Conversion of CO2 to higher alcohols on K-CuZnAl/Zr-CuFe composite

IF 20.2 1区化学 Q1 CHEMISTRY, PHYSICAL Applied Catalysis B: Environmental Pub Date : 2024-01-18 DOI:10.1016/j.apcatb.2024.123748

Qian Zhang , Sen Wang , Xuerong Shi , Mei Dong , Jiangang Chen , Juan Zhang , Jianguo Wang , Weibin Fan

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Abstract

Direct conversion of CO₂ into higher alcohols (C₂₊OH) is highly desirable, but rather challenging due to requiring the synergetic action of C-C coupling and CO insertion. Here, we developed a new K-CuZnAl/Zr-CuFe composite, which gave CO₂ conversion and C₂₊OH selectivity of 40.6% and 22.4% respectively, while CO selectivity is only 10.3% at 320 °C, 4 MPa and 6000 mL g_cat⁻¹ h⁻¹. The C₂₊OH STY can reach 195.1 mg g_cat^–1 h^–1, and is well maintained within 200 h at higher GHSV of 24000 mL g_cat⁻¹ h⁻¹. Introduction of K-CuZnAl and decrease of the contact distance of K-CuZnAl and Zr-CuFe boost the formation and subsequent conversion of CO* intermediate. In addition, doping small amounts of Zr into CuFe catalyst hinders the phase separation of Cu and Fe species by enhancing their interface interaction. As a result, the CH_x * species generated on iron carbide through CO* dissociative activation quickly reacts with the non-dissociative adsorbed CO* on adjacent Cu to produce more C₂₊OH.

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在 K-CuZnAl/Zr-CuFe 复合材料上将 CO2 转化为高级醇

直接将 CO2 转化为高级醇（C2+OH）是非常理想的，但由于需要 C-C 偶联和 CO 插入的协同作用，因此颇具挑战性。在此，我们开发了一种新型 K-CuZnAl/Zr-CuFe 复合材料，在 320 ℃、4 MPa 和 6000 mL gcat-1 h-1 条件下，其 CO2 转化率和 C2+OH 选择性分别为 40.6% 和 22.4%，而 CO 选择性仅为 10.3%。C2+OH STY 可达到 195.1 mg gcat-1 h-1，并且在更高的 GHSV（24000 mL gcat-1 h-1）条件下可在 200 小时内保持稳定。K-CuZnAl 的引入以及 K-CuZnAl 和 Zr-CuFe 接触距离的减小促进了 CO* 中间体的形成和后续转化。此外，在 CuFe 催化剂中掺入少量 Zr 会增强 Cu 和 Fe 的界面相互作用，从而阻碍它们的相分离。因此，碳化铁上通过 CO* 解离活化产生的 CHx * 物种会迅速与相邻 Cu 上非解离吸附的 CO* 发生反应，产生更多的 C2+OH 。

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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.