The direct production of liquid fuels from CO2 hydrogenation has attracted enormous interest for its significant roles in mitigating CO2 emissions and reducing dependence on petrochemicals. Here we report a highly efficient, stable and multifunctional Na–Fe3O4/HZSM-5 catalyst, which can directly convert CO2 to gasoline-range (C5–C11) hydrocarbons with selectivity up to 78% of all hydrocarbons while only 4% methane at a CO2 conversion of 22% under industrial relevant conditions. It is achieved by a multifunctional catalyst providing three types of active sites (Fe3O4, Fe5C2 and acid sites), which cooperatively catalyse a tandem reaction. More significantly, the appropriate proximity of three types of active sites plays a crucial role in the successive and synergetic catalytic conversion of CO2 to gasoline. The multifunctional catalyst, exhibiting a remarkable stability for 1,000 h on stream, definitely has the potential to be a promising industrial catalyst for CO2 utilization to liquid fuels.
Although considerable efforts have been made in converting carbon dioxide to hydrocarbons via hydrogenation processes, precise control of CC coupling towards heavy olefins remains a challenge. Here we report a carbon dioxide hydrogenation to olefin process that achieves 72% selectivity for alkenes and 50.3% selectivity for C 4-18 alkenes, of which formation of linear α-olefins accounts for 80%. The process is catalyzed by carbon-supported iron, commonly used in CC coupling reactions, with multiple alkali promoters extracted from corncob. The design is based on the synergistic catalysis of mineral elements in biomass enzyme on which carbon dioxide can be directly converted into carbohydrate. The mineral elements from corncob may promote the surface enrichment of potassium, suppressing the secondary hydrogenation of alkenes on active sites. Furthermore, carburization of iron species is enhanced to form more Fe 5 C 2 species, promoting both the reverse water-gas shift reaction and subsequent CC coupling.
Mn acted as a promoter by forming a Mn-rich layer around a core rich in Fe. The outer layer hindered the formation of magnetite, and impeded H2 adsorption whilst encouraging CO dissociative adsorption, which gave the perfect conditions for olefin production.
Spinel-like ZnFe2O4 is tailor-made synthesized for catalyzing CO2 hydrodenation, achieving an ultra-high yield of full spectrum alkene over a three-stage reactor system (1858.1 g/kgcat h). This study can provide a...
Pd
has been regarded as one of the alternatives to Pt as a promising
hydrogen evolution reaction (HER) catalyst. Strategies including Pd–metal
alloys (Pd–M) and Pd hydrides (PdH
x
) have been proposed to boost HER performances. However, the stability
issues, e.g., the dissolution in Pd–M and the hydrogen releasing
in PdH
x
, restrict the industrial application
of Pd-based HER catalysts. We here design and synthesize a stable
Pd–Cu hydride (PdCu0.2H0.43) catalyst,
combining the advantages of both Pd–M and PdH
x
structures and improving the HER durability simultaneously.
The hydrogen intercalation is realized under atmospheric pressure
(1.0 atm) following our synthetic approach that imparts high stability
to the Pd–Cu hydride structure. The obtained PdCu0.2H0.43 catalyst exhibits a small overpotential of 28 mV
at 10 mA/cm2, a low Tafel slope of 23 mV/dec, and excellent
HER durability due to its appropriate hydrogen adsorption free energy
and alleviated metal dissolution rate.
High‐rate electrochemical CO2‐to‐CO conversion provides a favorable strategy for carbon neutrality. Molecular catalysts, especially those with isolated metal active centers, are known to be the efficient CO2‐to‐CO electrocatalysts due to their high selectivity and outstanding instinct activity; however, the controllable scale‐up synthesis and durable utilization at industrial current densities still remain a challenge. Here, it is developed a molecularly dispersed cobalt phthalocyanine loaded on carbon nanotube for high‐current long‐term CO2‐to‐CO electrolysis. The resultant catalyst exhibits a high CO selectivity with a maximum Faradaic efficiency of 97% and performs a current density of −200 mA cm−2 in a flow cell with a TOF of 83.9 s−1, which is among the best of CO‐selective electrocatalysts. With a series of impregnation loading experiments, the process of molecular‐dispersion or aggregation is investigated. In addition, the application of selective and durable electrolysis at a current of 0.25 A is realized up to 38.5 h in a scale‐up MEA configuration. Subsequent characterization shows robust durability closely related to the dispersion of CoPc. This study provides a triumph to catalyze commercial‐scale CO production using molecularly dispersed phthalocyanine electrocatalysts.
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