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Chemoselective hydrogenation of 3‐nitrostyrene over supported gold catalysts: Effect of loadings of gold
Journal of the Chinese Chemical Society ( IF 1.6 ) Pub Date : 2020-12-16 , DOI: 10.1002/jccs.202000512 Yuan Tan 1, 2 , Xing Chi Li 1, 3 , Xiao Yan Liu 1
Journal of the Chinese Chemical Society ( IF 1.6 ) Pub Date : 2020-12-16 , DOI: 10.1002/jccs.202000512 Yuan Tan 1, 2 , Xing Chi Li 1, 3 , Xiao Yan Liu 1
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The chemoselective hydrogenation from 3‐nitrostyrene to 3‐vinylaniline is quite challenging due to coexistence of the C=C bond and the –NO2 group in the same molecule. Previously, we found that the selectivity to the 3‐vinylaniline is very high in wide temperature and time windows when taking the ZnAl‐hydrotalcite supported Au25 nanoclusters as the precatalyst. Here, we investigated the loading effect of gold on the catalytic performance for the chemoselectivity of this reaction. The loadings of gold ranged from 0.5 to 10 wt%. The results showed that the reaction rate decreased greatly with the increasing loading of gold, and selectivity dropped obviously after the loading of gold attaining 10 wt%. The UV–Vis (ultraviolet visible absorption spectroscopy), XRD (X‐ray diffraction), and HAADF‐STEM (high angle annular dark field‐scanning transmission electronic microscope) results suggested that the gold nanoparticles aggregated with the increasing loading of gold. The X‐ray absorption near edge structure (XANES) and in situ CO‐DRIFTS (diffuse reflectance infrared Fourier transform spectroscopy) results indicated that the valent state of gold tended to be slightly positively charged when the loading of gold increased. The origin of the high selectivity to the 3‐vinylaniline was discussed subsequently based on the above results.
中文翻译：
负载型金催化剂上3-硝基苯乙烯的化学选择性加氢：金负载量的影响
由于同一分子中C = C键和–NO 2基团的共存，从3-硝基苯乙烯到3-乙烯基苯胺的化学选择性氢化非常具有挑战性。以前，我们发现当使用ZnAl-水滑石负载的Au 25时，在较宽的温度和时间范围内，对3-乙烯基苯胺的选择性非常高。纳米簇作为前催化剂。在这里，我们研究了金的负载效应对该反应的化学选择性的催化性能。金的负载量为0.5至10重量％。结果表明，随着载金量的增加，反应速率大大降低，当载金量达到10 wt％时，选择性明显下降。UV-Vis（紫外可见吸收光谱），XRD（X射线衍射）和HAADF-STEM（高角度环形暗场扫描透射电子显微镜）结果表明，金纳米颗粒随着金的负载增加而聚集。X射线吸收近边缘结构（XANES）和原位CO-DRIFTS（漫反射红外傅里叶变换光谱法）结果表明，当金的负载量增加时，金的价态趋于稍微带正电。随后根据上述结果讨论了对3-乙烯基苯胺的高选择性的起源。
更新日期：2020-12-16
中文翻译：
负载型金催化剂上3-硝基苯乙烯的化学选择性加氢：金负载量的影响
由于同一分子中C = C键和–NO 2基团的共存，从3-硝基苯乙烯到3-乙烯基苯胺的化学选择性氢化非常具有挑战性。以前，我们发现当使用ZnAl-水滑石负载的Au 25时，在较宽的温度和时间范围内，对3-乙烯基苯胺的选择性非常高。纳米簇作为前催化剂。在这里，我们研究了金的负载效应对该反应的化学选择性的催化性能。金的负载量为0.5至10重量％。结果表明，随着载金量的增加，反应速率大大降低，当载金量达到10 wt％时，选择性明显下降。UV-Vis（紫外可见吸收光谱），XRD（X射线衍射）和HAADF-STEM（高角度环形暗场扫描透射电子显微镜）结果表明，金纳米颗粒随着金的负载增加而聚集。X射线吸收近边缘结构（XANES）和原位CO-DRIFTS（漫反射红外傅里叶变换光谱法）结果表明，当金的负载量增加时，金的价态趋于稍微带正电。随后根据上述结果讨论了对3-乙烯基苯胺的高选择性的起源。
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