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Facile Strategy for Efficient Charge Separation and High Photoactivity of Mixed-Linker MOFs.
Chen, Teng-Fei; Wang, Lin-Yang; Wang, Yi-Fan; Gao, Hui; He, Jing; Wang, Guo; Meng, Xiang-Fu; Wu, Yi-Shi; Deng, Yu-Heng; Wan, Chong-Qing.
Afiliación
  • Chen TF; Beijing Key Laboratory for Optical Materials and Photonic Devices, Department of Chemistry, Capital Normal University, Beijing 100048, China.
  • Wang LY; Beijing Key Laboratory for Optical Materials and Photonic Devices, Department of Chemistry, Capital Normal University, Beijing 100048, China.
  • Wang YF; Beijing Key Laboratory for Optical Materials and Photonic Devices, Department of Chemistry, Capital Normal University, Beijing 100048, China.
  • Gao H; Beijing Key Laboratory for Optical Materials and Photonic Devices, Department of Chemistry, Capital Normal University, Beijing 100048, China.
  • He J; Beijing Key Laboratory for Optical Materials and Photonic Devices, Department of Chemistry, Capital Normal University, Beijing 100048, China.
  • Wang G; Beijing Key Laboratory for Optical Materials and Photonic Devices, Department of Chemistry, Capital Normal University, Beijing 100048, China.
  • Meng XF; Beijing Key Laboratory for Optical Materials and Photonic Devices, Department of Chemistry, Capital Normal University, Beijing 100048, China.
  • Wu YS; Beijing Key Laboratory for Optical Materials and Photonic Devices, Department of Chemistry, Capital Normal University, Beijing 100048, China.
  • Deng YH; Beijing Key Laboratory for Optical Materials and Photonic Devices, Department of Chemistry, Capital Normal University, Beijing 100048, China.
  • Wan CQ; Beijing Key Laboratory for Optical Materials and Photonic Devices, Department of Chemistry, Capital Normal University, Beijing 100048, China.
ACS Appl Mater Interfaces ; 13(17): 20897-20905, 2021 May 05.
Article en En | MEDLINE | ID: mdl-33896173
Two new sets of UiO-Zr metal-organic framework (MOF) bearing mixed linkers BDC-(SCH3)2 and BDC-(SOCH3)2 that have different band gaps and edges were prepared through post oxidation and direct methods, namely, UiO-66-(SCH3)2-xh (x = 4, 9, 12 oxidation hours) and UiO-66-(SOCH3)x(SCH3)2-x (x = 0, 0.4, 0.6, 2), respectively. These composites with stoichiometric components were fully characterized via proton nuclear magnetic resonance (1H NMR) spectroscopy, powder X-ray diffraction (PXRD), transmission electron microscopy (TEM), Fourier-transform infrared (FT-IR) spectra, Brunauer-Emmett-Teller (BET), photo electrochemical measurements, and femtosecond transient absorption (fs-TA) spectroscopy. The structure, electronic property, and photoresponsive and catalytic ability as the functions of the molar ratio of linkers and the synthetic protocol were first investigated. The mixed-linker UiO-66-(SCH3)2-xh and UiO-66-(SOCH3)x(SCH3)2-x exhibited improved performances as compared to the UiO-66-(SCH3)2 and UiO-66-(SOCH3)2 possessing neat linkers only. Their photo response and catalytic activity varied with different linker ratios. For UiO-66-(SCH3)2-xh, the performance increased with the increasing linker BDC-(SOCH3)2 ratio upon oxidation but reached the highest as the BDC-(SOCH3)2 being of 24.4% in UiO-66-(SCH3)2-9h. In comparison, the best photocurrent (80.74 uA/cm-2) and the highest H2 generation rate (2018.8 µmol g-1 h-1) (λ > 400 nm) in UiO-66-(SCH3)2-9h are about twice those of UiO-66-(SOCH3)0.4(SCH3)1.6 obtained by direct synthesis, although the linker BDC-(SOCH3)2 ratio of those two composites is almost the same (24.4% vs 23.9%). Recorded shorter lifetime and higher charge separation efficiency of the former than those of the latter suggest the postsynthetic protocol as the efficient method for achieving the mixed-liner-MOF-based photocatalyst with high performance. A new type-II tailored homojunction is proposed in these mixed-linker MOFs for their efficient charge separation and improved activity.
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Texto completo: 1 Colección: 01-internacional Banco de datos: MEDLINE Idioma: En Revista: ACS Appl Mater Interfaces Asunto de la revista: BIOTECNOLOGIA / ENGENHARIA BIOMEDICA Año: 2021 Tipo del documento: Article País de afiliación: China

Texto completo: 1 Colección: 01-internacional Banco de datos: MEDLINE Idioma: En Revista: ACS Appl Mater Interfaces Asunto de la revista: BIOTECNOLOGIA / ENGENHARIA BIOMEDICA Año: 2021 Tipo del documento: Article País de afiliación: China