二维共价有机框架材料的可控合成及其光催化应用研究进展

doi:10.6023/A22070303

化学学报 ›› 2022, Vol. 80 ›› Issue (11): 1494-1506.DOI: 10.6023/A22070303 上一篇下一篇

综述

二维共价有机框架材料的可控合成及其光催化应用研究进展

于潇涵, 黄伟^*(), 李彦光^*()

苏州大学功能纳米与软物质研究院江苏苏州 215123

投稿日期:2022-07-12 发布日期:2022-08-30
通讯作者: 黄伟, 李彦光

作者简介:

于潇涵, 苏州大学功能纳米与软物质研究院硕士研究生. 2020年本科毕业于苏州大学纳米科学技术学院, 现主要从事有机聚合物半导体材料的合成及其光催化应用研究.

黄伟, 副教授, 硕士生导师, 苏州大学优秀青年学者. 2017年于德国马普高分子研究所获化学博士学位, 2018年至2021年于苏州大学从事博士后研究, 2021年入职苏州大学功能纳米与软物质研究院, 担任副教授. 近年来主要从事多孔有机聚合物材料的可控合成及光催化应用研究. 在材料的分子设计、可控合成、光驱动太阳能燃料制备和有机质转化方面取得了一系列创新成果. 在Angew. Chem., Mater. Today, ACS Catal.等材料、化学领域权威期刊发表学术论文30余篇, 其中2篇论文入选ESI高被引论文, 多篇论文被Angew. Chem.选为热点和封面文章. 获国家自然科学基金青年基金和中国博士后面上项目资助.

李彦光教授于2005年获得复旦大学化学系理学学士学位, 2010年获得美国俄亥俄州立大学化学系化学博士学位, 2010年至2013年在美国斯坦福大学化学系从事博士后研究, 2013年10月入职苏州大学功能纳米与软物质研究院, 被聘为教授、博士生导师. 到目前为止, 共发表学术论文150余篇, 论文总他引36000余次, ESI高被引论文40余篇, 在2017~2021年连续入选科睿唯安(Clarivate Analytics)“全球高被引学者”榜单(材料、化学).

Controllable Synthesis and Photocatalytic Applications of Two-dimensional Covalent Organic Frameworks

Xiaohan Yu, Wei Huang(), Yanguang Li()

Institute of Functional Nano & Soft Materials (FUNSOM), Soochow University, Suzhou 215123

Received:2022-07-12 Published:2022-08-30
Contact: Wei Huang, Yanguang Li

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摘要/Abstract

通过模拟自然界光合作用, 将太阳能转化为方便存储的化学能是缓解未来能源短缺和环境污染问题的理想途径之一. 二维共价有机框架材料(2D COFs)是近年来发展起来的一类新型有机半导体材料, 具有结晶度高、结构精确以及化学组分灵活可调等优势, 在光催化领域展现出巨大应用潜力, 受到了研究者们的广泛关注. 对2D COFs的可控制备以及电子结构调控方法进行了系统总结, 并重点介绍了它们在光催化水分解、CO₂还原以及H₂O₂合成领域的最近研究进展, 讨论了材料结构和催化性能之间的关系, 最后对2D COFs在光催化应用领域存在的机遇和挑战进行了展望.

