CN101861198B - 用于捕获和螯合气体及其衍生组分的***和方法 - Google Patents
用于捕获和螯合气体及其衍生组分的***和方法 Download PDFInfo
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- CN101861198B CN101861198B CN2008801161840A CN200880116184A CN101861198B CN 101861198 B CN101861198 B CN 101861198B CN 2008801161840 A CN2008801161840 A CN 2008801161840A CN 200880116184 A CN200880116184 A CN 200880116184A CN 101861198 B CN101861198 B CN 101861198B
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- 229910052707 ruthenium Inorganic materials 0.000 description 1
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- 229910052706 scandium Inorganic materials 0.000 description 1
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- 238000005201 scrubbing Methods 0.000 description 1
- 239000004065 semiconductor Substances 0.000 description 1
- 229910052851 sillimanite Inorganic materials 0.000 description 1
- 229910052709 silver Inorganic materials 0.000 description 1
- 239000004332 silver Substances 0.000 description 1
- 229910001923 silver oxide Inorganic materials 0.000 description 1
- 238000004088 simulation Methods 0.000 description 1
- 239000002893 slag Substances 0.000 description 1
- 238000007582 slurry-cast process Methods 0.000 description 1
- 235000011121 sodium hydroxide Nutrition 0.000 description 1
- 235000019795 sodium metasilicate Nutrition 0.000 description 1
- NTHWMYGWWRZVTN-UHFFFAOYSA-N sodium silicate Chemical compound [Na+].[Na+].[O-][Si]([O-])=O NTHWMYGWWRZVTN-UHFFFAOYSA-N 0.000 description 1
- 229910052911 sodium silicate Inorganic materials 0.000 description 1
- 238000001778 solid-state sintering Methods 0.000 description 1
- 239000002904 solvent Substances 0.000 description 1
- 229910052596 spinel Inorganic materials 0.000 description 1
- 239000011029 spinel Substances 0.000 description 1
- 238000010561 standard procedure Methods 0.000 description 1
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- 238000006467 substitution reaction Methods 0.000 description 1
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- YTZVWGRNMGHDJE-UHFFFAOYSA-N tetralithium;silicate Chemical compound [Li+].[Li+].[Li+].[Li+].[O-][Si]([O-])([O-])[O-] YTZVWGRNMGHDJE-UHFFFAOYSA-N 0.000 description 1
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- 238000010792 warming Methods 0.000 description 1
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- UGZADUVQMDAIAO-UHFFFAOYSA-L zinc hydroxide Chemical compound [OH-].[OH-].[Zn+2] UGZADUVQMDAIAO-UHFFFAOYSA-L 0.000 description 1
- 229910021511 zinc hydroxide Inorganic materials 0.000 description 1
- 229940007718 zinc hydroxide Drugs 0.000 description 1
- NWONKYPBYAMBJT-UHFFFAOYSA-L zinc sulfate Chemical compound [Zn+2].[O-]S([O-])(=O)=O NWONKYPBYAMBJT-UHFFFAOYSA-L 0.000 description 1
- 229910000368 zinc sulfate Inorganic materials 0.000 description 1
- 229960001763 zinc sulfate Drugs 0.000 description 1
- 229910052726 zirconium Inorganic materials 0.000 description 1
