Preparation of tungstophosphoric acid intercalated MgAl layered double hydroxides with a tunable interlayer spacing and their catalytic esterification performance in the deacidification of crude oil

WANG Hao; LI Dong-mei; WU Yan; DING Yu

Volume 48 Issue 1

Jan. 2020

Turn off MathJax

Article Contents

Article Navigation > Journal of Fuel Chemistry and Technology > 2020 > 48(1): 44-51

WANG Hao, LI Dong-mei, WU Yan, DING Yu. Preparation of tungstophosphoric acid intercalated MgAl layered double hydroxides with a tunable interlayer spacing and their catalytic esterification performance in the deacidification of crude oil[J]. Journal of Fuel Chemistry and Technology, 2020, 48(1): 44-51.

Citation:

WANG Hao, LI Dong-mei, WU Yan, DING Yu. Preparation of tungstophosphoric acid intercalated MgAl layered double hydroxides with a tunable interlayer spacing and their catalytic esterification performance in the deacidification of crude oil[J]. Journal of Fuel Chemistry and Technology, 2020, 48(1): 44-51.

Citation:

WANG Hao, LI Dong-mei, WU Yan, DING Yu. Preparation of tungstophosphoric acid intercalated MgAl layered double hydroxides with a tunable interlayer spacing and their catalytic esterification performance in the deacidification of crude oil[J]. Journal of Fuel Chemistry and Technology, 2020, 48(1): 44-51.

PDF( 1812 KB)

Preparation of tungstophosphoric acid intercalated MgAl layered double hydroxides with a tunable interlayer spacing and their catalytic esterification performance in the deacidification of crude oil

WANG Hao¹,
LI Dong-mei¹,
WU Yan^{1
,
,},
DING Yu²

1.
School of Chemistry and Chemical Engineering, Southwest Petroleum University, Chengdu 610500, China
2.
State Key Laboratory of Oil and Gas Reservoir Geology and Exploitation, Southwest Petroleum University, Chengdu 610500, China

Funds:

National Natural Science Foundation of China 21506176

More Information

Corresponding author: WU Yan, E-mail: wyana524@163.com
Received Date: 2019-08-12
Rev Recd Date: 2019-10-05

Available Online: 2021-01-23

Publish Date: 2020-01-10

Abstract

Abstract

This study demonstrates the synthesis of MgAl layered double hydroxides (LDHs) intercalated with tungstophosphoric acid (H₃PW₁₂O₄₀, HPW) by an ion exchange method, and different interlayer spacings (d₀₀₃) are obtained by adjusting the ion exchange temperature and time. The crystalline structures, molecular structures, atomic compositions, acidity, and specific surface areas of the LDH samples are rigorously characterized. A relatively high ion exchange temperature is demonstrated to be favorable for the formation of a large d₀₀₃ value of around 1.46 nm, while a long exchange time is favorable for the formation of a small d₀₀₃ value of around 1.05 nm. The different values of d₀₀₃ are the result of different orientations of HPW anions within the interlayer space. Here, d₀₀₃=1.46 nm is obtained when P₂W₁₈O₆₂^6- and PW₁₁O₃₉^7- anions are arranged in the interlayer with their C₂ axes respectively tilted toward and perpendicular to the LDH layer planes. In contrast, d₀₀₃=1.05 nm is obtained when PW₁₂O₄₀^3- anions are grafted onto the LDH layers with their C₂ axis perpendicular to the layer planes. Furthermore, the catalytic esterification performance of the samples is investigated for the deacidification of a model crude oil. Compared with PW₁₂O₄₀^3- anions, the presence of P₂W₁₈O₆₂^6- and PW₁₁O₃₉^7- anions in the interlayer produce a higher proportion of sites with intermediate acidity that function as catalytic sites. Moreover, a large value of d₀₀₃ facilitates the diffusion of reactants into the interlayer, which enhances their contact with the catalytic sites, and thereby increases the catalytic esterification performance of the LDHs in the deacidification of crude oil.
- tungstophosphoric acid,
- layered double hydroxides (LDHs),
- interlayer spacing,
- esterification,
- deacidification

FullText(HTML)

References(32)

