TWI634929B - 經改良之酸性氣體吸附 - Google Patents
經改良之酸性氣體吸附 Download PDFInfo
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- TWI634929B TWI634929B TW103144350A TW103144350A TWI634929B TW I634929 B TWI634929 B TW I634929B TW 103144350 A TW103144350 A TW 103144350A TW 103144350 A TW103144350 A TW 103144350A TW I634929 B TWI634929 B TW I634929B
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Abstract
本發明揭示一種用於從液體或氣體中移除酸性氣體污染物之吸附方法,該方法包括提供活性氧化鋁吸附劑,該吸附劑經選自由一或多種鹼金屬化合物、一或多種鹼土金屬化合物、或此等化合物之混合物組成之群的化合物浸漬;使該含有酸性氣體污染物之液體或氣體與該活性氧化鋁吸附劑接觸以充分吸附該液體或氣體中酸性氣體污染物以降低該液體或氣體之污染物含量,該氧化鋁吸附劑係由聚結之經煅燒氧化鋁粉末形成及具有至少0.10cc/g之大於500埃孔隙之汞孔隙體積。
Description
本發明係關於藉由在氧化鋁吸附劑上選擇性吸附酸性氣體而從液體或氣體物流中移除酸性氣體。
酸性氣體係諸如例如石油烴之材料中之非所需雜質,因為若干此等氣體諸如COS及H2S係硫源及由此係潛在大氣污染物。COS及H2S亦用作工業製程之非所需污染物,諸如例如,當該污染物存在於諸如丙烯之石油衍生之可聚合烯烴時藉由使聚合觸媒中毒而非所需。該酸性氣體可作為起初存在於原料中之污染物引入此等製程,或其等因二氧化碳與硫化氫或其他硫化合物之分子篩催化反應而在處理製程中形成。例如,酸性氣體可在天然氣物流中發現,及除成為污染物外,酸性氣體諸如COS、H2S、CO2、CS2、SO2、HCl、HF及HBr可腐蝕天然氣管道、管道設備、及其他化學處理裝置。
根據製程及需要之產物純度,起始材料中COS含量可需要減少至低於1重量百萬分率(ppmw)及有時至低於100重量十億分率(ppbw)之含量。在數ppmw範圍內之COS濃度不能有效地藉由分餾從諸如丙烯之石油原料中分離,此係由於COS之沸點與丙烯相差僅3.4℃。
Khclghatian於美國專利第3,315,003號教示一種用於從烴中移除COS之方法,該方法藉由首先使該烴與諸如單乙醇胺之液體接觸,該單乙醇胺擦洗該烴以移除酸性氣體諸如H2S及CO2及部分COS。隨後
蒸餾該烴。若干後續蒸餾後,該液體底部產物經鹼石灰處理以移除任何殘留COS。
然而,此外,藉由包括蒸餾之方法分離COS係非常昂貴,此歸因於用於蒸發實質上全部該液體之能量成本。由此,需要提供其他用於從有機液體中移除COS雜質之方法。
吾人亦提議藉由催化水解形成H2S而從烴中移除COS,例如,使用氧化鋁作為觸媒。Frcvcl等人於美國專利第3,265,757號教示包含於液體烴中之COS的水解,其藉由使該液體烴及水之混合物於20至50℃之溫度下與含有0.15至3重量%之鈉或鉀之高表面積鹼性、活性氧化鋁接觸。該專利權人申明,然而,若氧化鋁完全乾燥,則水解反應將不會開始。他們建議或者在反應前用無離子水潤濕該氧化鋁觸媒,或者使無離子水及該液體烴之混合物流經觸媒床直至充分數量水積累在氧化鋁上以允許水解反應進行。然而,雖然該方法確實移除COS(藉由將其轉化為H2S),但是該方法並沒有從烴中移除硫,而僅改變該硫化合物之形式,該硫化合物仍必須隨後藉由另一處理步驟從該烴中移除。
