Chemisorption‐Induced and Plasmon‐Promoted Photofixation of Nitrogen on Gold‐Loaded Carbon Nitride Nanosheets. Issue 13 (12th May 2020)

• Record Type: Journal Article
• Authors: Wu, Shiqun; Chen, Ziyu; Liu, Kaida; Yue, Wenhui; Wang, Lingzhi; Zhang, Jinlong
• Is Part Of: ChemSusChem. Volume 13:Issue 13(2020)
• Page Start: 3455
• Page End: 3461
• Publication Date: 2020-05-12
• Subjects: carbon nitride -- gold -- nitrogen fixation -- photocatalysis -- surface plasmon resonance; Green chemistry -- Periodicals; Sustainable engineering -- Periodicals; Chemistry -- Periodicals; Chemical engineering -- Periodicals; 660
• DOI: 10.1002/cssc.202000818
• Languages: English
• ISSNs: 1864-5631

Abstract

Abstract: Photocatalytic fixation of nitrogen is a promising method for green conversion of solar light, but has been substantially limited by inefficient activation of the nonpolar N≡N bond and the poor utilization of visible light. In this study, carbon nitride nanosheet composites with abundant nitrogen vacancies and strong plasmonic resonance absorption of visible light have been fabricated through the combination of hydrogen treatment and loading of Au nanoparticles. Ammonia yields of 184 μmol g −1 and 93 μmol g −1 are obtained without any sacrificial agent under full‐light and visible‐light irradiation, respectively. In particular, the visible‐light activity is enhanced tenfold with the help of Au. Combining the experimental results and theoretical calculations, both the hydrogen treatment and Au loading help form nitrogen vacancies on the carbon nitride nanosheets, which promote N2 activation by enhancing the chemisorption. Furthermore, the Au loading further improves the nitrogen reduction efficiency through charging the excited hot electrons formed from the surface plasmonic resonance to the adsorbed N2 molecules. Abstract : So hot right now : Efficient nitrogen photofixation is carried out on Au‐loaded carbon nitride under visible‐light excitation through the coupling of strong N2 activation by nitrogen vacancies and accelerated N2 reduction by hot electrons from Au with surface plasmon resonance effect. An ammonia yield of 184 μmol g −1 and 93 μmol g −1 is obtained without any sacrificial agent under full‐light and visible‐light irradiation, respectively