References

[1]	SLAVCHEVA E, SHONE B, TURNBULL A. Review of naphthenic acid corrosion in oilrefining[J]. Brit Corros J, 1999, 34(2):125-131. doi: 10.1179/000705999101500761
[2]	FU X, DAI Z, TIAN S, LONG J, WANG X. Catalytic decarboxylation of petroleum acids from high acid crude oils over solid acid catalysts[J]. Energy Fuels, 2008, 22(3):1923-1929. doi: 10.1021/ef7006547
[3]	DASTJERDI Z, DUBÉ M A. Acid-catalyzed esterification of naphthenic acids[J]. Environ Prog Sustainable Energy, 2013, 32(2):406-410. doi: 10.1002/ep.11606
[4]	WANG Y Z, LI J Y, SUN X Y, DUAN H L, SONG C M, ZHANG M M, LIU Y P. Removal of naphthenic acids from crude oils by fixed-bed catalytic esterification[J]. Fuel, 2014, 116:723-728. doi: 10.1016/j.fuel.2013.08.047
[5]	CAVANI F, TRIFIRÒ F, VACCARI A. Hydrotalcite-type anionic clays:Preparation, properties and applications[J]. Catal Today, 1991, 11(2):173-301. http://d.old.wanfangdata.com.cn/NSTLQK/NSTL_QKJJ029328183/
[6]	段雪, 张法智.插层组装与功能材料[M].北京:化学工业出版社, 2007. DUAN Xue, ZHANG Fa-zhi. Intercalation Assembly and Functional Materials[M]. Beijing:Chemistry Industry Press, 2007.
[7]	王恩波, 胡长文.多酸化学导论[M].北京:化学工业出版社, 1998. WANG En-bo, HU Chang-wen. Introduction of Polyacid Chemistry[M]. Beijing:Chemistry Industry Press, 1998.
[8]	WU Y, LIU X Y, LEI Y Q, QIU Y, WANG M L, WANG H. Synthesis and characterization of 12-tungstophosphoric acid intercalated layered double hydroxides and their application as esterification catalysts for deacidification of crude oil[J]. Appl Clay Sci, 2017, 150:34-41. doi: 10.1016/j.clay.2017.09.007
[9]	POPE M T. Heteropoly and Isopoly Oxometalates[M]. Berlin:Springer, 1983.
[10]	吴雁, 雷艳清, 刘新月, 邱月, 王豪. 12-磷钨酸插层MgAl水滑石的合成、表征及催化酯化原油脱酸性能[J].燃料化学学报, 2017, 45(9):1049-1055. doi: 10.3969/j.issn.0253-2409.2017.09.004 WU Yan, LEI Yan-qing, LIU Xin-yue, QIU Yue, WANG Hao. Synthesis and characterization of 12-tungstophosphoric acid intercalated MgAl layered double hydroxides and their application as esterification catalysts for deacidification of crude oil[J]. J Fuel Chem Technol, 2017, 45(9):1049-1055. doi: 10.3969/j.issn.0253-2409.2017.09.004
[11]	WANG H, DUAN W, WU Y, TANG Y, LI L. Synthesis of magnesium-aluminum layered double hydroxide intercalated with ethylene glycol by the aid of alkoxides[J]. Inorg Chim Acta, 2014, 418:163-170. doi: 10.1016/j.ica.2014.04.031
[12]	JIA Y, FANG Y, ZHANG Y, MIRAS H N, SONG Y F. Classical Keggin intercalated into layered double hydroxides:Facile preparation and catalytic efficiency in Knoevenagel condensation reactions[J]. Chem-Eur J, 2015, 21(42):14862-14870. doi: 10.1002/chem.201501953
[13]	MA J J, YANG M, CHEN Q, ZHANG S S, CHENG H, WANG S Y, LIU L, ZHANG C Y, TONG Z W, CHEN Z. Comparative study of Keggin-type polyoxometalate pillared layered double hydroxides via two synthetic routes:Characterization and catalytic behavior in green epoxidation of cyclohexene[J]. Appl Clay Sci, 2017, 150:210-216. doi: 10.1016/j.clay.2017.09.030
[14]	ARCO M D, CARRIAZO D, GUTIÉRREZ S, MARTÍN C, RIVES V. Synthesis and characterization of new Mg₂Al-paratungstate layered double hydroxides[J]. Inorg Chem, 2004, 43(1):375-384. doi: 10.1021/ic0347790
[15]	WEIR M R, KYDD R A. Synthesis of heteropolyoxometalate-pillared Mg/Al, Mg/Ga, and Zn/Al layered double hydroxides via LDH-hydroxide precursors[J]. Inorg Chem, 1998, 37(21):5619-5624. doi: 10.1021/ic9805067
[16]	YANG Q Z, SUN D J, ZHANG C G, WANG X J, ZHAO W A. Synthesis and characterization of polyoxyethylene sulfate intercalated Mg-Al-nitrate layered double hydroxide[J]. Langmuir, 2003, 19(14):5570-5574. doi: 10.1021/la034526j
[17]	BAJUK-BOGDANOVIĆ D, POPA A, USKOKOVIĆ-MARKOVIĆ S, HOLCLAJTNER-ANTUNOVIĆ I. Vibrational study of interaction between 12-tungstophosphoric acid and microporous/mesoporous supports[J]. Vib Spectrosc, 2017, 92:151-161. doi: 10.1016/j.vibspec.2017.06.007
