Enhanced Catalytic Performance of UiO-67 Supported Pd Catalyst for Toluene Degradation

IF 2.3 4区 化学 Q3 CHEMISTRY, PHYSICAL Catalysis Letters Pub Date : 2024-06-28 DOI:10.1007/s10562-024-04712-z
Chunzhi Zhao, Dongsen Mao, Tao Meng, Qiangsheng Guo, Jun Yu
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Abstract

Owing to the intrinsic nature of the uniformed topologies and ultrasmall Zr6 nodes of Zr-MOFs, herein, we employed Zr-MOFs (UiO-66 and UiO-67), as opposed to the support of traditional ZrO2, to prepare the Pd catalysts for toluene degradation. Compared with the catalysts of Pd/UiO-66 and Pd/ZrO2, Pd/UiO-67 catalyst boosted an excellence catalytic performance for toluene degradation, giving the lowest T90% value of 235 °C with long-term stability. With the assisting of the cavity confinement of Zr-MOFs, Pd nanoparticles are prone to be encapsulated in the 3D frameworks of Zr-MOFs, and the bigger micropores of UiO-67 are more conducive to the formation of larger Pd nanoparticles. The in situ FT-IR results further declared that although the active sites are partly sacrificed due to the larger Pd nanoparticles formed in UiO-67, the stable adsorbed toluene on Pd/UiO-67 boosted the quick degradation of toluene in the reaction interval even without undergoing intermediate processes of benzoate and benzaldehyde.

Graphical Abstract

UiO-66, UiO-67 and ZrO2 were employed to prepare the Pd catalysts for toluene degradation, Pd/UiO-67 catalyst boosted an excellence catalytic performance with long-term stability.

Abstract Image

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增强 UiO-67 支持的钯催化剂在甲苯降解中的催化性能
由于 Zr-MOFs 具有均匀拓扑结构和超小 Zr6 节点的固有特性,与传统的 ZrO2 相比,我们采用 Zr-MOFs(UiO-66 和 UiO-67)制备了用于甲苯降解的钯催化剂。与 Pd/UiO-66 和 Pd/ZrO2 催化剂相比,Pd/UiO-67 催化剂对甲苯降解的催化性能更为优异,其最低 T90% 值为 235 ℃,且具有长期稳定性。在 Zr-MOFs 的空腔约束辅助下,Pd 纳米颗粒容易被包裹在 Zr-MOFs 的三维框架中,而 UiO-67 较大的微孔更有利于形成较大的 Pd 纳米颗粒。原位傅立叶变换红外光谱结果进一步表明,虽然 UiO-67 中形成的较大 Pd 纳米颗粒牺牲了部分活性位点,但 Pd/UiO-67 上稳定吸附的甲苯促进了反应区间内甲苯的快速降解,甚至无需经过苯甲酸酯和苯甲醛的中间过程。图解摘要 利用 UiO-66、UiO-67 和 ZrO2 制备了用于甲苯降解的钯催化剂,Pd/UiO-67 催化剂具有优异的催化性能和长期稳定性。
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来源期刊
Catalysis Letters
Catalysis Letters 化学-物理化学
CiteScore
5.70
自引率
3.60%
发文量
327
审稿时长
1 months
期刊介绍: Catalysis Letters aim is the rapid publication of outstanding and high-impact original research articles in catalysis. The scope of the journal covers a broad range of topics in all fields of both applied and theoretical catalysis, including heterogeneous, homogeneous and biocatalysis. The high-quality original research articles published in Catalysis Letters are subject to rigorous peer review. Accepted papers are published online first and subsequently in print issues. All contributions must include a graphical abstract. Manuscripts should be written in English and the responsibility lies with the authors to ensure that they are grammatically and linguistically correct. Authors for whom English is not the working language are encouraged to consider using a professional language-editing service before submitting their manuscripts.
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