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Synthesis of palladium-rhodium bimetallic nanoparticles for formic acid dehydrogenation

Journal of Energy Chemistry 2021年第1期30卷 301-309,I0010页

作者： Ilaria Barlocco sofia capelli Elisa Zanella Xiaowei Chen Juan JDelgado Alberto Roldan Nikolaos Dimitratos Alberto Villa Dipartimento di Chimica Universitàdegli Studi di MilanoMilan I-20133Italy Departamento de Ciencia de los Materiales Ingeniería Metalúrgica y Química InorgánicaFacultad de CienciasUniversidad de CádizCampus Río San PedroPuerto Real(Cádiz)E-11510Spain School of Chemistry Cardiff UniversityMain BuildingPark PlaceCF103AT CardiffUnited Kingdom Dipartimento di Chimica Industriale e dei Materiali Alma Mater Studiorum Universitàdi BolognaViale Risorgimento 4I-40136 BolognaItaly

Herein,we report for the first time the synthesis of preformed bimetallic Pd-Rh nanoparticles with different Pd:Rh ratios(nominal molar ratio:80-20,60-40,40-60,20-80) and the corresponding Pd and Rh monometallic ones by sol immobilization using polyvinyl alcohol(PVA) as protecting agent and NaBH4 as reducing agent,using carbon nanofibers with high graphitization degree(HHT) as the desired support.The synthesized catalysts were characterized by means of Transmission Electron Microscopy(TEM) and inductively coupled plasma optical emission spectroscopy(ICP-OES).TEM shows that the average particle size of the Pd-Rh nanoparticles is the range of 3-4 nm,with the presence of few large agglomerated nanoparticles.For bimetallic catalysts,EDX-STEM analysis of individual nanoparticles demonstrated the presence of random-alloyed nanoparticles even in all cases Rh content is lower than the nominal one(calculated Pd:Rh molar ratio:90-10,69-31,49-51,40-60).The catalytic performance of the Pd-Rh catalysts was evaluated in the liquid phase dehydrogenation of formic acid to H2.It was found that Pd-Rh molar ratio strongly influences the catalytic performance.Pd-rich catalysts were more active than Rh-rich ones,with the highest activity observed for Pd90:Rh10(1792 h^(-1)),whereas Pd69:Rh31(921 h^(-1)) resulted the most stable during recycling tests.Finally,Pd90:Rh10 was chosen as a representative sample for the liquid-phase hydrogenation of muconic acid using formic acid as hydrogen donor,showing good yield to adipic acid.

关键词： Palladium Rhodium Alloy Formic acid Hydrogen Muconic acid

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