JP2000178566A - Method for hydrotreatment of hydrocarbon oil - Google Patents
Method for hydrotreatment of hydrocarbon oilInfo
- Publication number
- JP2000178566A JP2000178566A JP10378020A JP37802098A JP2000178566A JP 2000178566 A JP2000178566 A JP 2000178566A JP 10378020 A JP10378020 A JP 10378020A JP 37802098 A JP37802098 A JP 37802098A JP 2000178566 A JP2000178566 A JP 2000178566A
- Authority
- JP
- Japan
- Prior art keywords
- catalyst
- hydrocarbon oil
- alumina
- hydrotreatment
- oil
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Pending
Links
Landscapes
- Production Of Liquid Hydrocarbon Mixture For Refining Petroleum (AREA)
Abstract
Description
【0001】[0001]
【発明の属する技術分野】本発明は、炭化水素油の水素
化処理方法に関し、さらに詳しくは、触媒のコークによ
る失活を低減し、触媒寿命を伸ばすことにより水素化処
理の運転期間を長くする炭化水素油の水素化処理方法に
関する。[0001] The present invention relates to a method for hydrotreating a hydrocarbon oil, and more particularly, to extending the operating period of the hydrotreating by reducing the deactivation of the catalyst by coke and extending the life of the catalyst. The present invention relates to a method for hydrotreating a hydrocarbon oil.
【0002】[0002]
【従来技術】従来、炭化水素油の水素化処理方法は、原
油、減圧残渣油、常圧残渣油、減圧軽油、常圧軽油など
の供給原料炭化水素油を加熱して、水素加圧下に水素化
処理触媒が充填された反応塔に導入して、水素化脱メタ
ル、水素化脱硫、水素化脱窒素、水素化分解などの反応
を行っている。2. Description of the Related Art Conventionally, a method for hydrotreating hydrocarbon oils is to heat a feedstock hydrocarbon oil such as crude oil, vacuum residue, normal pressure residue, vacuum gas oil, normal pressure gas oil, etc. It is introduced into a reaction column filled with a hydrotreating catalyst, and performs reactions such as hydrodemetallization, hydrodesulfurization, hydrodenitrogenation, and hydrocracking.
【0003】しかし、従来の方法では、供給原料炭化水
素油中に含まれる多環芳香族化合物は、加熱されること
により重合し、さらに触媒反応で重合してコークを生成
して触媒上に析出するため触媒活性の低下(コーク失
活)が起きるので、触媒寿命が短くなるという問題があ
った。[0003] However, in the conventional method, the polycyclic aromatic compound contained in the feedstock hydrocarbon oil is polymerized by heating, and further polymerized by a catalytic reaction to form coke and precipitate on the catalyst. As a result, the catalyst activity is reduced (deactivation of coke), so that there is a problem that the catalyst life is shortened.
【0004】[0004]
【発明が解決しようとする課題】本発明は、前述のコー
ク失活の問題を解決し、触媒寿命を伸ばすことにより水
素化処理期間を長くできる炭化水素油の水素化処理方法
を提供することを目的とする。また、本発明の他の目的
は、多環芳香族化合物の含有量が少ない炭化水素油を生
成することにある。An object of the present invention is to provide a method for hydrotreating a hydrocarbon oil which solves the above-mentioned problem of coke deactivation and can extend the hydrotreating period by extending the life of the catalyst. Aim. Another object of the present invention is to produce a hydrocarbon oil having a low content of a polycyclic aromatic compound.
【0005】[0005]
【課題を解決するための手段】本発明者らは、供給原料
炭化水素油中の多環芳香族化合物を予め除去した炭化水
素油を水素化処理することにより、触媒のコーク失活が
防止しされ、触媒寿命を伸ばすことができることを見出
し本発明を完成するに至った。Means for Solving the Problems The present inventors hydrotreat a hydrocarbon oil from which a polycyclic aromatic compound in a feedstock hydrocarbon oil has been removed in advance to prevent deactivation of coke in the catalyst. As a result, they found that the life of the catalyst could be extended, and completed the present invention.
【0006】本発明に係わる炭化水素油の水素化処理方
法は、供給原料炭化水素油を吸着剤と接触させて、該炭
化水素油中の多環芳香族化合物を吸着除去して減少させ
た後、触媒の存在下に水素化処理することを特徴とす
る。The method for hydrotreating hydrocarbon oil according to the present invention comprises the steps of: contacting a feed hydrocarbon oil with an adsorbent to adsorb and remove polycyclic aromatic compounds in the hydrocarbon oil; And hydrotreating in the presence of a catalyst.
