The effect of acid-base synergistic catalysis on upgrading of volatiles from coal pyrolysis over Mg-Al composite oxides

•MgxAl-LDOs with tunable acid-base property were prepared for pyrolysis volatiles upgrading.•The quality of tar and gas was improved over MgxAl-LDOs with less carbon deposition.•The content of light aromatic hydrocarbons increased by 79.8% over Mg4Al-LDO catalyst.•The acid-base synergistic effect of...

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Veröffentlicht in:Fuel (Guildford) 2022-08, Vol.321, p.124030, Article 124030
Hauptverfasser: Yang, Hang, Zhang, Jiehan, Li, Changming, Chen, Zhaohui, Wang, Demin, Wang, Deliang, Ibrahim Sharif, Munnir, Li, Jianling, Yu, Jian, Gao, Shiqiu
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container_issue
container_start_page 124030
container_title Fuel (Guildford)
container_volume 321
creator Yang, Hang
Zhang, Jiehan
Li, Changming
Chen, Zhaohui
Wang, Demin
Wang, Deliang
Ibrahim Sharif, Munnir
Li, Jianling
Yu, Jian
Gao, Shiqiu
description •MgxAl-LDOs with tunable acid-base property were prepared for pyrolysis volatiles upgrading.•The quality of tar and gas was improved over MgxAl-LDOs with less carbon deposition.•The content of light aromatic hydrocarbons increased by 79.8% over Mg4Al-LDO catalyst.•The acid-base synergistic effect of MgxAl-LDOs plays the key role in the upgrading of volatiles. Catalytic upgrading of coal pyrolysis volatiles is one of the most promising technical routes to achieve graded utilization of low-rank coal resource. In this work, a series of Mg-Al composite oxide catalysts (MgxAl-LDOs) were synthesized with tunable acid-base properties for upgrading the volatiles from coal pyrolysis by adjusting the Mg/Al ratio in Mg-Al hydrotalcite precursors (MgxAl-LDHs). The NH3-TPD and CO2-TPD analysis results showed the quantity of acidity sites decrease together with an increase of basicity sites as the Mg/Al ratio increased in MgxAl-LDOs. MgxAl-LDOs possessed weaker acidity strength and more acidity sites than pure Al2O3, but less basicity sites than pure MgO. The catalytic performances illustrated that the increased acidity sites in MgxAl-LDOs promoted the cracking of heavy components and reduced the yield of heavy tar. Meanwhile, the weakened acidity strength and the introduction of basicity sites by Mg in MgxAl-LDOs enhanced the strong resistance to carbon deposition. Moreover, the CO2 yield and the content of light aromatic hydrocarbons in tar increased obviously after upgrading, which can be attributed to the acid-base synergistic effect of the MgxAl-LDOs. Particularly, the Mg4Al-LDO catalyst selectively improved the relative contents of light aromatic hydrocarbons, and the content of benzene, toluene, ethylbenzene, xylene, naphthalene and indene increased by 1.48, 1.54, 0.76, 2.56, 0.19 and 2.14 times (compared with the inert quartz sand), respectively. The unique catalytic behaviors of MgxAl-LDO catalysts will provide a new insight into the effect of acid-base synergistic catalysis on upgrading of volatiles from coal pyrolysis.
