JP2019173020A - 燃料および燃料の製造方法 - Google Patents
燃料および燃料の製造方法 Download PDFInfo
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- JP2019173020A JP2019173020A JP2019096577A JP2019096577A JP2019173020A JP 2019173020 A JP2019173020 A JP 2019173020A JP 2019096577 A JP2019096577 A JP 2019096577A JP 2019096577 A JP2019096577 A JP 2019096577A JP 2019173020 A JP2019173020 A JP 2019173020A
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Classifications
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Abstract
Description
本願は、2011年12月12日に出願された米国仮特許出願第61/569,712号、および2012年5月11日に出願された米国仮特許出願第61/646,152号、および2012年6月19日に出願された米国仮特許出願第61/673,683号への優先権を主張する。仮特許出願各々への優先権は、明示的に主張されており、各仮特許出願の個別における開示は、全ての目的に対し、全範囲において参照することにより、本明細書中に援用される。
本開示は、精製システムまたはフィールド改良設備への原料として、再生可能燃料または再生可能油の導入に概ね関する。より具体的には、本開示は、石油留分、石油留分の反応物質、および/または石油留分原料と共処理するために、例えば精製の流動式接触分解(FCC)、コークス器、フィールド改良システム、水素添加分解装置、および/または水素処理ユニット等の石油転換ユニットにバイオマスから熱的に製造された液体を導入する方法、およびその生成物(例えば、燃料)、ならびに当該生成物の使用および価値に関する。
バイオマスは、人類史の殆どにおいて、主要なエネルギー源であった。1800年代の終わり頃および1900年代の間に、バイオマスから調達される世界でのエネルギー割合は降下し、同時に、化石燃料の商業的な発展および活用により、石炭および石油の製品のための市場が優位になった。それでもなお、世界のエネルギーのおよそ15%はバイオマスから調達され続けており、発展途上国におけるバイオマスの寄与は非常に高く、38%である。加えて、化石燃料の利用が与える環境への影響が新たに意識されている。特に、化石燃料を消費する結果生じる温暖化ガスという負担である。
一実施形態において、本発明は、石油留分原料および再生可能燃料油原料から生成される燃料組成物に関する。一実施形態において、本発明は、触媒の存在下で共処理された石油留分原料および再生可能燃料油原料から生成される燃料組成物に関する。一実施形態において、本発明は、再生可能燃料油を含む原料から生成される、流動式接触分解装置の生成物の組成物に関する。一実施形態において、本発明は、触媒の存在下で変換ユニットにおいて処理され得る80重量%よりも多い石油留分原料および20重量%よりも少ない再生可能燃料油原料から生成される燃料組成物に関する。
材料、システム、方法、製品、用途および数ある中の応用例の多くの利点は、添付の図および要約書を含めて本出願にて提供されている概要および詳細を検討することにより、容易に認識および理解され得る。
2005年に、環境保護局(EPA)は、米国における最初の再生可能燃料の指令である「再生可能燃料の基準」(RFS1)を発表した。RFSは、2012年までに7.5Bガロンの再生可能燃料をガソリンに混合することを要求した。2年後、計画は、2022年までに36Bガロンの再生可能燃料を目標にするよう、2007年の「エネルギーの独立および安全性議定書」(EISA)の下で拡大された。さらに、EISAは、ガソリン同様、ディーゼル燃料もカバーするようRFSを拡大し(ジェット燃料は、RFS下で最初は含まれなかった)、異なるタイプの再生可能燃料について個々の体積の目標を定めた(例えば、RFS2は、新型バイオ燃料について、2022年までに21Bガロンを要求している)。
・水、砂、物理的な屑およびより軽い生成物を除去する;
・水素化処理する;および、
・炭素除去または接触水素化分解(HCR)によって水素付加する。
(評価設備)
