Journal
RSC ADVANCES
Volume 7, Issue 30, Pages 18340-18346Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c6ra28742e
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- Ministry of Science and Technology (Taiwan, R.O.C.) [MOST 105-2628-E-155-002-MY3, MOST 105-2221-E-155-014-MY3, MOST 105-2622-E-155-011-CC2, MOST 105-2218-E-155-007]
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This study elucidates how the nitrogen functionalities affect the UV-visible absorption and photoluminescence (PL) emission of N-modified graphene quantum dots (NGQDs). An electrochemical exfoliation technique incorporated with an in situ amino-functionalization is adopted to synthesize N-modified graphene nanosheets (GNs) with different amidation levels. The applied voltage plays a crucial role in tuning the N/C atomic ratio on the GN product. The maximal N/C atomic ratio reaches 8.4% when exfoliating the GNs at 5 V. The nitrogen functionalities on the GNs include (i) amide/amino functional groups, decorated to the edge sites of GNs, and (ii) pyridinic/pyrrolic/quaternary N, planar to the GNs. The tunable PL emission is strongly affected by the n-pi* transitions, forming an interstate transition. The N chemical doping in C=C sp(2) domains and amino edge functional groups strongly influences the bonding and anti-bonding of molecular orbits, leading to different electronic transition n-states. Thus, the N dopant and edge N functionalities serve as new radiative sites to tune the PL emission. The surface coverage of sp(2) carbon bonding decreased with an increase in the number of N functional groups, inducing a red shift. Therefore, the color-tunable emission from blue to greenish color and the increase of absorption in the visible region can be done by tuning appropriate amidation level on the NGQD specimens.
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