- 229910001928 zirconium oxide Inorganic materials 0.000 description 1
- OMQSJNWFFJOIMO-UHFFFAOYSA-J zirconium tetrafluoride Chemical compound F[Zr](F)(F)F OMQSJNWFFJOIMO-UHFFFAOYSA-J 0.000 description 1
- ZXAUZSQITFJWPS-UHFFFAOYSA-J zirconium(4+);disulfate Chemical compound [Zr+4].[O-]S([O-])(=O)=O.[O-]S([O-])(=O)=O ZXAUZSQITFJWPS-UHFFFAOYSA-J 0.000 description 1
- GFQYVLUOOAAOGM-UHFFFAOYSA-N zirconium(iv) silicate Chemical compound [Zr+4].[O-][Si]([O-])([O-])[O-] GFQYVLUOOAAOGM-UHFFFAOYSA-N 0.000 description 1
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Abstract
本发明描述了螯合温室气体的方法,所述方法包括:(i)提供含有第一试剂的溶液,所述第一试剂能够与温室气体反应;(ii)在促进至少第一试剂与温室气体反应以生成至少第一反应物的条件下,使所述溶液与温室气体接触;(iii)提供具有间隙并且包括至少第二反应物的多孔基质;(iv)在促进所述至少第一反应物与所述至少第二反应物反应以提供第一产物的条件下,让含有所述至少第一反应物的溶液渗入所述多孔基质的至少大部分间隙;以及(v)允许所述至少第一产物形成并填充所述多孔基质的至少部分内部空隙,从而螯合温室气体。
Description
相关申请
本申请要求2007年11月15日提交的美国临时专利申请第60/988,122号的优先权,其全部内容在此通过引用并入本文。
背景技术
由于提出了更为人们接受的理论,全球变暖(包括温室气体二氧化碳的释放增加)已受到越来越多的关注。2004年,全球释放的二氧化碳为490亿吨,这相对于1970年的水平增加了80%。2005年,仅在美国排放的二氧化碳为60亿吨。建筑工业中,诸如钢铁和水泥之类的材料产生非常大量的二氧化碳(其他有毒气体和/或温室气体之一)。2002年,EPA估算水泥生产占二氧化碳世界产量的5wt%并且与钢铁工业并列为最突出的二氧化碳的工业贡献者。二氧化碳的释放归因于三个方面:第一,石灰石分解,其中碳酸钙被煅烧(加热)为CaO。第二,加热(驱动)吸热的石灰石分解需要能量(约5百万BTU/公吨水泥)。第三,驱动加工仪器(例如回转煅烧窑和研磨仪器)需要电能。总而言之,生产每一吨水泥,生成1.08吨二氧化碳。
再者,常规陶瓷制造包括高温过程,例如煅烧和烧结。原料通常被转化为通过诸如研磨之类的制粉过程制造的活性材料,其中陶瓷碎片(水泥工业中称为熟料)从厘米尺寸被研磨为微米尺寸。甚至这些过程也是能量密集的。1980年,陶瓷化学品的研磨过程约占国家能量消耗的0.5%。
因此,需要用于制造陶瓷的更好的***和/或方法,所述***和/或方法也可最小化碳足迹(footprint),或者甚至捕获和/或螯合生产中所生成的温室气体。
此外,燃烧后(post-combustion)捕获废气中的CO2仍然是挑战。例如,诸如背压之类的问题可限制发电机组的输出。此外,捕获方法经常受燃烧条件的限制,由所燃烧的燃料的化学作用和所选择的燃烧条件来确定捕获方法。例如,对于高CO2捕获效率而言,基于胺(amine-based)的捕获方法需要低温条件,这个方法引入了用于冷却燃料气体的能量消耗以及与能量结合的CO2足迹。
因此,存在建立下述方法的需求:该方法可在大多数的燃料和燃烧条件下运行而对于使用那种燃烧方法的制造企业没有任何效率上的不利结果,所述方法可以经济的方式除去气流中所有CO2,在已考虑对CO2产生的所有作用时消耗CO2,该方法可通过销售可用物品回收的成本来处理材料,并且以可溶形式提供CO2。
发明内容
一种实施方式提供了螯合温室气体的方法,所述方法包括:(i)提供含有第一试剂的溶液,所述第一试剂能够与温室气体反应;(ii)在促进至少第一试剂与温室气体反应以生成至少第一反应物的条件下,使所述溶液与温室气体接触;(iii)提供具有间隙并且包括至少第二反应物的多孔基质;(iv)在促进所述至少第一反应物与所述至少第二反应物反应以提供至少第一产物的条件下,让含有所述至少第一反应物的溶液渗入所述多孔基质的至少大部分间隙;以及(v)允许所述至少第一产物形成并填充所述多孔基质的至少部分内部空隙,从而螯合温室气体。反应可包括,例如,溶解、离子加成(ionaddition)、离子取代、沉淀、歧化作用或者它们的组合。
另一种实施方式提供由碳捕获方法、碳螯合方法或者它们的组合生成的陶瓷,所述方法包括让多孔基质的至少一种组分与渗入介质所含有的至少第一反应物反应以提供至少第一产物,在所述反应过程中,所述多孔基质的剩余部分作为支架用于促进从反应混合物中形成所述第一产物,从而生成陶瓷。
在另一种实施方式中,提供制造陶瓷的方法,所述方法包括:(i)提供具有间隙并且包括至少第一反应物的多孔基质;(ii)使所述多孔基质与含有至少第二反应物的渗入介质接触,所述渗入介质包括温室气体;(iii)在促进所述至少第一反应物与所述至少第二反应物反应以提供至少第一产物的条件下,让渗入介质渗入所述多孔基质的至少部分内部空隙;以及(iv)允许所述至少第一产物形成并填充所述多孔基质的至少部分间隙,从而生成陶瓷,其中所述方法消耗大量温室气体并且不释放大量温室气体。
一种实施方式提供水泥,所述水泥基本不包括水硬性结合(hydraulicbond)。水硬性结合一般可被称为水介导结合(water-mediated bond),例如,包括至少水分子或部分水分子的结合。例如,它可以是氢结合。
另一种实施方式公开了包括陶瓷结合的陶瓷,其中所述陶瓷包括相互连接的网络微结构。陶瓷结合一般可被称为具有共价键合、离子键合或混合离子-共价键合的金属与非金属或非金属与非金属之间的化学键合。在优选的实施方式中,所述化学键合基本上基于相邻的多孔结构中的沉积物质而不是基于范德华键合或氢键合。一般而言,相互连接的网络微结构可被称为具有一些孔隙度和/或通道的微结构,所述通道相互连接并且从表面可进入所述通道。
附图说明
图1提供在一种实施方式中基于热力学计算产生的、用于选择HLPS中使用的反应物种类的FeO相图。
图2提供在一种实施方式中基于热力学计算产生的、用于选择HLPS中使用的反应物种类的Ca(OH)2相图。
