MIME-Version: 1.0 Content-Type: multipart/related; boundary="----=_NextPart_01D5E5AD.468609B0" This document is a Single File Web Page, also known as a Web Archive file. If you are seeing this message, your browser or editor doesn't support Web Archive files. Please download a browser that supports Web Archive, such as Windows® Internet Explorer®. ------=_NextPart_01D5E5AD.468609B0 Content-Location: file:///C:/AAC9D4D2/Manuscript2.htm Content-Transfer-Encoding: quoted-printable Content-Type: text/html; charset="windows-1252" Ali Akbar Miran Beigi et al.

Room temperature imidazolium-based ionic liquids as scavengers for hydrogen sulfide removal = of crude oil

 

Ali Akbar Mi= ran Beigi*,a,= Maryam Yousefia,b, Majid Abd= oussb

a Research Institute of Petroleum Industry, = West Blvd. of Azadi Sport Complex, Tehran, Iran=

bDepartment<= /span> of Chemistry, Amirkabir University of Technology, P.O. Box 15875-4413, Tehran, Iran=


=  

=  

= Article history:

= Received 20 Aug 2018

= Received in revised form 24 Oct 2018

= Accepted 30 Oct 2018

= Available online 25 Dec 2018

=  

= ------------------------

=  

= Keywords:

H2S removal

Crude oil

Ionic liquids

Commercial scavengers

Petroleum refining

=  

=  

=  

=  

=  

=  

=  

=                                                 =                  

Abstract

Determination of H2S amounts in crude oil was performed by a precise method instead of UOP163 that were developed in our pervious works. Evaluation of ILs and scavengers were done by two ways. The first one was based on variable concentration of ILs as the scavenger (dyna= mic method) and the second one was based on a constant concentration of the scavenger during H2S removal process (static method). In the static method, design of experiments was performed for all three tested ILs and three parameters such as time, temperature and dosage (injection volume) of ILs w= ere investigated. A wide range of time and temperature was also studied accordi= ng to operating conditions in petroleum terminals. Dose of ILs, was obtained f= rom the dynamic method. According to the obtained results, these ILs had a significant effect on H2S reduction in crude oil, so that H2S concentration= in some conditions was less than 1 ppm. In comparison between ILs and commerci= al scavengers’s performance can be properly understood t= hat not only ILs reduced H2S concentration, but also their dosage was very low,= and mole ratio of [IL]/[H2S] was 1-3 that it was negligible compared with commercial scavengers. Also the results showed that [EMIM][NTf2] was more effective than the other I= Ls in H2S removal.


 


. Introduction

In contrast ionic liquids (ILs) provides a vaporless, thermally stable [18, 19], reusable “green” solvent and catalyst for chemic= al reactions, so ILs has very possibility for removal of H2S. ILs are molten salts composed entirely of ions, and many o= f them are liquids at room temperature. Room temperature ionic liquids (RTILs), often referred to as ‘designer solvents’, have been= the great focus of scientists in various fields since they can be tuned for specific applications [20-27]. Nowadays, the most commonly studied ILs norm= ally contain, imidazolium, ammonium, phosphonium, pyridinium, and pyrrolidinium cations, and tetrafluoroborate, hexafluoropho= sphate, bistrifluorosulfonylimide and triflate anions [20, 25, 28-30].The physicochemical properties of ILs can be finely tuned by slight structural changes of the corresponding cations and anions [23–26]. To better understand the nature of ionic liquids and rationally ex= pand their applications especially as pollutant scavenger and electrolyte, knowl= edge of their thermophysical and electrochemical properties is required. In this work [<= span class=3DSpellE>Hmim][BF4], [Emim][Ntf2] and [Bmim][MeSO4] were used as scavengers for H= 2S removal from crude oil and then the results were compared with several commercial scavengers. Molecular structures of the three ILs are shown in Fig.1.

