A general bottom-up synthesis of CuO-based trimetallic oxide mesocrystal superstructures for efficient catalytic production of trichlorosilane
A general bottom-up synthesis of CuO-based trimetallic oxide mesocrystal superstructures for efficient catalytic production of trichlorosilane
复制标题
CuO基三金属氧化物介晶超结构的通用自下而上合成用于高效催化生产三氯硅烷
DOI：
10.1007/s12274-020-2934-2
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发表时间：
2020-07-25
期刊：
影响因子：
9.9
通讯作者：
Su, Fabing
中科院分区：
文献类型：
--
作者：
Liu, Hezhi;Ji, Yongjun;Su, Fabing
介晶是一种具有高度有序纳米粒子超结构的非经典晶体，由于其新的集体特性，在许多应用中显示出巨大的潜力。然而，仍然缺乏一种简便和通用的合成策略来将不同的组分组织和整合到复杂的介晶中，也缺乏它们在工业催化反应中的应用的报道。在此，我们报告了一种通用的自下而上合成的 CuO 基三金属氧化物介晶（表示为 CuO-M1Ox-M2Oy，其中 M1 和 M2 = Zn、In、Fe、Ni、Mn 和 Co），使用简单的沉淀方法，然后进行水热处理和通过煅烧进行拓扑转变。当这些介晶用作催化剂通过硅氢氯化反应生产三氯硅烷（TCS）时，它们表现出优异的催化性能，大大提高了硅转化率和TCS选择性。特别是，TCS 产率比无催化剂工艺提高了 19 倍。后者是当前的工业流程。这些介晶的高效催化性能归因于明确的纳米级异质界面的形成，可以有效促进电荷转移，以及在不同金属氧化物之间的界面附近的 CuO 上产生压缩和拉伸应变。这里开发的合成方法可适用于制造通用的复杂金属氧化物介晶作为各种工业化学反应的新型催化剂。
Mesocrystals, the non-classical crystals with highly ordered nanoparticle superstructures, have shown great potential in many applications because of their newly collective properties. However, there is still a lack of a facile and general synthesis strategy to organize and integrate distinct components into complex mesocrystals, and of reported application for them in industrial catalytic reactions. Herein we report a general bottom-up synthesis of CuO-based trimetallic oxide mesocrystals (denoted as CuO-M1Ox-M2Oy, where M1 and M2 = Zn, In, Fe, Ni, Mn, and Co) using a simple precipitation method followed by a hydrothermal treatment and a topotactic transformation via calcination. When these mesocrystals were used as the catalyst to produce trichlorosilane (TCS) via Si hydrochlorination reaction, they exhibited excellent catalytic performance with much increased Si conversion and TCS selectivity. In particular, the TCS yield was increased 19-fold than that of the catalyst-free process. The latter is the current industrial process. The efficiently catalytic property of these mesocrystals is attributed to the formation of well-defined nanoscale heterointerfaces that can effectively facilitate the charge transfer, and the generation of the compressive and tensile strain on CuO near the interfaces among different metal oxides. The synthetic approach developed here could be applicable to fabricate versatile complicated metal oxide mesocrystals as novel catalysts for various industrial chemical reactions.