石油留分原料と様々な量の再生可能燃料油(RFO)との共処理、(または、比較として石油留分原料のみの処理)を、Model R+ Kayser Technology Advanced Cracking Evaluation(ACE) FCCユニット(本明細書中において「ACE評価ユニット」または「FCCユニット」と称する)において、FCC触媒を用いて実施した。
全範囲において参照されることによって本明細書中に援用される米国特許第7,905,990号、米国特許第5,961,786号および米国特許5,792,340号に従い、以下に示す実施例において使用した再生可能燃料油(RFO)原料を、工業的な高速の熱分解処理における廃材の原料の急速な熱処理によって生成した。再生可能燃料油(RFO)原料の特性を以下の表1に要約した。
(1)石油留分原料として、100重量%の水素処理していない減圧軽油(VGO)原料(「VGO原料」と本明細書中において称する);
(2)98重量%のVGO原料および2重量%の再生可能燃料油(RFO)原料;
(3)95重量%のVGO原料および5重量%の再生可能燃料油(RFO)原料;および、
(4)90重量%のVGO原料および10重量%の再生可能燃料油(RFO)原料。
これらの原料および原料の組み合わせ各々に、510℃(950°F)という一定の分解温度にて、ACE評価ユニットによって処理または共処理を行なった。
これらの原料または原料の組み合わせ各々に対して、4:1〜11.25:1の範囲、より具体的には、4:1、6:1、8:1、10:1、および11.25:1といった異なる触媒と油との比率(「触媒/油比」)を独立して採用し、いくつかの操作を行なった。
ACE評価ユニットにおいて、原料または原料の組み合わせを処理または共処理することによって得られた液体サンプル各々を回収し、分析に用いた。ドライガスの生成に対して、ガスクロマトグラフィーによる分析を実施した。コークスの含有量は、評価手順における再生工程にて生成される二酸化炭素の量を分析することによって定量した。各操作に対するACE評価の結果は、ドライガス、液化した石油ガス(LPG、C3−C4)、ガソリン(C5−221℃)、ライトサイクル油(LCO、221−343℃)、ヘビーサイクル油(HCO、343℃+)およびコークスの転換と収量とを含んでいる。原料または原料の組み合わせの転換は、原料または原料の組み合わせの量と、221℃より上で沸騰する液体の生成物として規定した未転換の材料の量との間の差を計算することによって定量した。
等価エネルギー供給ベースまたは等量炭素供給ベースで表される転換と収量との曲線は、FCC型のユニット(ACE評価ユニット)における、再生可能燃料油(RFO)原料とVGO原料の様々な量の組み合わせに起因する予想外の効果を実証している。再生可能燃料油(RFO)原料は、VGO原料のおよそ1/2の炭素とエネルギーの含有量を有している(等価な重量に対して)。例えば、98重量%のVGO原料と2重量%の再生可能燃料油(RFO)との原料の組み合わせからの結果は、100重量%のVGO原料のそれらに対して比較すると、2重量%の再生可能燃料油(RFO)原料は、2重量%のVGO原料の代わりに置き換えられ得、それは、およそ1%より少ない炭素と1%より少ないエネルギーとがFCCユニットにおいて、後に続く所望の生成物への転換に利用できることを意味する。2重量%の再生可能燃料油(RFO)原料の組み合わせの場合において、重量または体積の合計の等量をFCCユニットに供給すれば、再生可能燃料油(RFO)原料の炭素およびエネルギーが、VGO原料の炭素およびエネルギーと同じ割合においてガソリンに転換されると、その結果、ガソリンの収量が1%程度に低下すると予想されるであろう。しかしながら、1%よりも少ない程度にガソリンの収量は低下し、この場合、その現象は、全ての代替のレベル(すなわち、2重量%、5重量%および10重量%の再生可能燃料油(RFO)原料の組み合わせ)に対して観察された。従って、供給量が、FCCユニットへの炭素またはエネルギーの等価な量に基づいて表されていれば(すなわち、品質の良いVGO原料、またはVGO原料と再生可能燃料油(RFO)原料との組み合わせ(ブレンド)のいずれが供給されるかに関わらず、炭素の供給またはエネルギーの供給を一定に維持すること)、再生可能燃料油(RFO)原料をVGO原料に組み合わせまたはブレンドすると、ガソリンの収量の測定可能な増量が生じ得る。収量がFCCユニットへの一定の炭素またはエネルギーの供給量に基づいて表されると、FCCへの重量または体積の合計の供給量が、再生可能燃料油(RFO)原料の代替に伴い増加するであろうことがこの条件において示唆されている。2重量%の再生可能燃料油(RFO)原料の組み合わせ(ブレンド)の場合において、FCCユニットへのおよそ1%の追加的な量の供給が、100%のVGO供給と同じ炭素とエネルギーの供給量を得るために求められ得る。体積の追加に関して、VGOとRFOとの間の密度の違いを考慮すれば、FCCユニットへの2重量%の再生可能燃料油(RFO)原料の組み合わせ(ブレンド)の1%よりも少ない体積の追加が、FCCユニットへの品質の良いVGO原料と同じ炭素またはエネルギーの供給量を得るために生じ得る。