图3提供在一种实施方式中基于热力学计算产生的、用于选择HLPS中使用的反应物种类的FeTiO3相图。
图4提供在一种实施方式中基于热力学计算产生的、用于选择HLPS中使用的反应物种类的Fe3O4相图。
图5提供在一种实施方式中基于热力学计算产生的、用于选择HLPS中使用的反应物种类的Fe3O4相图。提供CaSO4和K2CO3的热力学计算结果。
图6提供在一种实施方式中基于热力学计算产生的、用于选择HLPS中使用的反应物种类的CaSO4和K2CO3相图。
图7提供在一种实施方式中基于热力学计算产生的、用于选择HLPS中使用的反应物种类的CaSO4和C2H2O4相图。
图8提供在一种实施方式中基于热力学计算产生的、用于选择HLPS中使用的反应物种类的MgO和C2H2O4相图。
图9提供在一种实施方式中基于热力学计算产生的、用于选择HLPS中使用的反应物种类的Ca(OH)2和C2H2O4相图。
图10提供在一种实施方式中基于热力学计算产生的、用于选择HLPS中使用的反应物种类的CaSO4和K2H2O4相图。
图11提供在一种实施方式中基于热力学计算产生的、用于选择HLPS中使用的反应物种类的Ca(OH)2和K2H2O4相图。
图12提供在一种实施方式中基于热力学计算产生的、用于选择HLPS中使用的反应物种类的CaCO3和H2C2O4相图。
图13提供在一种实施方式中基于热力学计算产生的、用于选择HLPS中使用的反应物种类的0.1mol CaCO3和K2C2O相图。
图14提供在一种实施方式中与pH有关的CaCO3的分解。
图15提供在一种实施方式中与pH有关的CaC2O4的分解。
具体实施方式
全部参考文献在此通过引用并入本文。
水热液相烧结的通用条件
在水热液相烧结(HLPS)的优选实施方式中,具有相邻间隙孔的、“未烧结(green)”或部分烧结的、多孔的、固体基质可通过液相渗入介质的作用转变为烧结陶瓷。在相对温和的条件下可进行HLPS,通常不超过高压釜运行中所遇到的温度和压力。HLPS可在宽的温度和压力范围内进行。例如,在一些实施方式中,HLPS条件可包括温度低于约2000℃,例如低于约1000℃、例如低于约500℃、例如低于约200℃、例如低于约100℃、例如低于约50℃、例如室温。反应压力可小于约100000psi,例如小于70000psi、例如小于约50000psi、例如小于约10000psi、例如小于约5000psi、例如小于约1000psi、例如小于约500psi、例如小于约100psi、例如小于约50psi、例如小于约10psi。在一种实施方式中,可在温度为约80℃至约180℃范围内以及压力为约1大气压至约3大气压(1大气压为约15psi)范围内进行水热烧结方法。
理论上,能够与渗入物发生水热反应以生成不同物质的任何起始材料可被用于生成水热烧结产物。因此,根据预期的最终用途可选择多种起始材料,成型为具有所需形状和尺寸的多孔固体基质并且随后进行用于转化为烧结最终产物的本发明方法的步骤。
在一种实施方式中,所述多孔固体基质从金属氧化物粉末得到。所述粉末可以是无定形的或者结晶的,优选结晶的。而且,所述金属氧化物粉末可具有宽的粒度范围,平均粒度范围为约0.01微米至约100微米,包括例如约0.02微米至约50微米,例如约0.04微米至约20微米,例如约0.08微米至约10微米。在一种实施方式中,所述粉末的平均粒度为约0.1微米至约5微米。
所述金属氧化物中的金属可选自:IIa族金属的氧化物、IIb族金属的氧化物、IIIb族金属的氧化物、IVb族金属的氧化物、Vb族金属的氧化物、过渡金属的氧化物、镧系金属的氧化物、锕系金属的氧化物或者它们的混合物。优选地,所选的金属氧化物或烧结最终产物可在化学、陶瓷、磁性、电子、超导、机械、建筑或者甚至生物学方面具有潜在的应用。所述烧结最终产物可具有工业实用性或家用实用性。所述最终产物不一定需要包括与反应物相同的材料。例如,可由包括钡和/或钛的反应物生成基本不含钛酸钡(BaTiO3)的产物。然而,在不同的实施方式中,反应物中所含的钡和/或钛可主要作为中间反应物,因此最终产物不一定包括所述钡和/或钛。
本申请所述的“水热反应”可包括在含水介质或非水液态介质中发生的转化。而且,这种转化可包括相同化学物质的溶解和再沉淀,一种化学物质的溶解及其与第二化学物质的结合以形成复合材料,复合材料中起始化学物质仍然不同,或者一种化学物质与第二化学物质反应以生成不同于起始物质的新化学成分。因此,所述水热烧结方法可用通过沉淀(或再沉淀)、离子加成、离子取代或它们的组合得到的成分填充多孔固体基质中的间隙或空隙。所述成分可包括与固体基质中的成分相同的化学物质、由两种不同的化学物质共同-再沉淀得到的复合物、由两种化学物质之间的反应得到的新产物、由介质中含有的浸渗剂类物质得到的再沉淀材料或者它们的组合。
在一种实施方式中,在至少大部分未烧结多孔固体基质与流体介质中存在的预选的浸渗剂类物质反应以生成新产物的条件下,可进行HLPS方法。
HLPS反应
所述水热反应方法可通过溶解-再沉淀反应机理发生。可选地,所述反应可通过离子取代反应发生。对于前者,少部分压制的多孔固体基质可溶解提供可与浸渗剂溶液中的离子反应的溶解物质;浸渗剂溶液中的离子可以是金属离子。在一种实施方式中,添加的浸渗剂的量可足以在单一步骤中产生完全反应。可选地,也可包括多个步骤。例如,可包括多次渗入。在一种实施方式中,从氧化钛基质可形成钛酸锶,此后,通过另一渗入可形成锶磷灰石。可选地,通过多次渗入可形成碳酸盐,然后该碳酸盐可形成保护性的草酸盐层。在另一种实施方式中,可部分地渗入和干燥压坯(compact),并且所述渗入步骤可重复直至生成最终产物。
所述产物的形状可保持固体基质的形状。在一种实施方式中,当所述产物的摩尔体积大于氧化物的摩尔体积(即,正摩尔体积变化-即,转化为较大摩尔体积)时,成核形成的产物(nucleated product)填充压坯的孔隙并且增加所述压坯的密度。所述摩尔体积变化不是必须为正;它也可以为负(即,转化为较小摩尔体积)或无变化,这取决于离子种类和反应机理。例如,部分基质在反应过程中可溶解消失,孔隙度提高,同时产生新化学键合和负摩尔体积变化。类似地,如果新材料的形状与基质损失的形状具有相同的体积,那么基本没有摩尔体积变化。
HLPS反应可通过例如离子加成和/或离子取代发生。在加成反应中,可将渗入介质中的离子(阴离子或阳离子)加至基质主体而不取代基质中另外的离子。离子加成的例子可包括氧化物转化至氢氧化物或氧化物转化至碳酸盐。离子取代的例子可包括氢氧化物转化至碳酸盐或氢氧化物转化至草酸盐。此外,所述反应可通过歧化作用发生,其中不可溶的无机主体/基质材料可被分离为两种不可溶的无机产物。例如,对于氧化物、氟化物、氢氧化物、硫酸盐、混合的金属氧化物、硅酸盐、羟磷灰石而言可进行歧化作用。
非均质成核现象还可在反应过程中发生。如先前所描述的,密度的变化可依赖于基质材料的类型和/或形成的产物的类型。一旦水热反应完成,可进一步通过例如时效来除去开孔。
