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Coupling Molecular and Nanoparticle Catalysts on Single Metal–Organic Framework Microcrystals for the Tandem Reaction of H2O2 Generation and Selective Alkene Oxidation
ACS Catalysis ( IF 11.3 ) Pub Date : 2017-09-05 00:00:00 , DOI: 10.1021/acscatal.6b03632 Rungmai Limvorapitux 1 , Lien-Yang Chou 2, 3 , Allison P. Young 2 , Chia-Kuang Tsung 2 , SonBinh T. Nguyen 1
ACS Catalysis ( IF 11.3 ) Pub Date : 2017-09-05 00:00:00 , DOI: 10.1021/acscatal.6b03632 Rungmai Limvorapitux 1 , Lien-Yang Chou 2, 3 , Allison P. Young 2 , Chia-Kuang Tsung 2 , SonBinh T. Nguyen 1
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A molecular catalyst, (sal)MoVI, and a heterogeneous catalyst, either Pd or Au nanoparticles (NPs), were integrated into one UiO-66 MOF microcrystal. The resulting dually functionalized catalysts, Pd@UiO-66-(sal)Mo and Au/UiO-66-(sal)Mo, have been utilized for a one-pot tandem reaction of H2O2 generation and selective liquid-phase alkene oxidation. The NPs serve as catalysts for the production of H2O2 from H2 and O2 gases, while the (sal)Mo moieties function as the oxidation catalyst. When the metal NPs are fully encapsulated within the MOF microcrystals, the alkene hydrogenation side reaction is largely suppressed, with a 6-fold decrease in the hydrogenation/oxidation product ratio for 5-bromo-1-cyclooctene favoring the epoxide as the major product. For Au/UiO-66-(sal)Mo, where the two catalysts are in close proximity on the MOF microcrystal, the enhancement in oxidation productivity is increased by 10 times in comparison to the [Au/UiO-66-NH2 + UiO-66-sal(Mo)] physical mixture of the two singly functionalized MOFs.
中文翻译：
在金属-有机骨架微晶上偶联分子和纳米颗粒催化剂，用于H 2 O 2生成和选择性烯烃氧化的串联反应
将分子催化剂（sal）Mo VI和非均相催化剂Pd或Au纳米颗粒（NPs）集成到一个UiO-66 MOF微晶中。生成的双功能催化剂Pd @ UiO-66-（sal）Mo和Au / UiO-66-（sal）Mo已用于H 2 O 2生成和选择性液相烯烃的一锅串联反应。氧化。NP用作由H 2和O 2产生H 2 O 2的催化剂（sal）Mo部分起氧化催化剂的作用。当金属NP被完全封装在MOF微晶中时，烯烃氢化副反应被大大抑制，5-溴-1-环辛烯的氢化/氧化产物比降低6倍，有利于环氧化物作为主要产物。对于Au / UiO-66-（sal）Mo，其中两种催化剂都紧靠MOF微晶，与[ Au / UiO-66-NH 2 + UiO -66-sal（Mo）]两个单官能化MOF的物理混合物。
更新日期：2017-09-05
中文翻译：
在金属-有机骨架微晶上偶联分子和纳米颗粒催化剂，用于H 2 O 2生成和选择性烯烃氧化的串联反应
将分子催化剂（sal）Mo VI和非均相催化剂Pd或Au纳米颗粒（NPs）集成到一个UiO-66 MOF微晶中。生成的双功能催化剂Pd @ UiO-66-（sal）Mo和Au / UiO-66-（sal）Mo已用于H 2 O 2生成和选择性液相烯烃的一锅串联反应。氧化。NP用作由H 2和O 2产生H 2 O 2的催化剂（sal）Mo部分起氧化催化剂的作用。当金属NP被完全封装在MOF微晶中时，烯烃氢化副反应被大大抑制，5-溴-1-环辛烯的氢化/氧化产物比降低6倍，有利于环氧化物作为主要产物。对于Au / UiO-66-（sal）Mo，其中两种催化剂都紧靠MOF微晶，与[ Au / UiO-66-NH 2 + UiO -66-sal（Mo）]两个单官能化MOF的物理混合物。
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