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首页> 外文期刊>Catalysis science & technology >Direct coating copper-zinc-aluminum oxalate with H-ZSM-5 to fabricate a highly efficient capsule-structured bifunctional catalyst for dimethyl ether production from syngas
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Direct coating copper-zinc-aluminum oxalate with H-ZSM-5 to fabricate a highly efficient capsule-structured bifunctional catalyst for dimethyl ether production from syngas

机译：直接涂层copper-zinc-aluminum草酸H-ZSM-5制造高效capsule-structured双功能催化剂二甲醚生产合成气

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摘要

Dimethyl ether (DME) has been considered as an industrially important intermediate and clean alternative fuel. The development of a highly efficient syngas-to-DME bifunctional catalyst is of great importance but remains a challenge. In this work, we reported a facile and robust strategy for preparing a highly efficient CZA-oa@H-ZSM-5 capsule-structured bifunctional catalyst by coating an H-ZSM-5 shell on millimeter-sized copper-zinc-aluminum oxalate (CZA-oa) but not on copper-zinc-aluminum oxide (CZA-oxi) via the hydrothermal crystallization process with the subsequent calcination at 500 degrees C for 5 h in air. From the characterization and reaction results, we inferred that the direct use of CZA-oa as a replacement of CZA efficiently inhibited Cu leaching in the coating process, besides turning down the necessity of using a rotary oven for the good coating of the H-ZSM-5 shell on the core owing to high hydrophilic property. The developed CZA-oa@H-ZSM-5 capsule bifunctional catalyst showed 5.0 times higher turnover frequency (TOF, 1.5 min(-1)) with 93.7% of DME selectivity as compared to CZA-oxi@H-ZSM-5 R (0.3 min(-1) of TOF and 92.5% of DME selectivity) prepared by a similar procedure except for the use of mixed oxide as a core to replace CZA-oa. The improvement in the intrinsic activity of the developed CZA-oa@H-ZSM-5 capsule bifunctional catalyst originated from appropriate Cu-Zn interactions. Interestingly, owing to the excellent hydrophilic property of CZA-oa, the use of the rotary oven in the coating process of the H-ZSM-5 shell can be avoided if oxalate is used to replace oxide as a core. Compared to CZA-oxi@H-ZSM-5 R (0.031 mmol m(Cu)(-2) h(-1)), CZA-oa@H-ZSM-5 showed a much higher DME formation rate (R-DME = 0.122 mmol m(Cu)(-2) h(-1)), which allowed it to be a promising catalyst for DME production from syngas. Moreover, this work also opens a new window for designing outstanding bifunctional catalysts for other applications.
机译：二甲醚(测距装置)已经被视为一个工业上重要的中间和清洁替代燃料。高效syngas-to-DME双功能催化剂重视,但仍然是一个挑战。这项工作,我们报道一个肤浅和鲁棒性准备一个高效的策略CZA-oa@H-ZSM-5 capsule-structured双官能催化剂通过涂层H-ZSM-5壳效果copper-zinc-aluminum草酸(CZA-oa),但不是copper-zinc-aluminum氧化物通过水热结晶(CZA-oxi)过程和随后的煅烧,享年500岁度5 h在空气中。表征和反应的结果,我们直接使用CZA-oa作为推断更换CZA有效地抑制铜浸在涂层过程中,除了转向使用旋转烤箱的必要性好的涂料H-ZSM-5壳的核心由于高亲水属性。CZA-oa@H-ZSM-5胶囊双功能催化剂显示高5.0倍营业额频率(TOF、1.5分钟(1))的测距装置选择性为93.7%相比CZA-oxi@H-ZSM-5 TOF的R(0.3分钟(1)和92.5%的测距装置选择性)准备的类似的过程,除了使用混合氧化物作为核心来取代CZA-oa。改进的内在活性开发CZA-oa@H-ZSM-5胶囊双官能起源于适当Cu-Zn催化剂交互。优秀的亲水性CZA-oa的属性,使用的旋转烤箱的镀膜工艺如果使用草酸H-ZSM-5壳是可以避免的取代氧化作为核心。CZA-oa@H-ZSM-5显示更高的测距装置的形成率(R-DME = 0.122更易与m h(铜)(2)(1)),使它成为一个有前途的测距装置的催化剂从合成气生产。打开一个新窗口的设计突出双功能催化剂的其他应用程序。

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