| 噻吩环掺杂氮化碳纳米片的制备及光催化性能 |
| Preparation and Photocatalytic Performance of Thiophene-Ring Doped Carbon Nitride Nanosheets |
|
| 摘要: 二次热剥离是合成二维氮化碳纳米片(CNN)的有效方法，进一步拓宽其可见光响应并优化光电转化效率是提升CNN光催化性能的有效策略。本工作采用原位聚合分子掺杂和二次热剥离相结合的方法，以2-氨基噻吩-3-甲腈为分子掺杂源，将噻吩环原位掺杂引入并稳定存在于CNN共轭杂环，制备了噻吩环掺杂的氮化碳纳米片光催化剂(CNN-Thx)。经过二次热剥离后，产物保持二维杂化共轭聚合结构且噻吩环依然稳定掺杂于CNN共轭杂环。噻吩环掺杂引起π共轭体系进一步扩展，降低了产物禁带宽度，拓宽了可见光吸收范围，增强了光电转换效率；同时，二次热剥离协同噻吩掺杂引起更显著的n-π*跃迁，大幅提升了催化剂的光催化活性。在可见光照下对催化剂进行光解水制H2及活化O2制H2O2的性能测试。结果表明，CNN-Thx具有显著增强的光催化还原性能，其中，CNN-Th10的产氢活性达到322.8 μmol·h-1，4 h后生成H2O2浓度达到223.1 μmol·L-1，分别是CNN的3.6和22.3倍。 |
| 关键词: 氮化碳纳米片 掺杂 光催化 制H2 制H2O2 |
| 基金项目: 江苏省自然科学基金(No.BK20190981)和福州大学能源与环境光催化国家重点实验室开放课题(No.SKLPEE-KF202103)资助。 |
| Abstract: Secondary thermal exfoliation is an effective method to synthesize 2D carbon nitride nanosheets (CNN). Further broadening the visible light response and optimizing the photoelectric conversion efficiency are effective strategies to improve the photocatalytic performance of CNN materials. In this work, we report thiophene-ring doped carbon nitride nanosheet photocatalysts (CNN-Thx) prepared from in situ polymerization doping and secondary thermal exfoliation using 2-aminothiophene-3-carbonitride as the molecular doping source. Thiophene-ring with excellent chemical properties was stably doped into conjugated CNN nanosheets. After secondary thermal exfoliation, the products maintained 2D hybrid conjugated polymer structures, and the thiophene-ring was still stably doped in the CNN conjugated heterocyclic skeleton. Thiophene-ring doping causes the further expansion of the π-conjugated system, reduces the bandgap, broadens the visible light absorption range, and accelerates the photoelectric conversion efficiency of the catalysts. At the same time, thermal exfoliation cooperated with thiophene doping leads to a more significant n-π* transition, which greatly improves the photocatalytic activity of the catalysts. The results showed that CNN-Thx had significantly enhanced photocatalytic reduction performance, in which the H2 evolution activity of CNN-Th10 reached 322.8 μmol·h-1, and the generated H2O2 concentration reached 223.1 μmol·L-1 after 4 h, which were 3.6 and 22.3 times that of CNN, respectively. |
| Keywords: carbon nitride nanosheets doping photocatalysis H2 evolution H2O2 production |
| 投稿时间：2021-11-05 修订日期：2022-02-06 |
| 摘要点击次数: 1945 |
| 全文下载次数: 911 |
| 李雪,徐红赟,王乙舒,宋艳华,崔言娟.噻吩环掺杂氮化碳纳米片的制备及光催化性能[J].无机化学学报,2022,38(4):654-664. |
| 查看全文 查看/发表评论 下载PDF阅读器 |
| Support information: |
|
|
|
|
|
|
