Eco-Materials and Renewable Energy Research Center (ERERC), College of Engineering and Applied Sciences, Nanjing University, NO. 22, Hankou Road, Nanjing, Jiangsu 210093, P.R. China.
Phys Chem Chem Phys. 2013 Nov 7;15(41):18077-84. doi: 10.1039/c3cp53774a.
The development of efficient photocatalytic material for converting solar energy to hydrogen energy as viable alternatives to fossil-fuel technologies is expected to revolutionize energy shortage and environment issues. However, to date, the low quantum yield for solar hydrogen production over photocatalysts has hindered advances in the practical applications of photocatalysis. Here, we show that a carbon nitride intercalation compound (CNIC) synthesized by a simple molten salt route is an efficient polymer photocatalyst with a high quantum yield. We found that coordinating the alkali metals into the C-N plane of carbon nitride will induce the un-uniform spatial charge distribution. The electrons are confined in the intercalated region while the holes are in the far intercalated region, which promoted efficient separation of photogenerated carriers. The donor-type alkali metal ions coordinating into the nitrogen pots of carbon nitrides increase the free carrier concentration and lead to the formation of novel nonradiative paths. This should favor improved transport of the photogenerated electron and hole and decrease the electron-hole recombination rate. As a result, the CNIC exhibits a quantum yield as high as 21.2% under 420 nm light irradiation for solar hydrogen production. Such high quantum yield opens up new opportunities for using cheap semiconducting polymers as energy transducers.
开发高效的光催化材料,将太阳能转化为氢能,作为化石燃料技术的可行替代品,有望彻底改变能源短缺和环境问题。然而,迄今为止,光催化剂用于太阳能制氢的量子产率低,阻碍了光催化实际应用的发展。在这里,我们展示了一种通过简单的熔融盐路线合成的氮化碳插层化合物(CNIC)是一种高效的聚合物光催化剂,具有高量子产率。我们发现,将碱金属配位到氮化碳的 C-N 平面中会引起非均匀的空间电荷分布。电子被限制在插层区域,而空穴在远插层区域,这促进了光生载流子的有效分离。供体型碱金属离子配位到氮化碳的氮锅中会增加自由载流子浓度,并导致形成新的非辐射路径。这有利于改善光生电子和空穴的输运,并降低电子-空穴复合速率。因此,在 420nm 光照射下,CNIC 用于太阳能制氢的量子产率高达 21.2%。如此高的量子产率为使用廉价的半导体聚合物作为能量转换器开辟了新的机会。