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Highly Selective Catalysis at the Liquid–Liquid Interface Microregion
ACS Catalysis ( IF 11.3 ) Pub Date : 2021-01-14 , DOI: 10.1021/acscatal.0c04604 Yabin Zhang 1 , Rammile Ettelaie 2 , Bernard P. Binks 3 , Hengquan Yang 1
ACS Catalysis ( IF 11.3 ) Pub Date : 2021-01-14 , DOI: 10.1021/acscatal.0c04604 Yabin Zhang 1 , Rammile Ettelaie 2 , Bernard P. Binks 3 , Hengquan Yang 1
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Liquid–liquid interfaces in principle have the potential to regulate the selectivity of chemical reactions because of highly anisotropic microenvironments but have not yet been well exploited. Here, we present a liquid–liquid interface-based strategy to boost catalytic selectivity, exemplified by selective hydrogenation of α,β-unsaturated aldehydes. The key to this success is the spatially controlled assembly of tubular catalyst particles, just at the narrow inner interfacial layer of Pickering emulsion water droplets. The catalyst particles that are assembled at the inner interfacial layer of water droplets exhibit much higher selectivity to C═O hydrogenation than ones located either at the outer interfacial layer, in the interior of droplets, or at the conventionally called Pickering emulsion interface. A selectivity of 92.0–98.0% to the thermodynamically and kinetically unfavorable C═O hydrogenation over the C═C hydrogenation was achieved unexpectedly. Our strategy and the phenomena of interfacial catalysis reported here constitute an important supplement to the existing methods for tuning catalytic selectivity, providing tremendous opportunities to construct highly selective catalytic systems.
中文翻译：
液-液界面微区的高选择性催化
由于高度各向异性的微环境，液-液界面原则上具有调节化学反应选择性的潜力，但尚未得到充分利用。在这里，我们提出了一种基于液-液界面的策略来提高催化选择性，以α，β-不饱和醛的选择性加氢为例。成功的关键在于管状催化剂颗粒的空间控制组装，恰好在Pickering乳液水滴的狭窄内界面层。组装在水滴的内界面层上的催化剂颗粒对C = O氢化的选择性比位于外界面层，液滴内部或常规称为Pickering乳液界面的催化剂颗粒高得多。选择性为92.0–98。出乎意料地实现了相对于C andC氢化而言热力学和动力学上不利的C═O氢化0％。本文报道的我们的策略和界面催化现象构成了现有用于调节催化选择性的方法的重要补充，为构建高选择性催化系统提供了巨大的机会。
更新日期：2021-02-05
中文翻译：
液-液界面微区的高选择性催化
由于高度各向异性的微环境，液-液界面原则上具有调节化学反应选择性的潜力，但尚未得到充分利用。在这里，我们提出了一种基于液-液界面的策略来提高催化选择性，以α，β-不饱和醛的选择性加氢为例。成功的关键在于管状催化剂颗粒的空间控制组装，恰好在Pickering乳液水滴的狭窄内界面层。组装在水滴的内界面层上的催化剂颗粒对C = O氢化的选择性比位于外界面层，液滴内部或常规称为Pickering乳液界面的催化剂颗粒高得多。选择性为92.0–98。出乎意料地实现了相对于C andC氢化而言热力学和动力学上不利的C═O氢化0％。本文报道的我们的策略和界面催化现象构成了现有用于调节催化选择性的方法的重要补充，为构建高选择性催化系统提供了巨大的机会。
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