在處理相同類型反應之後續專利中,Pollcck等人於美國專利第4,491,516號教示若水與COS比範圍為1至10莫耳水/莫耳COS,較佳地1.5至6莫耳水/莫耳COS,或該烴之約30%飽和,無論何者上限提供較少量水,則利用水經氧化鋁水解COS之反應速率可極大提升。
Brownell等人於美國專利第4,455,446號教示藉由水解經氧化鋁上含硫化鉑之觸媒從丙烯中移除COS。該專利權人申明,水解反應可在氣相或液相進行,其中用於液相之溫度為35至65℃。亦必須存在至少兩倍於待水解COS化學計量量之水量。
Harris等人於美國專利第4,391,677號描述一種用於使包含亞硫雜質諸如H2S、COS、及CH3SH之富含丁烯-1原料脫硫之方法。該方法
包括使進料物流流經維持在脫硫條件下,及包含至少一種能將H2S、COS、及CH3SH吸附、吸收、或轉化為高沸點亞硫化合物之脫硫介質之進料之脫硫區。現基本上不含H2S、COS、及CH3SH之由此處理之進料物流隨後流經蒸餾區,及作為呈含高沸點亞硫化合物之富含丁烯-2物流之底部產物回收。該脫硫區包括活性氧化鋁床,接著氧化鋅床。據稱活性氧化鋁在20至1000ppm水存在時將COS水解為H2S及部分移除H2S及甲基硫醇。據稱氧化鋅移除未經氧化鋁床移除之全部H2S及甲基硫醇。
COS亦已藉由吸附在沸石吸附劑上而從液體烴中移除。Collins於美國專利第3,654,144號揭示藉由將COS吸附在經特定修飾之沸石A吸附劑上而移除COS,該吸附劑包括沸石A之鹼金屬陽離子形式,其已與鹼土金屬陽離子,較佳地鈣陽進行離子交換,交換程度至20至約100當量%。
Innes於美國專利第4,098,684號描述藉由使COS及其他硫化合物流經沸石雙床而移除COS及其他硫化合物,該等床分別包括13X分子篩、及具有4埃之孔隙尺寸之沸石A篩。據稱市售13X沸石移除任何存在之H2S及硫醇。據稱藉由13X篩之COS吸附之能力較小。該13X沸石經描述為具有通過孔隙開口獲得之含相互連接晶體內孔隙的三維網狀結構,其將容許臨界尺寸上至10埃及具有一般化學式0.83+-0.05Na2O/1.00Al2O3/2.48+-0.038SiO2之分子。該分子篩床可藉由使於約177至316℃之溫度下之實質上不可吸附之熱淨化氣體流經該床而再生。
雖然沸石材料由此已用作吸收劑以從液體烴中移除諸如COS之亞硫化合物,但是已發現具有籠狀結構之沸石在環境溫度下具有低吸附速率及因此在此等溫度下處理液體係不實用的。
由此,迫切需要提供一種用於從液體或氣體中移除酸性氣體包
括亞硫雜質諸如COS之方法,較佳地在不存在水時,使用具有高吸附特性亦能在上不實質損失吸附能力下再生之氧化鋁吸附劑。亦需要從液體或氣體中移除除COS外之酸性氣體至最低ppm含量。
Liu於U.S.4,835,338中提供一種經改良之從液體烴中移除羰基硫化物之方法,其藉由吸附在包括活性氧化鋁吸附劑之吸附介質上,隨後在達到吸附能力後使該活性氧化鋁再生。該活性氧化鋁吸附劑經選自由一或多種鹼金屬化合物、一或多種鹼土金屬化合物、或任何二或多種此等化合物之混合物組成之群的化合物預處理;隨後使用以從烴中吸附羰基硫化物;及隨後藉由使氣體流經該吸附劑而再生。可用活性氧化鋁係揭示為具有範圍為1/4英寸至100網目(150微米)之粒度之市售產品。在實務中,氧化鋁粒子藉由使5微米氧化鋁粉末聚結成適用於該吸附方法之較大粒子而形成。