关键词: 共价有机框架材料, 光催化, 析氢, CO₂还原, 氧还原

In the past century, the extensive consumption of fossil fuels has caused significant environmental pollution and energy resource crisis. As a result, seeking to develop clean and renewable alternatives to traditional fossil fuels has recently aroused great concern. Clean and abundant solar energy is undoubtedly an ideal solution. Inspired by natural photosynthesis, tremendous efforts have been devoted over past decades to build artificial photocatalytic systems that aims to convert solar energy to valuable chemical energy, such as H₂, CO, CH₄ and H₂O₂ etc. To do this, developing advanced semiconductor photocatalysts with superior optoelectronic properties is of fundamental importance and has become one of the main challenges. Two-dimensional covalent organic frameworks (2D COFs), as a new class of crystalline, organic porous materials, have recently attracted increasing attention for photocatalytic applications. Specially, they feature periodic molecular architectures and π-unit arrays that are assembled from organic subunits via covalent bonds and π-π interaction. Benefiting from these unique structural characters, 2D COFs usually possess broad visible light absorption range and much enhanced charge separation efficiency in comparison with their amorphous counterparts. Moreover, their molecular topology structures and optoelectronic properties can be readily tuned by selecting suitable monomers and synthetic procedures, making them to be a versatile platform for task-oriented synthesis of advanced photocatalysts with predesigned structures and functionalities. Therefore, the development of 2D COFs photocatalysts will undoubtedly provide new opportunities for efficient utilization of solar energy. In this paper, we first overviewed the synthetic methods of 2D COFs and the viable strategies for modulating their optoelectronic properties, and subsequently summarized current research advances of 2D COFs on photocatalytic water splitting, CO₂ reduction and H₂O₂ production. Finally, the opportunities and challenges in this emerging field are prospected.

Key words: covalent organic frameworks, photocatalysis, H₂ evolution, CO₂ reduction, O₂ reduction

引用此文

于潇涵, 黄伟, 李彦光. 二维共价有机框架材料的可控合成及其光催化应用研究进展[J]. 化学学报, 2022, 80(11): 1494-1506.

Xiaohan Yu, Wei Huang, Yanguang Li. Controllable Synthesis and Photocatalytic Applications of Two-dimensional Covalent Organic Frameworks[J]. Acta Chimica Sinica, 2022, 80(11): 1494-1506.

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图/表 5

图1. 用于2D COFs合成的常见反应类型

Figure 1. Typical chemical reactions for the synthesis of 2D COFs

图2. 2D COFs光电性质调控策略. (a)含有D-A结构的COFs中电子分离和转移示意图以及常见的电子供体、受体基团[83]. (b)重组COFs (RC-COF)的设计思路及相应的高分辨透射电镜(HR-TEM)图像和粉末X射线衍射(PXRD)图谱[79]. (c) NH2-UiO-66/TpPa-1-COF异质结中的电荷转移路径[58]. (d) aza-CMP/C2N异质结的TEM图像以及能带结构示意图[82]

Figure 2. Strategies for tuning the photoelectronic properties of 2D COFs. (a) Schematic diagram of charge separation and transfer in D-A 2D COFs and some typical electron donor and acceptor groups. Reproduced with permission[83]. Copyright 2019, Wiley-VCH. (b) Synthetic procedure of reconstructed COFs (RC-COF) and its corresponding high resolution tunneling electron microscopy (HR-TEM) image and powder X-ray diffraction (PXRD) pattern. Reproduced with permission[79]. Copyright 2022, Springer Nature. (c) Facilitated charge separation across NH2-UiO-66/TpPa-1-COF heterojunction. Reproduced with permission[58]. Copyright 2018, Wiley-VCH. (d) TEM image and electronic band structures of aza-CMP /C2N heterojunction. Reproduced with permission[82]. Copyright 2018, Wiley-VCH

图3. (a) FS-COF的分子结构及空间堆砌模型[90]. (b) BD-COF和CYANO-COF的化学结构. (c) CYANO-COF在不同光照波长下光催化析氢的AQE[91]. (d) PY-DHBD-COF的化学结构[92]. (e)剥离的2D CTF-1纳米片的TEM图片(插图为剥离前后材料的光学照片). (f)块状CTF-1及其2D纳米片的光催化析氢性能[62]. (g)不同碱催化剂合成的CTF-1的XRD图谱. (h)高结晶性CTF-1样品的TEM图像及其(i)光催化全解水性能[53]

