TW200813209A - Operation of a steam methane reformer by direct feeding of steam rich producer gas from steam hydro-gasification - Google Patents

Operation of a steam methane reformer by direct feeding of steam rich producer gas from steam hydro-gasification Download PDF

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TW200813209A
TW200813209A TW096126103A TW96126103A TW200813209A TW 200813209 A TW200813209 A TW 200813209A TW 096126103 A TW096126103 A TW 096126103A TW 96126103 A TW96126103 A TW 96126103A TW 200813209 A TW200813209 A TW 200813209A
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Taiwan
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steam
gas
syngas
smr
pressure
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TW096126103A
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English (en)
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Joseph M Norbeck
Chan-Seung Park
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Univ California
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Publication of TW200813209A publication Critical patent/TW200813209A/zh

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Description

200813209 九、發明說明： 相關申请案之相互參照 本案係2006年7月 11/489,3〇8的部分連續案， 【發明所屬之技術領域】 本發明的領域為從碳 料。 18曰申請的專利申請案序號 並且主張該案之優先權。 質原料（feed stock)合成運輸燃 【先前技術】 的以石、、由2包料境、健康、安全議題及將來無可避免 因而需要鐘別新的==的許多關心的 料的方法。全世及將其轉化成錢性運輸燃 增長，特ft ΐ料的内燃機交通"·具的數目持續 要使用柴油的交通工種。關以外全世界主 進使用$人 ，、矢群成長侍比美國内地更快。當引 工呈以π : 1及/或柴油引擎技術之更具燃料效率的交通 ，、乂同日文降低燃料消耗及 改變。因為用於^ 文’此情;兄將可獲得 當中，因此除非門私山北 科之貝源正逐漸耗竭 燃燒的合成柴油 ，枓，将別是潔淨 問通。再者，傳統引擎中以石油為主 的 造成嚴重的璟产+ α \ 的正常燃燒會 法。潔淨^嚴袼的廢氣排放控制辦 放。义、口成木油燃料將會助於降低柴油引擎的排 潔淨鐵燒的運輸燃料之製造需要重新調配現有以石油 94049 5 200813209 ‘為主的燃料或者於 '料的新方法。