本發明之目的係提供一種經改良之從液體或氣體中移除酸性氣體之方法,其包括將該酸性氣體吸附在吸附介質上,該介質包括經一或多種鹼金屬化合物、一或多種鹼土金屬化合物、或其混合物預處理之活性氧化鋁。已發現若該氧化鋁吸附劑由經聚結氧化鋁粉末形成及經鹼金屬及/或鹼土金屬化合物處理後,具有至少0.10cc/g之大於500埃孔隙之汞孔隙體積,則達成經改良之針對酸性氣體之吸附劑能力。
本發明包括一種經改良之移除酸性氣體之方法,諸如上文描述包括藉由在活性氧化鋁吸附劑上吸附而從液體或氣體中移除羰基硫化物(COS)。當達成該吸附劑之能力時,該吸附劑之再生可達成及實施。用於本發明方法之活性氧化鋁吸附劑包括具有粒度範圍為約1/4"至約100網目(U.S.Series)之活性微粒氧化鋁。此等粒子由具有平均尺寸約1至10微米之經聚結氧化鋁粉末形成。氧化鋁粒子形成為具有至
少0.45cc/g,一般至少0.50cc/g,較佳至少0.60cc/g,更佳至少0.70cc/g之總汞孔隙體積。
期望之氧化鋁粒子孔隙體積可藉由若干種方法獲得,包括聚結具有平均尺寸範圍從約1至4微米之氧化鋁粉末。若使用較大氧化鋁粉末,例如,高於4微米,則可將燒除添加劑與該等粉末聚結。在隨後煅燒期間移除及/或碳化該燒除添加劑。
適宜用於本發明實務之起始材料包括偽勃姆石、三水鋁石、三羥鋁石及任何其他形式之氧化鋁,其當經適當處理獲得之吸附劑具有0.10至2.5重量%(1100℃基於煅燒)之氧化鈉濃度,2.0至9.0重量%之LO1(藉由從400加熱至1100℃測定之羥基含量),及100至500m2/g(BET)之表面積。
本發明之起始材料可具有粒度為75微米或更高之粒子。此等粒子應經研磨至約1至10微米之粒度以獲得特別有利之吸附劑。可使用熟習此項技術者熟知之任何研磨技術。
一旦該氧化鋁起始材料具有約1至10微米之平均粒度,該氧化鋁藉由暴露於高溫一段短時間迅速活化。此迅速活化之方法在此項技術中熟知。一種已發現特別有用之技術係描述於美國專利第2,915,365號中者。依照此專利揭示,將氧化鋁注入處於高於300℃,諸如300℃至1000℃之氣體溫度之經高度加熱氣體(例如空氣)流。氧化鋁與熱氣體間接觸持續時間可少於一分鐘,諸如從分秒至幾秒,其中2至3秒係較佳接觸時間。一旦活化,該氧化鋁係γ相或者非晶相或其混合物。
在本發明之一較佳實施例中,經迅速活化之氧化鋁係在水存在時形成(聚結)之球及隨後藉由熟習此項技術者熟知之多種方法中之任一種再活化。一種產生良好活性氧化鋁之方法係將經老化氧化鋁暴露於範圍為300至800℃之溫度持續10分鐘至約4小時,其中350至450℃之溫度持續15分鐘至2小時係典型條件。適當的最終活化(如粉末活
化)在形成具有低LO1、但高表面積之吸附劑時係重要的。
一般而言,燒除添加劑係基於碳之材料。燒除添加劑之實例包括糖、澱粉、及木質素或穀粉諸如木材、小麥、玉米、黑麥等等。亦可使用水溶性聚合物諸如聚環氧乙烷、聚乙烯醇等等。
活性氧化鋁較佳地經一或多種鹼金屬化合物、一或多種鹼土金屬化合物或其混合物浸漬,浸漬含量範圍可為約0.01至約15重量%,較佳地約1.0至約8.0重量%,更佳地約2.0至約8.0重量%及最佳地約3.0至約6.0重量%,其中重量%係測量為呈氧化物之經浸漬鹼金屬或鹼土金屬相對於經浸漬氧化鋁吸附劑之總重量之重量百分比。該鹼金屬化合物或鹼土金屬化合物較佳將包括具有可分解陰離子之物質,使得浸漬後沒有非所需其他材料殘留在氧化鋁中。此等鹼金屬/鹼土金屬化合物之實例包括例如鈉、鉀、鋰、鈣及鎂之氫氧化物、碳酸鹽及硝酸鹽。
活性氧化鋁可藉由在含有溶解之鹼金屬/鹼土金屬化合物之水溶液中浸泡該活性氧化鋁至少5分鐘上至1小時或更長及隨後乾燥該經浸漬氧化鋁及在300至450℃下再活化1至2小時,而經該鹼金屬/鹼土金屬化合物浸漬。若需要,可使用多於一次浸漬及乾燥之循環。若需要,該化合物亦可藉由噴霧等施加於該活性氧化鋁。