Figure 3. (a) Molecular structure and the spatial stacking model of FS-COF. Reproduced with permission[90]. Copyright 2018, Springer Nature. (b) Chemical structures of BD-COF and CYANO-COF and (c) wavelength-dependent AQE of photocatalytic H2 production for CYANO-COF. Reproduced with permission[91]. Copyright 2022, Springer Nature. (d) Chemical structure of PY-DHBD-COF. Reproduced with permission[92]. Copyright 2022, Springer Nature. (e) A TEM image of the exfoliated 2D CTF-1 nanosheets (the insert is the photographs of the bulk and exfoliated CTF-1). (f) Comparison of photocatalytic H2 production rates of the bulk and exfoliated CTF-1. Reproduced with permission[62]. Copyright 2022, Wiley-VCH. (g) XRD patterns of CTF-1 synthesized in presence of different bases. (h) A TEM image of the highly crystalline CTF-1 and (i) its photocatalytic performance for overall water splitting. Reproduced with permission[53]. Copyright 2020, Wiley-VCH

图4. (a) CT-COF的化学结构以及电荷转移路径示意图[102]. (b) Re-COF的化学结构及其(c)光催化CO2还原产CO性能[104]. (d)含不同金属中心的TTCOF-M在气固相光催化CO2还原反应中的性能. (e) TTCOF-M在CO2还原和水氧化中的反应机理. (f)模拟的TTCOF-Zn紫外-可见光漫反射吸收光谱(UV-Vis DRS)以及光生电子的转移路径[105]. (g) TCOF-POM的合成及其(h)光催化CO2还原产CO性能[106]

Figure 4. (a) Molecular structure of CT-COF and the proposed electron transfer pathway. Reproduced with permission[102]. Copyright 2020, Wiley-VCH. (b) Chemical structure of Re-COF and (c) its photocatalytic CO2-to-CO performance. Reproduced with permission[104]. Copyright 2018, American Chemical Society. (d) Photocatalytic CO2 reduction and water oxidation using different TTCOF-M and (e) the proposed catalytic mechanism. (f) Simulated UV-Vis DRS of TTCOF-Zn indicates the photo-induced electron transfer route. Reproduced with permission[105]. Copyright 2019, Wiley-VCH. (g) Synthetic procedure of TCOF-POMs and (h) their photocatalytic CO evolution rates. Reproduced with permission[106]. Copyright 2022, American Chemical Society

图5. (a) TAPD-R2 COF (R=Me, OMe)的化学结构[119]. (b)含氟TF50-COF的化学结构及其(c)在纯水中的光催化氧还原产H2O2性能[120]. (d) CHF-DPDA用于光催化两电子氧还原和两电子水氧化生成H2O2示意图及其(e)在纯水中的H2O2生成速率[121]. (f)在不同温度下COF-TfpBpy光催化产H2O2效率及相应的太阳能-化学能转换(SCC)效率, (g)生成的H2O2可直接用于染料降解和杀菌, (h) COF-TfpBpy在纯水中光催化产H2O2的反应机理示意图[122]

Figure 5. (a) Chemical structure of TAPD-R2 COF (R=Me, OMe). Reproduced with permission[119]. Copyright 2020, American Chemical Society. (b) Chemical structure of TF50-COF and (c) its photocatalytic H2O2 production rate in pure water. Reproduced with permission[120]. Copyright 2022, Wiley-VCH. (d) Schematic illustration of the two reaction pathways for photocatalytic H2O2 production using CHF-DPDA and (e) the photocatalytic H2O2 production rates of the samples. Reproduced with permission[121]. Copyright 2022, Wiley-VCH. (f) Photocatalytic H2O2 production rates of COF-TfpBpy at different temperatures and the corresponding solar-to-chemical conversion (SCC) efficiencies, (g) the formed H2O2 can be directly used for the degradation of RhB and sterilization of E. coli and (h) the proposed photocatalytic mechanism. Reproduced with permission[122]. Copyright 2022, Wiley-VCH

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二维共价有机框架材料的可控合成及其光催化应用研究进展

Controllable Synthesis and Photocatalytic Applications of Two-dimensional Covalent Organic Frameworks

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