CN109789365A - 从垃圾填埋气体中除去硅氧烷的方法 - Google Patents
从垃圾填埋气体中除去硅氧烷的方法 Download PDFInfo
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- -1 siloxanes Chemical class 0.000 title claims abstract description 51
- 238000000034 method Methods 0.000 title claims abstract description 21
- PNEYBMLMFCGWSK-UHFFFAOYSA-N Alumina Chemical compound [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 claims abstract description 26
- 239000003054 catalyst Substances 0.000 claims abstract description 22
- 230000000694 effects Effects 0.000 claims abstract description 8
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 claims abstract description 7
- 239000010813 municipal solid waste Substances 0.000 claims abstract description 5
- ZWYDDDAMNQQZHD-UHFFFAOYSA-L titanium(ii) chloride Chemical compound [Cl-].[Cl-].[Ti+2] ZWYDDDAMNQQZHD-UHFFFAOYSA-L 0.000 claims abstract description 5
- 238000011068 loading method Methods 0.000 claims abstract description 4
- 229910021536 Zeolite Inorganic materials 0.000 claims abstract description 3
- HNPSIPDUKPIQMN-UHFFFAOYSA-N dioxosilane;oxo(oxoalumanyloxy)alumane Chemical compound O=[Si]=O.O=[Al]O[Al]=O HNPSIPDUKPIQMN-UHFFFAOYSA-N 0.000 claims abstract description 3
- 239000004408 titanium dioxide Substances 0.000 claims abstract description 3
- 239000010457 zeolite Substances 0.000 claims abstract description 3
- 239000007789 gas Substances 0.000 claims description 32
- 239000003463 adsorbent Substances 0.000 claims description 11
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 claims description 8
- XLOMVQKBTHCTTD-UHFFFAOYSA-N Zinc monoxide Chemical compound [Zn]=O XLOMVQKBTHCTTD-UHFFFAOYSA-N 0.000 claims description 8
- ZOKXTWBITQBERF-UHFFFAOYSA-N Molybdenum Chemical compound [Mo] ZOKXTWBITQBERF-UHFFFAOYSA-N 0.000 claims description 6
- 229910052750 molybdenum Inorganic materials 0.000 claims description 6
- 239000011733 molybdenum Substances 0.000 claims description 6
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 claims description 5
- 239000003546 flue gas Substances 0.000 claims description 5
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 claims description 4
- PWHULOQIROXLJO-UHFFFAOYSA-N Manganese Chemical compound [Mn] PWHULOQIROXLJO-UHFFFAOYSA-N 0.000 claims description 4
- 239000010941 cobalt Substances 0.000 claims description 4
- 229910017052 cobalt Inorganic materials 0.000 claims description 4
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 claims description 4
- 229910052802 copper Inorganic materials 0.000 claims description 4
- 239000010949 copper Substances 0.000 claims description 4
