4.6 Article

Greener and facile synthesis of Cu/ZnO catalysts for CO2 hydrogenation to methanol by urea hydrolysis of acetates

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RSC ADVANCES
卷 11, 期 24, 页码 14323-14333

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ROYAL SOC CHEMISTRY
DOI: 10.1039/d1ra02103f

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  1. Swiss National Science Foundation [CRSII5-183495]
  2. MINECO, Spain [CTQ2016-75499-R]
  3. Swiss National Science Foundation (SNF) [CRSII5_183495] Funding Source: Swiss National Science Foundation (SNF)

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In this study, sodium- and nitrate-free hydroxy-carbonate precursors were successfully prepared via urea hydrolysis co-precipitation of acetate salt, simplifying the catalyst preparation process and making the synthesis more sustainable. The Cu/ZnO catalysts derived from these precursors showed comparable catalytic performance to commercial catalysts in CO2 hydrogenation, even without the need for a washing step and pH control.
Cu/ZnO-based catalysts for methanol synthesis by COx hydrogenation are widely prepared via co-precipitation of sodium carbonates and nitrate salts, which eventually produces a large amount of wastewater from the washing step to remove sodium (Na+) and/or nitrate (NO3-) residues. The step is inevitable since the remaining Na+ acts as a catalyst poison whereas leftover NO3- induces metal agglomeration during the calcination. In this study, sodium- and nitrate-free hydroxy-carbonate precursors were prepared via urea hydrolysis co-precipitation of acetate salt and compared with the case using nitrate salts. The Cu/ZnO catalysts derived from calcination of the washed and unwashed precursors show catalytic performance comparable to the commercial Cu/ZnO/Al2O3 catalyst in CO2 hydrogenation at 240-280 degrees C and 331 bar. By the combination of urea hydrolysis and the nitrate-free precipitants, the catalyst preparation is simpler with fewer steps, even without the need for a washing step and pH control, rendering the synthesis more sustainable.

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