【0007】前述の炭化水素油の水素化処理方法におい
ては、供給原料炭化水素油を加熱する前に吸着剤と接触
させることが好ましい。In the process for hydrotreating hydrocarbon oils described above, it is preferred that the feedstock hydrocarbon oil be contacted with the adsorbent before heating.
【0008】[0008]
【発明の実施の形態】以下、本発明に係わる炭化水素油
の水素化処理方法の好適な実施形態について、詳細に説
明する。DETAILED DESCRIPTION OF THE PREFERRED EMBODIMENTS Preferred embodiments of the method for hydrotreating hydrocarbon oil according to the present invention will be described in detail below.
【0009】本発明での供給原料炭化水素油としては、
原油、減圧残渣油、常圧残渣油、接触分解軽油、熱分解
軽油、直留軽油、コーカーガスオイル、水素化処理軽
油、脱硫軽油などの水素化処理に付される炭化水素油が
使用可能である。In the present invention, the feedstock hydrocarbon oils include:
Hydrocarbon oils to be subjected to hydrotreatment such as crude oil, vacuum residue oil, atmospheric residue, catalytic cracking gas oil, pyrolysis gas oil, straight run gas oil, coker gas oil, hydrotreated gas oil, and desulfurized gas oil can be used. is there.
【0010】本発明の方法では、前述の供給原料炭化水
素油を水素化処理に付する前に吸着剤と接触させて、該
炭化水素油中の多環芳香族化合物を吸着除去するが、多
環芳香族化合物は熱によっても重合反応を起こしてコー
クを生成するので、熱履歴を受ける前に吸着剤と接触さ
せることが好ましい。本発明の方法では、供給原料炭化
水素油中の多環芳香族化合物は当初含有量の60重量%
以下、好ましくは40重量%以下まで吸着除去すること
が望ましい。In the process of the present invention, the above-mentioned feedstock hydrocarbon oil is brought into contact with an adsorbent before being subjected to hydrotreating to adsorb and remove polycyclic aromatic compounds in the hydrocarbon oil. Since the ring aromatic compound causes a polymerization reaction even by heat to generate coke, it is preferable that the ring aromatic compound be brought into contact with the adsorbent before receiving the heat history. In the process of the present invention, the polycyclic aromatic compound in the feed hydrocarbon oil is 60% by weight of the initial content.
Below, it is desirable to remove by adsorption to preferably 40% by weight or less.
【0011】本発明での多環芳香族化合物の吸着除去
は、二基並列に吸着剤が充填された吸着塔を配置し、吸
着、脱着を交互に繰り返し使用することが望ましい。本
発明で使用される吸着剤としては、活性炭、アルミナ、
シリカ−アルミナ、ゼオライトなどが例示される。特
に、固体酸量を0.15mmol/g(アンモニア吸着
法で測定)以上有する吸着剤が好ましく、アルミナ含有
量20〜40wt%のシリカ−アルミナが好適である。For the adsorption and removal of the polycyclic aromatic compound in the present invention, it is desirable to arrange an adsorption tower filled with an adsorbent in parallel with two units and use the adsorption and desorption alternately and repeatedly. As the adsorbent used in the present invention, activated carbon, alumina,
Examples thereof include silica-alumina and zeolite. In particular, an adsorbent having a solid acid content of 0.15 mmol / g or more (measured by an ammonia adsorption method) or more is preferable, and silica-alumina having an alumina content of 20 to 40% by weight is preferable.
【0012】多環芳香族化合物が吸着除去された供給原
料炭化水素油は、加熱炉で加熱されて、水素と伴に水素
化処理触媒が充填された反応塔に導入され、水素化処理
に付される。本発明での水素化処理は、通常の水素化処
理装置を使用して、通常の水素化処理触媒を使用し行う
ことができる。The feed hydrocarbon oil from which the polycyclic aromatic compound has been adsorbed and removed is heated in a heating furnace, introduced into a reaction column filled with a hydrotreating catalyst together with hydrogen, and subjected to hydrotreating. Is done. The hydrotreating in the present invention can be carried out by using a normal hydrotreating apparatus and a normal hydrotreating catalyst.
