gas as raw material through the component units of synthesis gas alkene system processed andAnnexation schematic diagram;
Fig. 2 is composition and the annexation schematic diagram of the Fischer-Tropsch olefin unit processed of embodiment 1;
Fig. 3 is that comparative example 1 a kind of is taking coal as raw material through the component units of methanol-to-olefins system and connect and closeIt is schematic diagram;
Figure labeling description is as follows: 1-water-coal-slurry prepare unit, 2-air gas separation unit, 3-coal gasification unit,4-Water gas shift/WGS unit, 5-purified synthesis gas unit, 6-Fischer-Tropsch olefin unit processed, the dry reformer unit of 7-methane,8-synthesis gas blender, 9-methane blended device, 10-carbon dioxide mix device, 11-feed coal entrance, 12-raw materialWater inlet, 13-air intake, the outlet of 14-nitrogen purge gas, the outlet of 15-purified oxygen, 16-water-coal-slurry entrance,17-steam entry, 18-synthesis gas from coal gasification entrance, 19-conversion synthesis gas entrance, 20-purification of carbon dioxideOutlet, the outlet of 21-sulfide, the outlet of 22-decontaminating syngas, 23-mixed synthesis gas entrance, 24-unreacted closeBecome gas outlet, the outlet of 25-Fischer-Tropsch synthesizing methane, the synthetic carbon dioxide outlet of 26-Fischer-Tropsch, 27-mixing methane to enterMouth, 28-carbon dioxide entrance, 29-methane dry weight are integrated into gas outlet, the additional methane entrance of 30-, 31-dioxyChange carbon evacuation port, 32-First Heat Exchanger, 33-Fischer-Tropsch synthesis device, 34-carbon dioxide eliminating tower, 35-solutionAnalysing tower, 36-drying tower, 37-the first compressor, 38-methane separation tower, 39-gas-liquid separation tower, 40-gasoline dividesFrom tower, 41-debutanizing tower, 42-the second compressor, 43-domethanizing column, 44-dethanizer, 45-ethylene distillationTower, 46-propylene rectification tower, 47-Fischer-Tropsch synthesis device entrance, the outlet of 48-Fischer-Tropsch synthesis device, 49-gasLiquid knockout tower entrance, 50-gas-liquid separation tower tower top outlet, the outlet of 51-gas-liquid separation tower tower reactor, 52-oil product go outMouth, the outlet of 53-alcohols, 54-carbon dioxide eliminating column overhead export, 55-carbon dioxide eliminating tower tower reactor exports,The outlet of 56-low-temp methanol, 57-drying tower tower top outlet, 58-wastewater outlet, 59-debutanizing tower entrance, 60-Debutanizing tower tower top outlet, 61-C 4 mixture floss hole, 62-domethanizing column entrance, 63-demethanizerEject mouthful, the outlet of 64-domethanizing column tower reactor, the outlet of 65-deethanizer overhead, the outlet of 66-dethanizer tower reactor,The outlet of 67-ethene, the outlet of 68-ethane, the outlet of 69-propylene, the outlet of 70-propane, the dry reforming reactor of 71-methane,72-heat supply JI, 73-heat supply JO, 74-methyl alcohol synthesis unit, 75-methanol-to-olefins unit.
Detailed description of the invention
Below in conjunction with embodiment and accompanying drawing, the present invention is described in further detail, but enforcement side of the present inventionFormula is not limited to this.