上述反应完成之后,可在溶液中冲洗或浸泡致密整体基质以冲走过量的渗入溶液。冲洗用溶液可以是pH为5的醋酸铵。在一种实施方式中,随后可在约90℃至约250℃的温度下,在烘箱中干燥所述致密基质。在烧结陶瓷中可能存在的残余孔隙度可进一步通过加热至更高温度(例如加热至约600℃或低于600℃)来除去。
通过HLPS方法烧结的陶瓷产品可具有各种应用。例如,它可用于建筑、化学(例如,催化剂、过滤)、电子元件、半导体材料、电气材料或它们的组合。
多孔固体基质的制备
固体基质可包括不易在溶液中溶解的材料。在一种实施方式中,所述多孔固体基质由粉末得到。所述粉末可以是任何种类。例如,它可以是金属氧化物粉末。合适的金属氧化物粉末的例子可包括,铍氧化物(例如,BeO),镁氧化物(例如,MgO)、钙氧化物(例如,CaO,CaO2)、锶氧化物(例如,SrO)、钡氧化物(BaO)、钪氧化物(例如,Sc2O3)、钛氧化物(例如,TiO,TiO2,Ti2O3)、铝氧化物(例如,Al2O3)、钒氧化物(例如,VO,V2O3,VO2,V2O5)、铬氧化物(例如,CrO,Cr2O3,CrO3,CrO2)、锰氧化物(例如,MnO,Mn2O3,MnO2,Mn2O7)、铁氧化物(例如,FeO,Fe2O3)、钴氧化物(例如,CoO,Co2O3,Co3O4)、镍氧化物(例如,NiO,Ni2O3)、铜氧化物(例如,CuO,Cu2O)、锌氧化物(例如,ZnO)、镓氧化物(例如,Ga2O3,Ga2O)、锗氧化物(例如,GeO,GeO2)、锡氧化物(例如,SnO,SnO2)、锑氧化物(例如,Sb2O3,Sb2O5)、铟氧化物(例如,In2O3)、镉氧化物(例如,CdO)、银氧化物(例如,Ag2O)、铋氧化物(例如,Bi2O3,Bi2O5,Bi2O4,Bi2O3,BiO)、金氧化物(例如,Au2O3,Au2O)、锌氧化物(例如,ZnO)、铅氧化物(例如,PbO,PbO2,Pb3O4,Pb2O3,Pb2O)、铑氧化物(例如,RhO2,Rh2O3)、钇氧化物(例如,Y2O3)、钌氧化物(例如,RuO2,RuO4)、锝氧化物(例如,Tc2O,Tc2O3)、钼氧化物(例如,MoO2,Mo2O5,Mo2O3,MoO3)、钕氧化物(例如,Nd2O3)、锆氧化物(例如,ZrO2)、镧氧化物(例如,La2O3)、铪氧化物(例如,HfO2)、钽氧化物(例如,TaO2,Ta2O5)、钨氧化物(例如,WO2,W2O5)、铼氧化物(例如,ReO2,Re2O3)、锇氧化物(例如,OsO,OsO2)、铱氧化物(例如,IrO2,Ir2O3)、铂氧化物(例如,PtO,PtO2,PtO3,Pt2O3,Pt3O4)、汞氧化物(例如,HgO,Hg2O)、铊氧化物(例如,TlO2,Tl2O3)、钯氧化物(例如,PdO,PdO2)、镧系氧化物、锕系氧化物,等等。而且,依赖于所涉及的具体应用,金属氧化物的混合物也可用于制造预成型件。
所述基质也可包括氢氧化物,例如金属氢氧化物。例如,它可包括氢氧化镁(例如,Mg(OH)2)、氢氧化钙(例如,Ca(OH)2)、氢氧化锶(例如,Sr(OH)2)、和氢氧化钡(例如,Ba(OH)2)、氢氧化铬(例如,Cr(OH)2)、氢氧化钛(例如,Ti(OH)2)、氢氧化锆(例如,Zr(OH)4)、氢氧化锰(例如,Mn(OH)2)、氢氧化铁(例如,Fe(OH)2)、氢氧化铜(例如,Cu(OH)2)、氢氧化锌(例如,Zn(OH)2)、氢氧化铝(例如,Al(OH)3)或者它们的组合。
所述基质也可包括氟化物,例如金属氟化物。例如,它可包括氟化镁(例如,MgF2)、氟化钙(例如,CaF2)、氟化锶(例如,SrF2)、以及氟化钡(例如,BaF2)、氟化铬(例如,CrF2)、氟化钛(例如,TiF3)、氟化锆(例如,ZrF4)、氟化锰(例如,MnF2)、氟化铁(例如,FeF2)、氟化铜(例如,CuF2)、氟化镍(例如,NiF2)、氟化锌(例如,ZnF2)、氟化铝(例如,AlF3)或者它们的组合。
所述基质也可包括混合金属氧化物,例如金属钛酸盐。例如,它可包括钛酸镁(例如,MgTiO3)、钛酸钙(例如,CaTiO3)、钛酸锶(例如,SrTiO3)、钛酸钡(例如,BaTiO3)或者它们的组合。
所述基质也可包括硫酸盐,例如金属硫酸盐。例如,它可包括硫酸镁(例如,MgSO4)、硫酸钙(例如,CaSO4)、硫酸锶(例如,SrSO4)、和硫酸钡(例如,BaSO4)、硫酸铬(例如,Cr2(SO4)3)、硫酸钛(例如,TiSO4,Ti2(SO4)3)、硫酸锆(例如,ZrSO4)、硫酸锰(例如,MnSO4)、硫酸铁(例如,FeSO4)、硫酸铜(例如,CuSO4)、硫酸镍(例如,NiSO4)、硫酸锌(例如,ZnSO4)、硫酸铝(例如,Al2(SO4)3)或者它们的组合。
所述基质也可包括硅酸盐,例如金属硅酸盐。例如,它可包括偏硅酸锂、原硅酸锂、偏硅酸钠、硅酸铍、硅酸钙、原硅酸锶、偏硅酸钡、硅酸锆、偏硅酸锰、硅酸铁、原硅酸钴、原硅酸锌、偏硅酸镉、红柱石、硅线石、蓝晶石(hyanite)、高岭石或者它们的组合。
0046所述基质也可包括羟磷灰石,例如金属羟磷灰石。例如,它可包括碳酸钙、四水合硝酸钙、氢氧化钙或者它们的组合。
所述基质除了上述任何材料外还可包括惰性填充材料以及其他材料。惰性填充材料可以是被合并进入固体基质以填充孔并且与用于化学键合的浸渗剂实质上不发生反应的任何材料。例如,所述惰性材料可以是木材、塑料、玻璃、金属、陶瓷、灰烬或者它们的组合。
所述粉末以平均粒度、粒度分布以及具体的表面积来表征,所述平均粒度可在约0.005μm至500μm的范围内,例如约0.01μm至约100μm。对于提高溶解而言,细的平均粒度和窄的粒度分布可能是理想的。
通过任何常规技术(包括挤出成型,注射成型,模压成型,等静压成型以及泥浆浇注)所述粉末可成型为任何期望形状和尺寸的生坯。也可成型为陶瓷薄膜。在压坯成型中所使用的任何润滑剂、粘合剂的类似材料可被使用并且它们应当对所得材料无有害效果。这些材料的优选类型为在相对较低的温度(优选的低于500℃)下加热时,蒸发或烧掉所述材料而不留下明显的残渣。
所述基质可包括,例如,矿物、工业废物或工业化学材料。矿物可以是例如矿物硅酸盐或石膏。工业废物可以是例如飞尘、矿渣或废电池。工业化学品一般可以是通过工厂或工业合成或制备的任何化学品。
所述压坯可成型为产品材料的预定形状和尺寸。所述压坯可以是任何形状。所述压坯的开孔率的体积(0-80%)可依赖于反应产物的摩尔体积与粉末的摩尔体积的比例。产物材料可以是例如整体(例如整体致密体)。在一种实施方式中,在所述压坯的孔内形成的反应产物可具有大于粉末的摩尔体积。反应产物可具有大于氧化物粉末的摩尔体积以填充反应过程中压坯的孔隙。例如,如果反应产物的摩尔体积是氧化物粉末摩尔体积的两倍,所述压坯应当具有约50%(按体积计)的开孔率。