若該經處理之吸附劑具有至少0.4cc/g,通常至少0.45cc/g,較佳至少0.5cc/g及,更佳至少0.55cc/g之總汞孔隙體積,則該經浸漬及再活化之氧化鋁吸附劑得以改良。進一步而言,若該經浸漬及再活化氧化鋁吸附劑具有至少0.1cc/g,通常至少0.15cc/g,較佳至少0.30cc/g,更佳至少0.40cc/g之大於500埃孔隙之孔隙體積,則可達成經極大改良之酸性氣體之吸附。
該等經改良之活性氧化鋁吸附劑能處理含高達200ppm之酸性氣體雜質濃度的氣體或液體及將該濃度降低至低於1ppm。由於從其中
含此等雜質之液體或氣體中移除COS或其他酸性氣體原則上係經由吸附,則存在或不存在任何特定量水分對於本方法之操作係不關鍵的。
然而,由於已發現該吸附劑對酸性氣體之能力與存在之水量呈反比例變化,較佳地在儘可能少水存在的情況下操作。亦應注意,對於該吸附方法無需存在水以成功地操作。
在一較佳實施例中,該酸性氣體雜質從液體或氣體烴流中移除。待純化之烴流可首先流經乾燥床諸如分子篩或矽石或類似物以在該烴流經過該吸附劑之前移除大部分(若非全部)存在之水分,以避免正如上文所之討論般降低吸附能力。待藉由本發明之吸附劑移除之污染物係酸性氣體或溶解於液體中之酸性氣體,其包括COS、H2S、CO2、CS2、SO2、HCl、HF、HBr,其中該等物流之主要成分主要由乙烯、丙烯、丁烷、或各種烯烴之混合物、天然氣、源自生質之合成氣體、氫氣、氮氣、或空氣組成。該等物流之主要成分可呈氣體或者液體形式。
若該烴流中存在水分,則一些酸性氣體可藉由水解轉化為其他反應產物,其可隨後吸附在經鹼金屬浸漬之活性氧化鋁吸附劑上。若需要,在隨後使該吸附劑再生時,此等經吸附之反應產物可隨後移除,連同所吸附之酸性氣體。
該吸附方法可在環境溫度下進行,雖然若方便可使用15至100℃之溫度,例如,若經污染液體或氣體在先前處理後處於此溫度,則不需要在流經該吸附劑前進行加熱或冷卻。
吸附可有利地在填充塔中進行,雖然可採用維持吸附劑與經酸性氣體污染之進料間接觸之任何替他方便之形式,諸如漿料方法。該進料經過吸附劑之流動速率應足夠緩慢,以允許來自進料之酸性氣體在經鹼金屬/鹼土金屬浸漬之活性氧化鋁上發生期望吸附的足夠接觸時間。接觸時間之實際長度將隨該吸附劑粒度變化。
用於含硫酸性氣體之經鹼金屬/鹼土金屬浸漬之活性氧化鋁吸附劑的吸附能力係藉由監測該吸附劑流出物之硫含量測定。在達到其吸附能力之前,該流出物將含有低於1ppm硫。在此監測指示已達到該吸附劑之能力,即,藉由流出物硫含量之升高後,該吸附劑可藉由使經加熱氣體諸如空氣、烴氣體、氮氣、或其他惰性氣體流經該吸附劑而再生。該經加熱氣體較佳地加熱至約100至300℃,更佳約150至250℃,及最佳約250℃之溫度,及以約1至10cc/min之速率流經該吸附劑,直至移除大量吸附於其上的硫。大量係該經吸附硫之約40重量%或更高。此可藉由分析吸附劑中殘留硫之量而輕易測定。該再生氣體經過吸附劑之流動方向可與進料流動方向相同,例如,當該吸附劑係填充在塔中時,或者該再生氣體可與其中進料經過之正常流動方向相反之方向流經該吸附劑。其他酸性氣體之吸附能力可藉由用於測量其他陰離子種類,例如Cl、F等等之熟知方法測定。
以下實例將用於更好地闡明本發明之方法。
COS吸附劑係如下文描述製備。將吸附劑置於各自床中及經歷如下文描述之迅速老化及滲漏試驗之測試條件。
