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Hollow Flower-Like Cu–Co Catalysts Derived from Layered Double Hydroxides for CO2 Hydrogenation to Ethanol
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DOI:10.1021/acssuschemeng.6c01997.png)
Abstract
En 中文
The selective hydrogenation of CO2 to value-added C2+ oxygenates is a promising route toward carbon neutrality but is complicated by the parallel pathways to hydrocarbons and methanol. Herein, a precursor-topology strategy is employed to construct the hollow flower-like Cux–Coy catalysts derived from layered double hydroxide (LDH) precursors for CO2 hydrogenation to ethanol. The three-dimensional architectural Cux–Coy offers a high surface area and open mesopores while promoting a homogeneous distribution of Cu–Co interfacial sites on the Al2O3 matrix. Cu1–Co3 achieves a CO2 conversion of 16.9% and an ethanol selectivity of 16.5%, with the stability over 100 h when CO2 is hydrogenated at 260 °C and 1.5 MPa under a gas hourly space velocity of 12,000 mL·gcat–1·h–1 and a H2/CO2 volume ratio of 3:1. Multitechnique characterization by XRD, SEM/TEM, EPR, XPS, CO2-TPD, H2-TPR, H2-TPD, N2O pulse titration, and in situ DRIFTS suggests that the optimized Cu1–Co3 catalyst possesses a hollow flower-like architecture, enhancing the Cu dispersion, increasing the abundant defect/basic sites, improving the CO2 reducibility and H2 activation ability, and accessing the Cu–Co interfacial ensembles. Cu–Co interfacial sites favor the formation and preservation of *CO and *CHx species required for C–C coupling for ethanol formation while suppressing excessive hydrogenation to CH4.
Keywords:
CO2 hydrogenation
ethanol
LDHs
Cu−Co
spatial construction
Journal
A
IF:
0
Papers:
554
Citations:
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