Monolayer CoMoS Anchored on Hydrophobic Reduced Graphene Nanoribbons for Efficient Hydrodeoxygenation

IF 7.1 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

ACS Sustainable Chemistry & Engineering Pub Date : 2024-11-14 DOI:10.1021/acssuschemeng.4c05233

Cen Zhang, Tianyi Liu, Siyan Zou, Xinyi Liu, Binbin Zhou, Jiali Mu, Jing Cao

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Abstract

Improving both the activity and stability is of great importance for MoS₂-based catalysts in the hydrodeoxygenation (HDO) reaction. Herein, we report the construction of monolayer CoMoS anchored on hydrophobic-reduced graphene nanoribbons (ML-CoMoS/rGNRs) which exhibited excellent activity and stability in the HDO of 4-methylphenol. The superior HDO activity was attributed to the single layer structure of MoS₂, which allows the good exposure of abundant edge sites for accommodating Co promoters to form the Co–Mo–S active phase. Besides, the hydrophobicity of rGNRs enables the fast removal of H₂O during the HDO reaction, which alleviates the sulfur loss and endows the excellent stability of supported CoMoS monolayers. Consequently, ML-CoMoS/rGNRs afforded 97.3% conversion and 98.4% toluene selectivity at 220 °C for at least five reaction cycles. This work provides novel insights for designing highly active and stable metal sulfide catalysts for the application in the HDO reaction.

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锚定在疏水性还原石墨烯纳米带上的单层 CoMoS 实现高效氢脱氧反应

提高活性和稳定性对于基于 MoS2 的加氢脱氧反应 (HDO) 催化剂非常重要。在此，我们报告了锚定在疏水还原石墨烯纳米带（ML-CoMoS/rGNRs）上的单层 CoMoS 的构建情况，该催化剂在 4-甲基苯酚的 HDO 反应中表现出优异的活性和稳定性。优异的 HDO 活性归功于 MoS2 的单层结构，这种结构允许大量边缘位点暴露出来，以容纳 Co 促进剂形成 Co-Mo-S 活性相。此外，rGNRs 的疏水性可以在 HDO 反应过程中快速去除 H2O，从而减少硫的损失，并赋予支撑 CoMoS 单层优异的稳定性。因此，ML-CoMoS/rGNRs 在 220 ℃ 条件下进行至少五个反应循环，可获得 97.3% 的转化率和 98.4% 的甲苯选择性。这项工作为设计用于 HDO 反应的高活性、高稳定性金属硫化物催化剂提供了新的见解。

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来源期刊

ACS Sustainable Chemistry & Engineering CHEMISTRY, MULTIDISCIPLINARY-ENGINEERING, CHEMICAL

CiteScore

13.80

自引率

4.80%

发文量

1470

审稿时长

1.7 months

期刊介绍： ACS Sustainable Chemistry & Engineering is a prestigious weekly peer-reviewed scientific journal published by the American Chemical Society. Dedicated to advancing the principles of green chemistry and green engineering, it covers a wide array of research topics including green chemistry, green engineering, biomass, alternative energy, and life cycle assessment. The journal welcomes submissions in various formats, including Letters, Articles, Features, and Perspectives (Reviews), that address the challenges of sustainability in the chemical enterprise and contribute to the advancement of sustainable practices. Join us in shaping the future of sustainable chemistry and engineering.