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1. 发明公开

EP2684856A1 A method for methanation of gasification derived producer gas on metal catalysts in the presence of sulfur 审中-公开
标题翻译：一种用于气体从气化制造商在硫的存在下得到的上金属催化剂甲烷化过程
公开(公告)号：EP2684856A1
公开(公告)日：2014-01-15
申请号：EP12175567.2
申请日：2012-07-09
申请人： Paul Scherrer Institut
发明人： König, Christian Felix Julian , Schildhauer, Tilman J. , Nachtegaal, Maarten , Kaufman Rechulski, Marcelo Daniel , Biollaz, Serge
IPC分类号： C07C1/04 , C07C9/04 , C10L3/06
CPC分类号： C10L3/08 , C10L3/103 , C10L3/104
摘要： The present invention discloses a method for catalytic production of a methane-rich gas mixture from sulfur-containing synthesis gas with simultaneous at least partial sulfur removal, thereby:
a) producing a synthesis gas mixture;
b) bringing said synthesis gas mixture into a contact with a methanation catalyst thereby continuously deactivating the methanation catalyst by sulfur and/or carbon species comprised in the synthesis gas mixture in one part of the methanation process, while a part of said depleted methanation catalyst is simultaneously regenerated by oxidation in a different part of the process;
c) the methanation catalyst is a metal, a metal oxide, a metal sulfide or a mixture of metals, metal oxides or metal sulfide/nitride/phosphide on a support;
d) said metal or metals are selected from a group comprising Ni, Ru, Mo, Co, Fe, Rh, Pd, Pt, Ir, Os, W, V, wherein the support is an oxide of a group comprising Al 2 O 3 , SiO 2 , TiO 2 , CeO 2 , ZrO 2 , carbides, nitrides, phosphides or a mixture thereof, wherein
e) the metal or metals can be promoted by one or more of the following elements: K, P, Na, Ba, Ni, Ru, Rh, Co, Pt, Pd, Ir, W, Os, V, Mn.
The method achieves a nearly complete methanation of CO in the presence of both organic and inorganic sulfur compounds, such as olefins, tars etc., combined with an at least partial uptake of sulfur followed by a relatively fast oxidative regeneration of the methanation catalyst (bed material) and sulfur release, preferably at a temperature level near the methanation temperature.
摘要翻译：本发明盘松动了一种用于催化生产由含硫合成气的富含甲烷的气体混合物与同时至少部分脱硫的，从而：a）生产的合成气混合物; b）使所述合成气混合物与甲烷化催化剂从而连续停用通过硫和/或在甲烷化过程的一个部分中的合成气混合物由碳物种的甲烷化催化剂的接触，而所述的部分耗尽甲烷化催化剂是通过在过程中的不同部分氧化同时再生; c）该甲烷化催化剂是金属，金属氧化物，金属硫化物或金属，金属氧化物或金属硫化物在载体上的/氮化物/磷化物的混合物; d）所述金属或金属选自一组包含Ni，钌，钼，钴，铁，铑，钯，铂，铱，锇，W，V，worin支承是一组由Al 2 O 3的氧化物中选择的SiO 2，TiO 2的，的CeO 2，ZrO 2的，碳化物，氮化物，磷化物或它们的混合物，worin E）的金属或多种金属可以被一个或多个下列元素来促进：K，P，钠，钡，的Ni，钌，铑，钴，铂，钯，铱，W，锇，V，Mn等。该方法实现了CO的有机和无机硫化合物，发色的存在几乎完全甲烷化：如烯烃，焦油等，具有组合（用于随后一个甲烷化催化剂床的相对几乎氧化再生硫的至少部分吸收材料）和硫释放，优选地在靠近甲烷化温度的温度水平。