Embodiment 1
Taking coal and natural gas as raw material is through a system for synthesis gas alkene processed, as shown in Figure 1, comprise water coalIt is clean that slurry is prepared unit 1, air gas separation unit 2, coal gasification unit 3, Water gas shift/WGS unit 4, synthesis gasChange unit 5, Fischer-Tropsch olefin unit 6 processed and the dry reformer unit 7 of methane, purified synthesis gas unit and Fischer-Tropsch alkene processedSynthesis gas blender 8 is set between hydrocarbon unit, before the dry reformer unit of methane, methane blended device 9 and titanium dioxide is setCarbon blender 10, water-coal-slurry is prepared unit feed coal entrance 11 and raw water entrance 12 is set; Air separationUnit arranges air intake 13, nitrogen purge gas outlet 14 and purified oxygen outlet 15, and nitrogen purge gas outlet connectsReceive purified synthesis gas unit, purified oxygen outlet is connected to coal gasification unit; Coal gasification unit arranges water coalSlurry entrance 16 is prepared unit outlet with water-coal-slurry and is connected; Water gas shift/WGS unit arrange steam entry 17 andExport with coal gasification unit the synthesis gas from coal gasification entrance 18 being connected; It is synthetic that purified synthesis gas unit arranges conversionGas entrance 19, purification of carbon dioxide outlet 20, sulfide outlet 21 and decontaminating syngas outlet 22, conversionSynthesis gas entrance is connected with the outlet of Water gas shift/WGS unit; Fischer-Tropsch olefin unit processed arranges mixed synthesis gas entrance23, the synthetic carbon dioxide outlet 26 of unreacted synthesis gas outlet 24, the outlet 25 of Fischer-Tropsch synthesizing methane and Fischer-Tropsch;The dry reformer unit of methane arranges and mixes methane entrance 27, carbon dioxide entrance 28 and methane dry weight and be integrated into gas and go outMouth 29; Synthesis gas mixer entrance and decontaminating syngas outlet, methane dry weight are integrated into gas outlet and unreactedSyngas outlet is connected, and its outlet is connected with mixed synthesis gas entrance; Methane blended device entrance and additional methaneOutlet is connected entrance 30 with Fischer-Tropsch synthesizing methane, and its outlet is connected with mixing methane entrance; Carbon dioxide mixDevice entrance is connected with the synthetic carbon dioxide outlet of purification of carbon dioxide outlet and Fischer-Tropsch, its outlet and carbon dioxideEntrance is connected with carbon dioxide evacuation port 31;
The composition of described Fischer-Tropsch olefin unit processed and annexation as shown in Figure 2, comprise First Heat Exchanger 32,Fischer-Tropsch synthesis device 33, carbon dioxide eliminating tower 34, Analytic Tower 35, drying tower 36, the first compressor37, methane separation tower 38, gas-liquid separation tower 39, gasoline separation tower 40, debutanizing tower 41, the second compressionMachine 42, domethanizing column 43, dethanizer 44, ethylene rectifying column 45 and propylene rectification tower 46; The first heat exchangeThe tube side entrance of device is connected with synthesis gas mixer outlet, and tube side outlet connects with Fischer-Tropsch synthesis device entrance 47Connect, its shell side entrance is connected with Fischer-Tropsch synthesis device outlet 48, shell side outlet and gas-liquid separation tower entrance 49Be connected; Gas-liquid separation tower tower top outlet 50 is connected with carbon dioxide eliminating tower entrance, tower reactor outlet 51 and vapourOil knockout tower entrance is connected, and gasoline separation tower tower top arranges oil product outlet 52, and tower reactor arranges alcohols outlet 53;Carbon dioxide eliminating column overhead outlet 54 is connected with drying tower entrance, tower reactor outlet 55 and Analytic Tower entrance phaseConnect; Analytic Tower tower top arranges the synthetic carbon dioxide outlet of Fischer-Tropsch and is connected with carbon dioxide mix device entrance, tower reactorLow-temp methanol outlet 56 is set; Drying tower tower top outlet 57 is connected with the first suction port of compressor, and tower reactor arranges uselessWater out 58; The first compressor outlet is connected with debutanizing tower entrance 59, debutanizing tower tower top outlet 60 withThe second suction port of compressor is connected, and tower reactor arranges C 4 mixture floss hole 61; The second compressor outlet and piptonychiaAlkane tower entrance 62 is connected, and demethanizer column overhead outlet 63 is connected with methane separation tower entrance, tower reactor outlet 64Be connected with dethanizer entrance; The outlet of Fischer-Tropsch synthesizing methane and the methane blended device entrance of methane separation column overheadBe connected, the unreacted synthesis gas outlet of tower reactor is connected with synthesis gas mixer entrance; Deethanizer overhead outlet65 are connected with ethylene rectifying column entrance, and tower reactor outlet 66 is connected with propylene rectification tower entrance; Ethylene rectifying column towerTop arranges ethene outlet 67, and tower reactor arranges ethane outlet 68, and propylene rectification tower tower top arranges propylene outlet 69,Tower reactor arranges propane outlet 70; The dry reformer unit of described methane comprises the dry reforming reactor 71 of methane, and methane is dryReforming reactor arranges for thermal jacket, and this entrance 72 for thermal jacket is connected with the outlet of coal gasification unit, suppliesThe outlet 73 of thermal jacket is connected with synthesis gas from coal gasification entrance.