起始粉末压坯中的孔可以较小,例如约0.01微米(μm)至约100微米(μm),例如约0.1μm至约1μm,并且在整个压坯中均匀分布,从而能够使浸渗剂溶液完全渗透粉末压坯。可通过标准方法来确定孔体积量(闭孔率和开孔率)和孔尺寸。例如,压汞孔径测试仪(mercury intrusion pore sizer)可用于评价这三个参数。
然后,上面得到的预成型件进行下面讨论的步骤。
渗入介质的制备
如先前所描述的,水热烧结可利用含水介质或非水介质。液体溶剂的选择可基于浸渗剂物质,所述浸渗剂可以是渗入介质的一部分。在水热烧结方法的条件下,所述浸渗剂物质在液体溶剂中可具有较大的溶解度。例如,如果所述浸渗剂物质是离子型的,那么液体溶剂可以是水。某些非离子型的浸渗剂也可在含水介质中具有足够的溶解度。
此外,诸如醇类(例如,甲醇、乙醇、丙醇、异丙醇等等)、多元醇类(例如,乙二醇、1,2-丙二醇、1,3-丙二醇等等)、某些低分子量醚类(例如,呋喃、四氢呋喃)、胺类(例如,甲基胺、乙基胺、吡啶等等)、低分子量酮类(例如,丙酮)、亚砜类(例如,二甲亚砜)、乙腈等等之类的水溶性有机溶剂也可在含水混合物中存在。在某些实施例中,可将表面活性剂(例如,聚硅氧烷、聚乙二醇以及氧化烷基二甲基胺)加至含水混合物。
所述渗入介质优选地含有水溶性金属盐类(即,离子形式的金属)。这些盐的阳离子可来自例如下列金属:铍、镁、钙、锶、钡、钪、钛、钒、铬、锰、铁、钴、镍、铜、锌、铝、镓、锗、锡、锑、铟、镉、银、铅、铑、钌、锝、钼、钕、锆、镱、镧、铪、钽、钨、铼、锇、铱、铂、金、汞、铊、钯、镧系金属的阳离子、锕系金属的阳离子或者它们的混合物。一般而言,溶解于渗入溶液中的盐的阴离子,可来自例如下列基团:氢氧化物、硝酸盐、氯化物、醋酸盐、甲酸盐、丙酸盐、苯基乙酸盐、苯甲酸盐、羟基苯甲酸盐、胺基苯甲酸盐、甲氧基苯甲酸盐、硝基苯甲酸盐、硫酸盐、氟化物、溴化物、碘化物、碳酸盐、草酸盐、磷酸盐、柠檬酸盐以及硅酸盐或者它们的混合物。可选择浸渗剂中含有的金属离子与氧化物粉末中的金属离子的摩尔比例以获得理想的化学计量反应产物。溶液中需要过量的金属离子以帮助达到反应完全。
依赖于渗入介质和基质材料,得到的烧结产物可以是,例如,钛酸盐(如果涉及包括钛的材料)。例如,可从水中TiO2和Fe2+、Mg2+、Mn2+、Co2+、Ni2+的盐或者它们的组合的盐得到具有钛铁矿结构的钛酸盐。可从Ca2+、Sr2+、钡离子的盐水溶液或者它们的组合的盐水溶液制备具有钙钛矿结构的钛酸盐。而且,可得到具有尖晶石结构的化合物(包括Mg2TiO4、Zn2TiO4和Co2TiO4)。此外,可通过本发明的方法得到例如具有通式BaxTiyOx+2y(其中x和y是整数)的钛酸钡的不同相。
可选地,所得的烧结产物可以是碳酸盐、硫酸盐、草酸盐或者它们的组合;如果使用常规的烧结方法,可使用的材料可包括在该材料能烧结之前可能分解的材料;例如,在常规烧结方法中,当在能够烧结之前加热时,碳酸盐将分解为它的氧化物。所述碳酸盐、硫酸盐、草酸盐可以是例如,金属碳酸盐、金属硫酸盐、金属草酸盐,分别包括元素周期表中发现的元素的阳离子。
烧结材料的表征
烧结材料的孔隙度
HLPS可生成具有非常均匀和非常细小的微结构的烧结产物。烧结材料的孔隙度可以是,例如小于约15%,例如小于约10%,例如小于约5%,或者甚至实际上完全致密。压坯的总孔隙度可使用标准技术中例如压汞孔径测定仪来确定。密度可使用诸如阿基米德压汞孔径测定仪之类的常规技术来估算。
烧结材料的尺寸和形状
由HLPS方法得到的烧结材料的一个特征是所述烧结材料可具有与起始的压坯相同的形状或者甚至相同的尺寸。在一种实施方式中,其中所述产物基本无摩尔体积变化,不会引起压坯收缩,这与许多陶瓷的制造过程相反,因此,几乎不需要或根本不需要加工烧结材料。
烧结材料的组分
如实施例中所示例的,很多化学组分可用来制造烧结材料。此外,形成烧结材料所涉及的不同的金属氧化物和盐的数目不一定以特定的方式来限制。此外,最终产物的化学计量可由生坯和渗入介质中存在的反应物的摩尔比例来决定。烧结材料的组分可使用X射线衍射定量分析(QXRD)和感应耦合等离子体(ICP)来估算。
微结构和相关机械性能
HLPS方法的烧结产物可具有基本类似网状的互相连接的网络微结构。从HLPS方法获得的整体也可表现出诸如核-壳结构之类的复合结构。此外,所述产物可具有优异的机械性能,例如高的抗拉强度、抗压强度和理想的拉伸模量。这种加强可由化学键合产生,所述化学键合在物理结合的颗粒之间形成并且所述化学键合在离子取代、离子加成、Ostwald熟化(即,可形成新的网络的重结晶)或它们的组合的过程中形成。在一种实施方式中,Ostwald熟化可包括在碱性介质中时效碳酸盐材料。此外,如先前所描述的,在具有正摩尔体积变化的例子中,可实现致密化。
由HLPS制造水泥
常规地,水泥可由两个步骤制造:(i)用高温方法合成以及(ii)然后加固并与水结合以制造整体结构。
HLPS可使制造水泥的合成和加固/结合步骤集成,提供紧凑、能效高并且环境友好的方法。HLPS可以是多功能的,使用很多原料,这将让该方法用于可方便得到的成分(例如,工厂废弃物),从而使运输成本最小化。
HLPS可提供在温和的温度和/或压力条件下在流体中形成各种有利的陶瓷材料的选择,而不需要制造陶瓷所使用的高温方法。不使用如常规工序中的“修正式”研磨方法即可制造陶瓷晶体,并且所述陶瓷晶体具有用于制造材料的合适反应性的晶体尺寸和形态。此外,通过HLPS生成的产物的化学结合可以是陶瓷结合或可基本不含水硬性结合,如,常规建筑材料(即,水泥)制造方法通常生成水硬性结合。常规水泥具有水硬性结合,因此,就常规水泥的机械强度而言,约200℃开始可降低其机械强度-1000℃常规水泥损失几乎全部的强度。通过使水硬性结合(即,涉及水分子或部分水分子的键合)的形成基本上最小化,由HLPS生成的陶瓷经得起至少约1000℃的温度。
一般而言,使用HLPS生产水泥或陶瓷的其他好处可包括形成陶瓷产物的反应时间更短。水热反应可基于水溶液反应,其中,典型地在温度低于约400℃(例如低于300℃或大约室温)条件下,可从溶液中直接形成陶瓷。
生成的陶瓷也可以是非常致密的,基本不含水硬性结合并且主要含有陶瓷结合。例如,水泥中的结合可由水中浆状粉末的水合作用产生。常规陶瓷具有的大多数结合是通过高温烧制引起的扩散产生的。相反,可由粉末或固体基质的整体压坯与渗入介质的反应以填充颗粒间隙(即,孔)来形成HLPS陶瓷。在这些间隙中成核并且生长的晶体可形成彼此的化学键合以及粉末基质的化学键合以制造陶瓷结合的整体。因此,不同于水硬性水泥接合方法,可形成无水的陶瓷结合,所述无水的陶瓷结合的稳定性可以是至少约1000℃,例如约2000℃。此外,不同于常规致密化方法(例如,固态烧结),反应温度可低于约90℃,例如室温。