doi_str_mv 10.1016/j.fuel.2022.124030
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Catalytic upgrading of coal pyrolysis volatiles is one of the most promising technical routes to achieve graded utilization of low-rank coal resource. In this work, a series of Mg-Al composite oxide catalysts (MgxAl-LDOs) were synthesized with tunable acid-base properties for upgrading the volatiles from coal pyrolysis by adjusting the Mg/Al ratio in Mg-Al hydrotalcite precursors (MgxAl-LDHs). The NH3-TPD and CO2-TPD analysis results showed the quantity of acidity sites decrease together with an increase of basicity sites as the Mg/Al ratio increased in MgxAl-LDOs. MgxAl-LDOs possessed weaker acidity strength and more acidity sites than pure Al2O3, but less basicity sites than pure MgO. The catalytic performances illustrated that the increased acidity sites in MgxAl-LDOs promoted the cracking of heavy components and reduced the yield of heavy tar. Meanwhile, the weakened acidity strength and the introduction of basicity sites by Mg in MgxAl-LDOs enhanced the strong resistance to carbon deposition. Moreover, the CO2 yield and the content of light aromatic hydrocarbons in tar increased obviously after upgrading, which can be attributed to the acid-base synergistic effect of the MgxAl-LDOs. Particularly, the Mg4Al-LDO catalyst selectively improved the relative contents of light aromatic hydrocarbons, and the content of benzene, toluene, ethylbenzene, xylene, naphthalene and indene increased by 1.48, 1.54, 0.76, 2.56, 0.19 and 2.14 times (compared with the inert quartz sand), respectively. 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Catalytic upgrading of coal pyrolysis volatiles is one of the most promising technical routes to achieve graded utilization of low-rank coal resource. In this work, a series of Mg-Al composite oxide catalysts (MgxAl-LDOs) were synthesized with tunable acid-base properties for upgrading the volatiles from coal pyrolysis by adjusting the Mg/Al ratio in Mg-Al hydrotalcite precursors (MgxAl-LDHs). The NH3-TPD and CO2-TPD analysis results showed the quantity of acidity sites decrease together with an increase of basicity sites as the Mg/Al ratio increased in MgxAl-LDOs. MgxAl-LDOs possessed weaker acidity strength and more acidity sites than pure Al2O3, but less basicity sites than pure MgO. The catalytic performances illustrated that the increased acidity sites in MgxAl-LDOs promoted the cracking of heavy components and reduced the yield of heavy tar. Meanwhile, the weakened acidity strength and the introduction of basicity sites by Mg in MgxAl-LDOs enhanced the strong resistance to carbon deposition. Moreover, the CO2 yield and the content of light aromatic hydrocarbons in tar increased obviously after upgrading, which can be attributed to the acid-base synergistic effect of the MgxAl-LDOs. Particularly, the Mg4Al-LDO catalyst selectively improved the relative contents of light aromatic hydrocarbons, and the content of benzene, toluene, ethylbenzene, xylene, naphthalene and indene increased by 1.48, 1.54, 0.76, 2.56, 0.19 and 2.14 times (compared with the inert quartz sand), respectively. The unique catalytic behaviors of MgxAl-LDO catalysts will provide a new insight into the effect of acid-base synergistic catalysis on upgrading of volatiles from coal pyrolysis.</description><subject>Acid-base synergy</subject><subject>Acidity</subject><subject>Acids</subject><subject>Aluminum oxide</subject><subject>Ammonia</subject><subject>Aromatic hydrocarbons</subject><subject>Basicity</subject><subject>Benzene</subject><subject>Carbon dioxide</subject><subject>Catalysis</subject><subject>Catalysts</subject><subject>Catalytic upgrading</subject><subject>Chemical synthesis</subject><subject>Coal</subject><subject>Coal pyrolysis</subject><subject>Ethylbenzene</subject><subject>Hydrocarbons</subject><subject>Hydrotalcites</subject><subject>Indene</subject><subject>Magnesium</subject><subject>Naphthalene</subject><subject>Pyrolysis</subject><subject>Synergistic