2. 发明公开

EP4450483A1 METHOD AND SYSTEM FOR FLEXIBLE PRODUCTION OF HYDROGEN AND HYDROCARBONS FROM PRODUCT GAS 审中-公开
公开(公告)号：EP4450483A1
公开(公告)日：2024-10-23
申请号：EP23168162.8
申请日：2023-04-17
申请人： PAUL SCHERRER INSTITUT
发明人： Schildhauer, Tilman J.
IPC分类号： C07C29/151 , C10B53/00 , C10B53/02 , C10B53/07 , C10J3/00 , C10K1/02 , C10K1/32 , C10K3/04 , B01D53/14
CPC分类号： C10B53/00 , C10B53/07 , C10B53/02 , C10K1/32 , C10K1/024 , C10K3/04 , B01D53/1462 , C10K1/30 , C10J3/46 , C10J2300/09220130101 , C10J2300/091620130101 , C10J2300/097620130101 , C10J2300/161220130101 , C10J2300/165620130101 , C10J2300/166520130101 , C10K1/004 , C10K1/005 , C10J2300/095620130101 , C10J2300/095920130101 , C10J2300/180720130101 , B01J23/80 , B01J23/28 , C10K1/18 , C10K1/16 , C10J3/463 , C10J3/06 , C10K1/26 , C07C29/1518
摘要： It is desirable to design a plant such that it is flexible with respect to the product spectrum and to flexible integration of hydrogen as fuel besides biomass, while minimizing the capital costs by e.g. multipurpose reactors. Even on the feedstock side, some flexibility could be useful, i.e. using besides hydrogen also CO2 as feed for the production of storable energy carriers, e.g. hydrocarbons, while using the stored energy carrier at least as partial feedstock in times when hydrogen production is desired.
This objective is achieved according to the present invention by a method/system for producing hydrogen and/or methanol, comprising :
a) thermochemically converting in terms of gasification and/or pyrolysis a carbonaceous feedstock from biomass or wastes yielding a product gas that comprises at least CO, H2 and optionally unsaturated hydrocarbons, such as ethylene, acetylene, benzene;
b) optionally providing a gas cleaning section to remove catalyst poisons, e.g. Sulphur species, from the product gas;
c) bringing the product gas into a fluidized bed reactor and reacting the product gas in the presence of a catalyst and/or a sorbent based on e.g. copper, molybdenum and/or iron that supports the conversion of CO and H2O to hydrogen and CO2 or to methanol depending on the operation conditions that are controllable in terms of the catalyst and/or sorbents used and/or the pressure and/or the temperature and/or the heat exchange in the fluidized bed reactor;
d) guiding the reacted product gas to an upgrading section that comprises a particle filter, an optional condensation step and at least one separation unit, such as a membrane, a scrubber, an absorption, a pressure swing adsorption or a temperature swing adsorption, a chemisorption, a liquefaction or combinations thereof, thereby separating a hydrogenrich stream or a methanol-rich stream from the effluent of the fluidized bed reactor.
This method and this system thus allow to use one single fluidized bed reactor to flexibly decide for the production of hydrogen or methanol thereby enabling a production that for example is enabled to reflect the availability of green hydrogen and/or renewable energy.

