• Medientyp: E-Book
  • Titel: Intermolecular Hydrogen Bond Modulating the Selective Coupling of Protons and Co2 to Ch4 Over Nitrogen-Doped Carbon Layers Modified Cobalt
  • Beteiligte: Ma, Minzhi [VerfasserIn]; Chen, Jiahao [VerfasserIn]; Huang, Zeai [VerfasserIn]; Fa, Wenjun [VerfasserIn]; Wang, Fang [VerfasserIn]; Rao, Zhiqiang [VerfasserIn]; Wang, Rui [VerfasserIn]; Zhang, Ruiyang [VerfasserIn]; Cao, Yuehan [VerfasserIn]; Zou, Yanzhao [VerfasserIn]; Zhou, Ying [VerfasserIn]
  • Erschienen: [S.l.]: SSRN, [2022]
  • Umfang: 1 Online-Ressource (31 p)
  • Sprache: Englisch
  • DOI: 10.2139/ssrn.4022172
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  • Beschreibung: Photocatalytic reduction of CO 2 with H 2 O to CH 4 is a promising route to complete the carbon neutrality goal. Nevertheless, one of the biggest challenges for this elegant strategy is that the coupling of the protons and CO 2 to form CH 4 is fiercely competed with proton-proton couplings to form H 2 or CO generation, leading to extremely low CH 4 selectivity. Herein, we designed and fabricated the nitrogen-doped carbon layers modified cobalt (N-CCo) photocatalyst for modulating the selective coupling of protons and CO 2 to CH 4 during photocatalytic reduction of CO 2 . In situ DRIFTS and DFT calculations revealed that the formation of intermolecular hydrogen bond between the as-prepared N-C@Co and H 2 O molecule was found to suppress the mass transfer of the generated protons and promote the adsorption of CO 2 molecule. More crucially, it was conducive to suppress the desorption of the CO intermediate product that was typically recognized as the decisive specie for CH 4 generation. As a result, the H 2 selectivity (9.1 %) and activity (17.3 µmol g -1 ) of the as-prepared N-C@Co were reduced by a factor of 9.2 and 17.6, respectively, as compared to that of bulk Co. The CH 4 selectivity of N-C@Co was boosted 6.2 times from13.3% of bulk Co to 82.0 % of N-C@Co with the generation rate of 155.7 μmol g −1 . This work provides a fresh insight into the photocatalyst design for improving CH 4 selectivity and suppressing the competing H 2 and CO generation
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