In our previous work, physical and electrochemical properties of these ILs were investigated. Viscosity, solubility, thermal decomposition and electrochemical window of three ILs were studied more than the other properties. So these mentioned properties have been applied for H= 2S removal. For example, the viscosity of selected ILs was fully compatible wi= th the crude oil. Therefore, use of them in crude oil was not a problem. The thermal stability of ILs was very high and their ability at high temperatur= es was excellent. ILs may be hydrophilic or lipophilic.

1-Hexyl-3-Methylimidazolium Tetrafuoroborate=

[HMIM][BF4]

C10H19BF4N2

M.W. =3D 254.08

IL1

1-Buthyl-3-Methylimidazolium Methylsulfate

[BMIM][MeSO4]

C9H18N2O4S

M.W. =3D 250.32

IL3

1-Ethyl-3-Methylimidazolium bis(trifluoromethylsulfonyl)imide

[EMIM][NTf2]

C8H11F6N3O4S2

M.W. =3D 391.32

IL2

Hydrophilic Property                                              =                                            Lipophilic Property                               

 

 

 

 

 


 

 

Molecular structures of the three ILs


 

The hydrophilic and lipophilic ILs can remove H2S of aqueous and organic parts of crude oil respectively. The decomposition temperature ranges of three ILs are shown in Table 1. Also the experimental values of physicochemical properties of [HMIM][B= F4], [EMIM][NTf2] and [BMIM][MeSO4], such as density, refractive index, dynamic = and kinematic viscosities, pH, and surface tension are listed in Table 2. [20]. According to our previous studies these ILs are very suitable for H2S scavenging and to the best of our knowledge we didn’t find any paper relate= d to H2S removal from crude oil by using ILs. In addition, these ILs unlike other scavengers don’t have any disadvantages such as slow synthetics, high consumption, unstable in high temperatures, or increase salt and sediments content. Of course the elimination reaction mechanism is unknown and our further studies certainly will be in this field.

 

In present work determination of H2S amounts in crude= oil was performed by the method that was presented by researchers at Research Institute of Petroleum Industry method (RIPI). [Ref. 31] Then ILs was used = in two different ways as scavengers for H2S removal. Finally, the results of b= oth methods were compared with several commercial scavengers. Also in our next work, metallic nanoparticles will be synthesized in ionic liquids media for= H2S removal from crude oil.

 

= Table 1. Thermal decomposition for investigated ionic liquids

Ionic Liquid

       Decomposition            Temperature Range/ºC

[HMIM][BF4]

310-500

[EMIM][NTf2]

390-510

[BMIM][MeSO4]

317-438

 

t (oC)

r  (g mL-1= )

h  (mPa s)=

= nD

s (mN m= -1)

104 ap  (K)=

pH of 1% Solution

[HMIM][BF4]

10

1.1562

608.1

1.4265

41.4

5.343

&n= bsp;

20

1.1492

311.7

1.4241

40.6

5.525

6.41

25

1.1461

220.0

1.4223

40.4

5.623

6.25

30

1.1425

167.3

1.4211

40.0

5.718

&nb= sp;

40

1.1355

103.3

1.4183

39.8

5.909

5.77

50

1.1280

63.77

1.4158

39.0

6.104

 

60

1.1214

52.22

1.4137

38.2

6.302

5.12

70

1.1122

28.48

1.4106

37.2

6.504

 

80

1.1004

21.39

1.4080

36.6

6.709

4.49

90

1.0874

15.87

1.4051

36.3

6.918

4.17

95

1.0838

13.92

1.4038

35.9

7.025

&n= bsp;

[EMIM][= NTf2]

10

1.5311

55.92

1.4254

40.2

4.706

&n= bsp;

20

1.5220

37.27

1.4232

39.8

5.518

6.48

25

1.5168

31.13

1.4220

39.4

5.929

6.5

30

1.5117

26.28

1.4206

39.0

6.344

&n= bsp;

40

1.5020

19.67

1.4179

38.8

7.186

6.54

50

1.4907

14.96

1.4153

38.6

8.045

&n= bsp;

60

1.4780

11.84

1.4127

38.0

8.925

6.60

70

1.4651

9.506

1.4101

37.2

9.828

&n= bsp;

