Surface-modified, dye-sensitized niobate nanosheets enabling an efficient solar-driven Z-scheme for overall water splitting.

Nishioka, Shunta; Hojo, Koya; Xiao, Langqiu; Gao, Tianyue; Miseki, Yugo; Yasuda, Shuhei; Yokoi, Toshiyuki; Sayama, Kazuhiro et al. · Sci Adv · 2022

basic_science · Level V

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Abstract

While dye-sensitized metal oxides are good candidates as H<sub>2</sub> evolution photocatalysts for solar-driven Z-scheme water splitting, their solar-to-hydrogen (STH) energy conversion efficiencies remain low because of uncontrolled charge recombination reactions. Here, we show that modification of Ru dye-sensitized, Pt-intercalated HCa<sub>2</sub>Nb<sub>3</sub>O<sub>10</sub> nanosheets (<b>Ru</b>/Pt/HCa<sub>2</sub>Nb<sub>3</sub>O<sub>10</sub>) with both amorphous Al<sub>2</sub>O<sub>3</sub> and poly(styrenesulfonate) (PSS) improves the STH efficiency of Z-scheme overall water splitting by a factor of ~100, when the nanosheets are used in combination with a WO<sub>3</sub>-based O<sub>2</sub> evolution photocatalyst and an I<sub>3</sub><sup>-</sup>/I<sup>-</sup> redox mediator, relative to an analogous system that uses unmodified <b>Ru</b>/Pt/HCa<sub>2</sub>Nb<sub>3</sub>O<sub>10</sub>. By using the optimized photocatalyst, PSS/<b>Ru</b>/Al<sub>2</sub>O<sub>3</sub>/Pt/HCa<sub>2</sub>Nb<sub>3</sub>O<sub>10</sub>, a maximum STH of 0.12% and an apparent quantum yield of 4.1% at 420 nm were obtained, by far the highest among dye-sensitized water splitting systems and comparable to conventional semiconductor-based suspended particulate photocatalyst systems.