Microenvironment regulation of Ru(bda)L2 catalyst incorporated in metal-organic framework for effective photo-driven water oxidation

doi:10.1016/S1872-2067(23)64411-0

Abstract

Abstract:

A Ru(bda)L₂ molecular catalyst (H₂bda = 2,2′-bipyridine-6,6′-dicarboxylic acid, L represents ligands) was incorporated into a UiO-66 metal-organic framework (MOF) as isolating sites for chemical- and photo-driven water oxidation with the water nucleophilic attack mechanism. An impressive turn-over number of 566 was obtained for photo-driven water oxidation in the phosphate buffer saline, which was nearly 20 times that of the homogenous counterpart in the presence of ruthenium tris(bipyridine) and sodium persulfate. Infrared spectroscopy, X-ray diffraction and X-ray spectroscopy techniques were used to characterize the composition and structure of the catalysts. Kinetic isotope effect (KIE), proton inventory experiment and proton nuclear magnetic resonance were conducted to understand the photo-driven O₂ evolution mechanism. It was observed that the protons participated in O₂ evolution with a normal KIE value, and the uptake of phosphates by UiO-66 matrix improved the affinity towards H₂O via hydrogen bonding. The high O₂ output and the limited photosensitizer oxidative decomposition in PBS suggest that the phosphate acted as a proton mediator to assist proton and/or proton-couple electron transfer through a hydrogen-bonded network of water molecules. This study uses a heterogenous matrix to emulate an enzyme-like microenvironment capable of achieving efficient artificial photosynthesis.

Key words: Ru(bda)L₂ catalyst, Isolating site, Photo-driven water oxidation, Proton mediator, Microenvironment

Jianxin Feng, Xuan Li, Yucheng Luo, Zhifang Su, Maoling Zhong, Baolan Yu, Jianying Shi. Microenvironment regulation of Ru(bda)L₂ catalyst incorporated in metal-organic framework for effective photo-driven water oxidation[J]. Chinese Journal of Catalysis, 2023, 48: 127-136.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(23)64411-0

https://www.cjcatal.com/EN/Y2023/V48/I5/127

Figures/Tables 10

Scheme 1. Illustration showing the incorporation of the Ru(bda)L2 molecular catalyst into the UiO-66 framework.

Fig. 1. HAADF-STEM images and corresponding elemental maps of Ru(bda)L2@UiO-66.

Fig. 2. Three reaction cycles (20 min in every run) driven by low concentration of CeIV (0.1 mol L-1) (a) and single-pass reaction driven by the high concentration of CeIV (0.3 mol L-1) (b) in Ru(bda)L2@UiO-66, Ru(bda)L2 and Ru(bda)L2/UiO-66 catalyzing chemical water oxidation for oxygen evolution in 5 mL of HNO3 aqueous solution (0.1 mol L-1). In the recycling experiment, Ce(NH4)2(NO3)6 solid was directly added into the previous reaction solution to restart the following cycles.

Fig. 3. Photocatalytic oxygen evolution (a) and TON (3 h) (b) comparison for Ru(bda)L2@UiO-66 (5 mg), Ru(bda)L2/UiO-66 (5 mg) and Ru(bda)L2 (equivalent) in PBS solution. TON = n(O2)/n(Ru(bda)L2); (c) Photocatalytic oxygen evolution in PBS solution with different amounts of Ru(bda)L2@UiO-66. (d) The dependence of the initial O2 evolution rate (10 min) on the Ru(bda)L2@UiO-66 concentration. Reaction condition: Ru(bpy)32+ (2.6 mmol L-1), Na2S2O8 (0.12 mol L-1), PBS solution (5 mL), visible light (λ > 420 nm) irradiated at 100 mW cm-2 intensity.

Fig. 4. Oxygen evolution (a) and CO2 evolution (b) against time in photocatalytic water oxidation by Ru(bda)L2@UiO-66 in three different solvents of PBS, BBS and H2O. Reaction conditions: 5 mg of catalyst dispersed in 5 mL of solution, in the presence of Ru(bpy)32+ (2.6 mmol L-1) and Na2S2O8 (0.12 mol L-1), visible light (λ > 420 nm) irradiated at 100 mW cm-2 intensity.

Fig. 5. UV-vis diffuse reflectance spectra of Ru(bda)L2@UiO-66, Ru(bda)L2/UiO-66, UiO-66 and Ru(bda)L2.

Fig. 6. XRD patterns (a,b) and IR spectra (c,d) of pristine catalysts of UiO-66, Ru(bda)L2@UiO-66 and Ru(bda)L2/UiO-66 (a,c), and recycled Ru(bda)L2@UiO-66 catalysts (b,d) after chemical-driven oxidation in Ce4+ solution and photo-driven oxidation in H2O, BBS, and PBS solutions. Terephthalic acid (TA) was added to the recycled samples (b,d) for comparison.

Fig. 7. Ru 3p (a), S 2p (b) and P 2p (c) XPS spectra of pristine Ru(bda)L2@UiO-66 and recycled Ru(bda)L2@UiO-66 after photo-driven oxidation in H2O, BBS, PBS solutions and chemical-driven oxidation in Ce4+ solution.

Fig. 8. (a) The kinetic isotope effect of Ru(bda)L2@UiO-66 (5 mg) in 5 mL of non-deuterated and deuterated PBS solution in the presence of Ru(bpy)32+ (PS, 2.6 mmol L-1) and Na2S2O8 (SA, 0.12 mol L-1), visible light (λ > 420 nm) irradiated at 100 mW cm-2 intensity. (b) The dependence of rate constant ratio (kn/k0) in non-deuterated and deuterated mixed solvent (kn) and in non-deuterated solvent (k0) on D2O molar fractions (n). (c) 1H NMR spectra of water molecules in CDCl3 before and after the addition of Ru(bda)L2@UiO-66 and Ru(bda)L2@UiO-66 (P).

Fig. 9. Illustration of the derived microenvironment (left panel) with the phosphate proton-mediator and preorganized water-networks around Ru(bda)L2 catalysts (middle panel) to promote proton transport and/or electron transfer during photo-driven O2 evolution with the WNA mechanism (right panel).

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Microenvironment regulation of Ru(bda)L₂ catalyst incorporated in metal-organic framework for effective photo-driven water oxidation

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