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Preparation and Study of Pd Catalysts Supported on Activated Carbon Cloth (ACC) for Direct Synthesis of H2O2 from H2 and O2

机译:活性炭布(ACC)担载的Pd催化剂的制备及由H2和O2直接合成H2O2的研究

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Activated carbon cloths (ACCs) were used as supports for Pd catalysts. The catalyst preparation was carried out by the impregnation method using acidic solution of palladium dichloride (PdCl2) as metal precursor. The effects of the oxidation state of the loaded metal, heat treatment of the catalysts in different atmosphere (H2, air) at different temperatures and surface chemistry of the support on the catalyst characterizations and the catalytic activities were investigated. Wet oxidation of ACC was done by nitric acid in order to induce oxygen-containing surface functional groups. Surface chemistry of the support and oxidation state of the metallic phase was investigated by means of XPS, TPD, SEM, DTA and TGA tests. Direct synthesis of hydrogen peroxide from H2 and O2 was performed batch wise in a stainless steel autoclave. The reactions were conducted under high pressure (38 bar) at 0 °C and methanol was used as reaction medium. The direct synthesis results showed that the oxygen-containing surface functional groups increase the selectivity of the catalysts by reducing the rate of water production. Existence of the oxidized state of Pd (PdO) also makes the catalyst more selective than the corresponding zerovalent state (PdO). PdO affected on selectivity by increasing the rate of H2O2 production and reducing the amount of production of water, simultaneously.
机译:活性炭布(ACC)用作Pd催化剂的载体。使用二氯化钯(PdCl 2)的酸性溶液作为金属前体,通过浸渍法进行催化剂的制备。研究了负载金属的氧化态,在不同温度(H2,空气),不同温度下催化剂的热处理以及载体的表面化学性质对催化剂性能和催化活性的影响。 ACC的湿氧化是通过硝酸进行的,以诱导含氧的表面官能团。通过XPS,TPD,SEM,DTA和TGA测试研究了载体的表面化学性质和金属相的氧化态。在不锈钢高压釜中分批从氢气和氧气直接合成过氧化氢。反应在0℃在高压(38bar)下进行,甲醇用作反应介质。直接合成结果表明,含氧表面官能团可通过降低水的生成速率来提高催化剂的选择性。 Pd(PdO)氧化态的存在也使催化剂比相应的零价态(PdO)更具选择性。 PdO通过同时增加H2O2的产生速率和减少水的产生量而影响选择性。

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