Adopt said system to prepare a technique for alkene, be specifically implemented as follows:
The feed coal flow that enters technique of the present invention is 250t/h, and additional methane flow is 365t/h, feed coalThan being 0.68:1, the constituent of feed coal is in table 1 with additional methane feed.
The composition of table 1 feed coal
| Composition | Lime-ash | Carbon | Hydrogen | Nitrogen | Sulphur | Oxygen |
| Mass fraction % | 7.53 | 73.64 | 5.24 | 1.13 | 2.63 | 9.83 |
Feed coal is prepared and in unit, is mixed and made into water coal in water-coal-slurry with raw water after washing grinds to form coal dustSlurry; Air is divided into nitrogen purge gas and purified oxygen after air gas separation unit, and wherein nitrogen purge gas enters and closesBecome gas clean unit, purified oxygen enters coal gasification unit; Water-coal-slurry directly enters coal gasification unit and oxygenBe 1350 DEG C in temperature, pressure be under 3.0Mpa condition high-temperature gasification reaction to make temperature be the height of 1350 DEG CTemperature synthesis gas from coal gasification; Described synthesis gas from coal gasification enters from the heat supply JI of dry reforming reactor, forAfter the whole unit heating of methane dry weight, temperature is reduced to 500 DEG C, enters from entering waste heat boiler for the outlet of thermal jacketOne step reclaims after heat, enters Water gas shift/WGS unit and adjusts hydrogen-carbon ratio, and the conversion synthesis gas obtaining enters and closesBecome gas clean unit to remove sulfide and be purified the decontaminating syngas that carbon dioxide and hydrogen-carbon ratio are 1:1, described inDecontaminating syngas enters synthesis gas blender by pipeline; The first that additional methane and Fischer-Tropsch olefin unit processed generatesAlkane passes into the dry reforming reactor of methane after mixing in methane blended device, the purification dioxy of purified synthesis gas unitChange carbon and mix in carbon dioxide mix device with the carbon dioxide that Fischer-Tropsch olefin unit processed generates, by 80% volumeMixed carbon dioxide passes into the dry reforming reactor of methane, and other 20% is emptying by carbon dioxide evacuation port;Methane and carbon dioxide reacts and obtains methane dry weight and be integrated into gas, methane dry weight in the dry reforming reactor of methaneOperation temperature in whole reactor is 750 DEG C, pressure 1.0MPa, and methane dry weight is integrated into gas by pipeRoad enters synthesis gas blender; Decontaminating syngas, methane dry weight are integrated into gas and unreacted synthesis gas is synthesizingIn gas blender, be mixed to get the mixed synthesis gas that hydrogen-carbon ratio is 1:1, mixed synthesis gas passed into Fischer-Tropsch synthetic anti-Answering device is to carry out Fischer-Tropsch synthesis, reacted product under 350 DEG C and the pressure condition that is 2.5MPa in temperatureThing is through cooling and separate the product G&O that obtains removing after oil product with gasoline separation tower through gas-liquid separation towerProduct, gas product enters carbon dioxide eliminating tower and Analytic Tower after being cooled to-21 DEG C, in Analytic Tower tower reactorAfter the low-temp methanol absorbing and removing carbon dioxide of-50 DEG C, enter drying tower, in drying tower, remove moisture and doneDry gas product, described dry gas product is cooled to 12 DEG C and 2.1Mpa by the first compressor compresses, entersDebutanizing tower separates the C 4 mixture that obtains tower top debutanization gas product and tower reactor, described debutanization gas productBe cooled to enter domethanizing column after 3Mpa and-100 DEG C by the second compressor compresses, tower top is methane and not anti-Answer synthesis gas, tower reactor is demethanation gas product; Methane and unreacted synthesis gas enter into methane separation tower,After synthesis gas blender mixes, enter Fischer-Tropsch synthesis device to unreacted synthesis gas, demethanation gas product entersEnter to dethanizer, tower top obtains deethanization gas product and enters into ethylene rectifying column and obtain ethene and ethane, towerStill obtains propane and propylene mixtures and enters into propylene rectification tower and obtain propylene and propane.
