采用一种新颖有效的席夫碱化学法合成吡啶共聚改性的g-C3N4,其可见光催化产氢性能较(由尿素为前驱物制备的)纯g—C3N4显著增强。在此基础上,又进一步通过一步煅烧的方法构建了毗啶改性g—CaN4和N掺杂还原氧化石墨烯(N-rGO)的复合物,其产氢活性得到了进一步地提高,氢气产量最高达到304pmol·h-1,分别为纯g.C3N4和吡啶改性g-C3N4的11.7倍和3.1倍。除了其增强的可见光吸收能力,增大的表面积,我们认为:吡啶环作为分子内电子受体,N—rGO作为“电子转移活性位”,二者共同促进了光生载流子分离和转移,从而显著增强了该复合体系的光催化活性。
Here, we fabricated a pyridine-copolymerized g-C3N4 by a novel and cost-effective approach based on Schiff-base chemistry. Thus produced g-C3N4 showed significantly enhanced and stable visible-light photocatalytic H2 evolution performance compared to pristine g-C3N4 obtained from urea. Subsequently, we constructed a composite of pyridine-modified g-C3N4 and N-doped reduced graphene oxide (N-rGO) by facile one-pot calcination to elevate the photocatalytic efficiency further. The peak H2 production rate achieved using this composite was 304 μmol.h--1, about 11.7 and 3.1 times as those obtained using pure g-C3N4 and pyridine-modified g-C3N4, respectively. In addition to enhanced visible light absorbance and enlarged surface area, the promoted separation, transfer, and surface reactivity of photogenerated charge carriers by the pyddine ring as intramolecular electron acceptor and N-rGO as "electron-transfer activation region" are considered responsible for the remarkably enhanced photocatalytic activity.