PdFe Alloy-Fe5C2 interfaces for efficient CO2 hydrogenation to higher alcohols

IF 20.2 1区化学 Q1 CHEMISTRY, PHYSICAL

Applied Catalysis B: Environmental Pub Date : 2024-01-03 DOI:10.1016/j.apcatb.2024.123691

Yanqiu Wang , Ying Zhou , Xinxin Zhang , Mingrui Wang , Tangkang Liu , Jinxing Wei , Guanghui Zhang , Xinlin Hong , Guoliang Liu

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Abstract

Direct CO₂ hydrogenation to higher alcohols (HA) is a promising route for high-value utilization of waste CO₂, but developing active and stable catalysts remains a grand challenge. For this reaction, constructing multifunctional interfaces as active sites is required to fulfill controllable C-C coupling of alkyl and CO*/CH_xO* species. Herein, we report a PdFe catalyst with abundant PdFe alloy-Fe₅C₂ interfaces via a PdFe alloy induced FeO_x carbidization process, which can achieve HA yield of 86.5 mg g_cat⁻¹ h⁻¹ with 26.5% selectivity at 300 ºC, 5 MPa, and 6000 mL g_cat⁻¹ h⁻¹. The accelerated deactivation test unveils the PdFe catalyst exhibits better durability than the widely studied CuFe based catalysts against harsh conditions. Multiple in-situ characterization results unveil a synergetic mechanism for HA synthesis at the PdFe alloy-Fe₅C₂ interfaces, where PdFe alloy is responsible for CO formation and non-dissociative activation, while Fe₅C₂ phase promotes CO dissociation and chain propagation.

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用于高效 CO2 加氢制取高级醇的钯铁合金-Fe5C2 介面

直接将二氧化碳加氢转化为高级醇（HA）是一条很有前景的高价值利用废弃二氧化碳的途径，但开发活性和稳定的催化剂仍然是一项巨大的挑战。对于该反应，需要构建多功能界面作为活性位点，以实现烷基和 CO*/CHxO* 物种的可控 C-C 偶联。在此，我们通过钯铁合金诱导的 FeOx 碳化过程，报告了一种具有丰富钯铁合金-Fe5C2 界面的钯铁催化剂，该催化剂可在 300 ºC、5 MPa 和 6000 mL gcat-1 h-1 条件下实现 86.5 mg gcat-1 h-1 的 HA 产率和 26.5% 的选择性。加速失活测试表明，与广泛研究的基于铜铁的催化剂相比，钯铁催化剂在恶劣条件下表现出更好的耐久性。多种原位表征结果揭示了钯铁合金-Fe5C2 界面合成 HA 的协同机制，其中钯铁合金负责 CO 的形成和非解离活化，而 Fe5C2 相则促进 CO 的解离和链的扩展。

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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.

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