State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, 350108, P. R. China.
College of Chemical Engineering, Fuzhou University, Fuzhou, 350108, P. R. China.
Angew Chem Int Ed Engl. 2021 Jan 18;60(3):1235-1243. doi: 10.1002/anie.202009267. Epub 2020 Nov 13.
The design and synthesis of two semiconducting bis (4-ethynyl-bridging 1, 8-naphthalimide) bolaamphiphiles (BENI-COO and BENI-NH ) to fabricate supramolecular metal-insulator-semiconductor (MIS) nanostructures for biomimetic hydrogen evolution under visible light irradiation is presented. A H evolution rate of ca. 3.12 mmol g ⋅h and an apparent quantum efficiency (AQE) of ca. 1.63 % at 400 nm were achieved over the BENI-COO -NH -Ni MIS photosystem prepared by electrostatic self-assembly of BENI-COO with the opposite-charged DuBois-Ni catalysts. The hot electrons of photoexcited BENI-COO nanofibers were tunneled to the molecular Ni collectors across a salt bridge and an alkyl region of 2.2-2.5 nm length at a rate of 6.10×10 s , which is five times larger than the BENI-NH nanoribbons (1.17×10 s ). The electric field benefited significantly the electron tunneling dynamics and compensated the charge-separated states insufficient in the BENI-COO nanofibers.
设计并合成了两种半导体双（4-乙炔基-桥连 1,8-萘二甲酰亚胺）双（酰胺） bolaamphiphiles（BENI-COO 和 BENI-NH），以在可见光照射下仿生制氢来制备超分子金属-绝缘体-半导体（MIS）纳米结构。通过静电自组装将带相反电荷的 DuBois-Ni 催化剂与 BENI-COO 组装，制备了 BENI-COO-NH-Ni MIS 光系统，在该光系统上实现了约 3.12mmol·g ⋅h 的 H 2 演化速率和约 1.63%的表观量子效率（AQE）在 400nm 处。光激发的 BENI-COO 纳米纤维中的热电子通过盐桥和长度为 2.2-2.5nm 的烷基区域以 6.10×10 s的速率隧穿到分子 Ni 收集器，这比 BENI-NH 纳米带（1.17×10 s）快五倍。电场显著促进了电子隧穿动力学，并补偿了 BENI-COO 纳米纤维中电荷分离状态的不足。
