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首页> 外文期刊>Journal of Materials Chemistry, A. Materials for energy and sustainability >(100) surface-exposed CeO2 nanocubes as an efficient heterogeneous catalyst in the tandem oxidation of benzyl alcohol, para-chlorobenzyl alcohol and toluene to the corresponding aldehydes selectively
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(100) surface-exposed CeO2 nanocubes as an efficient heterogeneous catalyst in the tandem oxidation of benzyl alcohol, para-chlorobenzyl alcohol and toluene to the corresponding aldehydes selectively

机译:(100)表面暴露的CeO2纳米立方作为一种有效的多相催化剂,可选择性地将苄醇,对氯苄醇和甲苯串联氧化为相应的醛

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摘要

A new synthesis strategy has been developed to synthesize exclusively (100)-surface-exposed CeO2 nanocubes (similar to 90 nm), formed through three dimensional (3D) self-assembly of smaller ceria nanocrystal building blocks, as an efficient heterogeneous catalyst for multiple selective oxidation reactions. To compare the effect of morphology on catalysis, 1D CeO2 nanorods have also been tested in parallel. The as-synthesized CeO2 nanocubes acted as a breakthrough catalyst in the quantitative conversion of benzyl alcohol and para-chlorobenzyl alcohol with absolute selectivity to their respective aldehydes (>99%) under very mild reaction conditions in water at 35 degrees C. The same ceria nanocubes acted as an efficient catalyst in the oxidation of toluene to benzaldehyde selectively. The preferentially exposed (100) surfaces, the presence of a high concentration of oxygen vacancies (2.11 x 10(21) cm(-3)), the small size of the nanoscale building blocks and the corresponding high surface area and porosity have been reasoned to produce the observed high catalytic activity parameter and turn over frequency (TOF). Further characterization of the recovered catalysts after five cycles confirmed the retention of the original morphology, crystal structure and, most importantly, catalytic properties with no significant activity loss, confirming the possibility of repeated use of the present CeO2 nanocubes without compromising their intrinsic qualities.
机译:已开发出一种新的合成策略,以独家合成(100个)表面暴露的CeO2纳米立方体(类似于90 nm),该纳米立方体是通过较小的二氧化铈纳米晶体构件的三维(3D)自组装形成的,作为多种催化剂的有效多相催化剂选择性氧化反应。为了比较形态学对催化的影响,还并行测试了一维CeO2纳米棒。在35摄氏度的水中非常温和的反应条件下,合成后的CeO2纳米立方体在突破苄基醇和对氯苄醇的转化率方面具有突破性催化剂的作用,对它们各自的醛(> 99%)具有绝对选择性。纳米立方体在将甲苯选择性氧化为苯甲醛中起着有效的催化剂的作用。可以推断出优先暴露的(100)表面,高浓度的氧空位(2.11 x 10(21)cm(-3)),纳米级结构块的尺寸较小以及相应的高表面积和孔隙率产生观察到的高催化活性参数和周转频率(TOF)。在五个循环后对回收的催化剂进行进一步表征,证实了其原始形态,晶体结构以及最重要的催化性能得以保留,而活性没有明显损失,从而证实了在不损害其内在质量的情况下重复使用本发明CeO2纳米立方体的可能性。

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