如先前所描述的,HLPS方法的产物可发生摩尔体积变化(增加或减小)或摩尔体积基本无变化。在一种实施方式中,其中,所述摩尔体积变化为正,也可产生致密化。在一种实施方式中,其中所述固体基质可要求作为支架用于形成结合结构,基本无尺寸变化发生。因此,基本不引发诸如裂纹或缺陷之类的缺陷。当不改变材料尺寸时,由所选择的化学反应来控制结构的相对孔隙度,在所述化学反应中,产物和反应物之间的摩尔体积变化的百分数可确定保留在结构中的孔隙度。例如,50%多孔结构可完全致密化,所述50%多孔结构反应形成具有100%摩尔体积变化的产物。在一种实施方式中,具有大孔尺寸可以是理想的以实现完全转化。请注意,可由基质粉末的选择和压紧粉末的成型技术来控制起始密度。
可设计许多体积增加或减小的反应以导致孔隙度改变(参见表1),而用从所述反应中形成的晶体来键合陶瓷。例如,CaSO4基质转化为CaC2O4·H2O基质可导致44.4vol%的摩尔体积增加(致密化),而CaSO4转化为CaCO3可导致-19.7vol%的摩尔体积减小(增加孔隙度)。通过混合负体积变化和正体积变化的成分以设计复合物可进一步控制该方法,所述复合物的净密度(孔隙率)变化为零、正值或负值。如表1所示,如同616vol%那么大的摩尔体积增加和50.2vol%的摩尔体积减小都是可能的。
减小或增加孔隙度的能力可具有很大的实用性。例如,在可容纳大的膨胀的低密度基质中,大的摩尔体积增加可具有实用性,例如,可加入道路建筑材料或建筑结构中的粒料。另一方面,大的体积减小可用于改善反应溶液的运输,所述反应溶液通过增加反应进行时的渗透率在反应进行时结合粒料。此外,复合物可包括降低密度增加(或减小)的额外的惰性粉末,所述惰性粉末可成比例地减少摩尔体积的增加(或减小)。一般而言,不论反应是否导致基质体积的膨胀或收缩,反应形成的晶体可用于结合基质,不论所述基质是否作为反应物、惰性成分或已从反应中形成的产物。
表1.HLPS起始材料的密度、HLPS起始材料的分子量、HLPS起始材料的摩尔体积、HLPS起始材料转化为其碳酸盐的%体积变化、HLPS起始材料转化为其草酸盐的%体积变化。
起始材料 | 摩尔体积(cc/mol) | 转化为碳酸盐的%摩尔体积变化 | 转化为草酸盐的%摩尔体积变化 |
CaSO4 | 45.99 | -19.7 | 44.4 |
CaSO4.2H2O | 74.21 | -50.23 | -10.51 |
FeO | 11.97 | 148.09 | 558.94 |
Fe2O3 | 15.21 | 95.33 | 418.8 |
Fe3O4 | 14.93 | 99 | 428.54 |
MgO | 11.2 | 146.92 | 616.28 |
Mg(OH)2 | 24.61 | 12.34 | 225.88 |
MgCO3 | 27.64 | 0 | 190.09 |
Ca(OH)2 | 33.68 | 9.66 | 97.2 |
FeTiO3 | 32.14 | -7.58 | 145.48 |
FeCO3 | 29.71 | 0 | 165.6 |
CaCO3(方解石) | 36.93 | 0 | 79.83 |
HLPS可提供用各种材料形成陶瓷结合的方法,所述材料包括那些不能通过任何常规方法制备的材料。因此,诸如大理石、天然形成的碳酸钙(CaCO3)之类的陶瓷可从非碳酸化的钙原料中合成。
由于HLPS方法的多功能性,所述方法可用于捕获温室气体,例如二氧化碳,而形成如先前所描述的致密陶瓷。所述方法可被进一步集成至散发温室气体的粉末生成设备中,其中,所述气体可被捕获并且作为反应物直接输入HLPS方法。
由气体捕获形成陶瓷
使用HLPS方法,可从大气中捕获气体并可在反应中使用气体以形成各种陶瓷(包括大理石或水泥)。所述气体可以是任何类型的气体,例如温室气体,包括二氧化碳或通常含有碳、硫、磷、氮、氢、氧或它们的组合的气体。
基于热力学计算所产生的相图可用来帮助选择用于HLPS方法合适的反应物。例如,尽管发现许多其他的反应***,CaSO4与CO2的反应不可能形成CaCO3。兼有热力学计算结果的下列化学反应是基质与CO2饱和溶液的反应,这表现出形成羧酸盐化合物和螯合二氧化碳的适用性。请注意,碳原料和它的浓度是可变的并且其他陶瓷反应物保持恒定的浓度。对于每一个前体***而言,温度范围(包括室温)内所产生的相被报道。
FeO+CO2→FeCO3 (图1)
Ca(OH)2+CO2→CaCO3+H2O (图2)
FeTiO3+CO2→FeCO3+TiO2 (图3)
Fe3O4+CO2→FeCO3+Fe2O3 (图4)
如钛铁矿(FeTiO3)、钙钛矿(CaTiO3)、榍石(CaTiSiO5)或碱土长石(CaAl2Si2O8)可分解为碳酸盐和各自的氧化物。对于具有合适的还原环境的反应(例如Fe2O4)而言,还原Fe3+类物质是可能的,这样所有铁类物质是二价的并且可适用于碳酸化作用。预计以Fe3+为基础的氧化物不形成铁碳酸盐。
对于某些材料而言,根据计算CO2不可能反应。例如,CaSO4不与可溶的CO2反应。在其他情况下,捕获CO2的其他方法可能更加有利。例如,通过电化学的方法可将钾转化为氢氧化钾,从而捕获二氧化碳气体以形成K2CO3,然后从CaSO4中沉淀CaCO3,如下所示:
CaSO4+K2CO3→CaCO3+K2SO4 (图5)
钠的碳酸盐或铵的碳酸盐可进行类似的反应。在一种实施方式中,多孔大理石(即,碳酸钙)可被制备,并且K2SO4可保留在结构中。其他非矿物反应物(例如Ca(OH)2)也可用于捕获CO2。
Ca(OH)2+K2CO3→CaCO3+2KOH (图6)
其他合适的碱金属碳酸盐可包括Na2CO3和NH4CO3。通常,碱金属碳酸盐可由碱金属氢氧化物得到。当发生碳酸化作用时,涉及氢氧化物的反应(例如上述反应)可再获得碱金属氢氧化物。因此,这种反应可让碱金属氢氧化物循环以捕获更多的CO2。在一种实施方式中,当使用碳酸化反应时,可使用矿物氧化物来再获得碱金属氢氧化物:
MO+M’2CO3+H2O→MCO3+2M’OH,
其中,M=Na+,K+,NH4 +
可使用地球上丰富的铁矿石(Fe2O4/Fe3O4)。可选地,可将Mg用于可以石灰石开始的反应烧结方法中,如下所示:
Mg2++K2CO3+CaCO3→MgCO3/CaCO3+2K+
因此可用MgCO3填充多孔石灰石体以制造复合材料。
制造捕获诸如二氧化碳之类的温室气体的结构材料(例如碳酸盐)的一个重要的优势是在制造材料的过程中消耗二氧化碳,并且制造材料的过程不生成大量的温室气体。
气体螯合作用
在一种实施方式中,使用诸如草酸盐(C2O4 2-)之类的多齿配体可螯合两个CO2分子。该反应物可包括通过碳-碳键结合在一起的两个CO2分子。在下列草酸盐***中进行模拟反应以确定上述反应的可行性,它们各自的结果如图所示:
H
2
C
2
O
4
CaSO4+H2C2O4→CaC2O4·H2O+H2SO4 (图7)