有二多的材:…力或合成燃 為經濟可行的方法 /茶物末產生5成燃料 有價值，當作廣辛物祐I原料已經被認定為幾乎沒 F仏莱物被抱棄，而且虛姐 — 可使用煤炭當作原料以將 1 、、二有万乐。或者， 加價值的傳缔生、…万木的固體燃料升級成具附 摘值的傳統澄清液態燃料，例 油或其他烴燃料。 、衣保的&成柴 幹輸燃料具有優於氣態燃料的固有優點，液態運 :燃=相同壓力與溫度時具有比氣態燃料更高的能量ί mi錢，㈣_則必須以高壓儲存在交通工且 的儲才曰中’且若發生线漏或突然破裂的狀況將會有安全的 ^慮。液態燃料的分配係使用簡單的泵及輸送管路，比氣 態燃料容易許多 '現有運輸部門的液態燃料補給基礎設施 (mf^tructure)將確保皆能輕易整合至任何潔淨燃燒的合 成液態運輸燃料製造的現有市場。 潔淨燃燒的液態運輸燃料的可取得性係國家級的優先 事務。由碳質來源潔淨地且有效地製造合成氣（氫與一氧化 碳的混合物，亦稱之為合成氣），該等碳質來源可經施行費 -托型製程（Fischer-Tropsch type process)而製造潔淨而且 有價值的合成汽油及柴油燃料，將同時有益於運輸部分及 社會健康。費-托型製程或反應器，在本文中將其界定為分 別包括費-托製程或反應器，為任何使用合成氣來製造液態 94049 6 200813209 燃料的製程或及雍哭、。m ^ , £製程或反應哭所二\ 型液態燃料為經由此 理法應一還原、將存在== 擎震氧中的母性微粒移除以及將正常 量，現有製程是藉由觸婵來6W 物万木物減 的硫迅速毒化寺觸媒會被任何存在 把在曰通石油衍生的柴油燃料原料的情 广而~低觸媒的效率。典型地，由合成 托型液態燃料為不含硫、入4 '、斤衣k之費_ >情妒中且不合方香族且在合成柴油燃料的 ~有起兩的十六焼值。 =質⑽mass)材料為詩製造可再生燃料中最常 被处理的石反質廢棄物原料。廢棄 物殘餘物、林*、_^伐物及來自廢水(二二二乍 生質固體物（biosolid)亦4 g # 处—— 貝原料可經轉化而產生電力、勿 料。在數種生物質利用w田有仏值的化學製品或燃 周宏H L 與發展方面，加州超越 S豕之上。母年在加孙|，丄 丄『夕私就！由廢棄物管制設備的處理而 a樾茶夕於45百萬噸的都市固靜淼*此 丰數f|帀口脰廢茱物。此廢棄物將近 手數取、、S都达到垃圾掩埋場。舉例 4 維塞德市（Riverside County)，據估二十々 口、土區的利 廢棄木料。根據其他的推估，每夭计告母天抱棄約4000 °頓的 ^ 推估母天超過1〇〇,〇〇〇噸的生物 質被傾倒到利維塞德市隼中 、〕生物 物勺人的M0/广古 圾掩埋場。此都市廢棄 物包含約30%廢棄紙張啖铋 ^飞、我板40%有機（綠色及食物）廢 Β Η、Λ,氏張、塑膠及金屬棄物的組合。若可將 其車Τ化為減淨燃燒燃料的話 活此廢茶材料的碳質成分將具 94049 7 200813209 有可用於降低其他能源需求 ‘棄物來源並非唯一可取…予一些碳質材料的廢 /輋純/ 的來源。儘管許多現有的碳質事 =，!Γ紙張’可經分類、再利用及再循環作為其他 造::二;Γ直接被運送至轉化設備的話，輸 it將不而要付垃圾傾倒費。 圾傾倒費，現在每们。至35:g制局通常要收取垃 ,^ ^ 主35吴兀，以彌補處理成本。因 棄物運輪至「廢棄物變合成燃料」加工廠不 僅月b IV低處理成本’由於降 能利用。 &的處理成本頜外的廢棄物還 例子盧中燃燒木料為使用生物質產生熱能的簡單 並非利用:開放式燃燒生物質廢棄物以獲得能量及執 非利用熱值㈣Grifie value)之潔淨且有效的方法。入 -種:ΐ::許多爾質廢棄物的新方式。舉例來說： ㈣化ίίΓ造合成液態運輸燃料，而另一方式為製造用 於轉化為電力的高能氣體。 氣體η自可再生生物質來源的燃料實際上可降低溫室 :义心：减碳的淨累積’同時提供用於運輸的潔淨、 ^效的此置。從生物質來源共同製造（co_produc—合成液 處之一為其可提供可儲存的運輪燃料同時 ““成王球暖化的溫室氣體效應。