Sustainable Production of 1-Propanol via the Selective Hydrogenolysis of Glycerol Over a Tailored Iridium–Rhenium Oxide Catalyst Supported on HUSY Zeolite

IF 3.9 3区 化学 Q2 CHEMISTRY, PHYSICAL
ChemCatChem Pub Date : 2025-07-31 DOI:10.1002/cctc.202500885
Supphathee Chaowamalee, Atikhun Chotirattanachote, Wongsakorn Khammee, Chanoknun Kalvibool, Chawalit Ngamcharussrivichai
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Abstract

1-Propanol (1-PO) is a widely used industrial solvent and an important chemical intermediate. In this study, the hydrogenolysis of glycerol to 1-PO was investigated over conventional proton-form ultrastable (HUSY) zeolite, monometallic Ir-loaded HUSY (Ir-HUSY), and Ir–ReOx metal–metal oxide supported on HUSY (IrRe-HUSY). The IrRe-HUSY catalysts, which were prepared via a sequential two-step incipient wetness impregnation method, exhibited favorable physicochemical properties, including improved acid properties and uniform metal dispersion. Therefore, the bimetallic IrRe-HUSY catalysts demonstrated a considerably higher catalytic performance, achieving a glycerol conversion of 78.9% and 1-PO yield of 39.2%, than HUSY zeolite and Ir-HUSY, which demonstrated only 32.9% glycerol conversion and 11.1% 1-PO yield. This improvement in the catalytic properties of the IrRe-HUSY catalysts was attributed to the synergistic effects among the three catalyst components: (1) ReOx clusters facilitated glycerol adsorption and activation; (2) Ir nanoparticles promoted C─O bond cleavage and hydrogenation; and (3) the acidic HUSY support enhanced dehydration steps. Additionally, the effects of operating conditions, such as catalyst loading, reaction time, and temperature, on 1-PO production were systematically investigated. The surface structure of IrRe-HUSY and the mechanistic pathway for glycerol hydrogenolysis over the IrRe-HUSY catalyst were elucidated.

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在HUSY分子筛负载的定制氧化铱铼催化剂上通过甘油选择性氢解可持续生产1-丙醇
1-丙醇(1-PO)是一种用途广泛的工业溶剂和重要的化工中间体。在本研究中,研究了常规质子型超稳定(HUSY)分子筛、单金属负载Ir-HUSY分子筛(Ir-HUSY)分子筛和负载Ir-ReOx金属-金属氧化物分子筛(IrRe-HUSY)分子筛上甘油氢解制1-PO的反应。采用连续两步湿浸渍法制备的IrRe-HUSY催化剂具有良好的理化性能,包括改善的酸性和均匀的金属分散。因此,双金属催化剂IrRe-HUSY表现出相当高的催化性能,甘油转化率为78.9%,1-PO收率为39.2%,而分子筛HUSY和Ir-HUSY的甘油转化率为32.9%,1-PO收率为11.1%。IrRe-HUSY催化剂催化性能的提高是由于三种催化剂组分之间的协同作用:(1)ReOx簇有利于甘油的吸附和活化;(2)纳米Ir促进了C─O键的裂解和氢化;(3)酸性HUSY支持强化脱水步骤。此外,系统地研究了催化剂负载、反应时间和温度等操作条件对1-PO生产的影响。研究了IrRe-HUSY催化剂的表面结构及其催化甘油氢解的机理。
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来源期刊
ChemCatChem
ChemCatChem 化学-物理化学
CiteScore
8.10
自引率
4.40%
发文量
511
审稿时长
1.3 months
期刊介绍: With an impact factor of 4.495 (2018), ChemCatChem is one of the premier journals in the field of catalysis. The journal provides primary research papers and critical secondary information on heterogeneous, homogeneous and bio- and nanocatalysis. The journal is well placed to strengthen cross-communication within between these communities. Its authors and readers come from academia, the chemical industry, and government laboratories across the world. It is published on behalf of Chemistry Europe, an association of 16 European chemical societies, and is supported by the German Catalysis Society.
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