| CuPd/MgO室温高效催化甲醛溶液产氢 |
| CuPd/MgO for Efficient Catalytic Hydrogen Production from Formaldehyde Solution at Room Temperature |
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| 摘要: 采用浸渍还原法制备了MgO负载纳米CuPd合金的复合催化剂(CuPd/MgO)。该催化剂在室温催化甲醛溶液重整产氢过程中表现出优异的催化性能，转换频率(TOF)高达812.6 h-1，分别是相同条件下Cu/MgO (TOF=356.7 h-1)和Pd/MgO (TOF=34.8 h-1)的2.3倍和23倍。基于实验测试和表征结果，发现CuPd/MgO催化剂中纳米CuPd合金与表面富集缺陷的MgO载体之间存在金属-载体强相互作用。这种相互作用能够促进氧气在催化剂表面吸附活化并生成活性氧物种(超氧阴离子自由基，·O2-)，·O2-先后促进甲醛中的C—H键断裂和水分子的解离，随后与反应体系中生成的质子及氢自由基(·H)依次结合，最终实现氢气的析出与氧气的再生。 |
| 关键词: 铜钯合金 氧化镁 甲醛 氢气 金属-载体强相互作用 |
| 基金项目: 国家自然科学基金(No.22172143， 52102316)资助。 |
| Abstract: The composite catalyst of CuPd alloy nanoparticles supported on MgO (CuPd/MgO) was prepared by an impregnation reduction method. CuPd/MgO showed excellent catalytic performance during formaldehyde reforming for hydrogen production at room temperature in the air. The turnover frequency (TOF) of CuPd/MgO was as high as 812.6 h-1, which was respectively 2.3 times and 23 times higher than that of Cu/MgO (TOF=356.7 h-1) and Pd/MgO (TOF=34.8 h-1) under the same reaction conditions. Based on the experimental observations and characterization results, we found that a strong metal support interaction (SMSI) between CuPd alloy nanoparticles and MgO support enriched with defects on the surface was present in CuPd/MgO. This interaction was conducive to the transfer and recombination of electrons on the catalyst, greatly promoting the adsorption, activation, and reduction of oxygen on the catalyst surface to form superoxide anion radical (·O2-). The ·O2- combined with the proton generated by the C—H bond breaking of formaldehyde to form superoxide radical (·OOH). The hydrogen radical (·H) dissociated from water molecules in the reaction system continuously combined with ·OOH to generate hydrogen and oxygen, leading to the generation of hydrogen and the regeneration of oxygen. |
| Keywords: CuPd alloy MgO formaldehyde hydrogen strong metal-support interactions |
| 投稿时间：2022-06-29 修订日期：2022-10-09 |
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| 黄铭浩,李卓,杜雷雷,金智康,李仁宏.CuPd/MgO室温高效催化甲醛溶液产氢[J].无机化学学报,2022,38(12):2452-2458. |
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