3. 发明公开

EP2977103A1 Synthetic natural gas production using a carbon resistant, promoted supported catalyst 审中-公开
标题翻译： Herstellung von synthetischem Erdgas mit einemkohlenstoffbeständigen，promoteierten undgeträgertenKatalysator
公开(公告)号：EP2977103A1
公开(公告)日：2016-01-27
申请号：EP14178004.9
申请日：2014-07-22
申请人： Paul Scherrer Institut
发明人： Schildhauer, Tilman J. , Kampolis, Anastasios , Kröcher, Oliver
IPC分类号： B01J23/755 , C10K3/04 , C10L3/08 , B01J21/04 , B01J21/02
CPC分类号： C10K3/04 , B01J23/002 , B01J23/755 , B01J37/0201 , B01J37/0205 , B01J37/18 , B01J2523/00 , C10L3/08 , Y02E50/343 , B01J2523/305 , B01J2523/31 , B01J2523/828 , B01J2523/847
摘要： It is therefore the objective of the present invention to provide a method for the production of SNG taking advantage from a catalyst which has a high selectivity for the catalytic reactions and achieves long lifetime of the catalyst due to minor clogging and strong carbon resistance to prevent its deactivation.
These objectives are achieved according to the present invention by a method to convert a CO and/or CO 2 comprising a gas mixture stemming from an industrial processes, such as gasification of carbonaceous feedstocks (i.e. biomass), pyrolysis, ore conversion, combustion, calcination or fermentation, wherein the gas mixture further comprises saturated hydrocarbons in concentrations above 15% and/or unsaturated hydrocarbons, such as olefins, tars and/or aromatic compounds, into a methane rich gas by bringing the gas mixture into a contact with a supported metal catalyst comprising:
a) as an active phase nickel and optionally cobalt, ruthenium, iridium, molybdenum, iron or any possible combination thereof,
b) as a promoter boron and optionally sodium, potassium, calcium, magnesium, boron, rubidium, barium, gallium, phosphorus or any possible combinations thereof, and
c) as a support alumina and optionally silica, titania, lanthana, zirconia, ceria, magnesia or any possible combination thereof.
The presented invention improves the carbon resistance of nickel catalysts for low temperature (250-400°C) applications such as the methanation. Polymeric carbon is formed by reaction of carbon atoms on the catalyst surface under locally hydrogen-deficient situations. These carbon atoms stem from dissociation of carbon oxides and hydrocarbons whereby unsaturated hydrocarbons (ethylene, acetylene) and CO lead to higher carbon deposition rates. Using presently the promoter boron in the nickel catalyst avoids the formation of intermediates for polymeric carbon. As a second benefit, the formation of nickel carbides and carbon whiskers is decreased, too.
摘要翻译：因此，本发明的目的是提供一种利用对催化反应具有高选择性的催化剂生产SNG的方法，并由于较小的堵塞和强的耐碳性而使催化剂寿命长，以防止其失活。根据本发明，通过转化CO和/或CO 2的方法来实现这些目的，所述CO和/或CO 2包括来自工业过程的气体混合物，例如碳质原料（即生物质）的气化，热解，矿石转化，燃烧，煅烧或发酵，其中气体混合物还包含浓度高于15％的饱和烃和/或不饱和烃如烯烃，焦碳和/或芳族化合物，通过使气体混合物与负载金属接触而进入富含甲烷的气体催化剂包括：a）作为活性相镍和任选的钴，钌，铱，钼，铁或其任何可能的组合，b）作为助催化剂硼和任选的钠，钾，钙，镁，硼，铷，钡，镓，磷或其任何可能的组合，和c）作为载体氧化铝和任选的二氧化硅，二氧化钛，氧化镧，氧化锆，二氧化铈，氧化镁或任何可能的组合复查。本发明改进了镍催化剂对于低温（250-400℃）应用如碳化反应的耐碳性。在局部氢缺陷的情况下，通过碳原子在催化剂表面上的反应形成聚合碳。这些碳原子源于碳氧化物和烃的解离，因此不饱和烃（乙烯，乙炔）和CO导致更高的碳沉积速率。目前使用镍催化剂中的促进剂硼避免形成聚合碳的中间体。作为第二个好处，镍碳化物和碳晶须的形成也减少了。