effect</subject><subject>Tar</subject><subject>Toluene</subject><subject>Upgrading</subject><subject>Volatiles</subject><subject>Xylene</subject><issn>0016-2361</issn><issn>1873-7153</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2022</creationdate><recordtype>article</recordtype><recordid>eNp9kLtOwzAUhi0EEqXwAkyWmFNsx05ciaWquElFLGW2HOc4uErjYCeFvj2uwsx0hvP95_IhdEvJghJa3O8WdoR2wQhjC8o4yckZmlFZ5llJRX6OZiRRGcsLeomuYtwRQkop-Ax9bz8Bg7VgBuwt1sbVWaUj4HjsIDQuDs5gowfdHqOL2Hd47Juga9c1J_7gWz24FiK2we-x8brF_TH4P_oAAb812apNnX3voxsA-x9XQ7xGF1a3EW7-6hx9PD1u1y_Z5v35db3aZIYJOWS8Kg23UuSEMG6p5EKYqqgZByIKJgjL049E6FLWIIxlQtvSGlvlrLRLKUw-R3fT3D74rxHioHZ-DF1aqVghlyXlXBaJYhNlgo8xgFV9cHsdjooSdRKsduokWJ0Eq0lwCj1MIUj3HxwEFY2DzkDtQtKpau_-i_8Ct72E6w</recordid><startdate>20220801</startdate><enddate>20220801</enddate><creator>Yang, Hang</creator><creator>Zhang, Jiehan</creator><creator>Li, Changming</creator><creator>Chen, Zhaohui</creator><creator>Wang, Demin</creator><creator>Wang, Deliang</creator><creator>Ibrahim Sharif, Munnir</creator><creator>Li, Jianling</creator><creator>Yu, Jian</creator><creator>Gao, Shiqiu</creator><general>Elsevier Ltd</general><general>Elsevier BV</general><scope>AAYXX</scope><scope>CITATION</scope><scope>7QF</scope><scope>7QO</scope><scope>7QQ</scope><scope>7SC</scope><scope>7SE</scope><scope>7SP</scope><scope>7SR</scope><scope>7T7</scope><scope>7TA</scope><scope>7TB</scope><scope>7U5</scope><scope>8BQ</scope><scope>8FD</scope><scope>C1K</scope><scope>F28</scope><scope>FR3</scope><scope>H8D</scope><scope>H8G</scope><scope>JG9</scope><scope>JQ2</scope><scope>KR7</scope><scope>L7M</scope><scope>L~C</scope><scope>L~D</scope><scope>P64</scope></search><sort><creationdate>20220801</creationdate><title>The effect of acid-base synergistic catalysis on upgrading of volatiles from coal pyrolysis over Mg-Al composite oxides</title><author>Yang, Hang ; 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Catalytic upgrading of coal pyrolysis volatiles is one of the most promising technical routes to achieve graded utilization of low-rank coal resource. In this work, a series of Mg-Al composite oxide catalysts (MgxAl-LDOs) were synthesized with tunable acid-base properties for upgrading the volatiles from coal pyrolysis by adjusting the Mg/Al ratio in Mg-Al hydrotalcite precursors (MgxAl-LDHs). The NH3-TPD and CO2-TPD analysis results showed the quantity of acidity sites decrease together with an increase of basicity sites as the Mg/Al ratio increased in MgxAl-LDOs. MgxAl-LDOs possessed weaker acidity strength and more acidity sites than pure Al2O3, but less basicity sites than pure MgO. The catalytic performances illustrated that the increased acidity sites in MgxAl-LDOs promoted the cracking of heavy components and reduced the yield of heavy tar. Meanwhile, the weakened acidity strength and the introduction of basicity sites by Mg in MgxAl-LDOs enhanced the strong resistance to carbon deposition. Moreover, the CO2 yield and the content of light aromatic hydrocarbons in tar increased obviously after upgrading, which can be attributed to the acid-base synergistic effect of the MgxAl-LDOs. Particularly, the Mg4Al-LDO catalyst selectively improved the relative contents of light aromatic hydrocarbons, and the content of benzene, toluene, ethylbenzene, xylene, naphthalene and indene increased by 1.48, 1.54, 0.76, 2.56, 0.19 and 2.14 times (compared with the inert quartz sand), respectively. The unique catalytic behaviors of MgxAl-LDO catalysts will provide a new insight into the effect of acid-base synergistic catalysis on upgrading of volatiles from coal pyrolysis.</abstract><cop>Kidlington</cop><pub>Elsevier Ltd</pub><doi>10.1016/j.fuel.2022.124030</doi></addata></record>
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identifier ISSN: 0016-2361
ispartof Fuel (Guildford), 2022-08, Vol.321, p.124030, Article 124030
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source Elsevier ScienceDirect Journals
subjects Acid-base synergy
Acidity
Acids
Aluminum oxide
Ammonia
Aromatic hydrocarbons
Basicity
Benzene
Carbon dioxide
Catalysis
Catalysts
Catalytic upgrading
Chemical synthesis
Coal
Coal pyrolysis
Ethylbenzene
Hydrocarbons
Hydrotalcites
Indene
Magnesium
Naphthalene
Pyrolysis
Synergistic effect
Tar
Toluene
Upgrading
Volatiles
Xylene
title The effect of acid-base synergistic catalysis on upgrading of volatiles from coal pyrolysis over Mg-Al composite oxides
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