Wang Lei, Guo Fei, Ren Shijie, Gao Rui-Ting, Wu Limin
College of Chemistry and Chemical Engineering, College of Energy Material and Chemistry, Inner Mongolia University, Hohhot, 010021, China.
Department of Materials Science and State Key Laboratory of Molecular Engineering of Polymers, Fudan University, Shanghai, 200433, China.
Angew Chem Int Ed Engl. 2024 Oct 24;63(44):e202411305. doi: 10.1002/anie.202411305. Epub 2024 Sep 12.
The productions of hydrogen peroxide (HO) and hydrogen (H) in a photoelectrochemical (PEC) water splitting cell suffer from an onset potential that limits solar conversion efficiencies. Moreover, the formation of HO through two-electron PEC water oxidation reaction competes with four-electron oxidation evolution reaction. Herein, we developed the surface selenium doped antimony trisulfide photoelectrode with the integrated ruthenium cocatalyst (Ru/Sb(S,Se)) to achieve the low onset potential and high Faraday efficiency (FE) for selective HO production. The photoanode exhibits an outstanding average FE of 85 % in the potential range of 0.4-1.6 V and the HO yield of 1.01 μmol cm min at 1.6 V, especially at low potentials of 0.1-0.55 V with 80.4 % FE. Impressively, an unassisted PEC system that employs light and electrolyte was constructed to simultaneously produce HO and H production on both the Ru/Sb(S,Se) photoanode and the Pt/TiO/SbS photocathode. The integrated system enables the average PEC HO production rate of 0.637 μmol cm min without applying any addition bias. To our knowledge, this is the first demonstration that SbS-based photoelectrodes exhibit HO/H two-side production with a strict key factor of the system, which represents its powerful platform to achieve high efficiency and productivity and the feasibility to facilitate value-added products in neutral conditions.
光电化学（PEC）水分解电池中过氧化氢（HO）和氢气（H）的产生存在起始电位，这限制了太阳能转换效率。此外，通过双电子PEC水氧化反应生成HO与四电子析氧反应相互竞争。在此，我们开发了集成钌助催化剂（Ru/Sb(S,Se)）的表面硒掺杂三硫化锑光电极，以实现选择性生成HO的低起始电位和高法拉第效率（FE）。该光阳极在0.4 - 1.6 V的电位范围内表现出85%的出色平均FE，在1.6 V时HO产率为1.01 μmol cm min，特别是在0.1 - 0.55 V的低电位下FE为80.4%。令人印象深刻的是，构建了一个采用光和电解质的无辅助PEC系统，在Ru/Sb(S,Se)光阳极和Pt/TiO/SbS光阴极上同时产生HO和H。该集成系统在不施加任何额外偏压的情况下，平均PEC HO产生速率为0.637 μmol cm min。据我们所知，这是首次证明基于SbS的光电极在系统的严格关键因素下表现出HO/H双侧产生，这代表了其实现高效率和高生产率的强大平台以及在中性条件下促进增值产品的可行性。
