Zeolite-13X loaded strong stable CoO single-atom catalysts for efficient peroxomonosulfate activation: Role of magnesium silicate and SiOH bonding

IF 13.2 1区 工程技术 Q1 ENGINEERING, CHEMICAL
Jiale Yu, Qing Sun, Mengxue Sun, Jian Zhang, Jiawei Sheng
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Abstract

Cobalt-based catalysts exhibit high activity in the removal of water pollutants. However, their practical application is significantly impeded by potential biotoxicity and stability issues. How to simply stabilize cobalt atoms at the carrier interface remains a challenge. Here, we loaded cobalt into zeolite-13X and coated thin nanosheets of magnesium silicate with 3D floral morphology on the Co/13X surface through hydrothermal treatment. Temperature-controlled calcination successfully stabilized the Co atoms by utilizing Si-OH groups on the surface of zeolite-13X, resulting in the formation of an efficient and stable CoAbstract ImageO single-atom catalyst (600CoMg/13X). Characterization analyses including FT-IR, XPS, and XAFS confirmed that magnesium silicate played a crucial role in this process. Characterization analyses using BET, SEM and TEM revealed that 600CoMg/13X possesses a highly developed porous structure with a Brunauer-Emmett-Teller (BET) specific surface area of 364.903 m2/g. During peroxymonosulfate (PMS) activation for tetracycline (TC) degradation, the 13X stretcher-loaded CoAbstract ImageO single atom catalyst exhibited excellent catalytic performance and stability. A TC removal rate exceeding 98 % was achieved within 10 min while maintaining a TC removal rate of 95.5 % after eight cycles of degradation. Furthermore, under real aqueous environmental conditions, the 600CoMg/13X catalyst demonstrated stable degradation performance and low biotoxicity. This work provides valuable insights into establishing stable bonding at metal-zeolite interfaces and offers a feasible methodology for developing efficient and environmentally friendly cobalt-based catalysts.

Abstract Image

负载沸石- 13x的强稳定CoO单原子催化剂用于高效过氧单硫酸盐活化:硅酸镁和SiOH键合的作用
钴基催化剂在去除水污染物方面表现出较高的活性。然而,它们的实际应用受到潜在的生物毒性和稳定性问题的严重阻碍。如何简单地稳定载流子界面上的钴原子仍然是一个挑战。在这里,我们将钴装入沸石-13X中,并通过水热处理在Co/13X表面涂覆具有3D花形态的硅酸镁纳米薄片。通过控温煅烧,利用沸石-13X表面的Si-OH基团,成功稳定了Co原子,形成了高效稳定的CoO单原子催化剂(600CoMg/13X)。包括FT-IR、XPS和XAFS在内的表征分析证实了硅酸镁在这一过程中起着至关重要的作用。通过BET、SEM和TEM表征分析表明,600CoMg/13X具有高度发达的多孔结构,BET比表面积为364.903 m2/g。在过氧单硫酸盐(PMS)降解四环素(TC)的活化过程中,负载13X拉伸器的CoO单原子催化剂表现出优异的催化性能和稳定性。在10 min内达到98% %以上的TC去除率,8次循环降解后TC去除率保持在95.5 %。此外,在真实水环境条件下,600CoMg/13X催化剂表现出稳定的降解性能和低生物毒性。这项工作为在金属-沸石界面建立稳定键提供了有价值的见解,并为开发高效环保的钴基催化剂提供了可行的方法。
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来源期刊
Chemical Engineering Journal
Chemical Engineering Journal 工程技术-工程:化工
CiteScore
21.70
自引率
9.30%
发文量
6781
审稿时长
2.4 months
期刊介绍: The Chemical Engineering Journal is an international research journal that invites contributions of original and novel fundamental research. It aims to provide an international platform for presenting original fundamental research, interpretative reviews, and discussions on new developments in chemical engineering. The journal welcomes papers that describe novel theory and its practical application, as well as those that demonstrate the transfer of techniques from other disciplines. It also welcomes reports on carefully conducted experimental work that is soundly interpreted. The main focus of the journal is on original and rigorous research results that have broad significance. The Catalysis section within the Chemical Engineering Journal focuses specifically on Experimental and Theoretical studies in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. These studies have industrial impact on various sectors such as chemicals, energy, materials, foods, healthcare, and environmental protection.
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