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Viologen-Based Covalent Organic Frameworks toward Metal-Free Highly Efficient Photocatalytic Hydrogen Evolution
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2023-04-05 , DOI: 10.1021/acsami.2c23233 Sinem Altınışık 1, 2 , Gizem Yanalak 3 , İmren Hatay Patır 4 , Sermet Koyuncu 1, 2
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2023-04-05 , DOI: 10.1021/acsami.2c23233 Sinem Altınışık 1, 2 , Gizem Yanalak 3 , İmren Hatay Patır 4 , Sermet Koyuncu 1, 2
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Covalent organic frameworks (COFs) have shown promise in the field of photocatalysts for hydrogen evolution. Many studies have been carried out using various electroactive and photoactive moieties such as triazine, imide, and porphyrin to produce COFs with different geometric structures and units. Electron transfer mediators like viologen and their derivatives can accelerate the transfer of electrons from photosensitizers to active sites. Herein, the combination of a biphenyl-bridged dicarbazole electroactive donor skeleton with a viologen acceptor structure is reported for the photocatalytic hydrogen evolution of novel COF structures with various alkyl linkers {TPCBP X-COF [X = ethyl (E), butyl (B), and hexyl (H)]}. The structures became more flexible and exhibited less crystal behavior as the length of the alkyl chain increased according to scanning and transmission electron microscopy images, X-ray diffraction analyses, and theoretical three-dimensional geometric optimization. In comparison, the H2 evolution rate of the TPCBP B-COF (12.276 mmol g–1) is 2.15 and 2.38 times higher than those of the TPCBP H-COF (5.697 mmol h–1) and TPCBP E-COF (5.165 mmol h–1), respectively, under visible light illumination for 8 h. The TPCBP B-COF structure is one of the best-performing catalysts for the corresponding photocatalytic hydrogen evolution in the literature, producing 1.029 mmol g–1 h–1 with a high apparent quantum efficiency of 79.69% at 470 nm. Our strategy provides new aspects for the design of novel COFs with respect to future metal-free hydrogen evolution by using solar energy conversion.
中文翻译：
基于紫精的共价有机骨架实现无金属高效光催化析氢
共价有机框架 (COF) 在用于析氢的光催化剂领域显示出前景。许多研究已经使用各种电活性和光活性部分（例如三嗪、酰亚胺和卟啉）来生产具有不同几何结构和单元的 COF。电子转移介质如紫精及其衍生物可以加速电子从光敏剂转移到活性位点。在此，报道了联苯桥接二咔唑电活性供体骨架与紫精受体结构的结合，用于光催化析氢具有各种烷基连接基团的新型 COF 结构 {TPCBP X-COF [X = 乙基 (E), 丁基 (B) , 和己基 (H)]}。根据扫描和透射电子显微镜图像、X 射线衍射分析和理论三维几何优化，随着烷基链长度的增加，结构变得更加灵活并且表现出更少的晶体行为。相比之下，HTPCBP B-COF (12.276 mmol g –1 ) 的2演化速率是TPCBP H-COF (5.697 mmol h –1 ) 和TPCBP E-COF (5.165 mmol h –1 )的2.15和2.38倍，分别在可见光照射下8 h。TPCBP B-COF 结构是文献中相应光催化析氢性能最佳的催化剂之一，产生 1.029 mmol g –1 h –1，在 470 nm 处具有 79.69% 的高表观量子效率。我们的策略为新型 COF 的设计提供了新的方面，涉及未来通过使用太阳能转换进行无金属氢析出。
更新日期：2023-04-05
中文翻译：
基于紫精的共价有机骨架实现无金属高效光催化析氢
共价有机框架 (COF) 在用于析氢的光催化剂领域显示出前景。许多研究已经使用各种电活性和光活性部分（例如三嗪、酰亚胺和卟啉）来生产具有不同几何结构和单元的 COF。电子转移介质如紫精及其衍生物可以加速电子从光敏剂转移到活性位点。在此，报道了联苯桥接二咔唑电活性供体骨架与紫精受体结构的结合，用于光催化析氢具有各种烷基连接基团的新型 COF 结构 {TPCBP X-COF [X = 乙基 (E), 丁基 (B) , 和己基 (H)]}。根据扫描和透射电子显微镜图像、X 射线衍射分析和理论三维几何优化，随着烷基链长度的增加，结构变得更加灵活并且表现出更少的晶体行为。相比之下，HTPCBP B-COF (12.276 mmol g –1 ) 的2演化速率是TPCBP H-COF (5.697 mmol h –1 ) 和TPCBP E-COF (5.165 mmol h –1 )的2.15和2.38倍，分别在可见光照射下8 h。TPCBP B-COF 结构是文献中相应光催化析氢性能最佳的催化剂之一，产生 1.029 mmol g –1 h –1，在 470 nm 处具有 79.69% 的高表观量子效率。我们的策略为新型 COF 的设计提供了新的方面，涉及未来通过使用太阳能转换进行无金属氢析出。
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