Comparative example 1
This comparative example a kind of through the system of methanol-to-olefins, as shown in Figure 3, comprises water coal taking coal as raw materialIt is clean that slurry is prepared unit 1, air gas separation unit 2, coal gasification unit 3, Water gas shift/WGS unit 4, synthesis gasChange unit 5, methyl alcohol synthesis unit 74 and methanol-to-olefins unit 75; Water-coal-slurry is prepared unit, air separationThe annexation of unit, coal gasification unit, Water gas shift/WGS unit and purified synthesis gas unit and embodiment 1Identical, the decontaminating syngas outlet 22 of purified synthesis gas unit is connected with methyl alcohol synthesis unit entrance, and methyl alcohol closesBecome unit outlet to be connected with methanol-to-olefins unit entrance.
Adopt the technique of preparing alkene taking coal as raw material through methanol-to-olefins system of this comparative example, concreteBe implemented as follows:
Feed coal is prepared and in unit, is mixed and made into water coal in water-coal-slurry with raw water after washing grinds to form coal dustSlurry; Air is divided into nitrogen purge gas and purified oxygen after air gas separation unit, and wherein nitrogen purge gas enters and closesBecome gas clean unit, purified oxygen enters coal gasification unit; Water-coal-slurry directly enters coal gasification unit and oxygenBe 1350 DEG C in temperature, pressure be under 3.0Mpa condition high-temperature gasification reaction to make temperature be the height of 1350 DEG CTemperature synthesis gas from coal gasification; After the cooling of high-temperature coal gasification synthesis gas, enter Water gas shift/WGS unit and adjust hydrogen-carbon ratio,The conversion synthesis gas obtaining enters purified synthesis gas unit and removes sulfide and be purified carbon dioxide and hydrogen-carbon ratioFor the decontaminating syngas of 1:1, described decontaminating syngas enters methyl alcohol synthesis unit synthesizing methanol by pipeline, closesThe methyl alcohol becoming enters methanol-to-olefins unit and catalyzes and synthesizes and obtain ethene and propylene.
CO2 emission, efficiency and the investment in fixed assets of embodiment 1 and comparative example 1 unit's of producing alkeneContrast is in table 1.
CO2 emission, efficiency and the fixed assets contrast of table 1 unit alkene
| CO2 emission | Efficiency | Investment in fixed assets | |
| Embodiment 1 | 1.2t/t | 49.3％ | 70％ |
| Comparative example 1 | 5.8t/t | 36.3％ | 100％ |
Can be found out by table 1 result: of the present inventionly taking coal and natural gas as raw material through synthesis gas alkene processed beSystem and technique and coal compared with the methanol-to-olefins technology, carbon dioxide emission reduction 80% left and right; Efficiency improves13 percentage points; Compared with the methanol-to-olefins, owing to having reduced methanol synthesizer, unit alkene is solid with coalDetermine assets investment and reduce approximately 30%.
Above-described embodiment is preferably embodiment of the present invention, but embodiments of the present invention are not subject to above-mentioned realityExecute routine restriction, other any do not deviate from the change done under Spirit Essence of the present invention and principle, modification,Substitute, combine, simplify, all should be equivalent substitute mode, within being included in protection scope of the present invention.