80

1.4494

7.820

1.4072

36.6

10.76

6.66

90

1.4292

6.539

1.4045

36.0

11.72

6.69

95

1.4230

6.054

1.4033

35.5

12.21

&n= bsp;

[BMIM][= MeSO4]

10

1.2117

220.6

1.4831

46.0

4.457

&n= bsp;

20

1.2053

122.3

1.4777

44.4

4.810

         7.60

25

1.2019

93.78

1.4771

43.7

4.988

7.55

30

1.1983

73.35

1.4765

43.4

5.167

&n= bsp;

40

1.1923

46.85

1.4745

42.6

5.530

7.39

50

1.1853

32.21

1.4719

42.0

5.899

&n= bsp;

60

1.1774

23.02

1.4694

41.2

6.274

7.18

70

1.1668

17.05

1.4673

39.8

6.656

&n= bsp;

80

1.1538

13.14

1.4650

39.0

7.0453<= o:p>

6.96

90

1.1400

10.34

1.4626

38.1

7.443

6.85

95

1.1356

9.257

1.4615

37.6

7.645

 

=  

=  

=  

=  

=  

 

 


Table2.<= /b> Density= r, dynamic viscosity h,  refractive index n<= sub>D, surface tension s, = thermal expansion ap, and pH of the ionic liquids at different temperatures


 

 

2. Experimental

2.1 Materia= ls

= All chemicals and three ionic liquids were purchased from Merck, Aldrich and Fluka companies. The chemicals were used without furt= her purification. Crude oil samples included exported crude oil such as Balarood, Masjed Soleyman, Soomar, Bahregan and Furoozan.

 =

2.2 Experimental procedure

= The RIPI method was applied for determination of H2S amounts in crude oil. As we have previously reported this method was based on preliminary extraction with voltammetric detection. This me= thod offers several inherent advantages for H2S determination. Voltammetric detection methods are specific, since ot= her species are electrochemically inactive at potentials where H2S is detected. Also, this technique is very sensitive. Apparatus for determinati= on of hydrogen sulfide in crude oil is shown in Fig.2.  After the measurement of H2S content in crude oil, evaluation of several commercial scavengers and the I= Ls was done. Unfortunately there was not a systematic and standardized method = to evaluate the efficiency of scavengers. In present work two methods was appl= ied for evaluation. One is related to RIPI, was based on constant concentration= of ILs or commercial scavengers and the other one was based on variable concentration of them that is related to oil export terminals. In the const= ant concentration method for ILs, design of experiment was applied by using Des= ign Expert software.

Fig. 2 The apparatus for determination of hydrogen sulfide in crude oil

 

3. Results and discussion

= 3.1 Evaluation of commercial scavengers

= Evaluation of commercial scavengers was developed by two methods.

= 3.1.1 First method (Variable concentration)

= This method has been developed by the RIPI, had high operating speed. The scaven= gers that were used had fast kinetic and high efficiency. Evaluation in this met= hod was based on measuring and following potential variations of crude oil duri= ng addition of scavengers in a specified time. A potential variation of crude = oil was shown in fig. 3.

Fig. 3 Potential variations of crude oil by addition of a commercial scavenger versus time

 =

=       In the RIPI method, usually in the = one minute intervals, approximately 50 µl of scavenger was added to the certain amount of crude oil (about 100 g) and potential changes versus time and vol= ume consumption of scavenger were recorded (Fig.3).  Mutations that occurred in the potential curves were related to the equivalent point of H2S titration by scavenger. In the equivalent point, almost all H2S contents were neutralized by scavenger and crude oil are free of H2S.