この実施例の目的として、図7および8に示す、原料の転換は、VGOまたはRFO/VGOブレンドの供給量から、ライトサイクル油(LCO)およびヘビーサイクル油(HCO)の両方の重量による収量を差し引いたものである。用いられたVGOまたはRFO/VGOに対する、FCCの反応温度、触媒の重量、および触媒の接触時間は全て一定にし、触媒:油比のみ変化させて、ACEの転換のデータを得た。
FCC操作の主な目的は、最適なガソリンの収量を実現することであり、この検討の目的として、ガソリンの留分は、C5−221℃の沸点として定義され得る。図9は、様々な供給に対する触媒:油比の作用としてのガソリンの収量を示している。触媒:油比がおよそ7:1〜8:1の最大値までは、触媒:油比の増大に伴い、ガソリンの収量は初期において増大することが見受けられた。触媒:油比のさらなる増大は、設定した反応器の条件下において、オーバークラッキングに起因すると判断し得るガソリンの収量の減少に帰結した。
FCC操作において、LPG(C3+C4炭化水素として定義される)は、アルキル化および石油化学製品の原料に用いられ得る成分を含んでいるため、価値のある生成物として考慮され得る。この実施例において、VGOにおけるRFOブレンドの増大は、LPGの収量(一定の供給エネルギーベースに基づく)の増大に帰結し、この効果を図11に示す。この傾向は、FCCへの一定の炭素の供給量に基づいても維持され、RFOの添加が優先的にLPGへのより高い炭素の転換をもたらすことを提示している。
この実施例において、ドライガスは、H2、H2S、二酸化炭素、およびC1−C2炭化水素の合計として定義され得る。FCCの良好な操作ではこれらの生成は最少に維持され得るのは、気体の圧縮に関し、過剰なドライガスの生成物は下流のプラントの操作に制限をもたらし得るからである。ドライガスの収量への効果は、図12に示すように、予想通り、触媒:油比の増大に伴い、ドライガスの収量は増大している。等価エネルギー供給量ベースに基づき(すなわち、RFO/VGOブレンドが、参照のVGOのエネルギー供給量に対して類似するエネルギー供給量を有することを評価する)、RFOの添加の比率が増大することに伴い、ドライガスの製造の増大が認められた。この実施例における全ての場合において、主なドライガスの成分は、エチレン、メタンおよびエタンであった。
この実施例において、ライトサイクル油(LCO)は、221〜343℃の間において沸騰するそれらの液体として定義され得、この生成の価値は、場所および再生の目的に依存し得る。通常、北アメリカにおいて、LCOは好ましいものとして考慮され得ない。しかしながら、ガソリンに需要が高くないときと場所において、FCCユニットはディーゼルおよびNo.2ガソリンに高品質化できる中間分留のLCOの源として使用され得る。この実施例において、等価エネルギー供給ベースでのLCO生成物へのRFOブレンドの効果(図13)は、2重量%のRFOの添加の水準において相対的に明確でないが、5重量%および10重量%のRFOの添加において、等価エネルギー供給(または炭素供給)ベースで表されるLCO生成物の測定可能な増大が認められた。
この実施例において、ヘビーサイクル油(HCO)は、343℃〜525℃の間において蒸留されるそれらの液体として定義され得る。この材料は、一般的に、比較的に高い芳香族と潜在的に高い硫黄の含有量を伴う転換できない生成物であり、相対的に好ましくないものとして精製所によって考慮され得る。可能であれば、FCCユニットにおけるVCOからのHCOの生成物は最少化されるべきである。この実施例において、図14に示すように、HCOの生成物の比率は、VGO原料における2重量%または5重量%のRFO(重量による)の添加によって、顕著に影響を受け得なかったが、10重量%のRFOの代替におけるHCOの生成物の増大が、エネルギー供給ベースで明確に確認された。
FCCの操作において、コークスは、反応を推進させるためのプロセス加熱を提供するため、一般的に利用される。しかしながら、コークスの生成物の増大は、最終的にFCCユニットの熱のバランスを乱し、触媒の再生器におけるより高い温度に帰結する。この実施例におけるコークスの生成物へのRFOブレンドの影響は、図15に示している。
