Ruidi Wang,Bei-Bei Xu,Jiachen Wang,Xue Lu Wang,Ye-Feng Yao
The relationship between the structural characteristics and photocatalytic reaction mechanisms of graphitic carbon nitride (g-C3N4) still remains unclarified at the molecular level, which severely hinders the further development of this field. The present study addresses this issue by employing an innovative strategy to investigate the relationship between the H-containing structures of g-C3N4 and its water splitting properties. The exchangeable and unexchangeable protons of the H-containing groups of g-C3N4 were differentiated by selective deuteration, providing a way to distinguish the hydrophilic and relatively non-hydrophilic H-containing groups of g-C3N4. A combination of advanced solid-state NMR approaches reveals that amino group defects (CN2(NHx)) on the C–N skeleton of the photocatalyst likely serve as hydrophilic active sites for facilitating the photocatalytic hydrogen evolution reaction. Accordingly, the newly synthesized g-C3N4 sample having a high concentration of CN2(NHx) by design demonstrates an enhanced H2 yield by a factor of 17 compared to that of pure g-C3N4.
Wenda Zhang,Jie Feng,Fengqi Lu,Alberto J. Fernández-Carrión,Hui Fu,Xiaojun Kuang
Na-doped melilite-type silicate Sr2MgSi2O7 was reported to display high oxide ion conductivity. In this work, through multiple complementary techniques including X-ray diffraction, scanning electron microscopy, transmission electron microscopy, solid-state 29Si and 23Na nuclear magnetic resonance spectroscopy, and DFT calculations of defect formation energies, we found that it is hard to replace Sr with Na in Sr2MgSi2O7, and the Sr2−xNaxMgSi2O7−0.5x compositions formed mixed crystalline Sr2MgSi2O7 and Na-containing glassy phases. AC impedance spectroscopy measurements indicated that the ionic conduction in Sr2−xNaxMgSi2O7−0.5x could be from Na+ ions in the glassy phase, instead of the oxide ions.
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