未來，這些共同雙造 的方法將可提供用於能持續不斷的可再生 二 燃燒燃料。禹之〆系乎 以多將煤及其他石炭質材料轉化為潔淨燃燒的運 輸九、、枓之方法，但是彼等都太責以致於在市場上無法與以 94049 8 200813209 I 石油為主的燃料競爭，或彼等將產生揮發性燃料，例如甲 ‘醇及乙醇’該等揮發性燃料具有太高的蒸氣壓值而無法用 於南污染區’例如南加州空氣域，以致於無法從 潔淨空氣法規立法豁免。近期方法的例子為Hyn〇1甲醇製 程’其使用加氫氣化及蒸汽重組器反應器利用固態碳質材 料與天然氣的共進料來合成曱醇，而且其在實驗室規模示 範時具有> 85%之經證實的碳轉化效率。 更近期地’我們的實驗室發展出製造合成氣的方法， 馨其中係在產生富含發生氣的條件下將含碳質材料粒子在水 中的漿液及來自内部源（internal source)的氫飼入加氫氣化 反應器中。在產生合成氣的條件下將此與蒸汽一同飼入蒸 汽熱解重組器（pyrolytic reformer)中。此方法在Norbeck等 人的美國專利申請案序號1〇/5〇3,435 (公開為US 2005/0256212)，發明名稱：「使用自持加氫氣化從碳質材 料製造合成運輸燃料（Production of Synthetic 馨 Transporation Fuels From Carbonaceous Material Using Self-Sustained Hydro-Gasification)」中有詳細說明。在本 方法的另一版本中，係使用蒸汽加氫氣化反應器（SHR)在 氫及蒸汽二者存在之下同時加熱該碳質材料而在單一步驟 中進行蒸汽熱解及加氫氣化。此方法在Norbeck等人美國 專利申請案序號10/911,348 (公開為US 2005/0032920)，發 明名稱：「增進碳質材料的加氫氣化之蒸汽熱解方法（Steam Pyrolysis As A Process to Enhance The Hydro-Gasification of Carbonaceous Material)」中有詳細說明。將美國專利申 9 94049 200813209 請案序號10/503,435及10/911,348的揭示内容以引用方式 併入本文。 經由氣化製造合成氣及從合成氣製造液態燃料為絕然 不同的方法。本發明特別感興趣的是使用曱烷蒸汽重組器 (SMR)(其為廣泛被用於製造供液態燃料及其他化學品用 的合成氣之反應器）來製造合成氣。在SMR中進行的反應 可寫出如下。 CH4+H20 + CO+3H2 (1) 或 CH4+2H2O ^ C02+4H2 (2) 經由使用蒸汽及曱烷當作進料在該SMR中製造一氧 化碳及氫。在蒸汽產生器中將製程水加熱而產生所需的蒸 汽。該曱烷通常以壓縮天然氣的形式供應，或藉由來自化 學或精製製程的輕分子量排氣流的形式供應。 【發明内容】 本發明提供將蒸汽及甲烷供應至SMR的改良的經濟 替代性方法。該方法係藉由新程序的組合而完成，其中經 由利用氣體淨化單元（gas cleanup unit)從該SHR的產物流 (product stream)移除雜質而以來自SHR的產物氣體 (product gas)當作該SMR的原料，該氣體淨化單元在製程 壓力下操作而且位於該SHR與SMR之間。 在本發明之一具體實例中，使用SHR的產物氣體當作 SMR的原料。如上所述，此富含蒸汽及甲烷的產物氣體係 藉由碳質材料與水的混合物之漿液的加氫氣化產生。此產 10 94049 200813209 物氣體為富含甲烷的氣體與蒸汽的混合物（其中該蒸汽係 由於過度加熱原料令的水而存在），係作為81\/1尺的理想進 料流。 其他的程序必需從該SHR的產物流（product stream) 移除雜質，例如灰燼及焦炭的微細粒子、硫化氫（H2S)及其 他無機成分。這些雜質必須予以移除以防止用於該SMR 的觸媒之毒化。習慣上，為達此目的，係使用微粒過濾器、 溶劑清洗（胺類、Selexol™、Rectisol™)及藉由Claus製程 ⑩的加氫脫硫化的組合。