Carrier-Induced Modification of Palladium Nanoparticles on Porous Boron Nitride for Alkyne Semi-Hydrogenation

被引:55
作者
Buchele, Simon [1 ]
Chen, Zupeng [1 ]
Fako, Edvin [2 ,3 ]
Krumeich, Frank [4 ]
Hauert, Roland [5 ]
Safonova, Olga, V [6 ]
Lopez, Nuria [2 ,3 ]
Mitchell, Sharon [1 ]
Perez-Ramirez, Javier [1 ]
机构
[1] Swiss Fed Inst Technol, Dept Chem & Appl Biosci, Inst Chem & Bioengn, Vladimir Prelog Weg 1, CH-8093 Zurich, Switzerland
[2] Inst Chem Res Catalonia, Av Paisos Catalans 16, Tarragona 43007, Spain
[3] Barcelona Inst Sci & Technol, Av Paisos Catalans 16, Tarragona 43007, Spain
[4] Swiss Fed Inst Technol, Lab Inorgan Chem, Dept Chem & Appl Biosci, Vladimir Prelog Weg 1, CH-8093 Zurich, Switzerland
[5] Swiss Fed Labs Mat Sci & Technol, Empa, Uberlandstr 129, CH-8600 Dubendorf, Switzerland
[6] Paul Scherrer Inst, Forsch Str 111, CH-5232 Villigen, Switzerland
基金
瑞士国家科学基金会;
关键词
boron nitride; doping; heterogeneous catalysis; palladium; selective hydrogenation; METAL-SUPPORT INTERACTIONS; SELECTIVE HYDROGENATION; STRUCTURE SENSITIVITY; CATALYSTS;
D O I
10.1002/anie.202005842
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Chemical modifiers enhance the efficiency of metal catalysts in numerous applications, but their introduction often involves toxic or expensive precursors and complicates the synthesis. Here, we show that a porous boron nitride carrier can directly modify supported palladium nanoparticles, originating unparalleled performance in the continuous semi-hydrogenation of alkynes. Analysis of the impact of various structural parameters reveals that using a defective high surface area boron nitride and ensuring a palladium particle size of 4-5 nm is critical for maximizing the specific rate. The combined experimental and theoretical analyses point towards boron incorporation from defects in the support to the palladium subsurface, creating the desired isolated ensembles determining the selectivity. This practical approach highlights the unexplored potential of using tailored carriers for catalyst design.
引用
收藏
页码:19639 / 19644
页数:6
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