使各個床裝載78g吸附劑。吸附劑床隨後經歷吸附、再生及冷卻循環。重複該三個步驟共35次。在第35次循環結束時,在270℃以0.5slpm之流量再加熱各個床2小時及隨後冷卻至環境溫度。在迅速老化之吸附步驟期間,向該床以8.7slpm之流量35℃之溫度及80psia之壓力饋入含於氮氣中之450ppm之COS,持續35分鐘。在再生步驟期間,該床處於15psia之壓力及270℃之溫度,同時流速為0.5slpm,氮氣進料與吸附步驟反向流動。在迅速老化之冷卻步驟期間,該床處於
15psia之壓力及35℃之溫度,同時流速為0.5slpm,氮氣進料與該吸附步驟反向流動。
在該床完成該迅速老化測試後,完成滲漏測試。在該測試期間,向該床以6.45slpm之流量及35℃之溫度饋入含於氮氣中之75ppm之COS。該床運行一段時間使得在該床出口之COS達到進料條件。
將15克孔隙形成劑與85克尺寸為約5微米之經急驟煅燒氧化鋁粉末混合,製備珠粒。該材料使用泛聚結技術形成為珠粒及篩選至7X14 Tyler網目。隨後在842℉之溫度下煅燒該材料2小時。隨後將該活性材料浸在9.8重量% NaOH溶液中20分鐘及該材料再次在572℉之溫度下活化2小時。所得之材料具有6重量%之Na2O含量。
使實例1之材料如迅速老化方案中描述般迅速老化。老化後,實例1之材料隨後在滲漏測試中進行測試,該材料在640分鐘內滲漏至2ppm COS及在880分鐘內滲漏至25ppmCOS。
藉由將約5微米之氧化鋁粉末研磨至約1.5微米之粉末,製備珠粒。該氧化鋁粉末使用泛聚結技術形成為珠粒及篩選至7X14 Tyler網目。隨後在700℉之溫度下煅燒該珠粒2小時。隨後將該活性珠粒浸在9.8重量%NaOH溶液中20分鐘及該珠粒再次在泛活化劑中於572℉之溫度下活化2小時。所得之材料具有6重量%Na2O含量。
使實例3之材料如在迅速老化方案中描述般迅速老化。老化後,實例3之材料隨後在滲漏測試中進行測試。該材料在640分鐘內滲漏至2ppm COS及在880分鐘內滲漏至25ppmCOS。
藉由急驟活化約5微米氧化鋁粉末及隨後使用泛聚結技術將該活性粉末形成為珠粒,製備珠粒。該珠粒經篩選至7X14 Tyler網目。隨後在760℉之溫度下煅燒該材料2小時。隨後將該活性材料浸在9.8重量%NaOH溶液中20分鐘及該材料再次在泛活化劑中於572℉之溫度下活化2小時。所得之材料具有4重量%Na2O含量。
使實例5之對照材料如迅速老化方案中描述般迅速老化。其隨後在滲漏測試中進行測試。該對照材料在250分鐘內滲漏至2ppm COS及在497分鐘內滲漏至25ppm COS。
藉由急驟活化大約5微米氧化鋁粉末及隨後使用泛聚結技術形成為珠粒,製備珠粒。該等珠粒經篩選至7X14網目。隨後在760℉之溫度下煅燒該材料2小時。隨後將該活性材料浸在12重量%NaOH溶液中20分鐘及該材料再次在572℉之溫度下活化2小時。所得之材料具有6重量Na2O含量。
使實例7之對照材料如迅速老化方案中描述經迅速老化,及隨後在滲漏測試中進行測試。該材料在300分鐘內滲漏至2pmm COS及在500分鐘內滲漏至25ppm COS。
實例1材料之孔隙體積係藉由汞孔隙對稱法使用微晶學儀器在浸前進行測量。該材料之總孔隙體積係0.63cc/g。大於500埃孔隙之孔隙體積係0.61cc/g。
實例3材料之孔隙體積係藉由汞孔隙對稱法使用微晶學儀器在浸
前進行測量。該材料之總孔隙體積係0.72cc/g。大於500埃孔隙之孔隙體積係0.29cc/g。
實例5與7對照材料之孔隙體積係藉由汞孔隙對稱法使用微晶學儀器在浸前進行測量。各材料之總孔隙體積係0.38cc/g。大於500埃孔隙之孔隙體積係0.11cc/g。
下表1匯總上文描述之測試結果。