在該Claus製程中，係利用在高溫 (1000至1400°〇的反應爐中的空氣局部氧化1128。形成 硫，但是有些H2S仍維持未反應，而且有些S02需要被製 造而使殘餘的H2S在較低溫度（約200至350°C)與S02在 觸媒上反應以製成更多硫。然而，因為該SMR進料流必 須維持在南溫，所以該氣流的再加熱將耗損相當大量的能 量。因此，這些傳統淨化技術就能量觀點來看係禁止的。 馨再者，喪失了經由保持來自該SHR產物流的蒸汽所提供的 益處。因此，在本發明的另一具體實例中，係提供在製程 壓力下操作而且位於該SHR與SMR之間的氣體淨化單元。 更特別的是，提供用於將碳質材料轉化成合成氣之方 法，該方法包含在足以產生富含曱烷及一氧化碳的氣體產 物流（其可被稱為發生氣（producer gas))的溫度與壓力下， 在氫及蒸汽二者存在之下同時加熱碳質材料。實質上是在 製程壓力以及比製程壓力時的水之沸點更高的溫度之下從 該發生氣流移除雜質，且在藉以產生包含氫及一氧化碳的 11 94049 200813209 ^ 合成氣之條件下對所得的發生氣體進行曱烷蒸汽重組。在 ‘ 一特定方法中，為了將都市廢棄物、生物質、木材、煤或 ， 天然或合成聚合物轉化成合成氣，係在約700t：至約900 °C的溫度及約132 psi (磅/平方吋）至560 psi (磅/平方吋） 的壓力下，在氳及蒸汽二者存在之下同時加熱碳質材料， 藉以產生富含曱烷及一氧化碳的發生氣流。在該製程壓力 及在比製程壓力時的水之沸點更高的溫度（可能實質上在 製程溫度）下從該發生氣流移除雜質，接著在藉以產生包含 •約3比1的H2 : CO莫耳比範圍之氫及一氧化碳的合成氣 之條件下對所得的發生氣進行甲烷蒸汽重組。具有鈷為主 的觸媒之費-托型反應器所需的H2 : CO莫耳比為2 : 1。因 此，有過量的氫，其可被分離並且飼入該SHR而進行自持 式製程（self-sustainable process)，亦即，不需要外部的氳 進料。經由該曱烷蒸汽重組所產生的合成氣可在藉以製造 液態燃料的條件下飼入費-托型反應器中。該費-托型反應 0的放熱可被轉移至該加氫氣化反應及/或甲烷蒸汽重組反 應。 【實施方式】 本發明提供程序的組合，其中，於本發明之一具體實 施例中，SMR的原料為藉由SHR中的碳質材料與水的混 合物之加氫氣化所產生之富含蒸汽與曱烷的產物氣體之混 合物。該蒸汽係由於過度加熱原料中的水而存在，而且係 作為SMR的理想進料流。 其他的程序需要從該SHR的產物流移除雜質的方 12 94049 200813209 p 法，該雜質為例如灰燼及焦炭的微細粒子、硫化氳（h2s) v 及其他無機成分。這些雜質必須予以移除以防止用於該 1 SMR的觸媒之毒化同時使該SMR進料流維持在其高製程 溫度。因此，在本發明的另一具體實施例中，提供了氣體 淨化單元，該氣體淨化單元係在製程壓力以及在比製程壓 力時的水之沸點更高的溫度下操作，而且係設置在該SHR 與SMR之間。 參照第1圖，顯示該方法的流程圖。將内部產生的氫 ⑩進料10連同碳質材料14及水16飼入SHR 12中，於菝SHR 12中將彼等在400磅/平方吋加熱至750°C。將所得的發生 氣引至在約400磅/平方吋及約35(TC的氣體淨化過濾器 1 8，例如燭式過濾器組合件（〇&11(116；[1116了&5 361111>1)0。從而， 移除硫及灰燼之後，將流出物引至SMR 20以產生合成氣 體並且飼入費-托型反應器22,從該費-托型反應器22獲得 純水24、柴油燃料及/或蠟26。將一部分氫從該SMR 20 參分流出，在28反饋入該SHR 12。使用來自該費-托型反應 器22的熱30來補充該SMR的熱。 在水的起泡溫度以上操作該單元，使水以蒸汽形式存 在於來自SHR的氣態產物流中，藉以使該方法（process)能 保有該流出物流大部分的顯熱。第2圖中顯示質量平衡方 法流程圖。該圖中提供該方法各階段的產物流質量百分 比。