Buffer anion effects on water oxidation catalysis: The case of Cu(III) complex

doi:10.1016/S1872-2067(20)63729-9

Abstract

Abstract:

Water oxidation is the bottleneck of artificial photosynthesis. Since the first ruthenium-based molecular water oxidation catalyst, the blue dimer, was reported by Meyer’s group in 1982, catalysts based on transition metals have been widely employed to explore the mechanism of water oxidation. Because the oxidation of water requires harsh oxidative conditions, the stability of transition complexes under the relevant catalytic conditions has always been a challenge. In this work, we report the redox properties of a Cu^III complex (TAML-Cu^III) with a redox-active macrocyclic ligand (TAML) and its reactivity toward catalytic water oxidation. TAML-Cu^III displayed a completely different electrochemical behavior from that of the TAML-Co^III complex previously reported by our group. TAML-Cu^III can only be oxidized by one-electron oxidation of the ligand to form TAML^•+-Cu^III and cannot achieve water activation through the ligand-centered proton-coupled electron transfer that takes place in the case of TAML-Co^III. The generated TAML^•+-Cu^III intermediate can undergo further oxidation and ligand hydrolysis with the assistance of borate anions, triggering the formation of a heterogeneous B/CuO_x nanocatalyst. Therefore, the choice of the buffer solution has a significant influence on the electrochemical behavior and stability of molecular water oxidation catalysts.

Key words: Artificial photosynthesis, Water oxidation, Redox-active ligand, Copper catalyst, Buffer anion effect

Qifa Chen, Haoyi Du, Mingtian Zhang. Buffer anion effects on water oxidation catalysis: The case of Cu(III) complex[J]. Chinese Journal of Catalysis, 2021, 42(8): 1338-1344.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(20)63729-9

https://www.cjcatal.com/EN/Y2021/V42/I8/1338

Figures/Tables 7

Fig. 1. Synthesis of TAML-CuIII.

Fig. 2. (a) Crystal structure of TAML-CuIII. All hydrogen atoms and Na+ counter cations are omitted for clarity. Selected bond distances (?) and angles (deg): Cu-N1 1.844(3), Cu-N2 1.816(3), Cu-N3 1.816(3); Cu-N4 1.844(3); N1-Cu-N4 100.4(2), N1-Cu-N2 86.7(3), N2-Cu-N3 85.9(8), N3-Cu-N4 86.7(3). (b) CV plots of TAML-CuIII (0.5 mM) in different solution types: PBS (0.2 M, pH 7), NaHCO3 (0.2 M, pH 8.6), and BB (0.2 M, pH 9). Conditions: WE: BDD (0.07 cm2), RE: SCE, CE: platinum, scan rate: 5 mV/s.

Fig. 3. (a) E vs. pH diagram of TAML-CuIII (0.5 mM) in BB (0.2 M), with pH values ranging from 7.4 to 9.1. CV (b) and DPV (c) plots of TAML-CuIII (0.5 mM) in buffer solutions (0.2 M, pH 9) with different BB:PBS ratios. Electrochemical conditions: WE: BDD (0.07 cm2), RE: SCE, CE: platinum, scan rate: 10 mV/s. (d) Plot of first oxidation peak currents at ~1.32 V and second peak currents (icat) at ~1.51 V vs. catalyst concentration ([TAML-CuIII]).

Fig. 4. (a) CPE curve of (blue line) TAML-CuIII (0.5 mM, 3 mL) in BB (0.2 M, pH 9) using ITO as working electrode; the black line represents the CPE curve of the used ITO after 20000 s CPE in BB containing TAML-CuIII, followed by rinsing with deionized water and immediate transfer to the BB without catalyst. Electrochemical conditions: WE: ITO (1 cm2), RE: SCE, CE: platinum, applied potential: 1.39 V vs. NHE. (b) O2 evolution curves during CPE at 1.39 V of bare ITO (black line) and coated ITO (blue line) in BB (0.2 M, pH 9), measured with a O2 detector (calibrated Ocean Optics FOXY probe).

Fig. 5. SEM image (top view) of ITO before (a) and after (b) 10 h of CPE in BB (0.2 M, pH 9) containing TAML-CuIII catalyst (0.5 mM). Electrochemical conditions: WE: ITO (1 cm2), RE: SC, CE: platinum, applied potential: 1.39 V vs. NHE. (c) SEM image (side view) of generated B/CuOx film on ITO electrode. (d) EDX analysis of generated B/CuOx film. XPS profiles of Cu 2p (e) and B 1s (f) levels of generated B/CuOx film.

Fig. 6. CPE curves of coated B/CuOx film on ITO electrode in different types of buffer solutions. (a) borate buffer (red line, 0.2 M, pH 9); (b) NaHCO3 solution (blue line, 0.2 M, pH 9); (c) PBS (black line, 0.2 M, pH 9).

Fig. 7. Proposed decomposition mechanism of TAML-CuIII for electro-catalyzing water oxidation in borate buffer.

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