MgO+H2C2O4+2H2O→MgC2O4·2H2O+H2O (图8)
Ca(OH)2+H2C2O4→CaC2O4·H2O+H2O (图9)
K
2
C
2
O
4
CaSO4+K2C2O4+H2O→CaC2O4·H2O+K2SO4 (图10)
Ca(OH)2+K2C2O4+H2O→CaC2O4·H2O+2KOH (图11)
在一些实施方式中,涉及碳酸盐的反应可再获得KOH作为反应产物,当螯合碳酸盐时,KOH可被再次用于其他反应。此外,也可使用诸如(NH4)2C2O4和Na2C2O4之类的其他草酸盐,同样可使用任何可提供游离的草酸盐阴离子的草酸盐前体。在室温下稳定的许多草酸盐可被使用。例如,每个铁原子获取六个CO2原子,含铁草酸盐[Fe(C2O4)3]-3是可溶阴离子,这对于二氧化碳的捕获和/或螯合是理想的。
草酸盐也可以是有用的,它们可形成草酸盐类并释放二氧化碳气体或可溶碳酸盐,如下所示:
CaCO3+H2C2O4→CaC2O4·H2O+CO2 (图12)
CaCO3+K2C2O4→CaC2O4·H2O+K2CO3 (图13)
相对于常规水泥,羧酸盐材料的使用可提供增强的化学耐久性。例如,在pH小于约6的条件下,常规大理石可开始分解,但是能耐久非常高的pH水平而不分解(图14)。例如,当将草酸盐用于草酸钙单水合物时,可耐久大于2的pH且小于13的pH水平而不分解(图15)。水硬性结合的缺乏也可使羧酸盐材料不易受用于冷表面防冻的盐的影响。
应用
通过HLPS方法捕获和/或螯合温室气体同时形成陶瓷的一个优势为所述方法的多功能性。例如,可在任何时间开始反应,允许快速就地安装结构件。例如,蒸汽-辊碾(steam-roller)型设备可用于压实粉末并随后加热***,同时蒸汽和CO2的混合物开始烧结反应。可选地,可将碳酸盐溶液注入多孔床,随后基于辊碾(roller-based)加固和加热。浇注模具可包括聚合物衬垫(polymerliner),所述聚合物衬垫波导微波能量以局部加热水以开始并完成反应,其中压制的结构中的局部压力可对应于亚临界反应条件或超临界反应条件。这种多功能性可允许建设项目几乎不需要或根本不需要固化材料的时间。而且,HLPS方法就地添加水的能力可减少需要运输的建筑材料的重量,从而降低成本并且减少能量消耗。此外,HLPS中的水可被用作渗入介质的溶剂而不是反应物(例如在常规水泥中)。具体而言,HLPS中的水可被再次使用或返回生态***。
在一种实施方式中,可将气体捕获方法和气体螯合方法结合为一个单独的方法。例如,可通过能与温室气体反应的反应物来捕获温室气体。随后,被捕获的气体(然后以水溶液的形式)可在溶液中成为反应物,然后所述反应物作为先前描述的渗入介质以螯合气体。可选地,在螯合作用之前不使用捕获方法。例如,渗入介质可容易地产生,所述渗入介质溶解了至少温室气体,因此,在这个实施方式中,仅使用温室气体的螯合作用。如果需要的话,所述介质可以是从商业上可获得的产品。
在一种实施方式中,建立无收缩处理的能力能够形成很多多组分结构,其中除了键合相之外的组分可被动地存在于结构中。这些组分可以是砂砾和沙子,所述组分可提供强的过滤网络,所述过滤网络可由结合的碳酸盐材料的相互连接的网络来加强,所述结合的碳酸盐材料遍及整个砂砾和沙子的孔结构。也可合并诸如钢筋之类的其他结构,其中界面反应可提供额外的加固。由砂砾和沙子得到的可溶硅酸盐可促进与钢铁的反应,也促进其他硅酸盐化合物的形成,所述其他硅酸盐化合物进一步提供基于碳酸盐的(carbonate-based)复合物结构中的键合相。无收缩也可促进低压力环境中设备的嵌入以有利于实时监测材料的机械稳定性和应力状态。
本申请描述的产物的另一个优势可包括耐火性,尤其对于碳酸盐而言。诸如碳酸钙之类的碳酸盐基本不分解直至达到相当高的温度(约800℃至1000℃,依赖于CaCO3粒度和CO2的分压-PCO2)。
惰性材料,例如无机反射材料、着色剂、乳浊剂或发光颗粒也可合并在这些羧酸盐陶瓷中。例如,较早提到的FeTiO3的分解可被用于由氧化钛和FeCO3制造复合建筑材料。
燃烧后捕获碳
诸如金属碳酸盐和金属草酸盐之类的羧酸盐可被用于HLPS方法中燃烧后捕获二氧化碳。经过如下快速反应可从CO2分子制备碳酸盐离子:
CO2+2OH-→CO3 2-+H2O
请注意,生成水作为副产物。因此,如果处理大量的CO2,由于水变得稀有,水的生成也是有益的。在一种实施方式中,对于每个碳酸盐离子而言,可使用1个至2个无机阳离子,如下所示:
xMz++CO3 2-→Mx(CO3)
例如,当无机离子为钠时,基于原子百分比,CO2与无机产物的比例为1∶2,而当无机离子为钙时,基于原子百分比,CO2与无机产物的比例为1∶1。单价碳酸盐会是理想的因为它们在水中可高度可溶。
也可使用金属草酸盐类。使用两分子CO2以制造一分子草酸盐离子,如下所示:
2CO2+2e-→C2O4 2-
草酸盐离子可从一氧化碳或通过生物学从大多数植物中的CO2来制造。对于每个草酸盐阴离子而言,草酸盐捕获两分子CO2的能力可提供用于捕获CO2的其他可能性。例如,诸如石灰石之类的矿物一般可分解释放CO2,如下所示:
CaCO3→CaO+CO2.
可选地,加入草酸盐可分解碳酸盐:
CaCO3+K2C2O4+H2O→CaC2O4·H2O+K2CO3.
因此,与生成需要捕获的CO2气体相反,可从石灰石中回收CO3 2-并可生成可进一步用于水热烧结的K2CO3前体。加入草酸也可发生该反应:
CaCO3+H2C2O4→CaC2O4·H2O+CO2
众所周知,由氧化钙在水中的水合可制备氢氧化钙。氢氧化钙可转化为碳酸盐,如下所示:
Ca(OH)2+CO2→CaCO3+H2O
因此,该反应是碳中和(carbon neutral)反应,一旦释放CO2形成CaO就消耗CO2。然而,如果使用草酸盐,所述反应可消耗碳,如下所示:
Ca(OH)2+H2C2O4→CaC2O4·H2O+H2O
或
Ca(OH)2+K2C2O4+H2O→CaC2O4·H2O+2KOH
在一种实施方式中,在反应中生成的腐蚀性碱可进一步用作CO2捕获溶液。因此,捕获CO2的一个HLPS过程可开始另一个HLPS过程。
燃烧后碳捕获溶液可基于可溶的氢氧化物,例如苛性钠。可溶的氢氧化物可用作经过洗涤塔的捕获溶液。
所提出的方法的一个优势是,所述方法可回收废气的所有热值、在高温下运行、与CO2定量反应并且使用可从任何海岸线提取的原料,也可便于运输。CO2足迹可以非常小,除非所述废气不能提供用于蒸发和碳酸化作用所需的热值。
非限定性实施例
实施例1.来自氢氧化钙和碳酸钾的碳酸钙