【0013】本発明で使用される水素化処理触媒として
は、例えば、無機酸化物担体に水素化活性金属成分を担
持した通常の水素化脱メタル触媒、水素化脱硫触媒、水
素化分解触媒が使用可能である。無機酸化物担体として
は、例えば、アルミナ、シリカ、チタニア、アルミナ−
シリカ、アルミナ−チタニア、アルミナ−ボリア、アル
ミナ−マグネシア、アルミナ−ジルコニア、アルミナ−
リン、シリカ−チタニア、アルミナ−シリカ−ボリア、
アルミナ−シリカ−リン、アルミナ−チタニア−シリ
カ、アルミナ−チタニア−リン、アルミナ−ボリア−リ
ンなどが挙げられ、中でもアルミナ、アルミナ−シリ
カ、アルミナ−チタニア、アルミナ−ボリア、アルミナ
−リンなどが好適である。また、分解成分であるゼオラ
イトを含有する、アルミナ、アルミナ−シリカ、アルミ
ナ−チタニア、アルミナ−ボリア、アルミナ−リンなど
の担体も好適である。As the hydrotreating catalyst used in the present invention, for example, a usual hydrodemetallizing catalyst, a hydrodesulfurizing catalyst, or a hydrocracking catalyst in which a hydrogenation active metal component is supported on an inorganic oxide carrier is used. It is possible. As the inorganic oxide carrier, for example, alumina, silica, titania, alumina-
Silica, alumina-titania, alumina-boria, alumina-magnesia, alumina-zirconia, alumina-
Phosphorus, silica-titania, alumina-silica-boria,
Alumina-silica-phosphorus, alumina-titania-silica, alumina-titania-phosphorus, alumina-boria-phosphorus, and the like, among which alumina, alumina-silica, alumina-titania, alumina-boria, alumina-phosphorus, and the like are preferable. is there. Carriers containing zeolite, which is a decomposition component, such as alumina, alumina-silica, alumina-titania, alumina-boria, and alumina-phosphorus are also suitable.
【0014】水素化活性金属成分としては、周期律表第
VIA族金属および第VIII族金属が例示され、中で
もニッケルおよび/またはコバルトとモリブデンおよび
/またはタングステンの組み合わせが好ましい。また、
水素化活性金属成分の担持量は、酸化物換算で、第VI
A族金属が8〜30重量%、第VIII族金属が1〜1
0重量%の範囲が好適である。Examples of the hydrogenation-active metal component include metals of Group VIA and VIII of the Periodic Table, and a combination of nickel and / or cobalt with molybdenum and / or tungsten is preferred. Also,
The supported amount of the hydrogenation-active metal component is represented by VI.
8-30% by weight of Group A metal, 1-1 of Group VIII metal
A range of 0% by weight is preferred.
【0015】本発明での水素化処理条件は、特に限定さ
れるものではなく、供給原料炭化水素油の種類、脱メタ
ル率、脱硫率、分解率などの目標値により通常の水素化
処理条件から適宜選択することができる。例えば、反応
温度250℃〜450℃、反応圧力2〜30Mpa、液
空間速度0.1〜10h−1、水素/オイル比50〜1
500nm3/klなどの条件が例示される。[0015] The hydrotreating conditions in the present invention are not particularly limited, and may be deviated from ordinary hydrotreating conditions by target values such as the kind of feedstock hydrocarbon oil, demetallization rate, desulfurization rate, and cracking rate. It can be selected as appropriate. For example, a reaction temperature of 250 ° C. to 450 ° C., a reaction pressure of 2 to 30 Mpa, a liquid hourly space velocity of 0.1 to 10 h −1 , and a hydrogen / oil ratio of 50 to 1
Conditions such as 500 nm 3 / kl are exemplified.
【0016】本発明の方法では、予めコーク生成の原因
となる多環芳香族化合物を吸着除去した炭化水素油を水
素化処理するため、触媒上へのコーク析出が少なく、触
媒のコーク失活が防止されるので、触媒寿命が長くな
り、水素化処理の運転期間を長くすることができる。In the method of the present invention, hydrocarbon oil from which a polycyclic aromatic compound causing coke formation has been adsorbed and removed in advance is subjected to hydrogenation treatment, so that coke deposition on the catalyst is small and coke inactivation of the catalyst is reduced. As a result, the life of the catalyst is prolonged, and the operation period of the hydrotreatment can be prolonged.
【0017】また、本発明の方法で軽油などの炭化水素
油を高温で超深度水素化脱硫しても、生成油は、軽油の
着色の原因となる2環、3環類の多環芳香族化合物が少
ないので、生成油は透明性を増し、また、芳香族化合物
成分の含有量も低減されるので、商品価値の高い高品質
の軽油を得ることができる。Even when a hydrocarbon oil such as a gas oil is subjected to ultra-deep hydrodesulfurization at a high temperature by the method of the present invention, the resulting oil still has a bicyclic or tricyclic polycyclic aromatic which causes coloring of the gas oil. Since the amount of the compound is small, the resulting oil increases the transparency and the content of the aromatic compound component is reduced, so that a high-quality light oil having high commercial value can be obtained.