- 229910052748 manganese Inorganic materials 0.000 claims description 4
- 239000011572 manganese Substances 0.000 claims description 4
- 229910052759 nickel Inorganic materials 0.000 claims description 4
- 239000011787 zinc oxide Substances 0.000 claims description 4
- XHCLAFWTIXFWPH-UHFFFAOYSA-N [O-2].[O-2].[O-2].[O-2].[O-2].[V+5].[V+5] Chemical compound [O-2].[O-2].[O-2].[O-2].[O-2].[V+5].[V+5] XHCLAFWTIXFWPH-UHFFFAOYSA-N 0.000 claims description 3
- 229910052760 oxygen Inorganic materials 0.000 claims description 3
- 239000001301 oxygen Substances 0.000 claims description 3
- 238000000746 purification Methods 0.000 claims description 3
- 229910001935 vanadium oxide Inorganic materials 0.000 claims description 3
- 239000004411 aluminium Substances 0.000 claims description 2
- 229910052782 aluminium Inorganic materials 0.000 claims description 2
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 claims description 2
- 229910000420 cerium oxide Inorganic materials 0.000 claims description 2
- BMMGVYCKOGBVEV-UHFFFAOYSA-N oxo(oxoceriooxy)cerium Chemical compound [Ce]=O.O=[Ce]=O BMMGVYCKOGBVEV-UHFFFAOYSA-N 0.000 claims description 2
- 238000011144 upstream manufacturing Methods 0.000 claims description 2
- MYMOFIZGZYHOMD-UHFFFAOYSA-N Dioxygen Chemical compound O=O MYMOFIZGZYHOMD-UHFFFAOYSA-N 0.000 claims 1
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- 229910003978 SiClx Inorganic materials 0.000 claims 1
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- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 abstract description 15
- 239000000377 silicon dioxide Substances 0.000 abstract description 7
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- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 4
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- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 2
- RWSOTUBLDIXVET-UHFFFAOYSA-N Dihydrogen sulfide Chemical compound S RWSOTUBLDIXVET-UHFFFAOYSA-N 0.000 description 2
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 2
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 description 2
- 229910002808 Si–O–Si Inorganic materials 0.000 description 2
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- 229910052710 silicon Inorganic materials 0.000 description 2
- 239000010703 silicon Substances 0.000 description 2
- 238000001179 sorption measurement Methods 0.000 description 2
- 229910052682 stishovite Inorganic materials 0.000 description 2
- 229910052717 sulfur Inorganic materials 0.000 description 2
- 239000011593 sulfur Substances 0.000 description 2