使用ASPEN PLUS™平衡製程模擬來計算這些值。 ASPEN PLUS™為商用電腦模擬程式ASPEN PLUS™，其能 經由載入該等化學成分及操作條件而建立製程模型。該程 13 94049 200813209 ，式記錄所有規格並且模擬該模型，執行要解析該系統的結 -果所需的所有必要計算’從而預測其表現。當該等計算完 •成之後，ASPEN PLUSTM將列出每種流及每個單元的結 果。如第2圖所示，氫及41%煤漿液的舰原料將導致該 通中產生具有氫對-氧化碳之莫耳比為34: i的合成 氣。該SHR所需的進料氫可經由外部機構（觸㈣或經由 該SMR所產生的部分氫之内部反饋供應。在特定的例子 中，使用41%煤、52%水及7%氫的黎液，該浆液係依循 Norbeck等人的美國專利序號1〇/911,348的程序獲得。 任何能在比於製程燃力時的水之沸點更高的溫度下操 作的過渡器都可使用。有一種此類商業上可講得的過滤器 為濁式過濾器，其在此技藝中眾所周知。舉例來說，來見 吴國專利案號5,474,586，其揭示内容在此以引用方式併入 可用於本發明之可購得的氣體淨化單元為據悉在過 ;思奋益中▼有一系列燭狀過濾器的燭式過濾器。該 過濾器係由不銹鋼金屬燒結體脚)製成以移除來自該= 流的微粒物質(灰燼、無機鹽及未反應的焦炭)。將該漿液 2:谷益的底部入口飼入並且在頂部出口取出遽液。微粒 慮餅形式從另-出口取出。存在於該shr產物氣體 、Ί、=部分呈硫化氫形式的硫雜質，係藉由使該產物氣體 =過該氣體淨化單元中的金屬氧化物吸附劑填充床而移 除，微粒物質從濾餅出口取出。 :性吸附劑包括’但不限於，以辞為主的氧化物例如 平、辛’由肯塔基州，路易斯維爾市的Sud_chemie販售。 94049 14 200813209 ^ 多孔性金屬過濾器構件可以適當的形式及尺寸自喬治亞 ' 州，瑪麗愛特市的Bekaert購得，例如Bekpor⑧Porous Media-其係由具有孔洞尺寸為1的不鎮鋼燒結纖維基質製 成。這些吸附劑及過濾器構件使壓降及氣-固質傳限制的效 應被降至最低。在28大氣壓的壓力時，以300°C至500°C 範圍的溫度及達到2000/小時的空間速度用於SHR產物氣 體的脫硫。該氣體的硫化氫含量係藉由該等吸附劑的硫化 而減小至低到足以避免該SMR觸媒去活化的程度。該氣 鲁體淨化單元中所用的吸附劑可使用新鮮的吸附劑來置換或 在並排的多吸覆床中利用稀釋的空氣在原地再生。 第3圖中顯示證實利用該SHR產物流的直接飼入而成 功操作SMR的實驗數據。以在該SMR出口測得的氣體濃 度對該SMR溫度作圖。當該SMR的溫度低時，在該SMR 出口觀察到的主要產物為曱烷（因為該SHR為唯一操作的 反應器）。當該SMR的溫度提高時，曱烷濃度將降低而且 書觀察到氫及一氧化碳濃度的相對應提高。該SMR中製成 的合成氣之最終組成具有3 : 1的H2 : CO莫耳比。更普遍 地，本發明的方法可製造具有2 : 1至6 : 1的H2 : CO莫 耳比範圍之合成氣組成。 所得的流出物為富含氫、一氧化碳及蒸汽的氣體之綜 合物（synthesis)。使該SMR中產生的氫中將近三分之一再 循環回該SHR。因此，不需要外界的氳來源來維持穩態操 作。因此，該SHR和SMR製程可視為化學自持性 (chemically self-sustaining)。剩餘的合成氣接著可用於燃 15 94049 200813209 一 料的製造及製程加熱。 在本舍明的具體貫例中，該合成氣係飼入可製造不含 •硫、超高十六烷值柴油類的燃料及有價值的石蠟產物的製程 之費-托型反應器中。硫不存在能實現排出低污染物及粒子 的柴油燃料。有用的副產物可被製成，舉例來說，純水，其 可被再循環以產生加入該製程的漿液進料。該費托反應亦 2衣、含有氫、CO、co2及-些輕質烴氣體的尾氣。氫可 從該尾氣被脫出來並且再循環至該·或費_托反應器。任 何小量的其他氣體例如C0及c〇2都可予以去除。 