【0018】[0018]
【実施例】以下に実施例を示し本発明を本発明を具体的
に説明するが、本発明はこれにより限定されるものでは
ない。EXAMPLES The present invention will be described below in detail with reference to Examples, but the present invention is not limited thereto.
【0019】実施例1 下記の性状を有する供給原料炭化水素油を、アルミナ含
有量28wt%のシリカ−アルミナ(1/16インチ、
ペレット)の吸着剤が充填された吸着塔に、液空間速度
4.0hr−1、吸着温度24℃、大気圧で通油し、次
いで、2.9wt%CoO−MoO3−Al2O3触媒
を400ml充填した脱硫反応塔に導入して水素化脱硫
反応を下記条件で、生成油中の硫黄濃度が0.25wt
%となるように反応温度を調節しながら寿命試験を実施
した。反応フローを図1に示す。 供給原料炭化水素油: 密度=0.9780(g/cm3@15℃) 硫黄濃度=4.10(wt%) バナジウム濃度=85(wtppm) ニッケル濃度=27(wtppm) アスファルテン含有量=7.8(wt%) 反応条件: LHSV=0.2(hr−1) H2/Oil=800(nM3/Kl) 水素圧=13.5(Mpa)EXAMPLE 1 A feedstock hydrocarbon oil having the following properties was prepared from silica-alumina (1/16 inch,
The oil is passed through an adsorption tower filled with an adsorbent (pellet) at a liquid hourly space velocity of 4.0 hr −1 , an adsorption temperature of 24 ° C. and an atmospheric pressure, and then a 2.9 wt% CoO—MoO 3 —Al 2 O 3 catalyst Was introduced into a desulfurization reaction tower filled with 400 ml of water, and the hydrodesulfurization reaction was carried out under the following conditions so that the sulfur concentration in the produced oil was 0.25 wt.
% While adjusting the reaction temperature so as to obtain%. The reaction flow is shown in FIG. Feed hydrocarbon oil: Density = 0.9780 (g / cm 3 @ 15 ° C) Sulfur concentration = 4.10 (wt%) Vanadium concentration = 85 (wtppm) Nickel concentration = 27 (wtppm) Asphaltene content = 7. 8 (wt%) Reaction conditions: LHSV = 0.2 (hr −1 ) H 2 / Oil = 800 (nM 3 / Kl) Hydrogen pressure = 13.5 (Mpa)
【0020】反応結果を図2に示す。2000時間の反
応後の触媒をトルエンで洗浄して油分を除去し、触媒に
堆積したコークを定量したところ、21wt%であっ
た。また、上記反応で得られた2000時間目の生成油
中のアスファルテンをn−ヘプタンで抽出し定量したと
ころ、2.4wt%であった。図2から本発明の方法
は、比較例1の従来の方法に比較して、0.25wt%
硫黄濃度の生成油を得る反応温度が低く、触媒寿命が長
いことが分かる。FIG. 2 shows the reaction results. After 2,000 hours of reaction, the catalyst was washed with toluene to remove oil, and the amount of coke deposited on the catalyst was determined to be 21% by weight. Further, asphaltene in the product oil obtained at the time of 2000 hours obtained by the above reaction was extracted with n-heptane and quantified, and it was 2.4 wt%. FIG. 2 shows that the method of the present invention is 0.25 wt% compared to the conventional method of Comparative Example 1.
It can be seen that the reaction temperature for obtaining a product oil having a sulfur concentration is low and the catalyst life is long.
【0021】比較例1 実施例1において、実施例1で使用した供給原料炭化水
素油を吸着剤が充填された吸着塔に通油しないで、2.
9wt%CoO−MoO3−Al2O3触媒を400m
l充填した脱硫反応塔に導入して、実施例1と全く同様
にして寿命試験を実施した。Comparative Example 1 In Example 1, the feedstock hydrocarbon oil used in Example 1 was not passed through an adsorption tower filled with an adsorbent, and
9wt% CoO-MoO 3 -Al 2 O 3 catalyst to 400m
Then, the product was introduced into the packed desulfurization reaction tower, and a life test was performed in exactly the same manner as in Example 1.
【0022】反応結果を図2に示す。2000時間の反
応後の触媒をトルエンで洗浄して油分を除去し、触媒に
堆積したコークを定量したところ、28wt%であっ
た。また、上記反応で得られた2000時間目の生成油
中のアスファルテンをn−ヘプタンで抽出し定量したと
ころ、2.7wt%であった。FIG. 2 shows the reaction results. After 2,000 hours of reaction, the catalyst was washed with toluene to remove oil, and the amount of coke deposited on the catalyst was determined to be 28% by weight. Further, asphaltene in the produced oil at the time of 2000 hours obtained by the above reaction was extracted with n-heptane and quantified, and it was 2.7 wt%.
