Controlling oxide promoter coverage and microstructure on metals of inverse catalysts: Application to liquid phase tetrahydrofurfuryl alcohol conversion to 1,5-pentanediol

IF 20.2 1区化学 Q1 CHEMISTRY, PHYSICAL

Applied Catalysis B: Environmental Pub Date : 2024-01-10 DOI:10.1016/j.apcatb.2024.123724

Jiahua Zhou , Jiayi Fu , Piaoping Yang , Kewei Yu , Stavros Caratzoulas , Weiqing Zheng , Dionisios G. Vlachos

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引用次数: 0

Abstract

Metal M₁/metal oxide M₂O_x (M₁M₂O_x) inverse catalysts, where the oxide layer rests atop metal, have gained attention for their distinct catalytic performance. They are intensively studied in biomass upgrading, e.g., the hydrogenolysis of tetrahydrofurfuryl alcohol to produce 1,5-pentanediol. Pt and MO_x (M = W, Mo, Re, Nb) exhibit remarkable synergism in activity and selectivity, but the active sites remain poorly understood. Here, we examine the influence of oxide loading on PtMO_x inverse catalysts and introduce a high-pressure wash treatment to leach the excess oxide from carbon and optimize their structure. The findings reveal a saturation sub-monolayer MO_x coverage with 2D atomic structure on Pt that is crucial for performance; excessive loading leads to nanocrystalline of lower activity, and low loading exposes unselective metal sites. Wash treatment selectively removes MO_x from carbon, enhances their dispersion on Pt, and improves, in most cases, the performance. Tuning the inverse structure advances structure-reactivity understanding.

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控制反相催化剂金属上的氧化促进剂覆盖率和微观结构：液相四氢糠醇转化为 1,5-戊二醇的应用

金属 M1/金属氧化物 M2Ox（M1M2Ox）反相催化剂（氧化层位于金属之上）因其独特的催化性能而备受关注。在生物质升级（如四氢糠醇加氢分解生成 1,5-戊二醇）方面，对它们进行了深入研究。铂和 MOx（M = W、Mo、Re、Nb）在活性和选择性方面表现出显著的协同作用，但人们对其活性位点仍然知之甚少。在此，我们研究了氧化物负载对 PtMOx 反相催化剂的影响，并引入高压洗涤处理以从碳中析出多余的氧化物并优化其结构。研究结果表明，铂上具有二维原子结构的饱和亚单层氧化物覆盖率对催化剂的性能至关重要；过高的负载量会导致活性较低的纳米晶，而过低的负载量则会暴露出非选择性金属位点。水洗处理可选择性地将 MOx 从碳中去除，提高它们在铂上的分散性，并在大多数情况下提高性能。调整反向结构有助于加深对结构-反应的理解。

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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.