Claims (6)
1. a technique for alkene is prepared in employing through the system of synthesis gas alkene processed taking coal and natural gas as raw material,It is characterized in that:
Described system comprises that water-coal-slurry prepares unit, air gas separation unit, coal gasification unit, Water gas shift/WGSUnit, purified synthesis gas unit, Fischer-Tropsch olefin unit processed and the dry reformer unit of methane, purified synthesis gas unitAnd between Fischer-Tropsch olefin unit processed, synthesis gas blender is set, before the dry reformer unit of methane, methane blended device is setWith carbon dioxide mix device, water-coal-slurry is prepared unit feed coal entrance and raw water entrance is set; Air separationUnit arranges air intake, nitrogen purge gas outlet and purified oxygen outlet, and nitrogen purge gas outlet is connected to syntheticGas clean unit, purified oxygen outlet is connected to coal gasification unit; Coal gasification unit arrange water-coal-slurry entrance withWater-coal-slurry is prepared unit outlet and is connected; Water gas shift/WGS unit arranges steam entry and goes out with coal gasification unitThe synthesis gas from coal gasification entrance that mouth is connected; Purified synthesis gas unit arranges conversion synthesis gas entrance, purifies dioxyChange carbon outlet, sulfide outlet and decontaminating syngas outlet, conversion synthesis gas entrance and Water gas shift/WGS unitOutlet is connected; Fischer-Tropsch olefin unit processed arranges the outlet of mixed synthesis gas entrance, unreacted synthesis gas, Fischer-Tropsch closesBecome the synthetic carbon dioxide outlet of methane outlet and Fischer-Tropsch; The dry reformer unit of methane arranges and mixes methane entrance, twoCarbonoxide entrance and methane dry weight are integrated into gas outlet; Synthesis gas mixer entrance and decontaminating syngas outlet,Methane dry weight is integrated into gas outlet, and outlet is connected with unreacted synthesis gas, its outlet and mixed synthesis gas entrance phaseConnect; Outlet is connected methane blended device entrance with Fischer-Tropsch synthesizing methane with additional methane entrance, and it exports and mixesMethane entrance is connected; Carbon dioxide mix device entrance and purification of carbon dioxide outlet and the synthetic carbon dioxide of Fischer-TropschOutlet is connected, and its outlet is connected with carbon dioxide evacuation port with carbon dioxide entrance; Described Fischer-Tropsch alkene list processedUnit comprises First Heat Exchanger, Fischer-Tropsch synthesis device, carbon dioxide eliminating tower, Analytic Tower, drying tower,One compressor, methane separation tower, gas-liquid separation tower, gasoline separation tower, debutanizing tower, the second compressor,Domethanizing column, dethanizer, ethylene rectifying column and propylene rectification tower; First Heat Exchanger tube side entrance is with syntheticGas mixer outlet connects, and tube side outlet is connected with Fischer-Tropsch synthesis device entrance, its shell side entrance and Fischer-TropschSynthesis reactor outlet connects, and shell side outlet is connected with gas-liquid separation tower entrance; Gas-liquid separation tower tower top outletBe connected with carbon dioxide eliminating tower entrance, tower reactor outlet is connected with gasoline separation tower entrance, gasoline separation tower towerTop arranges oil product outlet, and tower reactor arranges alcohols outlet; The outlet of carbon dioxide eliminating column overhead and drying tower entranceBe connected, tower reactor outlet is connected with Analytic Tower entrance; Analytic Tower tower top arrange the synthetic carbon dioxide outlet of Fischer-Tropsch withCarbon dioxide mix device entrance is connected, and tower reactor arranges low-temp methanol outlet; Drying tower tower top outlet and first is pressedContracting machine entrance is connected, and tower reactor arranges wastewater outlet; The first compressor outlet is connected with debutanizing tower entrance, de-The outlet of butane column overhead is connected with the second suction port of compressor, and tower reactor arranges C 4 mixture floss hole; Second pressesThe outlet of contracting machine is connected with domethanizing column entrance, and demethanizer column overhead outlet is connected with methane separation tower entrance, towerStill outlet is connected with dethanizer entrance; The outlet of Fischer-Tropsch synthesizing methane and the methane blended of methane separation column overheadDevice entrance is connected, and the unreacted synthesis gas outlet of tower reactor is connected with synthesis gas mixer entrance; Dethanizer towerEject mouth and be connected with ethylene rectifying column entrance, tower reactor outlet is connected with propylene rectification tower entrance; Ethylene rectifying columnTower top arranges ethene outlet, and tower reactor arranges ethane outlet, and propylene rectification tower tower top arranges propylene outlet, tower reactorPropane outlet is set; The dry reformer unit of described methane comprises the dry reforming reactor of methane, and methane is done reforming reactionDevice arranges for thermal jacket, and this is connected for the entrance of thermal jacket and the outlet of coal gasification unit, for going out of thermal jacketMouth is connected with synthesis gas from coal gasification entrance;