= Primary investigations showed that electrode potential was depended on H2S or S concentration in crude oil. As long as hydrogen sulfide was present in= the crude oil, electrode potential, depending on the H2S concentrati= on in the specified range was nearly between -900 up to -1200 mV. It should be noted that beside H2S concentration the electrode potential coul= d be a function of temperature and electrolyte.  Also according to the Nernst equation, t= he electrode potential is depend on oxidative and reductive concentration, ions mobility= and activity coefficient. Therefore, the potential ranges difference between -9= 00 to -1200 mV may be due to one of the items listed above. In this method, evaluation of H2S reduction was based on decreasing of the elect= rode potential. Experience indicated that when the crude oil was free of H2= S, electrode potential shifted to nearly less than -750 up to -800 mV. To more accurate investigations, 4 samples of commercial scavengers were tested usi= ng this method and the results are given in Table 3.


Sample name

Injection volume /ml

E(initial)/mv

E(final)/mv

Treatment time/min

sulfavent 32<= /b>

0.65

1100

805

15

sulfavent 42<= /b>

0.55

1080

810

10

sulfavent 43<= /b>

1

1000

860

7

sulfavent 44<= /b>

1

1100

945

12


As can be observed, sulfavent 32 an= d sulfavent 43 had better efficiency than the others. L= esser amounts of sulfavent 32 were used, on the other hand, Sulfavent 43 had higher spee= d. So that, for the neutralization of H2S in crude oil, only 1 ml of scavenger was needed during 7 minutes. Although, both methods = gave same results in selection of scavengers, but the RIPI method provided more information, such as the effective time of scavenger and equivalent point.<= o:p>

=  

3.1.2 Second method (Constant concentration)

 This method was based = on instructions of oil export terminals. = First, the amount of H2S was measured in crude oil and then specific do= sage of scavengers was added to the crude oil. The consumed volume of scavenger = (was related to H2S concentration.

sample name

H2S content in crude  befor treatment / ppm

H2S content in crude after 1 hour treatment / ppm

H2S content in crude after overnight treatment / ppm=

H2S content in crude before treatment after overnight / ppm<= b>

sulfavent 32<= /b>

75

10.5

< 1.0

43

sulfavent 42<= /b>

75

47

< 1.0

43

sulfavent 43<= /b>

75

5.4

< 1.0

43

sulfavent 44<= /b>

75

26

17

43

Here H2S concentration was based on the amount of hydrogen sulf= ide in crude oil, which is usually between 50 to 100 ppm of scavenger and                   depending on its efficiency, was about 2 to 5 times of the amount of H2S in crude oil.

= In a general evaluation, 100 g of a crude oil containing 75 ppm H2S, = was chosen. Then 225 ppm ([Scavenger]/[H2= S]:3) of the scavenger was added to it. After an hour stirring at room temperatur= e, the H2S concentration was measured with RIPI method. The same experimental conditions were done for an overnight and the results were reported and compared. Accordingly, all four samples were tested and the results are shown in Table 4.

 Since the experiments = were conducted on consecutive days, and there was no possibility of H2S amount stabilization. So, = the results were normalized in first and the last columns. As can be seen in the table, without any commercial scavenger, H2S concentration has reached to 43 ppm after an overnight, but by mistake this reduction was generally considered to be scavenger. As a result, long reaction time, was = one of disadvantages in this method.

 

 

 

The result showed that all scavengers, with the exception of Sulfavent 44, had the ability to remove H2= S from crude oil. Whereas Sulfavent 32 and 43, both had satisfactory results after an hour. It seems that this method, where to store crude oil before loading, is appropriate. In the sec= ond method, which was developed by RIPI, those of scavengers that had rapid reaction kinetics (less than 15 min) will be successful in reduction or elimination of H2S from crude oil.

 =

3.2 Evaluat= ion of Ionic Liquids

3.2.1 First method (Variable concentration)

= The basis of this method, as was explained in the case of scavengers, was based= on gradual addition of ionic liquids and measuring and following potential variations of crude oil. First, the amount of H2S was measured in crude oil, then 20 ml of isopropyl alcohol and 3= 0 ml of toluene was added to 50 g of crude oil that containing 100 ppm of H= 2S. At the beginning, electrode potential was read, then certain amount of ionic liquid (approximately 10 µl) was added to crude oil in the same time interv= als and potential variations was recorded. Fig. 4 shows the potential variations versus time for three ionic liquids. Also this method determined the requir= ed

volume of ionic liquid to minimize concentration to less than 15 ppm of H2S. When the electrode

potential shifted to less than -800 mV, H2S concentration was less than 15 ppm. =

