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作 者:程若霖 金锡雄 樊向前[1,2] 王敏[1,2] 田建建 张玲霞[1,2] 施剑林[1,2]
机构地区:[1]中国科学院上海硅酸盐研究所高性能陶瓷和超微结构国家重点实验室,上海200050 [2]中国科学院大学,北京100049
出 处:《物理化学学报》2017年第7期1436-1445,共10页Acta Physico-Chimica Sinica
基 金:supported by the State Key Program for Basic Research of China(2013CB933200)~~
摘 要: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-C_3N_4,其可见光催化产氢性能较(由尿素为前驱物制备的)纯g-C_3N_4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吡啶改性g-C_3N_4和N掺杂还原氧化石墨烯(N-r GO)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304μmol?h-1,分别为纯g-C_3N_4和吡啶改性g-C_3N_4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-r GO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.
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