[18]	ZOU K, ZHANG H, DUAN X. Studies on the formation of 5-aminosalicylate intercalated Zn-Al layered double hydroxides as a function of Zn/Al molar ratios and synthesis routes[J]. Chem Eng Sci, 2007, 62(7):2022-2031. doi: 10.1016/j.ces.2006.12.041
[19]	HOLCLAJTNER-ANTUNOVIĆ I, BAJUK-BOGDANOVIĆ D, POPA A, USKOKOVIĆ-MARKOVIĆ S. Spectroscopic identification of molecular species of 12-tungstophosphoric acid in methanol/water solutions[J]. Inorg Chim Acta, 2012, 383:26-32. doi: 10.1016/j.ica.2011.10.035
[20]	LI Z S, JIA Y, WANG J, YANG P P, JING X Y, ZHANG M L. Synthesis and characterization of tungstophosphoric acid intercalated Ni/Al HTlc with magnetite[J]. J Mater Process Technol, 2009, 209(5):2613-2619. doi: 10.1016/j.jmatprotec.2008.06.005
[21]	SMITH B J, PATRICK V A. Quantitative determination of aqueous dodecatungstophosphoric acid speciation by NMR spectroscopy[J]. Aust J Chem, 2004, 57(3):261-268. doi: 10.1071/CH02037
[22]	CHEN Y, YAN D P, SONG Y F. Tris (hydroxymethyl) aminomethane modified layered double hydroxides greatly facilitate polyoxometalate intercalation[J]. Dalton Trans, 2014, 43(39):14570-14576. doi: 10.1039/C4DT01827C
[23]	BALLESTEROS M A, ULIBARRI M A, RIVES V, BARRIGA C. Optimum conditions for intercalation of lacunary tungstophosphate (Ⅴ) anions into layered Ni (Ⅱ)-Zn (Ⅱ) hydroxyacetate[J]. J Solid State Chem, 2008, 181(11):3086-3094. doi: 10.1016/j.jssc.2008.07.037
[24]	XU L, HU C W, WANG E B. Advances in study of a new class of pillared layered microporous materials-polyoxometalate-type hydrotalcite-like catalysts[J]. J Nat Gas Chem, 1997, 6(2):155-168.
[25]	FUCHS V M, SOTO E L, BLANCO M N, PIZZIO L R. Direct modification with tungstophosphoric acid of mesoporous titania synthesized by urea-templated sol-gel reactions[J]. J Colloid Interface Sci, 2008, 327(2):403-411. doi: 10.1016/j.jcis.2008.08.045
[26]	ZHU Z, TAIN R, RHODES C. A study of the decomposition behaviour of 12-tungstophosphate heteropolyacid in solution[J]. Can J Chem, 2003, 81(10):1044-1050. doi: 10.1139/v03-129
[27]	ZHANG Y H, SU J X, WANG X P, PAN Q, QU W. Photocatalytic performance of polyoxometallate intercalated layered double hydroxide[C]//Materials Science Forum. Trans Tech Publications, 2011, 663: 187-190.
[28]	HIMENO S, TAKAMOTO M, UEDA T. Formation of α-and β-Keggin-type[PW₁₂O₄₀]^3- complexes in aqueous media[J]. Bull Chem Soc Jpn, 2005, 78(8):1463-1468. doi: 10.1246/bcsj.78.1463
[29]	LUO Q S, LI L, WANG Z X, DUAN X. Theoretical study of the layer-anion interactions in magnesium aluminum layered double hydroxides[J]. Chin J Inorg Chem, 2001, 17(6):835-842. http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=wjhxxb200106012
[30]	胡长文, 刘彦勇, 贺庆林, 张继余, 王恩波.新型层柱催化剂ZnAl-XW₁₁Z的酯化催化活性[J].催化学报, 1996, 17(3):237-240. http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=QK199600002923 HU Chang-wen, LIU Yang-yong, HE Qing-lin, ZHANG Ji-yu, WANG En-bo. Studies on the esterification activity of a new type layer-pillared catalysts ZnAl-XW₁₁Z[J]. Chin J Catal, 1996, 17(3):237-240. http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=QK199600002923
[31]	JACOBS P A, MORTIER W J, UYTTERHOEVEN J B. Properties of zeolites in relation to their electronegativity:Acidity, carboniogenic activity and strength of interaction in transition metal complexes[J]. J Inorg Nucl Chem, 1978, 40(11):1919-1923. doi: 10.1016/0022-1902(78)80256-5
[32]	AN Z, ZHANG W, SHI H, HE J. An effective heterogeneous L-proline catalyst for the asymmetric aldol reaction using anionic clays as intercalated support[J]. J Catal, 2006, 241(2):319-327. http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=699f0b4878ffc1e2cfbea41ba04b075e