Is platinum-loaded titania the best material for dye-sensitized hydrogen evolution under visible light?

doi:10.1016/S1872-2067(24)60092-6

Abstract

Abstract:

A dye-sensitized photocatalyst combining Pt-loaded TiO₂ and Ru(II) tris-diimine sensitizer (RuP) was constructed and its activity for photochemical hydrogen evolution was compared with that of Pt-intercalated HCa₂Nb₃O₁₀ nanosheets. When the sacrificial donor ethylenediaminetetraacetic acid (EDTA) disodium salt dihydrate was used, RuP/Pt/TiO₂ showed higher activity than RuP/Pt/HCa₂Nb₃O₁₀. In contrast, when NaI (a reversible electron donor) was used, RuP/Pt/TiO₂ showed little activity due to back electron transfer to the electron acceptor (I₃^-), which was generated as the oxidation product of I^-. By modification with anionic polymers (sodium poly(styrenesulfonate) or sodium polymethacrylate) that could inhibit the scavenging of conduction band electrons by I₃^-, the H₂ production activity from aqueous NaI was improved, but it did not exceed that of RuP/Pt/HCa₂Nb₃O₁₀. Transient absorption measurements showed that the rate of semiconductor-to-dye back electron transfer was slower in the case of TiO₂ than HCa₂Nb₃O₁₀, but the electron transfer reaction to I₃^- was much faster. These results indicate that Pt/TiO₂ is useful for reactions with sacrificial reductants (e.g., EDTA), where the back electron transfer reaction to the more reducible product can be neglected. However, more careful design of the catalyst will be necessary when a reversible electron donor is employed.

Key words: Artificial photosynthesis, Solar fuel, Water splitting, Z-scheme

Haruka Yamamoto, Langqiu Xiao, Yugo Miseki, Hiroto Ueki, Megumi Okazaki, Kazuhiro Sayama, Thomas E. Mallouk, Kazuhiko Maeda. Is platinum-loaded titania the best material for dye-sensitized hydrogen evolution under visible light?[J]. Chinese Journal of Catalysis, 2024, 63: 124-132.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(24)60092-6

https://www.cjcatal.com/EN/Y2024/V63/I8/124

Figures/Tables 10

Fig. 1. TEM images of Pt/TiO2 and Al2O3/Pt/TiO2.

Fig. 2. Steady-state emission spectra of RuP-sensitized Pt/TiO2 with various modifications. The samples were suspended in H2O (pH adjusted 4 by aqueous sulfuric acid) saturated with Ar.

Fig. 3. FT-IR spectra of polymer-modified RuP/Pt/TiO2.

Fig. 4. ζ-potentials of polymer-modified RuP/Pt/TiO2 as a function of pH.

Fig. 5. H2 evolution time courses from an aqueous NaI solution (5 mmo l L?1) over modified RuP/Pt/TiO2 (λ > 400 nm).

Fig. 6. Time courses of Z-scheme overall water splitting (λ > 400 nm) from an aqueous NaI solution over polymer modified RuP/Pt/TiO2 (a) and RuP/Al2O3/Pt/TiO2 (b).

Fig. 7. Normalized Δabsorbance at 475 nm of RuP-sensitized photocatalysts as a function of time. Experimental conditions: water (adjusted to pH 4.0 by addition of sulfuric aid); excitation wavelength, 532 nm.

Table 1 Back electron transfer kinetics of RuP adsorbed on Pt/TiO2 or Pt(in)/HCa2Nb3O10 in water a.

Catalyst	Absorption decay lifetimes / µs (%)
Catalyst	τ₁	τ₂	τ₃	τ₄
RuP/Pt/TiO₂	0.1	3.5 ± 0.4	50 ± 7	500 ± 60
RuP/Pt/TiO₂		(30)	(35)	(35)
RuP/Pt(in)/HCa₂Nb₃O₁₀	0.09	2.0 ± 0.5	20 ± 4	250 ± 50
RuP/Pt(in)/HCa₂Nb₃O₁₀		(27)	(29)	(44)

Fig. 8. Normalized Δabsorbance at 380 nm of RuP-sensitized photocatalysts as a function of time. Measurement conditions: aqueous 100 mmol L?1 NaI solution (adjusted to pH 4.0 by addition of sulfuric acid); excitation wavelength, 532 nm.

Table 2 Absorption decay lifetimes of I3-.

Catalyst	Absorption decay lifetimes / µs (%)
Catalyst	τ₁	τ₂	τ₃
RuP/Pt/TiO₂	0.2 ± 0.02	150 ± 30	900 ± 200
RuP/Pt/TiO₂	(48)	(31)	(21)
RuP/Pt(in)/HCa₂Nb₃O₁₀	0.5 ± 0.05	400 ± 140	3000 ± 1000
RuP/Pt(in)/HCa₂Nb₃O₁₀	(55)	(17)	(28)
PMA/RuP/Pt/TiO₂	5.0 ± 0.9	1500 ± 200	-
PMA/RuP/Pt/TiO₂	(43)	(57)	-
PSS/RuP/Pt/TiO₂	3.0 ± 0.3	500 ± 100	2000 ± 400
PSS/RuP/Pt/TiO₂	(52)	(24)	(24)

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