Experimental and in situ DRIFTs studies on confined metallic copper stabilized Pd species for enhanced CO2 reduction to formate
Xiao, Xin 1Gao, Jiajian 2Xi, Shibo 2Lim, San Hua 2Peng, Alyssa Kai Wen 1Borgna, Armando 2Liu, Yan 2Chu, Wei1
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作者信息
1. Sichuan Univ
2. ASTAR
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Abstract
Understanding the basic principle of Pd-based bimetallic catalysts design is essential in CO2 hydrogenation to formate. In this work, Cu partially replaced the bivalence position in MgAl hydrotalcite structure was developed for achieving the highly confined Cu species, whose interaction with Pd species was systematically studied and compared with the traditional co-impregnation or stepwise impregnation method. The stable and maximum formate formation rate of 12.8 mmol/h/g(metal) was obtained on Pd-0.4@CuMgAlOx catalyst under 100 degrees C, 4.0 MPa, H-2/CO2 ratio of 3, being about double of the sum of formate production rate over the monometallic Cu and Pd catalysts. Strong synergetic interaction between Pd and the confined Cu species was observed with Cu/Pd atomic ratios of 14-181. Extensive characterization using TEM, XPS, XANES, coupled with kinetic study and in situ DRIFTs analysis revealed that the superior performance of Pd-0.4@CuMgAlOx was attributed to the confined PdCu nanoparticles with electron-rich PdCu surface.
Key words
Enhanced CO2 hydrogenation to formate/Synergetic effect/PdCu bimetallic catalysts/Confined catalysts/In situ DRIFTS/HOLLOW CARBON SPHERES/FORMIC-ACID/CATALYTIC-ACTIVITY/HYDROGENATION/NANOPARTICLES/CU/CONVERSION/DEHYDROGENATION/PALLADIUM/SUPPORT