An insight into the effect of calcination conditions on catalytic cracking of toluene over 3Fe8Ni/palygorskite: Catalysts characterization and performance

An insight into the effect of calcination conditions on catalytic cracking of toluene over 3Fe8Ni/palygorskite: Catalysts characterization and performance
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深入了解煅烧条件对 3Fe8Ni/凹凸棒石上甲苯催化裂化的影响:催化剂表征和性能

DOI:
10.1016/j.fuel.2016.11.038
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发表时间:
2017-02
期刊:
影响因子:
7.4
通讯作者:
Chen Dong
Chen Dong
中科院分区:
工程技术1区
文献类型:
--
作者:
Zou Xuehua;Chen Tianhu;Liu Haibo;Zhang Ping;Ma Zhiyuan;Xie Jingjing;Chen Dong

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考察了焙烧条件对3Fe 8 Ni/PG(PG:凹凸棒石)催化剂上甲苯催化裂解反应的影响。考察了煅烧温度、煅烧时间、煅烧气氛和反应温度等实验参数对合成的影响。采用X射线衍射(XRD)、程序升温还原(TPR)、透射电子显微镜(TEM)和拉曼光谱对催化剂进行了表征。通过气相色谱(GC)分析气体组成。结果表明,3Fe 8 Ni/PG催化剂对甲苯的催化裂解反应活性高于石英催化剂上的热裂解反应活性。考虑到催化剂的热稳定性和催化活性,制备3Fe 8 Ni/PG催化剂时应选择合适的焙烧温度和时间。在氢气中在700 °C下还原2小时的3Fe 8 Ni/PG显示出最高的催化反应性,如在550 °C的反应温度下甲苯转化率为100%所证明的。经氢气还原的3 Fe 8 Ni/PG催化剂对甲苯的催化活性上级优于空气中焙烧的3 Fe 8 Ni/PG、3 Fe/PG和8 Ni/PG,表明铁钒矿(Nisingle键Fe)是甲苯分解的活性组分。甲苯水蒸气重整反应表明,3Fe 8 Ni/PG催化剂上的甲苯转化率可达80%,且大部分甲苯转化为H2和CO,催化反应后在3Fe 8 Ni/PG催化剂上生成了无定形碳和石墨碳物种。3Fe 8 Ni/PG催化剂的D/G比(D-带与G-带的相对强度之比)与催化活性呈正相关。
In this paper, the effect of calcination conditions on catalytic cracking of toluene over 3Fe8Ni/PG (PG: palygorskite) was investigated. The experimental parameters including the calcination temperature, time and atmosphere and reaction temperature were evaluated. The catalysts were characterized using X-ray diffraction (XRD), H2temperature-programmed reduction (TPR), transmission electron microcopy (TEM) and Raman spectroscopy. The gas composition was analyzed by a gas chromatograph (GC). The results showed that 3Fe8Ni/PG catalyst exhibited a higher catalytic reactivity for catalytic cracking of toluene than that of thermal cracking over quartz. In consideration of the thermal stability and catalytic reactivity of catalyst, a proper calcination temperature and time should be employed in the preparation of 3Fe8Ni/PG catalyst. The 3Fe8Ni/PG reduced in hydrogen at 700 °C for 2 h showed the highest catalytic reactivity as evidenced by the toluene conversion of 100% at the reaction temperature of 550 °C. The catalytic reactivity of 3Fe8Ni/PG reduced in hydrogen for toluene conversion was superior to that of 3Fe8Ni/PG calcinated in air, 3Fe/PG, and 8Ni/PG, which revealed that the awaruite (Nisingle bondFe) was the active component for the decomposition of toluene. Moreover, steam reforming of toluene over 3Fe8Ni/PG catalysts suggested that 80% toluene conversion can be achieved and most of toluene was converted into H2and CO. Both amorphous carbon and graphitic carbon species were formed on 3Fe8Ni/PG catalysts after the catalytic reaction. The D/G ratio (the relative intensity of D-band to G-band ratio) was positively correlated to the catalytic reactivity of 3Fe8Ni/PG catalysts.
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