Synergistic Regulation of Charge State and Electron-donating Ability via Heterojunctions Design for Fixation of Electronegative Greenhouse F-gases

IF 20.2 1区化学 Q1 CHEMISTRY, PHYSICAL Applied Catalysis B: Environmental Pub Date : 2024-01-09 DOI:10.1016/j.apcatb.2024.123709

Xiang Meng, Boxu Dong, Liang Zhao, Wenhui Zhou, Xinhao Li, Jiantao Zai, Xuefeng Qian

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Abstract

The net-zero greenhouse gas emission has now become a global strategy. In this context, electronegative fluorinated-gases such as sulfur hexafluoride (SF₆) and hydrofluorocarbon, have become important emission reduction objects due to their strong global warming potential. In this work, the MnOx@Mn/SiC heterojunction was rationally designed and prepared. Because of the high electron coupling, the positively charged active-site MnOx@Mn (δ⁺) not only promotes the adsorption of SF₆ but also acts as a donor to transport electrons to SF₆, so that the adsorption and activation of SF₆ are unified in one active site. Therefore, MnOx@Mn/SiC can effectively degrade SF₆ above 450℃, and the degradation amount for 12 vol.% SF₆ can reach 523.8 mL g^-1 at 600℃. Furthermore, it also has good degradation performance on hydrofluorocarbons (R-22 and R-410A) even at 100℃. Given the cheap and easy scale-up synthesis, MnOx@Mn/SiC has the potential to reduce the emission of multiple fluorinated-gases in practical applications.

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通过异质结设计协同调节电荷状态和电子供能能力以固定负电温室气体

温室气体净零排放现已成为一项全球战略。在此背景下，六氟化硫（SF6）和氢氟碳化物等电负性氟化气体因其强烈的全球变暖潜力而成为重要的减排对象。本研究合理设计并制备了 MnOx@Mn/SiC 异质结。由于电子耦合度高，带正电荷的活性位MnOx@Mn（δ+）不仅能促进SF6的吸附，还能作为供体向SF6输送电子，从而使SF6的吸附和活化统一在一个活性位上。因此，MnOx@Mn/SiC 能在 450℃ 以上有效降解 SF6，在 600℃ 时对 12 vol.% SF6 的降解量可达 523.8 mL g-1。此外，即使在 100℃，它对氢氟碳化合物（R-22 和 R-410A）也有良好的降解性能。由于 MnOx@Mn/SiC 的合成成本低廉且易于放大，因此有望在实际应用中减少多种含氟气体的排放。

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来源期刊

Applied Catalysis B: Environmental 环境科学-工程：化工

CiteScore

38.60

自引率

6.30%

发文量

1117

审稿时长

24 days

期刊介绍： Applied Catalysis B: Environment and Energy (formerly Applied Catalysis B: Environmental) is a journal that focuses on the transition towards cleaner and more sustainable energy sources. The journal's publications cover a wide range of topics, including: 1.Catalytic elimination of environmental pollutants such as nitrogen oxides, carbon monoxide, sulfur compounds, chlorinated and other organic compounds, and soot emitted from stationary or mobile sources. 2.Basic understanding of catalysts used in environmental pollution abatement, particularly in industrial processes. 3.All aspects of preparation, characterization, activation, deactivation, and regeneration of novel and commercially applicable environmental catalysts. 4.New catalytic routes and processes for the production of clean energy, such as hydrogen generation via catalytic fuel processing, and new catalysts and electrocatalysts for fuel cells. 5.Catalytic reactions that convert wastes into useful products. 6.Clean manufacturing techniques that replace toxic chemicals with environmentally friendly catalysts. 7.Scientific aspects of photocatalytic processes and a basic understanding of photocatalysts as applied to environmental problems. 8.New catalytic combustion technologies and catalysts. 9.New catalytic non-enzymatic transformations of biomass components. The journal is abstracted and indexed in API Abstracts, Research Alert, Chemical Abstracts, Web of Science, Theoretical Chemical Engineering Abstracts, Engineering, Technology & Applied Sciences, and others.