Preparation of Zr-Based Phosphotungstic Acid Catalyst, ZrPTAX-BTC, and Its Application in Ultradeep and Fast Oxidative Desulfurization of Fuels,Industrial & Engineering Chemistry Research

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Preparation of Zr-Based Phosphotungstic Acid Catalyst, ZrPTAX-BTC, and Its Application in Ultradeep and Fast Oxidative Desulfurization of Fuels
Industrial & Engineering Chemistry Research ( IF 3.8 ) Pub Date : 2021-12-22 , DOI: 10.1021/acs.iecr.1c03959
Jintian Zhong _{1,

2,

3} , Zhaoyang Qi _{1,

2,

3} , Yiyan Liu _{1,

2,

3} , Yixi Zhu _{1,

2,

3} , Jie Chen _{2,

3,

4} , Changshen Ye _{1,

2,

3} , Ting Qiu _{1,

2,

3}

Affiliation

Fuels with extremely low sulfur content are highly desirable as a result of the growing environmental concerns. In this work, a simple and novel method to connect a Zr^IV open site with polyoxometalates (POM) was introduced, which was used as an effective heterogeneous catalyst for oxidative desulfurization of fuel oil. ZrPTA_X-BTC composites were synthesized conveniently and rapidly at room temperature and atmospheric pressure using pyromellitic acid (BTC) as a linker. The products were characterized by XRD, TGA, FT-IR, NMR, SEM, and N₂ adsorption–desorption, which verified the successful preparation of ZrPTA_X-BTC composite. ZrPTA_X-BTC catalyst has high content of active components, and has excellent catalytic activity in oxidative desulfurization reaction. It achieves rapid and complete desulfurization under mild reaction conditions (T = 50 °C, O/S = 4, t = 30 min, DBT removal rate reaches 100%). Further studies show that the synergistic catalysis of a Zr^IV open site and PTA molecule is the reason for its high catalytic activity, in which the Zr^IV open site promotes the decomposition of H₂O₂ into O₂·, PTA molecules combine with O₂· to form peroxytungstate (W(O₂)_n), and the close distance between the Zr^IV open site and PTA in ZrPTA_X-BTC allows H₂O₂ to be efficiently utilized. In addition, ZrPTA_X-BTC can be easily recovered and reused for at least five times, and only a slight decrease in catalytic activity has occurred. Therefore, ZrPTA_X-BTC has high catalytic activity, high stability, and good reusability, which is a potential catalyst that can realize the application of fuel ultradeep desulfurization.

中文翻译：

Zr基磷钨酸催化剂ZrPTAX-BTC的制备及其在燃料超深快速氧化脱硫中的应用

由于日益增长的环境问题，非常需要具有极低硫含量的燃料。在这项工作中，介绍了一种连接 Zr ^IV开放位点与多金属氧酸盐 (POM)的简单而新颖的方法，该方法可用作燃料油氧化脱硫的有效多相催化剂。ZrPTA _X -BTC 复合材料在室温和大气压下以均苯四酸 (BTC) 为连接剂，方便快捷地合成。通过XRD、TGA、FT-IR、NMR、SEM、N ₂吸附-脱附对产物进行了表征，验证了ZrPTA _X -BTC复合材料的成功制备。ZrPTA _X-BTC催化剂活性成分含量高，在氧化脱硫反应中具有优异的催化活性。在温和的反应条件下（T = 50 ℃，O/S = 4，t = 30 min，DBT去除率达到100%）实现了快速彻底的脱硫。进一步的研究表明，Zr ^IV开放位点和 PTA 分子的协同催化是其催化活性高的原因，其中 Zr ^IV开放位点促进 H ₂ O ₂分解为 O ₂ ·，PTA 分子与 O 结合₂ ·形成过氧钨酸盐(W(O ₂ ) _n )，与Zr之间的距离较近ZrPTA _X -BTC 中的^IV open site 和 PTA允许 H ₂ O ₂得到有效利用。此外，ZrPTA _X -BTC 可以很容易地回收并重复使用至少 5 次，并且催化活性仅略有下降。因此，ZrPTA _X -BTC催化活性高、稳定性高、重复使用性好，是一种可实现燃料超深度脱硫应用的潜在催化剂。

更新日期：2022-01-12

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