The sintering resistance of supported Cu nanoparticle (NP) catalysts is crucial to their practical application in the dehydrogenation of diethanolamine (DEA). In this paper, co-precipitation, hydrothermal synthesis, and sol-gel condensation are used to form a new support material through chemical bonding between graphene oxide and ZrO2. The composite carriers prepared by the three methods are mixed with copper nitrate and ground using a ball mill. A series of Cu/ZrO2-reduced graphene oxide (RGO) composites were prepared by calcination under nitrogen at 450 °C for 3 h and hydrogen reduction at 250 °C for 4 h. The conversion of DEA to iminodiacetic acid (IDA) reached 96% with the Cu/ZrO2-RGO catalyst prepared by hydrothermal synthesis. The conversion rate of DEA is more than 80% following the reuse of the CZG-2 catalyst for twelve cycles. The various physicochemical characterization techniques show that the Cu/ZrO2-RGO layered and wrinkled nanostructures can improve catalytic stability and suppress the sintering of the supported Cu NPs during the catalytic dehydrogenation of diethanolamine. A synergistic effect between the RGO and the Cu nanoparticles is observed. The Cu nanoparticles with RGO have a better dispersibility, and a new nano-environment is created, which is the key to improving the efficiency of diethanolamine dehydrogenation. These new Cu/ZrO2-RGO catalysts show increased durability compared to commercially produced Cu/ZrO2 catalysts and show promise for practical applications involving diethanolamine dehydrogenation.
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