4. 发明公开

EP4311852A1 PROCESS IMPROVEMENT UPGRADING IN POWER-TO-X (PTX) PROCESSES 审中-公开
公开(公告)号：EP4311852A1
公开(公告)日：2024-01-31
申请号：EP22187488.6
申请日：2022-07-28
申请人： Paul Scherrer Institut
发明人： Schildhauer, Tilman J.
IPC分类号： C10L3/08 , C10L3/10 , B01D53/22
摘要： Thus, the objective of the present invention is to provide a method and a system for the optimization of the part load capabilities of a biogas based PtX conversion that offer a better capability of using hydrogen that is generated or has not been used in the methanation process for further process steps, such as a recycling into the methanation process.
This objective according to the present invention by a method and a system (2) for the optimization of the part load capabilities of a biogas based PtX conversion, comprising:
a) a fluidized bed reactor (18) enabled to convert biogas into a CH4-enriched product gas stream (16);
a) a regular membrane upgrading unit (6) enabled to treat the CH4-enriched product gas stream (16) wherein the regular membrane upgrading unit (6) at least comprises a main membrane (8) being enabled to separate CO2 from methane to yield injectable CH4 enriched gas and a CO2 cleaning membrane (10) being enabled to recover permeated methane downstream of the main membrane (8) from CO2; and
c) a polymeric gas separation membrane (4) being enabled to treat the CH4-enriched product gas stream (16) wherein the polymeric gas separation membrane (4) is in addition to the regular membrane upgrading unit (6) and is positioned downstream of the fluidized bed reactor (18) and upstream of the regular membrane upgrading unit (6).
By the provision of the additional polymeric gas separation membrane, the method and the system allow to increase the recycle rate of hydrogen in the process and therefore reduce its loss through the off gas stream. At the same time, the present invention also allows to decrease the slip of CH4 through the same path and reduce the energy loss through the off gas stream.

5. 发明公开

EP2484971A1 A process and a system for the gasification and/or combustion of biomass and/or coal with an at least partial carbon dioxide separation 审中-公开
标题翻译：方法和系统，用于气化和/或生物量和/或碳的燃烧与至少部分二氧化碳分离
公开(公告)号：EP2484971A1
公开(公告)日：2012-08-08
申请号：EP11153368.3
申请日：2011-02-04
申请人： Paul Scherrer Institut
发明人： Schildhauer, Tilman J.
IPC分类号： F23C10/02 , F23C10/04 , C10J3/84 , C10J3/48
CPC分类号： C10J3/84 , C10J3/463 , C10J3/725 , C10J2300/1246 , F23C10/005 , F23C10/04 , F23C99/00 , F23C2900/01001 , F23C2900/99008 , Y02E20/346 , Y02P20/145
摘要： A process for the gasification and/or combustion of biomass and/or coal with an at least partial carbon dioxide separation using a combined reactor (2) having a combustion part (6) and a gasification part (4), comprising the steps of:
a) feeding the coal and/or feeding biomass into the gasification part (4) of the combustion/gasification reactor (2);
b) in the gasification part (4) heating at an elevated temperature in order to generate a product gas (8);
c) filtering the product gas (8) to separate ash, soot and other solid particles from the product gas (8);
d) feeding the filtered product gas (8')and an oxidized bed material (20) into the combustion part (6) of the reactor (2);
e) in the combustion part (6), at least partially reducing the oxidized bed material (20) in order to generate heat that is being transferred partially into the gasification part (4);
f) leading the exhaust gas (16) of the combustion part (6) to a turbine or a heat exchanger or into a further combustion reactor (18) or a catalytic conversion and leading the at least partially reduced bed material (22) into an oxidation reactor 24 fed with air (26) in order to re-oxidize the bed material prior to its recirculation into the combustion part (6).
摘要翻译：一种用于气化和/或生物量和/或煤具有用于至少部分二氧化碳分离使用组合反应器的燃烧过程（2），其具有燃烧部分（6）和气化部分（4），包括以下步骤： a）将煤和/或生物质进料到气化部的燃烧/气化反应器（4）（2）; b）在气化部（4），以便产生一个产物气体在加热在升高的温度（8）; c）过滤所述产物气体（8）从产物气体（8）中分离灰，烟灰和其它固体颗粒; D）供给过滤的产物气体（8“），并在氧化床材料（20）进入反应器（2）的燃烧部（6）; E）（在燃烧部分（6），至少部分氧化的还原性的床材料20），以便产生热量被传送做部分地进入气化部（4）; F）导致燃烧部分（6）的涡轮机或热交换器或到另外的燃烧反应器（18）或一催化转化的废气（16）和至少部分还原的床料（22）通入在为了其再循环之前的床料再氧化到燃烧部分（6）与空气（26）进料到氧化反应器24。

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