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Linker length-dependent hydrogen peroxide photosynthesis performance over crystalline covalent organic frameworks
CrystEngComm ( IF 2.6 ) Pub Date : 2023-07-07 , DOI: 10.1039/d3ce00607g Tao Yang 1 , Yingchu Wang 1 , Yue Chen 1 , Xueqing Peng 1 , Hengqiang Zhang 2 , Aiguo Kong 1
CrystEngComm ( IF 2.6 ) Pub Date : 2023-07-07 , DOI: 10.1039/d3ce00607g Tao Yang 1 , Yingchu Wang 1 , Yue Chen 1 , Xueqing Peng 1 , Hengqiang Zhang 2 , Aiguo Kong 1
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Molecular engineering-tuned covalent organic frameworks (COFs) have been demonstrated as promising photocatalysts for photocatalytic hydrogen peroxide (H2O2) production by a two-electron oxygen reduction in water. Herein, a simple strategy by altering the linker length of the building units is developed to harvest efficient COF catalysts for H2O2 photosynthesis. Three imine-linked COFs with similar structures but varied amine linker lengths were prepared by the amine aldehyde condensation reactions. It was found that the resultant COF with a longer linker exhibited a higher H2O2 generation rate. The highest H2O2 production rate of the prepared COFs with the longest amine linker reached 1164 μmol h−1 gcat−1 in O2-presaturated pure water, together with better stability. The rising photocatalytic performance of COFs with longer linkers could be attributed to the tuning of their molecular structures and morphologies, including a more negative conductor band, higher specific surface area, and separation efficiency of photogenerated carriers. This study provides a simple strategy by facially varying linker lengths for gaining COF-based photocatalysts.
中文翻译：
结晶共价有机框架上连接子长度依赖性过氧化氢光合作用性能
分子工程调整的共价有机骨架（COF）已被证明是一种有前途的光催化剂，可通过水中的双电子氧还原来光催化过氧化氢（H 2 O 2 ）生产。在此，开发了一种通过改变构建单元的连接体长度的简单策略来收获用于H 2 O 2光合作用的高效COF催化剂。通过胺醛缩合反应制备了三种结构相似但胺连接体长度不同的亚胺连接的COF。发现具有较长连接体的所得COF表现出较高的H 2 O 2生成率。H 2 O 2最高所制备的具有最长胺连接体的COF在O 2预饱和纯水中的产率达到1164 μmol h -1 g cat -1 ，并且稳定性较好。具有较长连接体的COF光催化性能的提高可归因于其分子结构和形态的调整，包括更负的导体带、更高的比表面积和光生载流子的分离效率。这项研究提供了一种简单的策略，通过改变接头长度来获得基于 COF 的光催化剂。
更新日期：2023-07-07
中文翻译：
结晶共价有机框架上连接子长度依赖性过氧化氢光合作用性能
分子工程调整的共价有机骨架（COF）已被证明是一种有前途的光催化剂，可通过水中的双电子氧还原来光催化过氧化氢（H 2 O 2 ）生产。在此，开发了一种通过改变构建单元的连接体长度的简单策略来收获用于H 2 O 2光合作用的高效COF催化剂。通过胺醛缩合反应制备了三种结构相似但胺连接体长度不同的亚胺连接的COF。发现具有较长连接体的所得COF表现出较高的H 2 O 2生成率。H 2 O 2最高所制备的具有最长胺连接体的COF在O 2预饱和纯水中的产率达到1164 μmol h -1 g cat -1 ，并且稳定性较好。具有较长连接体的COF光催化性能的提高可归因于其分子结构和形态的调整，包括更负的导体带、更高的比表面积和光生载流子的分离效率。这项研究提供了一种简单的策略，通过改变接头长度来获得基于 COF 的光催化剂。
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