- 229910052905 tridymite Inorganic materials 0.000 description 2
- 241000894006 Bacteria Species 0.000 description 1
- 239000003082 abrasive agent Substances 0.000 description 1
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- 239000003513 alkali Substances 0.000 description 1
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 1
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- 239000003610 charcoal Substances 0.000 description 1
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- 125000004122 cyclic group Chemical group 0.000 description 1
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- 229910052500 inorganic mineral Inorganic materials 0.000 description 1
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- 238000004519 manufacturing process Methods 0.000 description 1
- 239000011707 mineral Substances 0.000 description 1
- 239000010841 municipal wastewater Substances 0.000 description 1
- 229910052757 nitrogen Inorganic materials 0.000 description 1
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- 239000002245 particle Substances 0.000 description 1
- 229920001296 polysiloxane Polymers 0.000 description 1
- 239000002516 radical scavenger Substances 0.000 description 1
- 230000001172 regenerating effect Effects 0.000 description 1
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- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 1
- 229910001845 yogo sapphire Inorganic materials 0.000 description 1
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Abstract
在从沼气流，特别是垃圾填埋气流或来自厌氧消化器的气流中去除硅氧烷的方法中，首先使气流通过常规的硅氧烷去除单元以除去大部分硅氧烷，随后使其通过选定的具有精处理效果的催化剂，从而除去残留的痕量硅氧烷。具有精处理效果的催化剂选自沸石、多孔二氧化硅、二氧化钛、以及氧化铝或二氧化钛负载的各种金属。
Description
技术领域
本发明涉及一种用于从垃圾填埋气体中除去硅氧烷的新方法以及在该·方法中使用的催化剂。
发明背景
垃圾填埋气体是源自垃圾填埋场的气体，该气体由垃圾填埋场本身的各种细菌消化过程中产生。该气体一般含有大约45-50％的CH4、45％-50％的CO2、至多1％的H2S、一些氮和硅氧烷以及低水平的有机硫组分和挥发性有机碳(VOC)化合物。垃圾填埋气体具有高的能量含量，通常用作燃气发动机的燃料，尽管较小的燃气涡轮机和锅炉也可以使用垃圾填埋气体进行运作。在一些情况下，气体被升级，并被输出到公共气体网格，或者将其用作其他工业过程中的燃料气体。目前的主导市场是美国，往复式燃气发动机在垃圾填埋气体利用市场中占主导地位。
硅氧烷是包含硅、碳、氢和氧的有机硅化合物，其具有Si-O-Si键。硅氧烷可以是线性的也可以是环状的。它们可以存在于沼气中，因为它们用于各种个人护理和美容产品，例如化妆品和洗发剂，其被冲洗排掉或以其他方式处理，藉此最终进入城市废水和垃圾填埋场。硅氧烷在厌氧消化过程中不会被分解，因此，从处理厂和垃圾填埋场捕获的废气通常会被这些化合物严重污染。
多年来，从填埋气体中除去硅氧烷成为一个越来越重要的问题。
已知通过使用具有活性炭或多孔二氧化硅作为吸附剂的非再生性填充床吸附可以除去硅氧烷。也可以使用再生性吸附剂，以及基于气体冷却至极低温度的单元，以将硅氧烷从气体中沉淀出来。此外，使用液体提取技术。此外，这些技术可以组合使用。
因此，除了提供具有足够低的硫含量(即小于几百ppm)的气流之外，来自填埋场和厌氧消化器的原料气的利用的主要问题是提供硅氧烷(通常为线性或环状二甲基Si-O-Si化合物)含量非常低的气流。特别地，硅氧烷会引起问题，因为它们在燃烧过程中会转化为SiO2，导致发动机内部的磨料固体沉积物累积，造成损坏，缩短使用时间，并增加许多部件如火花塞、阀门等的维护要求。除了造成损坏和缩短发动机的使用时间之外，为了控制废气排放而安装的任何催化剂也对夹带在气流中的SiO2敏感，实际上甚至比发动机本身更敏感。例如，对于SCR(选择性催化还原)催化剂，SiO2耐受性可低至250ppb。