η、儘管已經詳細說明本發明及其優點，但是應了解在此 可進行各種艾更、取代及替換而不會悖離後附申請專利範 圍=界定的發明精神及範蜂。再者，並不意欲將本申請案 的耗臂限於說明書中所敘述的方法及裝置的特定具體例。 由於普通熟悉此技藝者將可輕易理解本發明的揭示内容， 所以可以根據本發明利用現在已存在或後續被發展出來的 :及裝置’該等方法及裝置係實質上執行相同的功能或 只貝上達到與本文所說明的對應具體例相同的結果。因 此^附的申請專利範圍意欲將此等方法及此等裝置之使 用包括在其範疇内。 【圖式簡單說明】 為了更完整了解本發明，現在伴隨附圖參照下列說 明，其中： 第1圖為本發明方法的流程圖； 第2圖為該方法的質量平衡流程圖；以及 16 94049 200813209 第3圖以圖形描述使用本發明及未使用本發明所製造 的成分。 【主要元件符號說明】 10 氫進料 12 SHR 14 碳質材料 16 水 18 氣體淨化過濾器 20 SMR 22 費-托型反應器 24 純水 26 柴油燃料及/或壤 28 還流線 30 熱 17 94049

Claims (1)

  1. 200813209 十、申請專利範圍： • Κ 一種用於將碳質材料轉化成合成氣之方法，勹 • 在足以產生富含甲烷及一氧化#&々包括· 溫度與壓力下，在氫及墓汽二者厌、虱體產物流的 材料； 者存在之下同時加熱碳質 從該發生氣流移除雜質；以及 …在藉以產生包括氫及一氧化碳的合成 對该所得的產物氣體進行甲燒蒸汽重电。 卞 \如申請專利範圍第1項之方法，其/，該雜”在^ 3. 二!更高的溫度下從該發生氣流錄: 圍…之方法，其中’該溫度為約· 其中，該雜質係實質上 其中，該壓力為約132 其中，該f垸蒸汽重組 4. 如申請專利範圍第1項之方法 在該壓力下從該發生氣流移除 5·如申請專利範圍第4項之方法· 碎/平方吋至560磅/平方吋。 6.如申請專利範圍第4之方法，具卜該甲燒& ^在藉以使所製造之合成氣的組成具有2 :ι至6:1的 2. c〇莫耳比範圍之條件下進行。 料利範圍第Μ之方法，其中，該甲燒蒸汽重組 録糟以使所製造之合成氣的組成具有3 :1的 旲耳比之條件下進行。 2 L如申請專利範圚坌 都市廢棄物、生二::法心其中，該碳質材料包括 物貝木材、煤或天然聚合物或合成聚 94049 18 200813209 合物。 • 9.:申請專利範圍第！項之方法，其中，經由該甲烷蒸汽 、、且所產生的合成氣係在藉以製造液態燃料的條件下 弓入費·托型反應器（Fischer_T卿sdl type reaetor)。 ::Γ將都市廢棄物、生物質、木材、煤或天然聚合 物或5成聚合物轉化成合成氣之方法，包括： 在約70CTC至約900。〇的溫度及约i 32碎/平 ΓΓ/Γ忖的壓力下，在氣及蒸汽二者存在之下同時 物^貝材枓’猎以產生富含甲燒及—氧化碳的氣體產 ▲沾貝貝上在該壓力及在比製程壓力時的水之沸點更 向的溫度下從該發生氣流移除雜質； 在藉以產生包括2 : 1至6 1 AA TT ^ 圍之_ β 一 — / 6 . 1的仏：CO莫耳比範 虱乳化碳的合成氣之條件下對所得 進行曱烷蒸汽重組；以及 在藉以製造液態燃料的條件下將經由該甲烷蒸汽 組所產生的合成氣飼入費_托型反應哭。 請專利範圍第10項之方法，包括i來自該費-托型 =的放熱轉移至該加氳氣化反應及/或甲 反應。 12.-種用於將碳質材料轉化成合成氣之裝置，包括： =產生富含甲烷及一氧化碳的氣體產物流的 =;^:，在氫及蒸汽二者存在之下同時加熱破質 材枓的加虱氣化反應器。 94049 19 200813209 13·如申請專利範圍第12項之裝置，包含用於接收該曱烷 蒸汽重組器所產生的合成氣以製造液態燃料之費-托型 反應器。 14.如申請專利範圍第13項之裝置，包含將來自該費-托型 反應的放熱轉移至該加氫氣化反應器及/或曱烷蒸汽重 組器的機構。
    20 94049
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