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Low‐Temperature Catalytic Hydrogenolysis of Guaiacol to Phenol over Al‐Doped SBA‐15 Supported Ni Catalysts
ChemCatChem ( IF 3.8 ) Pub Date : 2020-06-29 , DOI: 10.1002/cctc.202000712 Qiuyue Wang 1 , Yufang Chen 1 , Guanheng Yang 1 , Ping Deng 1 , Xinqing Lu 1 , Rui Ma 1 , Yanghe Fu 1 , Weidong Zhu 1
ChemCatChem ( IF 3.8 ) Pub Date : 2020-06-29 , DOI: 10.1002/cctc.202000712 Qiuyue Wang 1 , Yufang Chen 1 , Guanheng Yang 1 , Ping Deng 1 , Xinqing Lu 1 , Rui Ma 1 , Yanghe Fu 1 , Weidong Zhu 1
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Selective hydrogenolysis of aromatic carbon‐oxygen (Caryl−O) bonds is a key strategy for the generation of aromatic chemicals from lignin. However, this process is usually operated at high temperatures and pressures over hydrogenation catalysts, resulting in a low selectivity for aromatics and an extra consumption of hydrogen. Here, a series of Al‐doped SBA‐15 mesoporous materials with different Si/Al molar ratios (Al‐SBA‐15) were prepared via a post‐synthesis method using NaAlO2 as the Al source, and then Al‐SBA‐15 supported Ni catalysts (Ni/Al‐SBA‐15) were prepared by a deposition‐precipitation method using urea as the hydrolysis reagent. The prepared supports and catalysts were extensively characterized using various techniques such as XRD, N2 adsorption/desorption, TEM, 27Al NMR, NH3‐TPD, XPS, H2‐TPR, and pyridine‐FT‐IR, and the catalysts were evaluated in the hydrogenolysis of the Caryl−O bond in guaiacol and lignin derived compounds under mild conditions. The effects of the Si/Al ratio in catalyst and reaction parameters on guaiacol conversion and product distribution were investigated in detail, associated with solvent effect. The incorporation of Al into the framework of SBA‐15 can improve the Lewis acidity and the dispersion of the supported Ni particles and yet modulate the metal‐support interactions, which are propitious to the hydrogenolysis of the Caryl−O bond in guaiacol. The catalyst Ni/Al‐SBA‐15 with a Si/Al molar ratio of 10 shows the best performance with a guaiacol conversion of 87.4 % and a phenol selectivity of 76.9 % under the mild conditions conducted, because of its proper acidity, suitable metal‐support interactions, and high dispersion of the active species. The present study would stimulate research and development in multi‐functional catalysts for the generation of valuable chemicals from biomass.
中文翻译：
Al掺杂的SBA-15负载Ni催化剂对愈创木酚的低温催化氢解反应生成苯酚
芳香族碳氧（C aryl -O）键的选择性氢解是从木质素生成芳香族化学品的关键策略。然而，该方法通常在高温和高压下在氢化催化剂上进行，导致对芳族化合物的选择性低和额外的氢消耗。在这里，使用NaAlO 2作为Al源，通过后合成方法制备了一系列具有不同Si / Al摩尔比的Al掺杂SBA-15介孔材料（Al-SBA-15），然后制备了Al-SBA-15负载型Ni催化剂（Ni / Al-SBA-15）是通过沉积沉淀法使用尿素作为水解试剂制备的。使用各种技术（例如XRD，N 2）对制得的载体和催化剂进行了广泛表征。吸附/解吸，TEM，27 Al NMR，NH 3 -TPD，XPS，H 2 -TPR和吡啶-FT-IR，并评估了愈创木酚和木质素衍生化合物中C芳基-O键的氢解反应在温和的条件下。详细研究了催化剂中Si / Al比和反应参数对愈创木酚转化率和产物分布的影响，以及溶剂效应。将Al掺入SBA-15框架中可以改善路易斯酸度和负载型Ni颗粒的分散性，但仍可调节金属与载体之间的相互作用，这有利于C芳基的氢解-O键在愈创木酚中。Si / Al摩尔比为10的Ni / Al-SBA-15催化剂表现出最佳的性能，在温和的条件下，愈创木酚的转化率为87.4％，苯酚的选择性为76.9％，这是因为它具有适当的酸度，适用于金属‐支持相互作用以及活性物质的高度分散。本研究将促进多功能催化剂的研究和开发，以从生物质中产生有价值的化学物质。
更新日期：2020-06-29
中文翻译：
Al掺杂的SBA-15负载Ni催化剂对愈创木酚的低温催化氢解反应生成苯酚
芳香族碳氧（C aryl -O）键的选择性氢解是从木质素生成芳香族化学品的关键策略。然而，该方法通常在高温和高压下在氢化催化剂上进行，导致对芳族化合物的选择性低和额外的氢消耗。在这里，使用NaAlO 2作为Al源，通过后合成方法制备了一系列具有不同Si / Al摩尔比的Al掺杂SBA-15介孔材料（Al-SBA-15），然后制备了Al-SBA-15负载型Ni催化剂（Ni / Al-SBA-15）是通过沉积沉淀法使用尿素作为水解试剂制备的。使用各种技术（例如XRD，N 2）对制得的载体和催化剂进行了广泛表征。吸附/解吸，TEM，27 Al NMR，NH 3 -TPD，XPS，H 2 -TPR和吡啶-FT-IR，并评估了愈创木酚和木质素衍生化合物中C芳基-O键的氢解反应在温和的条件下。详细研究了催化剂中Si / Al比和反应参数对愈创木酚转化率和产物分布的影响，以及溶剂效应。将Al掺入SBA-15框架中可以改善路易斯酸度和负载型Ni颗粒的分散性，但仍可调节金属与载体之间的相互作用，这有利于C芳基的氢解-O键在愈创木酚中。Si / Al摩尔比为10的Ni / Al-SBA-15催化剂表现出最佳的性能，在温和的条件下，愈创木酚的转化率为87.4％，苯酚的选择性为76.9％，这是因为它具有适当的酸度，适用于金属‐支持相互作用以及活性物质的高度分散。本研究将促进多功能催化剂的研究和开发，以从生物质中产生有价值的化学物质。
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