FCCの操作における第1の目的は、典型的には最適なガソリンの収量を実現することであり、この検討の目的において、ガソリンの留分はC5−221℃の沸点として定義され得る。図16は、触媒:油比に対するガソリンの収量を示しており、様々な供給のため、一貫した10,000bbl/日の供給量での水を含まないRFOベースに基づく様々な原料ブレンドを用いている。RFO/VGOブレンドの10,000bbl/日の供給量の供給におけるエネルギーおよび炭素の量は、参照のVGOよりも少ないという事実にも関わらず、この実施例におけるガソリンの収量は、参照のVGO原料の場合よりも、予想できない程に高いことが見受けられる。特に、この実施例において、RFOの代替のより高いレベルにおいて、ガソリンの収量の劇的な改善が認められた。
参照のVGOの1トン当たりにつき生成されたガソリンのガロンを用い、RFO/VGOの1トン当たりにつき生成されたガソリンのガロンを比較し、RFOの1トン当たりにつき生成されたガソリンのガロンへの貢献の評価を行なった。図17は、RFOの代替のレベルの作用としてのRFOの1トンに対するガソリンのガロンを示している。この実施例において、代替のレベルが、2重量%から10重量%に変化するに伴い、RFOの1トン当たりにつき生成されたガソリンのガロンは増大した。最初のバイオマスに換算すると、バイオマスの1トンに対するガソリンの収量は、より高いRFOの代替のレベルにおいて、90gals/tonを上回った。
精製所は、通常、石油の液体を操作し、輸送し、供給し、処理するとき、体積ベースで操作を行なう。従って、VGOでのガソリンの収量に対するRFOの添加を検討するときにおいて公平で、公正な比較を行なうために、エネルギー等価ベースおよび炭素等量ベースの少なくとも一方(すなわち、供給炭素または供給エネルギーの等しい量に由来する、VGOおよびRFOからのそれぞれのガソリンの収量であるもの)で収量を測定することが重要になり得る。加えて、この実施例において、RFOは、VGOのおよそ半分の炭素およびエネルギーを含んでおり、この実施例において、少量である付加的な原料の体積の合計がFCCに供給されるべきであったのは、RFOをVGOにブレンドするときに、供給する炭素またはエネルギーの等量を維持するためであった。
評価設備:再生可能燃料油(RFO)と石油留分原料との共処理(または、比較としての石油留分原料のみの処理)は、流動床であるMicroactivity Test reactor (MAT)ユニット(本明細書中において「MAT評価ユニット」と称する)によって実施し、商業的に利用できる平衡触媒を用いた。
FCCの操作において、コークスは、一般的に、原料を予備加熱し、分解するための熱を供給するために必要である。しかしながら、あまりに多いコークスは、触媒を深刻に害し、触媒の再生の間、送風機に過度な負担をかけ、再生器において過度に高い温度を引き起こす。ブレンドが0.27重量%というより高いコンラドソン残留炭素分を有しているにも関わらず、評価の間、ドライガスに類似し、両方の原料は、得られた転換において殆どの同一のコークスの収量を得た。
この実施例の目的において、気体および液体の生成物における酸素の分配も、注目すべきである。例えば、分解後のブレンドにおける酸素の大部分は、この実施例において、H2O(74.6〜94.1重量%)として発生することに伴い、残りがCO2を形成した(0.7〜5.3重量%)。液体の生成物は、酸素の含有量を分析したが、検出限界(0.25重量%)よりも低いと見受けられた。
一連の減圧軽油(VGO)のサンプルおよび5重量%の再生可能燃料油(RFO)ブレンドを、実施例2に類似する条件下において、MAT評価ユニットによって分解した。表2に用いられたVGOは、FHR CAT原料と称し、15.6℃において0.9196g/mLの密度を有している。RFO自身は、1.198g/mlの密度と、26.58(重量%)の水分含有量を有していた。表3に用いられた5重量%のRFOのVGOにおけるブレンドは、FHR CFにおいて5重量%のRFOと称し、15.6℃において0.9243g/mLの密度を有している。用いられた5重量%のRFOのVGOにおけるブレンドの100 lbsにおいて、水分の含有量は、およそ1.329 lbsであった。VGOに対する分析、定性、および結果は、表2、3(供給ベースとして)および表4(精製のフローの要約)において表し、5重量%のRFOのVGOにおけるブレンドに対する分析、定性、および結果は、表5および6(供給ベースとして)において表し、表7(水を含まない供給ベース)、表8(精製のフローの要約)、および表9はRFOの供給量に起因するガソリンのガロンの計算である。