 

The electrode response versus time during the gradual addition of t= he ionic liquid in crude oil

= As can be seen in this chart, the ILs have been abl= e to reduce H2S concentration to less than 1 ppm, in a short time (le= ss than 30 minutes). Also mole ratio of [IL]/ [H2S] was 2.3, 1.3 and 2.5 for [HMIM][BF4], [EMIM][NTf2= ] and [BMIM][MeSO4] respectively that these were equal to 75 µl, 4= 8 µl and 76 µl of ionic liquids. These values ​​were negligible in comparison to commercial scavengers. Also among the three ionic liquids, [E= MIM] [NTf2] had a higher efficiency in H2S removal from cr= ude oil. Since [EMIM] [NTf2] is lipophilic and its viscosity is clos= er to crude oil’s viscosity, it can be better H2S scavenger, moreover the consumed volume of IL2 is less than the others.

=  

3.2.1 Second method (Constant concentration)

= In this method, the H2S concentration was measured in 15 g of crude oil, then specific dosage or concentration of io= nic liquid was added to the crude oil. In fact, according to the dynamic method results and operating condition in crude oil terminals, the required time, temperature and dosage of ILs, were determined f= or H2S removal. Finally, after considering the conditions in crude oil terminals (crude oil temperature, scavenger dosage and duration the crude oil passes through pipeline) and according to dynamic method results, it can be conclu= ded that the required amount of ILs to remove H2S should be selected from 1 to 3 [IL]/ [H2S] mole ratio, the reaction time from 25 mi= n to 35 min and the temperature from 20 ° C to 50 ° C, should be selected. After identifying these factors design of experiment was performed for each IL, u= sing Design Expert software.

 

3.2.2 Design of experiment<= /span>

As mentioned, the effective parameters or factors on H2S concentration was detected by using dynamic method. Then design of experiment was performed using Expert design software that contained 20 runs or tests for each IL and various conditions such as dosage, temperature and reaction time, was applied separately for each run. The results are given in Table. 5. As can be seen = in this table, first the concentration of H2S was 100 ppm and after applying various conditions, such as dosage, time and temperature, H2<= /sub>S concentration was reduced even less than 1 ppm. Columns 5 to 8 were normali= zed, because in some cases, H2S concentration was more than 100 ppm, therefore all results were normalized to 100 ppm. It is obvious that if IL dosage, time and temperature was grater, H2= S concentration was lower.

Runs 4 and 14 for IL2, and crude oil sample without u= sing ionic liquids are briefly reviewed in Table 6. H2S concentration= at the beginning was 113.27 ppm that was normalized to 100 ppm after 35 min stirring at 30 oC, H2S concentration was reached to…. The electrode potential shifted to -675 mV indicated that H2S concentration was reached to less than 1 ppm. Also after run 14, H2S concentration was decreased from 113.27 p= pm to less than 1 ppm. The potentiometric curves for crude oil, runs 4 and 14<= /span> are presented respectively in Figure<= /span> 5.

The first chart showed H2S concentration before addition of ionic liquids and the second one showed H2S concentration after addition of ionic liquids in a special time and temperature. The electrode potential versus volume of silver nitrate was sh= own in Fig.5 and H2S concentration can be calculated before and afte= r of ILs addition, according to the following formula.

