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Fabrication of NanoCOF/Polyoxometallate Composites for Photocatalytic NADH Regeneration via Cascade Electron Relay
Solar RRL ( IF 6.0 ) Pub Date : 2020-12-01 , DOI: 10.1002/solr.202000641 He Li 1 , Jiali Liu 1, 2 , Maodi Wang 1, 2 , Xiaomin Ren 1, 2 , Chunzhi Li 1, 2 , Yiqi Ren 1, 2 , Qihua Yang 1
Solar RRL ( IF 6.0 ) Pub Date : 2020-12-01 , DOI: 10.1002/solr.202000641 He Li 1 , Jiali Liu 1, 2 , Maodi Wang 1, 2 , Xiaomin Ren 1, 2 , Chunzhi Li 1, 2 , Yiqi Ren 1, 2 , Qihua Yang 1
Affiliation
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Covalent organic frameworks (COFs) as novel visible‐light responsive photocatalysts confront the problem of low photocatalytic activity due to the difficulty in separation of photogenerated charge carriers. Herein, the fabrication of nanoCOF/polyoxometallate (POM) composites to enhance the charge separation efficiency via cascade electron relay is reported. It is found that the photogenerated electrons in the π orbitals of nanoCOF quickly transfer to POM (electron mediator and electron storage tank) to form heteropolyblue (HPB), which is verified by electron paramagnetic resonance and ultraviolet (UV)–vis characterizations. In photocatalytic NADH regeneration, nanoCOF/POM composites afford NADH yield of 97% with turnover frequency of 72.0 mmolgCOF−1 h−1, which is the highest ever reported for COFs and is more than 360‐fold that of COF counterpart. The high photocatalytic activity of nanoCOF/POM composites is mainly attributed to the high concentration of charge carriers and long lifetime of photogenerated charges on the basis of transient absorption spectroscopy, which are achieved by the cascade relay of photogenerated electrons. The primary results suggest that the integration of COFs with electron mediators is an efficient approach to increase the photocatalytic activity via promoted charge separation efficiency.
中文翻译：
级联电子继电器制备用于光催化NADH再生的NanoCOF /多金属氧酸盐复合材料
由于难以分离光生电荷载流子，因此作为新型可见光响应型光催化剂的共价有机骨架（COF）面临着光催化活性低的问题。本文中，报道了通过级联电子继电器制备纳米COF /多金属氧酸盐（POM）复合材料以提高电荷分离效率的方法。结果发现，nanoCOFπ轨道中的光生电子迅速转移到POM（电子介体和电子储罐）中，形成杂多蓝（HPB），这已通过电子顺磁共振和紫外（UV）表征进行了验证。在光催化NADH再生中，纳米COF / POM复合材料的NADH收率为97％，周转频率为72.0 mmolg COF -1 h -1，这是有史以来最高的COF报告数，是COF同类报告的360倍以上。纳米COF / POM复合材料的高光催化活性主要归因于瞬态吸收光谱学上的电荷载流子浓度高和光生电荷的寿命长，这是通过光生电子的级联传递实现的。主要结果表明，COF与电子介体的整合是一种通过提高电荷分离效率来提高光催化活性的有效方法。
更新日期：2021-01-07
中文翻译：
级联电子继电器制备用于光催化NADH再生的NanoCOF /多金属氧酸盐复合材料
由于难以分离光生电荷载流子，因此作为新型可见光响应型光催化剂的共价有机骨架（COF）面临着光催化活性低的问题。本文中，报道了通过级联电子继电器制备纳米COF /多金属氧酸盐（POM）复合材料以提高电荷分离效率的方法。结果发现，nanoCOFπ轨道中的光生电子迅速转移到POM（电子介体和电子储罐）中，形成杂多蓝（HPB），这已通过电子顺磁共振和紫外（UV）表征进行了验证。在光催化NADH再生中，纳米COF / POM复合材料的NADH收率为97％，周转频率为72.0 mmolg COF -1 h -1，这是有史以来最高的COF报告数，是COF同类报告的360倍以上。纳米COF / POM复合材料的高光催化活性主要归因于瞬态吸收光谱学上的电荷载流子浓度高和光生电荷的寿命长，这是通过光生电子的级联传递实现的。主要结果表明，COF与电子介体的整合是一种通过提高电荷分离效率来提高光催化活性的有效方法。
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