室温条件下,约5g氧化钙粉末与约100ml去离子水在Teflon罐中反应形成Ca(OH)2。将氢氧化钙与水的混合物冷却至室温。然后,将它摇晃并倒入胶体成型机(colloidal press)中直至填充了储存器的约75%。在胶体成型机上缓慢施加7000磅的负载。将200ml去离子水和30g溶解于去离子水中的K2CO3注入TeflonTM罐。将湿的Ca(OH)2小球置于Teflon盘上和Teflon罐中。关闭所述罐的盖子并且在室温保持4天。然后,取出所述小球并用去离子水清洗。反应产物经过x-射线衍射并且发现反应产物主要包括CaCO3带有少量Ca(OH)2。样品保持它的形状并且具有足够的机械强度以抵抗断裂。
实施例2.来自氢氧化钙和草酸的单水合草酸钙
室温条件下,约5g氧化钙粉末与约100ml去离子水在Teflon罐中反应形成Ca(OH)2。将氢氧化钙与水的混合物冷却至室温。然后,将它摇晃并倒入1”直径的胶体(过滤器)成型机中直至填充了储存器的约75%。在胶体成型机上缓慢施加7000磅的负载。用200ml去离子水填充TeflonTM罐并混合30gH2C2O4。将湿的Ca(OH)2小球置于Teflon盘上和Teflon罐中。关闭所述罐的盖子并且在室温保持4天。然后,取出所述小球并用去离子水清洗。X-射线衍射表明存在CaC2O4·H2O和Ca(OH)2。按压时,样品保持它的形状和尺寸并且水热液相烧结之后尺寸没有变化。材料是机械稳定的。如果在按压过程中将Ca(OH)2与草酸混合而不使用纯水,可导致更完全的反应以及甚至更强的材料。
上述实施例以及优选的实施方式意在示例性说明本发明的范围,不应当以任何方式以此限定本发明。由于在公开的内容中提供了详细的描述,其他实施方式对于本领域的普通技术人员将必然是明显的。这样的其他实施方式被认为落入本发明的范围和实质,本发明的范围和实质仅由下面的权利要求书限制。
Claims (35)
1.一种螯合温室气体的方法,所述方法包括:
(i)提供含有第一试剂的溶液,所述第一试剂能够与温室气体反应;
(ii)在促进至少第一试剂与温室气体反应以生成至少第一反应物的条件下,使所述溶液与温室气体接触;
(iii)提供具有预定形状和尺寸以及间隙并且包括至少第二反应物的多孔基质;
(iv)在促进所述至少第一反应物与至少第二反应物反应以提供至少第一产物的条件下,让含有所述至少第一反应物的溶液渗入所述多孔基质的至少大部分间隙;以及
(v)允许所述至少第一产物形成并填充所述多孔基质的至少部分内部空隙,从而螯合温室气体。
2.如权利要求1所述的方法,其中,所述温室气体包括二氧化碳。
3.如权利要求1所述的方法,其中,所述温室气体含有硫、磷、氮或它们的组合。
4.如权利要求1所述的方法,其中,步骤(v)之后所述固体基质的摩尔体积与步骤(v)之前所述固体基质的摩尔体积基本相同。
5.如权利要求1所述的方法,其中,步骤(v)之后所述固体基质的摩尔体积大于步骤(v)之前所述固体基质的摩尔体积。
6.如权利要求1所述的方法,其中,步骤(v)之后所述固体基质的摩尔体积小于步骤(v)之前所述固体基质的摩尔体积。
7.如权利要求1所述的方法,其中,步骤(v)之后所述固体基质的密度大于步骤(v)之前所述固体基质的密度。
8.如权利要求1所述的方法,其中,所述温室气体由工厂产生。
9.如权利要求1所述的方法,其中,所述第二反应物包括金属氧化物、金属氢氧化物、金属硫酸盐、金属氟化物、金属钛酸盐或它们的组合。
10.如权利要求1所述的方法,其中,所述第二反应物包括金属。
11.如权利要求1所述的方法,其中,所述第一反应物包括草酸盐、碳酸盐、硫酸盐、磷酸盐、柠檬酸盐、金属离子或它们的组合。
12.如权利要求1所述的方法,其中,所述第一产物由沉淀形成。
13.如权利要求1所述的方法,其中,所述第一产物包括碳酸钙。
14.如权利要求1所述的方法,其中,所述第一产物包括羧酸盐。
15.如权利要求1所述的方法,其中,所述第一产物包括金属碳酸盐、金属草酸盐或它们的组合。
16.如权利要求1所述的方法,其中,所述第一产物具有至少1000℃的分解温度。
17.如权利要求1所述的方法,其中,所述第一产物具有相互连接的网络微结构。
18.如权利要求1所述的方法,其中,所述第一试剂为含水形式。
19.如权利要求1所述的方法,其中,在温度低于300℃条件下进行所述方法。
20.如权利要求1所述的方法,其中,在室温条件下进行所述方法。
21.一种由碳捕获方法、碳螯合方法或它们的组合生成的陶瓷,所述方法包括让多孔基质的至少一个组分与渗入介质所含有的至少第一反应物反应以提供至少第一产物,在所述反应过程中所述多孔介质的剩余部分作为支架用于促进从反应混合物中形成所述第一产物,从而生成陶瓷,
其中所述多孔基质具有预定的形状和尺寸,
其中所述第一反应物包括至少温室气体,
其中所述陶瓷保持了所述多孔基质的形状和尺寸,
其中所述陶瓷包括陶瓷结合,且
其中所述陶瓷具有至少1000℃的分解温度。
22.如权利要求21所述的陶瓷,其中,所述陶瓷基本不包括水硬性结合。
23.如权利要求21所述的陶瓷,其中,所述陶瓷具有至少2000℃的分解温度。
24.如权利要求21所述的陶瓷,其中,所述第一产物由离子取代、离子加成、歧化作用或它们的组合生成。
25.如权利要求21所述的陶瓷,其中,所述第一产物由沉淀生成。
26.如权利要求21所述的陶瓷,其中,所述陶瓷是水泥。
27.如权利要求21所述的陶瓷,其中,所述第一产物包括羧酸盐。
28.一种制造陶瓷的方法,所述方法包括:
(i)提供具有预定形状和尺寸以及间隙的并且包括至少第一反应物的多孔基质;
(ii)使所述多孔基质与含有至少第二反应物的渗入介质接触,所述渗入介质包括温室气体;
(iii)在促进所述至少第一反应物与所述至少第二反应物反应以提供至少第一产物的条件下,让渗入介质渗入所述多孔基质的至少部分内部空隙;以及
(iv)允许所述至少第一产物形成并填充所述多孔基质的至少部分间隙,从而生成陶瓷,
其中,所述方法消耗大量温室气体并不释放大量温室气体,且其中所述陶瓷具有至少1000℃的分解温度。
29.如权利要求28所述的方法,其中,步骤(ii)至步骤(iv)重复至少一次。
30.如权利要求28所述的方法,其中,所述陶瓷基本不具有水硬性结合。
31.如权利要求28所述的方法,其中,所述陶瓷不含有大量钛酸钡。
32.如权利要求28所述的方法,其中,所述温室气体从工厂得到。
33.如权利要求28所述的方法,其中,所述陶瓷基本不含裂纹。
34.一种螯合温室气体的方法,所述方法包括:
(i)提供含有至少一种温室气体的溶液作为第一反应物;
(ii)提供具有预定形状和尺寸以及间隙并且包括至少第二反应物的多孔基质;
(iii)在促进至少第一反应物与所述至少第二反应物反应以提供至少第一产物的条件下,让含有所述至少第一反应物的溶液渗入所述多孔基质的至少大部分间隙;以及
(iv)允许所述至少第一产物形成并填充所述多孔基质的至少部分内部空隙,从而螯合温室气体。
35.如权利要求34所述的方法,其中,所述温室气体溶于所述溶液。
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