 

 

 


Table 5 Design of experiment for three ionic liqu= ids

Run Order

Temp/ oC

Time /min

Dose [IL]/[H2S= ]

ppm H2S before treatment

ppm H2S IL1

ppm H2S IL2

ppm H2S IL3


1

35

30

2

100

21.30

27.3

14.82

2

20

25

1

100

78.5

32.5

62.95

3

35

30

2

100

17.21

22.46

19.63

4

50

35

1

100

<1

<1

<1

5

20

35

3

100

<1

9.3

17.51

6

50

25

3

100

<1

4.02

<1

7

35

30

2

100

19.02

20.79

19.85

8

35

30

3.633

100

<1

7.3

3.1

9

35

30

0.367

100

38.5

48.9

27.46

10<= /p>

10.505

30

2

100

32.3

41.83

26.27

11<= /p>

35

30

2

100

18.44

18.55

19.04

12<= /p>

59.495

30

2

100

<1

3.93

<1

13<= /p>

35

21.835

2

100

21.47

30.47

35.79

14<= /p>

35

38.165

2

100

<1

8.2

4.34

15<= /p>

35

30

2

100

20.71

21.41

17.69

16<= /p>

35

30

2

100

19.21

19.10

15.60

17<= /p>

20

35

1

100

6.1

11.1

38.25

18<= /p>

50

35

3

100

<1

<1

<1

19<= /p>

50

25

1

100

8.4

11.3

<1

20<= /p> 20

25

3

100

23.28

14.32

24.55


 

 

 

 

 


Table 5 Continue of Design of experiment for three ionic liquids


 

weight

Volume consumption of AgNO3

Initial potential (mV)

H2S (ppm)=

Condition

Time (min)

Temperature (oC)

Dose [IL]/[H2S]

Crude oil

10.22

7.2353

-1100

113.27

-

-

-

IL2 (Run 4)

15

-

-670

<1

35

50

1

IL2 (Run 5)

15

-

-575

<1

35

20

3


 

Fig. 5 The electrode potential versus volume of silver nitrate for H<= sub>2S measurement in crude oil

 

 

H2S concentration before Run 4 and Run 14 = for [EMIM][NTf2] was 116.66 ppm as shown = in fig. 6a and 6b. H2S concentration was diminished to less than 10= ppm After Runs 4 and 14. Fig.7 and 8 showed the electrode potential versus volu= me consumption of silver nitrate for runs 4 and 14 respectively. The EP3 (third equivalent point) for run 4 and EP1 for run 14 showed the required volume consumption of silver nitrate that neutralized H2S amounts in cr= ude oil.

 

Fig. 6(a) The electrode potential versus volume of silver nitrate for H2S measurement in crude oil that contains IL= 2

 

Fig. 6(b) The electrode potential versus volume of silver nitrate for H2S measurement in crude oil that contains IL= 2

 =

Fig. 7 The electrode potential versus volume of silver nitrate for H2S measurement in crude oil that contains IL= 2

 

Because the electrode potential was started with -675= mV, as a result H2S concentrations is les= s than 1 ppm.

= We found that all three parameters had significant effect in H2S removal by obtained results of this software. Here a few charts are examined briefly in fig. 8.

Fig. 8 Curves of temperature versus time at constant dosage=

= These figures showed that at constant dosage, if temperature and time were grater, H2S concentration was less. Al= so [EMIM][NTf2] had

better efficiency than the other ILs in H2S removal, because it reduced H2S concentration to less than 15 ppm in a short time.

 

Conc= lusions

= The results showed that all three ionic liquids were chosen correctly, because = all of them are suitable for H2S removal from crude oil. The investigation of chemical and physical properties of ionic liquids that all results were presented in our previous work, were indicated that some properties such as high thermal stability, pH, solubility and wide electroc= hemical windows, defined them as a suitable scavenger to H2S removal. Us= ing ionic liquids in the limited situation, and at low concentrations of H= 2S, is effective for crude oil sweetening. In comparison between commercial scavengers and ionic liquids and according to the obtained results from dyn= amic method and design of experiments, we found that ILs is more effective than commercial scavengers because the volume consumption of ILs is less than the scavengers. Also ILs could reduce H2S concentration to less than= 1 ppm. In design of experiments, three parameters (dosage, time and temperatu= re) were investigated which all of them are effective in H2S removal= and time is the most effective parameter. In addition, the results of dynamic method and design of experiment show that [EMIM][NTf2] has better performance, also lower dosage of it, has been spent.

 

 


 

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