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首页> 外文期刊>Catalysis science & technology >Cu-Pd bimetallic nanoalloy anchored on a N-rich porous organic polymer for high-performance hydrodeoxygenation of biomass-derived vanillin
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Cu-Pd bimetallic nanoalloy anchored on a N-rich porous organic polymer for high-performance hydrodeoxygenation of biomass-derived vanillin

机译：Cu-Pd双金属nanoalloy N-rich锚定为高性能多孔有机聚合物hydrodeoxygenation biomass-derived的香兰素

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摘要

The structural composition, particle size on the nanoscale, phase state, and surface property have a significant impact on the performance of nanoalloy catalysts. Here we report a bimetallic Cu3Pd nanoalloy anchored on a N-rich porous organic polymer (BBA-1), Cu3Pd@BBA-1, which shows enhanced catalytic activity for the hydrodeoxygenation of vanillin, a typical compound of lignin-derived bio-oil. The prepared Cu3Pd@BBA-1 bimetallic nanocatalyst exhibits highly efficient catalytic performance in promoting biomass refining compared with its monometallic counterparts, providing 99.3% conversion of vanillin with an exclusive selectivity of 93.6% for the hydrogenolysis product 2-methoxy-4-methylphenol. This catalyst is also found to have superior stability (reproducible conversion values upon several cycles), which represents a significant step forward in promoting biomass refining. The Cu3Pd@BBA-1 and related Cu and Pd based catalysts with varying metallic molar ratios were synthesized by a polyol method using NaBH4 as a strong reducing agent. The specific textural and chemical characteristics of the as-synthesized nanohybrid materials were comprehensively investigated by performing X-ray photoelectron spectroscopy, Fourier transform infrared spectroscopy, synchrotron powder diffraction, X-ray absorption fine structure spectroscopy, C-13 cross polarization magic angle spinning nuclear magnetic resonance, nitrogen physisorption, high resolution transmission electron microscopy, and high angle annular dark field scanning transmission electron microscopy with the corresponding elemental mapping. The catalytic performance of Cu3Pd on other commercial supports such as Al2O3, TiO2 and N-doped carbon is found to be inferior to that on BBA-1, revealing the important role of the nitrogen-rich porous organic polymer matrix. The performance of a 3:1 mixture of the monometallic nanoalloys was substantially lower than that of Cu3Pd@ BBA-1. These results and the inputs from the experimental probes used for the characterization indicate that in Cu3Pd@BBA-1, alloying leads to improved surface conditions on the nanoscale and brings about a synergetic electronic effect, thus enabling an enhanced catalytic activity and good recyclability.
机译：结构组成、粒度上纳米级、阶段状态和表面性质的性能产生重大影响nanoalloy催化剂。Cu3Pd nanoalloy N-rich多孔锚定有机聚合物(BBA-1), Cu3Pd@BBA-1节目增强的催化活性香兰素的hydrodeoxygenation典型化合物的lignin-derived生物燃油。Cu3Pd@BBA-1双金属nanocatalyst展品高效的催化性能促进生物质精炼与它相比单本位制的同行,提供99.3%转换的香兰素独家氢解作用的选择性为93.6%产品2-methoxy-4-methylphenol。也发现有优越的稳定(可再生的转换值数周期),它代表了一个重要的一步在促进生物质精炼。Cu3Pd@BBA-1及相关铜和基于Pd的催化剂不同金属摩尔比率使用NaBH4作为多元醇合成的方法强还原剂。as-synthesized的化学特性nanohybrid材料综合调查通过执行x射线光电子傅里叶变换红外光谱光谱、同步加速器粉末衍射,x射线吸收精细结构光谱,c13交叉极化魔角旋转核磁共振、氮物理吸附,高分辨率的传播电子显微镜,高角度环形暗扫描透射电子显微镜与相应元素的映射。Cu3Pd其他的催化性能商业支持,如氧化铝、二氧化钛和n型碳发现不如BBA-1,露出的重要作用富氮多孔有机聚合物矩阵。性能单本位制的一个3:1混合的nanoalloys大大低于Cu3Pd@ BBA-1。用于实验调查在Cu3Pd@BBA-1表征表明,合金导致改善表面状况纳米尺度上,带来了一个协同作用的电子效应,从而使一个增强催化活性和良好的可回收性。

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