Microfibrous-Structured Pd/AlOOH/Al-Fiber for CO Coupling to Dimethyl Oxalate: Effect of Morphology of AlOOH Nanosheet Endogenously Grown on Al-Fiber
Microfibrous-Structured Pd/AlOOH/Al-Fiber for CO Coupling to Dimethyl Oxalate: Effect of Morphology of AlOOH Nanosheet Endogenously Grown on Al-Fiber
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用于 CO 偶联草酸二甲酯的微纤维结构 Pd/AlOOH/Al 纤维：内生生长的 AlOOH 纳米片形态对 Al 纤维的影响
DOI：
10.1021/acsami.7600889
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发表时间：
2017
影响因子：
9.5
通讯作者：
Lu Yong
中科院分区：
文献类型：
--
作者：
Wang Chunzheng;Ding Jia;Zhao Guofeng;Deng Tao;Liu Ye;Lu Yong
我们报告了一种绿色、无模板、通用的一锅法，通过 Al 金属和 H2O 之间的纯水水热氧化反应 (2Al + 4H2O → 2AlOOH + 3H2) 在 3D 网络 60 μm-Al 纤维毡上内源生长独立式勃姆石 (AlOOH) 纳米片。 AlOOH纳米片的含量和形貌可以通过调节水热氧化时间长度和温度来微调。通过初湿浸渍法，钯高度分散在铝纤维毡上内源形成的 AlOOH 上，并在 CO 偶联至草酸二甲酯 (DMO) 反应中检查所得的 Pd/AlOOH/Al 纤维催化剂。有趣的是，Pd 分散对 AlOOH 纳米片的厚度（26-68 nm）非常敏感，因此转换显示出强烈的 AlOOH-纳米片-厚度依赖性，而本征活性（TOF）则与 AlOOH-纳米片-厚度无关。最有前途的结构化催化剂是使用微纤维结构复合材料和最薄的 AlOOH 纳米片（26 nm）来负载仅 0.26 wt% 的少量 Pd 的催化剂。该催化剂具有高导热性和令人满意的结构坚固性，在 150 °C 下使用 CH3ONO/CO/N2(1/1.4/7.6, vol) 进料和 3000 L kg–1h–1 的气时空速时，CO 转化率达到 67%，DMO 选择性达到 96%，特别是在至少 150 小时内非常稳定，没有失活迹象。
We report a green, template-free, and general one-pot method of endogenous growth of free-standing boehmite (AlOOH) nanosheets on a 3D-network 60 μm-Al-fiber felt through water-only hydrothermal oxidation reaction between Al metal and H2O (2Al + 4H2O → 2AlOOH + 3H2). Content and morphology of AlOOH nanosheets can be finely tuned by adjusting the hydrothermal oxidation time length and temperature. Palladium is highly dispersed on such AlOOH endogenously formed on Al-fiber felt via incipient wetness impregnation method and as-obtained Pd/AlOOH/Al-fiber catalysts are checked in the CO coupling to dimethyl oxalate (DMO) reaction. Interestingly, Pd dispersion is very sensitive to the thickness (26–68 nm) of AlOOH nanosheet, and therefore the conversion shows strong AlOOH-nanosheet-thickness dependence whereas the intrinsic activity (TOF) is AlOOH-nanosheet-thickness independence. The most promising structured catalyst is the one using a microfibrous-structured composite with the thinnest AlOOH nanosheet (26 nm) to support a small amount of Pd of only 0.26 wt %. This catalyst, with high thermal-conductivity and satisfying structural robustness, delivers 67% CO conversion and 96% DMO selectivity at 150 °C using a feed of CH3ONO/CO/N2(1/1.4/7.6, vol) and a gas hourly space velocity of 3000 L kg–1h–1, and particularly, is very stable for at least 150 h without deactivation sign.