【0023】[0023]
【発明の効果】本発明の方法では、供給原料炭化水素油
中の多環芳香族化合物を予め除去した炭化水素油を水素
化処理することにより、触媒のコーク失活が防止しさ
れ、触媒寿命を伸ばすことができる。また、生成油中の
アスファルテン含有量をもすくないので、接触分解用供
給原料として好適な生成油が得られる。According to the method of the present invention, the coke deactivation of the catalyst is prevented by hydrotreating the hydrocarbon oil from which the polycyclic aromatic compounds in the feedstock hydrocarbon oil have been removed in advance, and the catalyst life is reduced. Can be extended. Further, since the content of asphaltenes in the product oil is small, a product oil suitable as a feedstock for catalytic cracking can be obtained.
【図1】図1は、実施例1で使用した炭化水素油の水素
化処理のフローを模式的に表した図面である。FIG. 1 is a drawing schematically showing a flow of hydrotreating a hydrocarbon oil used in Example 1.
【図2】図2は、実施例1および比較例1の寿命試験の
結果を示すグラフである。FIG. 2 is a graph showing the results of a life test of Example 1 and Comparative Example 1.
Claims (2)
て、該炭化水素油中の多環芳香族化合物を吸着除去して
減少させた後、触媒の存在下に水素化処理することを特
徴とする炭化水素油の水素化処理方法。Claims 1. A method comprising contacting a feed hydrocarbon oil with an adsorbent to adsorb and remove polycyclic aromatic compounds in the hydrocarbon oil to reduce the same, and then subjecting the hydrocarbon oil to hydrotreatment in the presence of a catalyst. A method for hydrotreating a hydrocarbon oil.
触は、該炭化水素油の加熱前に行うことを特徴とする請
求項1記載の炭化水素油の水素化処理方法。2. The method for hydrotreating a hydrocarbon oil according to claim 1, wherein the contact between the feed hydrocarbon oil and the adsorbent is performed before heating the hydrocarbon oil.
Priority Applications (1)
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JP10378020A JP2000178566A (en) | 1998-12-18 | 1998-12-18 | Method for hydrotreatment of hydrocarbon oil |
Applications Claiming Priority (1)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
JP10378020A JP2000178566A (en) | 1998-12-18 | 1998-12-18 | Method for hydrotreatment of hydrocarbon oil |
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Publication Number | Publication Date |
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JP2000178566A true JP2000178566A (en) | 2000-06-27 |
Family
ID=18509332
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JP10378020A Pending JP2000178566A (en) | 1998-12-18 | 1998-12-18 | Method for hydrotreatment of hydrocarbon oil |
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Cited By (4)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
JP2001279273A (en) * | 2000-03-31 | 2001-10-10 | Idemitsu Kosan Co Ltd | Kerosene-based fuel oil for fuel cell |
JP2010509440A (en) * | 2006-11-06 | 2010-03-25 | サウジ アラビアン オイル カンパニー | Process for the removal of nitrogen and polynuclear aromatics from hydrocrackers and FCC feedstocks |
US8828219B2 (en) | 2011-01-24 | 2014-09-09 | Saudi Arabian Oil Company | Hydrocracking process with feed/bottoms treatment |
CN111595928A (en) * | 2020-04-29 | 2020-08-28 | 中国石油天然气股份有限公司 | Method for judging thermal cracking degree of crude oil |
-
1998
- 1998-12-18 JP JP10378020A patent/JP2000178566A/en active Pending
Cited By (5)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
JP2001279273A (en) * | 2000-03-31 | 2001-10-10 | Idemitsu Kosan Co Ltd | Kerosene-based fuel oil for fuel cell |
JP2010509440A (en) * | 2006-11-06 | 2010-03-25 | サウジ アラビアン オイル カンパニー | Process for the removal of nitrogen and polynuclear aromatics from hydrocrackers and FCC feedstocks |
US8828219B2 (en) | 2011-01-24 | 2014-09-09 | Saudi Arabian Oil Company | Hydrocracking process with feed/bottoms treatment |
US9534179B2 (en) | 2011-01-24 | 2017-01-03 | Saudi Arabian Oil Company | Hydrocracking process with feed/bottoms treatment |
CN111595928A (en) * | 2020-04-29 | 2020-08-28 | 中国石油天然气股份有限公司 | Method for judging thermal cracking degree of crude oil |
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