在浸及活化後測試實例1、3、5與7之材料之孔隙體積。實例1材料在浸及活化後具有0.56cc/g之總孔隙體積及對於大於500埃孔隙具有0.15cc/g之孔隙體積。實例3材料在浸及活化後具有0.59cc/g之總孔隙體積及對於大於500埃孔隙具有0.41cc/g之孔隙體積。對照實例5材料在浸及活化後具有0.36cc/g之總孔隙體積及對於大於500埃孔隙具有0.07cc/g之孔隙體積。對照實例7材料在浸及活化後具有0.34cc/g之總孔隙體積及對於大於500埃孔隙具有0.04cc/g之孔隙體積。
Claims (25)
- 一種用於藉由吸附從液體或氣體中移除含硫酸性氣體污染物之方法,其包括:使含有該含硫酸性氣體污染物之該液體或氣體與經0.1至15重量%(基於該化合物中呈氧化物之該金屬與該經浸漬吸附劑之重量比)之金屬化合物浸漬之活性氧化鋁吸附劑接觸,以吸附該液體或氣體中該含硫酸性氣體污染物持續一段足以降低該液體或氣體中該含硫酸性氣體污染物含量之時間,其中該金屬化合物選自下列組成之群:一或多種鹼金屬化合物、一或多種鹼土金屬化合物、或此等化合物之混合物;及其中該經浸漬氧化鋁吸附劑具有至少0.10cc/g之大於500埃孔隙之汞孔隙體積。
- 如請求項1之方法,其中該經浸漬金屬化合物包括相對於該經浸漬吸附劑約1.0至約8.0重量%為金屬氧化物。
- 如請求項2之方法,其中該經浸漬金屬化合物包括相對於該經浸漬吸附劑約2.0至6.0重量%為金屬氧化物。
- 如請求項1之方法,其中在經該活性氧化鋁吸附劑中浸漬之該金屬化合物中之該金屬基本上由鈉組成。
- 如請求項1之方法,其中該液體或氣體係烴流。
- 如請求項5之方法,其中該烴流係烯烴流。
- 如請求項5之方法,其中該烴流係天然氣流。
- 如請求項1之方法,其中該氧化鋁吸附劑係藉由聚結具有平均粒度為1至10微米之經煅燒氧化鋁粉末形成。
- 如請求項1之方法,其中該氧化鋁吸附劑係藉由聚結具有平均粒度為1至4微米之經煅燒氧化鋁粉末形成。
- 如請求項8之方法,其中該經煅燒氧化鋁粉末具有平均粒度為大於約4.0微米至10微米及係經燒除添加劑聚結為珠粒,該等珠粒經煅燒以移除該添加劑。
- 如請求項10之方法,其中該燒除添加劑係基於碳之材料。
- 如請求項6之方法,其中該烯烴係乙烯及/或丙烯。
- 如請求項1之方法,其中該經浸漬吸附劑具有至少0.40cc/g之全部汞孔隙體積。
- 如請求項1之方法,其中該經浸漬吸附劑具有至少0.5cc/g之全部汞孔隙體積。
- 如請求項1之方法,其中該經浸漬吸附劑具有至少0.15cc/g之大於500埃孔隙之汞孔隙體積。
- 如請求項1之方法,其中該經浸漬吸附劑具有至少0.30cc/g之大於500埃孔隙之汞孔隙體積。
- 如請求項1之方法,其包括再生該活性氧化鋁吸附劑以移除吸附在其上之大量該含硫酸性氣體污染物。
- 如請求項17之方法,其中該活性氧化鋁吸附劑係藉由使加熱氣體流經該吸附劑而再生。
- 如請求項1之方法,其中該含硫酸性氣體污染物選自下列組成之群:COS、H2S、CS2及SO2。
- 如請求項19之方法,其中該含硫酸性氣體污染物係COS。
- 如請求項8之方法,其中在浸漬前該氧化鋁吸附劑具有至少0.45cc/g之總汞孔隙體積。
- 如請求項8之方法,其中在浸漬前該氧化鋁吸附劑具有至少0.5cc/g之總汞孔隙體積。
- 如請求項8之方法,其中在浸漬前該氧化鋁吸附劑具有至少0.6cc/g之總汞孔隙體積。
- 如請求項1之方法,其中該液體或固體係由生質形成之合成液體或氣體。
- 如請求項24之方法,其中該合成液體或氣體包含選自下列組成之群之含硫酸性氣體污染物:COS、H2S、CS2及SO2。
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