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Development of catalytic microreactors by plasma processes and sol-gel processes

Abstract : This work aims not only at designing and fabricating new microfluidic chips for benzyl alcohol oxidation, but also at developing a methodology of plasma devoted to the surface functionalization with linkage reagent in order to anchor catalyst particles in the next step. Results show that the PECVD method is a universal method that can deposit high amine content of APTES polymerized film on various substrate surfaces. Optimized plasma conditions for APTES deposition were found and lead to a better hydrophilicity of the substrates, a higher coating thickness, as well as a higher amine group density than the conventional wet chemistry method. In addition, the APTES depositions lead to a further higher coverage and amount of AuNPs when the pH value is 6.2. Moreover, the results of immobilizing AuNPs on zeolite indicate that APTES is a better linker than MPTES as it provides a higher amount of gold loading. For zeolite and AuNPs@zeolite deposition, the particles were functionalized with carboxyl group using CES as a linker for bounding the protonated amines on COC surface that is pre-modified using PECVD method. The latter coating is stable in hydrodynamic flows and could be further used in microfluidics. Finally, the gold \Y zeolite \AuNPs@zeolite microreactors are respectively connected into pre-designed microfluidic system. The gold type microreactor exhibits stable high selectivity to benzaldehyde (~94%). However, it also shows relative low benzyl alcohol conversion (~20%). The AuNPs@zeolites type microreactor performs the best catalytic activity in our study as a high benzaldehyde selectivity (>99%) is obtained with the highest benzyl alcohol conversion (~40%).
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Xi Rao. Development of catalytic microreactors by plasma processes and sol-gel processes. Analytical chemistry. Université Pierre et Marie Curie - Paris VI, 2016. English. ⟨NNT : 2016PA066145⟩. ⟨tel-01592658⟩

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