氮掺杂还原氧化石墨烯与吡啶共聚g-C<sub>3</sub>N<sub>4</sub>复合光催化剂及其增强的产氢活性

引用本文: 程若霖, 金锡雄, 樊向前, 王敏, 田建建, 张玲霞, 施剑林. 氮掺杂还原氧化石墨烯与吡啶共聚g-C₃N₄复合光催化剂及其增强的产氢活性[J]. 物理化学学报, 2017, 33(7): 1436-1445. doi: 10.3866/PKU.WHXB201704076 shu

Citation: CHENG Ruo-Lin, JIN Xi-Xiong, FAN Xiang-Qian, WANG Min, TIAN Jian-Jian, ZHANG Ling-Xia, SHI Jian-Lin. Incorporation of N-Doped Reduced Graphene Oxide into Pyridine-Copolymerized g-C₃N₄ for Greatly Enhanced H₂ Photocatalytic Evolution[J]. Acta Physico-Chimica Sinica, 2017, 33(7): 1436-1445. doi: 10.3866/PKU.WHXB201704076 shu

氮掺杂还原氧化石墨烯与吡啶共聚g-C₃N₄复合光催化剂及其增强的产氢活性

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
基金项目:
国家重点基础研究发展规划项目（2013CB933200）资助

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-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吡啶改性g-C₃N₄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304 μmol·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。

关键词:

English

Incorporation of N-Doped Reduced Graphene Oxide into Pyridine-Copolymerized g-C₃N₄ for Greatly Enhanced H₂ Photocatalytic Evolution

1.
State Key Laboratory of High Performance Ceramics and Superfine Microstruture, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai 200050, P. R. China;
2.
University of Chinese Academy of Sciences, Beijing 100049, P. R. China
Received Date: 27 December 2016
Revised Date: 15 March 2017
Available Online: 13 April 2017
Fund Project:
The project was supported by the State Key Program for Basic Research of China (2013CB933200).

Abstract: 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 pyridine ring as intramolecular electron acceptor and N-rGO as "electron-transfer activation region" are considered responsible for the remarkably enhanced photocatalytic activity.

Key words:

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通讯作者: 陈斌, bchen63@163.com

1.
沈阳化工大学材料科学与工程学院沈阳 110142

氮掺杂还原氧化石墨烯与吡啶共聚g-C₃N₄复合光催化剂及其增强的产氢活性

English

Incorporation of N-Doped Reduced Graphene Oxide into Pyridine-Copolymerized g-C₃N₄ for Greatly Enhanced H₂ Photocatalytic Evolution

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

氮掺杂还原氧化石墨烯与吡啶共聚g-C3N4复合光催化剂及其增强的产氢活性

English

Incorporation of N-Doped Reduced Graphene Oxide into Pyridine-Copolymerized g-C3N4 for Greatly Enhanced H2 Photocatalytic Evolution

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南： 你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

氮掺杂还原氧化石墨烯与吡啶共聚g-C₃N₄复合光催化剂及其增强的产氢活性

Incorporation of N-Doped Reduced Graphene Oxide into Pyridine-Copolymerized g-C₃N₄ for Greatly Enhanced H₂ Photocatalytic Evolution

CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs