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K-guided selective regulation mechanism for CO hydrogenation over Ni/CeO catalyst. | LitMetric
Regulating the selectivity between CO and CH during CO hydrogenation is a challenging research topic. Previous research has indicated that potassium (K) modification can adjust the product selectivity by regulating the adsorption strength of formate/CO* intermediates. Going beyond the regulation mechanism described above, this study proposes a K-guided selectivity control method based on the regulation of key intermediates HCO*/HCO* for Ni catalysts supported on reducible carrier CeO. By incorporating K, the CO selectivity of CO hydrogenation shifts from around 25.4% for Ni/CeO to approximately 93.8% for Ni/CeO-K. This can be attributed to K modification causes electron aggregation in the bonding regions of HCO* and HCO* intermediates, thus enhancing their adsorption strength. Consequently, the reaction pathway from HCO*/HCO* to CH is limited, favoring the decomposition of formates to CO products. Moreover, the addition of K leads to a moderate decrease in CO conversion from 55.2% to 48.6%, which still surpasses values reported in most other studies. This reduction is associated with a decline in reducible Ni species and oxygen vacancy concentration in Ni/CeO-K. As a result, the adsorption capacity for CO and H reduces, ultimately reducing CO hydrogenation activity.
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