在垃圾填埋气体工业中已知的是，吸附剂，如活性炭、二氧化硅或氧化可用于除去存在于气体中的硅氧烷。这些吸附剂可用作清除剂，或者它们可利用变温吸附来用于再生的工艺配置。
由于上述原因，期望从气流中除去硅氧烷和含硫化合物，以增加发动机的使用时间和催化剂寿命。因此，多个专利和专利申请都涉及这个问题。因此，WO2008/024329A1公开了一种系统，其包括用于将硅氧烷从沼气中除去至非常低的硅氧烷水平的吸附床，使得净化的沼气可用作设备(例如内燃机或燃气涡轮机)的进气。吸附床包含活性炭、硅胶和分子筛中的至少两种。
US 7.393.381 B2描述了使用称为选择性活性梯度(SAGTM)的基于矿物的吸附介质来从气流中除去硅氧烷，US 7.410.524 B2公开了用于除去硅氧烷和挥发性有机碳的可再生的纯化系统(SWOPTM)。这些系统可以组合成流化床中的连续SWOPTM吸附再生，然后是几个SAGTM容器。
US 2010/0063343A1描述了从填埋气体中净化和回收甲烷燃料，更具体地说，是从填埋气体中浓缩和去除某些常见污染物的方法。处理的有害成分包括水、颗粒、硫(作为硫化氢)和硅氧烷。
在US 9,039,807 B2中，描述了另一种用于除去硅氧烷的再生吸附方法。该方法使用具有中性表面的吸附剂，并且其在约35-50℃的温度下使用。当吸附床已经充满容量时，将其加热以除去硅氧烷并使床再生。
Urban.W等人在Journal of Power Sources vol.193,359-366(2009)中公开了一种从填埋气流中除去硅氧烷的方法，其中气流首先通过常规的硅氧烷去除单元(该单元是基于Al2O3的吸附剂)，以去除大部分硅氧烷，随后使其通过基于V2O5/TiO2的催化剂，以除去许多其它有害的有机次要化合物。
在US 9.217.116中公开了从沼气流中除去硅氧烷的类似方法，其中气流首先通过包含在金属氧化物载体上的V2O5的氧化催化剂，其中催化剂氧化85％或更多的硫和卤化化合物，随后使其通过含有碱浸渍的碳的污染物去除模块，该模块除去85％或更多的酸性反应产物。如果沼气中存在硅氧烷杂质，则可以使用含有Al2O3的污染物去除模块。
US 2012/0301366公开了沼气中硅氧烷和硫化氢的微波诱导破坏，而US 2015/0209717描述了通过吸附从气流中除去硅氧烷和相关化合物的方法。
EP 1 316 350 A1描述了将硅氧烷催化转化为极性化合物并随后进行洗涤，以及DE 10 2004 051 807 A1描述了在选择的疏水硅胶上进行吸附。
最后，从US 9,217,116 B2中已知在沼气净化系统中使用包含在金属氧化物载体上的V2O5的催化氧化催化剂。催化剂氧化沼气中存在的85％或更多的硫和卤化化合物。沼气净化系统可包括含有氧化铝的污染物去除模块，以在除去硫和卤化化合物之前除去部分(即其85-98％)硅氧烷化合物。硅氧烷引起锅炉、燃气发动机和燃气涡轮机的问题，导致设备过度磨损、结垢和频繁润滑换油。此外，已知硅氧烷严重毒害在填埋气体处理和烟道气处理中使用的催化剂。众所周知，基于氧化钒的金属氧化物催化剂容易被存在于从填埋气体到发电厂的烟道气中的硅氧烷毒害。
发明内容
本发明构思的基础在于：(1)使用在300至450℃的温度下操作的基于氧化铝的吸附剂，以吸附存在于填埋气体中的大部分硅氧烷；和，(2)随后使用也在300至450℃的温度下操作的特别选择的催化剂作为精处理剂(polisher)，以从气体中除去任何残留的痕量硅氧烷。该精处理催化剂更具体地选自沸石；多孔二氧化硅；二氧化钛；氧化铝负载的镍；氧化铝负载的锰；氧化铝负载的钼；氧化铝负载的钴；氧化铝负载的钴、钼和镍中的任何一个或全部的组合；氧化铝负载的铜和锰；二氧化钛负载的氧化钒；二氧化钛负载的钼；氧化锌；负载在氧化锌上的铜；以及氧化铈。
因此，本发明涉及从沼气流，特别是垃圾填埋气流或来自厌氧消化器的气流中除去硅氧烷的方法，其中气流首先通过常规的硅氧烷去除单元，然后通过选定的具有精处理效果的催化剂，从而去除任何残留的痕量硅氧烷，并且其中该具有精处理效果的催化剂选自上述提及的那些催化剂。
包含基于氧化铝的吸附剂的硅氧烷去除单元在300至450℃的温度下操作，在该温度下大部分硅氧烷被吸附。所选定的具有精处理效果的催化剂也在300至450℃的温度下操作。
在300至450℃的温度下进行硅氧烷去除所需的热量是通过燃烧来自该单元的一部分净化产物填埋气体来提供，该燃烧提供热的烟道气，该热的烟道气使硅氧烷去除反应器上游的工艺气体加热，并且以这种方式，其能够使用丰富的垃圾填埋气体作为燃料，而且同时避免二氧化硅在这种燃气加热器中沉积。
Claims (5)
1.一种用于从沼气流特别是垃圾填埋气流或来自厌氧消化器的气流中除去硅氧烷的方法，其中使气流首先通过常规的硅氧烷去除单元以除去大部分硅氧烷，随后使其通过选定的具有精处理效果的催化剂，从而除去任何残留的痕量硅氧烷。
2.根据权利要求1所述的方法，其中所述具有精处理效果的催化剂选自沸石；多孔二氧化硅；二氧化钛；氧化铝负载的镍；氧化铝负载的锰；氧化铝负载的钼；氧化铝负载的钴；氧化铝负载的钴、钼和镍中的任何一个或全部的组合；氧化铝负载的铜和锰；二氧化钛负载的氧化钒；二氧化钛负载的钼；氧化锌、氧化锌上负载的铜；以及氧化铈。
3.根据权利要求1所述的方法，其中所述硅氧烷去除单元包括基于氧化铝的吸附剂。
4.根据前述权利要求中任一项所述的方法，其中所述硅氧烷去除单元和具有精处理效果的催化剂均在300至450℃的温度下操作。
5.根据权利要求4所述的方法，其中通过燃烧来自所述硅氧烷去除单元的一部分净化产物填埋气体来提供在300至450℃的温度下去除硅氧烷所需的热量，并且提供使来自硅氧烷去除反应器上游的工艺气体加热的热的烟道气。
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| EP3525916A1 (en) | 2019-08-21 |
| US20190201842A1 (en) | 2019-07-04 |
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