Tang Jun, Zhou Xue, Cao Shixiong, Zhu Lingyu, Xi Lingling, Wang Jianli
State Key Laboratory Breeding Base of Green Chemistry-Synthesis Technology, Biodiesel Laboratory of China Petroleum and Chemical Industry Federation, Zhejiang Province Key Laboratory of Biofuel, College of Chemical Engineering , Zhejiang University of Technology , Hangzhou 310014 , China.
Department of Chemistry , Zhejiang University , Xixi Campus , Hangzhou 310028 , China.
ACS Appl Mater Interfaces. 2019 May 1;11(17):16156-16163. doi: 10.1021/acsami.9b00821. Epub 2019 Apr 17.
Pickering interfacial catalysis provides an excellent platform for biphasic reactions, but the separation and recycling of nanocatalysts is a challenge because of high adsorption energy of nanocatalysts at the liquid-liquid interface. In this work, we represent a new type of versatile Pickering emulsion based on magnetic and CO-responsive nanohybrids FeO@SiO@P(TMA-DEA). The smart nanoparticles can stabilize the water-in-oil Pickering emulsion in the biphasic system and achieve the subsequent demulsification by bubbling CO ascribed to their reversible switching surface. In the absence of energy barrier, the nanohybrids can be easily captured in situ by magnetic field in 2 min and showed excellent recyclability. In the Anelli system for alcohol oxidation, the nanocatalyst exhibited threefold enhancement in catalytic efficiency in comparison with an unemulsified two-phase and little loss on activity after five cycles. The conceptually novel dual-responsive system offers a green and energy-saving strategy for effective recycling of the nanocatalyst and intensification of biphasic reaction.
皮克林界面催化为双相反应提供了一个出色的平台，但由于纳米催化剂在液-液界面具有较高的吸附能，其分离和循环利用是一项挑战。在这项工作中，我们展示了一种基于磁性和CO响应性纳米杂化物FeO@SiO@P(TMA-DEA)的新型通用皮克林乳液。这种智能纳米颗粒可以在双相体系中稳定油包水型皮克林乳液，并通过鼓入CO实现随后的破乳，这归因于其可逆切换的表面。在没有能垒的情况下，纳米杂化物可以在2分钟内通过磁场轻松原位捕获，并表现出优异的可循环性。在用于醇氧化的阿内利体系中，与未乳化的两相相比，该纳米催化剂的催化效率提高了两倍，并且在五个循环后活性几乎没有损失。这种概念上新颖的双响应体系为纳米催化剂的有效循环利用和双相反应的强化提供了一种绿色节能策略。