The described technique of preparing alkene comprises the following steps:
Feed coal is prepared and in unit, is mixed and made into water coal in water-coal-slurry with raw water after washing grinds to form coal dustSlurry; Air is divided into nitrogen purge gas and purified oxygen after air gas separation unit, and wherein nitrogen purge gas enters and closesBecome gas clean unit, purified oxygen enters coal gasification unit; Water-coal-slurry directly enters coal gasification unit and oxygenHigh-temperature gasification reaction makes synthesis gas from coal gasification; After described synthesis gas from coal gasification is the whole unit heating of methane dry weightEnter Water gas shift/WGS unit and adjust hydrogen-carbon ratio, the conversion synthesis gas obtaining enters purified synthesis gas unit and removesSulfide is purified the decontaminating syngas that carbon dioxide and hydrogen-carbon ratio are 1:1～2:1, and described decontaminating syngas is logicalPiping enters synthesis gas blender; The methane that additional methane and Fischer-Tropsch olefin unit processed generates is in methane blendedAfter mixing in device, pass into the dry reforming reactor of methane, purification of carbon dioxide and the Fischer-Tropsch system of purified synthesis gas unitThe carbon dioxide that olefin unit generates passes into the dry reforming reactor of methane after carbon dioxide mix device mixes; FirstAlkane and carbon dioxide react and obtain methane dry weight and be integrated into gas in the dry reforming reactor of methane, and methane dry weight is wholeSynthesis gas enters synthesis gas blender by pipeline; Decontaminating syngas, methane dry weight are integrated into gas and unreactedSynthesis gas is mixed to get the mixed synthesis gas that hydrogen-carbon ratio is 1:1～2:1, mixed synthesis gas in synthesis gas blenderPass into Fischer-Tropsch synthesis device and carry out Fischer-Tropsch synthesis, reacted product is through cooling and through gas-liquid separationTower separates the gas product and the oil product that obtain removing after oil product with gasoline separation tower, after gas product is cooled, enter twoCarbonoxide enters drying tower after removing tower and Analytic Tower carbon dioxide removal, removes moisture and obtain in drying towerDry gas product, described dry gas product, after overcompression is cooling, enters debutanizing tower separation and obtains towerThe C 4 mixture of top debutanization gas product and tower reactor, described debutanization gas product enters domethanizing column, tower topFor methane and unreacted synthesis gas, tower reactor is demethanation gas product; Methane and unreacted synthesis gas enter into firstAlkane knockout tower, obtains unreacted synthesis gas and enter Fischer-Tropsch synthesis device after synthesis gas blender mixes, de-Methane product gas enters into dethanizer, and tower top obtains deethanization gas product and enters into ethylene rectifying column and obtain secondAlkene and ethane, tower reactor obtains propane and propylene mixtures and enters into propylene rectification tower and obtain propylene and propane.
2. according to claim 1ly a kind ofly adopt taking coal and natural gas as raw material through synthesis gas alkene processedSystem is prepared the technique of alkene, it is characterized in that: described carbon dioxide mix device passes into the dry reforming reaction of methaneCarbon dioxide in device is to mix 80% of rear carbon dioxide cumulative volume, and residue 20% is emptying.
3. according to claim 1ly a kind ofly adopt taking coal and natural gas as raw material through synthesis gas alkene processedSystem is prepared the technique of alkene, it is characterized in that: the charging mass ratio of described feed coal and additional methane is(0.5～1)：1。
4. according to claim 3ly a kind ofly adopt taking coal and natural gas as raw material through synthesis gas alkene processedSystem is prepared the technique of alkene, it is characterized in that: the charging mass ratio of described feed coal and additional methane is 0.68:1。
5. according to claim 1ly a kind ofly adopt taking coal and natural gas as raw material through synthesis gas alkene processedSystem is prepared the technique of alkene, it is characterized in that: in described coal gasification unit, the condition of high-temperature gasification reaction is:Temperature is 1200～1500 DEG C, and pressure is 2.8～3.2MPa; The temperature of described Fischer-Tropsch synthesis is300～450 DEG C, pressure is 2.0～3.0MPa; The condition of reacting in described dry reforming reactor is: temperatureBe 650～900 DEG C, pressure is 0.5～1.5MPa.
6. according to claim 5ly a kind ofly adopt taking coal and natural gas as raw material through synthesis gas alkene processedSystem is prepared the technique of alkene, it is characterized in that: in described coal gasification unit, the condition of high-temperature gasification reaction is:Temperature is 1350 DEG C, and pressure is 3.0MPa; The temperature of described Fischer-Tropsch synthesis is 350 DEG C, and pressure is2.5MPa; The condition of reacting in described dry reforming reactor is: temperature is 750 DEG C, and pressure is 1.0MPa.
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