Claims (19)
- 原料を共処理する流動式接触分解装置の生成物を含む燃料であって、
上記原料は、
i)石油留分;および、
ii)上記石油留分の重量に対して0.05〜20重量%の非濃縮再生可能燃料油を含み、
上記非濃縮再生可能燃料油は:
セルロースバイオマスの粉砕、および触媒によらない迅速熱処理により当該セルロースバイオマスの少なくとも60重量%が上記非濃縮再生可能燃料油に変換されることによる生成物を含み、かつ
無湿ベースにおいて少なくとも40重量%の炭素含有量、および無湿ベースにおいて20〜50重量%の範囲内の酸素含有量であり、
上記共処理は、上記酸素含有量の74.6〜94.1重量%を水に変換することを特徴とする燃料。 - 上記燃料は、輸送燃料であることを特徴とする請求項1に記載の燃料。
- 上記非濃縮再生可能燃料油は、水素化脱酸素化されない、脱酸素化されない、水素化処理されない、改良されない、または触媒処理されないで調製されることを特徴とする請求項1または2に記載の燃料。
- 上記非濃縮再生可能燃料油は、0.5重量%未満の固体含有量を有することを特徴とする請求項1〜3のいずれか1項に記載の燃料。
- 上記セルロースバイオマスは、木材、木材残渣、または木屑を含むことを特徴とする請求項1〜4のいずれか1項に記載の燃料。
- 上記非濃縮再生可能燃料油は、0.05重量%未満の灰分を有することを特徴とする請求項1〜5のいずれか1項に記載の燃料。
- 上記非濃縮再生可能燃料油は、0.1重量%未満の固体含有量を有することを特徴とする請求項1〜6のいずれか1項に記載の燃料。
- 上記セルロースバイオマスは、バガス、ヤシの葉、または空の果物の房を含むことを特徴とする請求項1〜4または請求項6〜7のいずれか1項に記載の燃料。
- 上記セルロースバイオマスの少なくとも70重量%が、上記非濃縮再生可能燃料油に変換されることを特徴とする請求項1〜8のいずれか1項に記載の燃料。
- 原料を、流動式接触分解触媒の存在下で共処理することを含み、
上記原料は、
i)石油留分と、
ii)上記石油留分の重量に対して0.05〜20重量%の非濃縮再生可能燃料油とを含み、
上記非濃縮再生可能燃料油は、セルロースバイオマスの粉砕、および触媒によらない迅速熱処理により当該セルロースバイオマスの少なくとも60重量%が上記非濃縮再生可能燃料油に変換されたことによる生成物を含み、
上記非濃縮再生可能燃料油は、
a)無湿ベースにおいて少なくとも40重量%の炭素含有量を有し、
b)無湿ベースにおいて20〜50重量%の範囲内の酸素含有量を有し、
上記共処理は、上記酸素含有量の74.6〜94.1重量%を水に変換することを特徴とする燃料の製造方法。 - 上記製造された燃料は輸送燃料であることを特徴とする請求項10に記載の製造方法。
- 上記非濃縮再生可能燃料油は、水素化脱酸素化されない、脱酸素化されない、水素化処理されない、改良されない、または触媒的に処理されないで調製されることを特徴とする請求項10または11に記載の製造方法。
- 上記非濃縮再生可能燃料油は、0.5重量%未満の固体含有量を有することを特徴とする請求項10〜12のいずれか1項に記載の製造方法。
- 上記セルロースバイオマスは、木材、バガス、ヤシの葉、または空の果物の房を含むことを特徴とする請求項10〜13のいずれか1項に記載の製造方法。
- 上記非濃縮再生可能燃料油は、0.05重量%未満の灰分含有量を有することを特徴とする請求項10〜14のいずれか1項に記載の製造方法。
- i)上記セルロースバイオマスは、バガス、ヤシの葉、または空の果物の房を含み、且つ、
ii)上記非濃縮再生可能燃料油は、0.5重量%未満の固体含有量と、0.1重量%未満の灰分含有量とを有することを特徴とする請求項10〜15のいずれか1項に記載の製造方法。 - i)上記石油留分は真空ガス油を含み、
ii)上記非濃縮再生可能燃料油は、0.5重量%未満の固体含有量と、0.1重量%未満の灰分含有量とを有し、且つ、
iii)流動式接触分解装置は、3〜5秒間の触媒接触時間で操作されることを特徴とする請求項10〜16のいずれか1項に記載の製造方法。 - 上記石油留分は、重ガスオイルまたは重−中間留分原料を含むことを特徴とする請求項10〜17のいずれか1項に記載の製造方法。
- 上記再生可能燃料油は、エタノールと混合されることを特徴とする請求項10〜18のいずれか1項に記載の製造方法。
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