Enhancing sulfur resistance of oxides in carbon monoxide oxidation by a high-entropy-stabilized strategy

IF 3.5 3区工程技术 Q2 ENGINEERING, CHEMICAL AIChE Journal Pub Date : 2024-05-07 DOI:10.1002/aic.18470

Shengyu Du, Pengfei Zhang

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Abstract

Industrial chemical processes require sulfur-resistant catalysts, which reduce catalyst replacement costs and simplify process operations. Herein, a high-entropy-stabilized strategy was put forward for sulfur-resistant catalysis. A spinel high entropy (Zn_0.2Mg_0.2Cu_0.2Mn_0.2Co_0.2Al₂O₄) was introduced by ball milling process with aluminum isopropoxide as the main precursor. Zn_0.2Mg_0.2Cu_0.2Mn_0.2Co_0.2Al₂O₄ possessed a high surface area of 171.2 m² g⁻¹, higher than typical high-entropy oxides (HEOs). The high-entropy spinel catalyst exhibited better SO₂-resistance performance in the oxidation of carbon monoxide, better than the simple oxides. The SO₂-resistance of Zn_0.2Mg_0.2Cu_0.2Mn_0.2Co_0.2Al₂O₄ was primarily improved by reinforcing the stability of the oxide using a high-entropy structure to decrease the absorption of SO₂ on its surface. Any adsorbed SO₂ on the surface of the HEO was then selectively trapped by sacrificial metal ions with stronger electron-withdrawing ability, protecting the active center (Cu²⁺, Co²⁺) from poisoning. This work reveals the significance of high-entropy structures in sulfur resistance.

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通过高熵稳定策略增强氧化物在一氧化碳氧化过程中的抗硫性

工业化工工艺需要抗硫催化剂，以降低催化剂更换成本并简化工艺操作。在此，我们提出了一种高熵稳定的抗硫催化策略。以异丙醇铝为主要前驱体，通过球磨工艺引入尖晶石高熵（Zn0.2Mg0.2Cu0.2Mn0.2Co0.2Al2O4）。Zn0.2Mg0.2Cu0.2Mn0.2Co0.2Al2O4 的比表面积高达 171.2 m2 g-1，高于典型的高熵氧化物（HEOs）。高熵尖晶石催化剂在氧化一氧化碳时表现出更好的抗二氧化硫性能，优于简单氧化物。Zn0.2Mg0.2Cu0.2Mn0.2Co0.2Al2O4的抗二氧化硫性能主要是通过使用高熵结构来增强氧化物的稳定性，从而减少其表面对二氧化硫的吸附来提高的。然后，高熵氧化物表面吸附的二氧化硫会被具有更强吸电子能力的牺牲金属离子选择性地捕获，从而保护活性中心（Cu2+、Co2+）免受毒害。这项工作揭示了高熵结构在抗硫方面的重要意义。

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来源期刊

AIChE Journal 工程技术-工程：化工

CiteScore

7.10

自引率

10.80%

发文量

411

审稿时长

3.6 months

期刊介绍： The AIChE Journal is the premier research monthly in chemical engineering and related fields. This peer-reviewed and broad-based journal reports on the most important and latest technological advances in core areas of chemical engineering as well as in other relevant engineering disciplines. To keep abreast with the progressive outlook of the profession, the Journal has been expanding the scope of its editorial contents to include such fast developing areas as biotechnology, electrochemical engineering, and environmental engineering. The AIChE Journal is indeed the global communications vehicle for the world-renowned researchers to exchange top-notch research findings with one another. Subscribing to the AIChE Journal is like having immediate access to nine topical journals in the field. Articles are categorized according to the following topical areas: Biomolecular Engineering, Bioengineering, Biochemicals, Biofuels, and Food Inorganic Materials: Synthesis and Processing Particle Technology and Fluidization Process Systems Engineering Reaction Engineering, Kinetics and Catalysis Separations: Materials, Devices and Processes Soft Materials: Synthesis, Processing and Products Thermodynamics and Molecular-Scale Phenomena Transport Phenomena and Fluid Mechanics.