Selective C2+ Alcohol Synthesis from Direct CO2 Hydrogenation over a Cs-Promoted Cu-Fe-Zn Catalyst

Higher alcohol (C2+) synthesis (HAS) from direct CO2 hydrogenation is a promising way to realize the fixation of CO2 to high-value chemicals; however, the identification of active catalysts to give satisfactory activity and selectivity is not yet achieved, let alone the elucidation of mechanism. Here, we report a working catalyst containing Cu-Fe-Zn that can efficiently and selectively synthesize C-2(+) alcohols from CO2 hydrogenation. The optimized catalyst-encoded CsC(0)(.)(8)F(1.0)Z(1.0) exhibits a high C2+ OH/ROH fraction (weight percent of C-2(+) alcohols in total C-1 and C-2(+) alcohols) of 93.8% with a high C2+OH space time yield (STY) of 73.4 mg g(cat)(-1) h(-1) (1.47 mmol g(cat)(-1) h(-1)).( )A( )mechanism study reveals that HAS experiences a tandem pathway of combining surface CO* formation on Cu-ZnO dual sites with surface hydrocarbon moieties on Cu-Fe7C3 dual sites at their material interfaces. A good balance of dissociative and nondissociative C-O bond activation in synergy results in the high HAS activity of Cs-C(0)(.)(8)F(1.0)Z(1.0).