文献类型：期刊文献

英文题名：Electrolyte-assisted polarization leading to enhanced charge separation and solar-to-hydrogen conversion efficiency of seawater splitting

作者：Li, Yiyang[1];Zhou, Hui[2];Cai, Songhua[3];Prabhakaran, Dharmalingam[4];Niu, Wentian[1];Large, Alexander[5];Held, Georg[5];Taylor, Robert A.[4];Wu, Xin-Ping[2];Tsang, Shik Chi Edman[1]

机构：[1]Univ Oxford, Wolfson Catalysis Ctr, Dept Chem, Oxford, England;[2]East China Univ Sci & Technol, Res Inst Ind Catalysis, Ctr Computat Chem, State Key Lab Green Chem Engn & Ind Catalysis, Shanghai, Peoples R China;[3]Hong Kong Polytech Univ, Dept Appl Phys, Hong Kong, Peoples R China;[4]Univ Oxford, Dept Phys, Clarendon Lab, Oxford, England;[5]Diamond Light Source Ltd, Harwell Sci & Innovat Campus, Didcot, England

年份：2024

卷号：7

期号：1

起止页码：77

外文期刊名：NATURE CATALYSIS

收录：;EI(收录号：20240115328711);WOS:【SCI-EXPANDED(收录号:WOS:001136622700002)】；

基金：Support for this project from the EPSRC in the UK (EP/K040375/1) and the National Natural Science Foundation of China for modelling (22003016) is gratefully acknowledged. S.C. acknowledges support from the General Research Fund (no. 15306021) from the Hong Kong Research Grant Council and the National Natural Science Foundation of China (grant no. 12104381). This work was carried out with the support of the Diamond Light Source (instrument B07/VerSoX, proposal SI29265).

语种：英文

外文关键词：Carrier lifetime - Conversion efficiency - Doping (additives) - Electrolytes - Nitrogen compounds - Polarization - Solar power generation - Titanium dioxide

摘要：Photocatalytic splitting of seawater for hydrogen evolution has attracted a great deal of attention in recent years. However, the poor energy conversion efficiency and stability of photocatalysts in a salty environment have greatly hindered further applications of this technology. Moreover, the effects of electrolytes in seawater remain controversial. Here we present electrolyte-assisted charge polarization over an N-doped TiO2 photocatalyst, which demonstrates the stoichiometric evolution of H2 and O2 from the thermo-assisted photocatalytic splitting of seawater. Our extensive characterizations and computational studies show that ionic species in seawater can selectively adsorb on photo-polarized facets of the opposite charge, which can prolong the charge-carrier lifetime by a factor of five, leading to an overall energy conversion efficiency of 15.9 +/- 0.4% at 270 degrees C. Using a light-concentrated furnace, a steady hydrogen evolution rate of 40 mmol g-1 h-1 is demonstrated, which is of the same order of magnitude as laboratory-scale electrolysers. Photocatalytic overall water splitting on particulate systems represents a possibility for clean energy storage, yet efficiencies for the process are typically low. Here, highly concentrated saltwater is used to polarize photoexcited N-doped TiO2, resulting in enhanced charge separation and a solar-to-hydrogen efficiency approaching 20%.