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Ultrahigh surface density of Co-N₂C single-atom-sites for boosting photocatalytic CO₂ reduction to methanol

Ma, Minzhi; Huang, Zeai; Doronkin, Dmitry E. ORCID iD icon 1,2; Fa, Wenjun; Rao, Zhiqiang; Zou, Yanzhao; Wang, Rui; Zhong, Yunqian; Cao, Yuehan; Zhang, Ruiyang; Zhou, Ying
1 Institut für Katalyseforschung und -technologie (IKFT), Karlsruher Institut für Technologie (KIT)
2 Institut für Technische Chemie und Polymerchemie (ITCP), Karlsruher Institut für Technologie (KIT)

Abstract:

Cobalt species as active sites for photocatalytic reduction of CO$_{2}$ to valuable products such as methanol have received increasing attention, however, it remains a huge challenge to achieve the high activity. Herein, a pyrolysis-induced-vaporization strategy was successfully employed to fabricate Co/g-C$_{3}$N$_{4}$ single-atom catalysts (Co/g-C$_{3}$N$_{4}$ SACs) with surface Co atom loading up to 24.6 wt%. Systematic investigation of Co/g-C$_{3}$N$_{4}$ SACs formation process disclosed that concentrated-H$_{2}$SO$_{4}$ exfoliation of g-C$_{3}$N$_{4}$ nanosheets (g-C$_{3}$N$_{4}$ NSs) as the substrate followed by a two-step calcination process is essential to achieve ultrahigh metal loading. It was found that the ultrahigh-density of Co single-atom sites were anchored on the g-C$_{3}$N$_{4}$ substrate surface and coordinated with two nitrogen and one carbon atoms (Co-N$_{2}$C). These single dispersed Co-N$_{2}$C sites on the g-C$_{3}$N$_{4}$ surface were found to act not only as electron gathering centers but also as the sites of CO$_{2}$ adsorption and activation, subsequently, boosting the photocatalytic methanol generation during light irradiation. ... mehr


Postprint §
DOI: 10.5445/IR/1000137304
Veröffentlicht am 13.09.2021
Originalveröffentlichung
DOI: 10.1016/j.apcatb.2021.120695
Scopus
Zitationen: 37
Web of Science
Zitationen: 35
Dimensions
Zitationen: 38
Cover der Publikation
Zugehörige Institution(en) am KIT Institut für Katalyseforschung und -technologie (IKFT)
Institut für Technische Chemie und Polymerchemie (ITCP)
Publikationstyp Zeitschriftenaufsatz
Publikationsmonat/-jahr 01.2022
Sprache Englisch
Identifikator ISSN: 0926-3373
KITopen-ID: 1000137304
HGF-Programm 38.03.02 (POF IV, LK 01) Power-based Fuels and Chemicals
Weitere HGF-Programme 56.98.01 (POF III, LK 01) Betrieb in MML
Erschienen in Applied catalysis / B
Verlag Elsevier
Band 300
Seiten Art.-Nr.: 120695
Vorab online veröffentlicht am 09.09.2021
Schlagwörter Cobalt, g-C$_{3}$N$_{4}$, single-atom catalysts, ultrahigh surface metal loading, photoreduction CO$_{2}$ to methanol
Nachgewiesen in Web of Science
Dimensions
Scopus
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