南京理工大学张侃团队报道了Cs掺杂促进太阳能水氧化CuWO₄光阳极的体电荷输运。相关研究成果于2023年12月15日发表在国际顶尖学术期刊《结构化学》。

钨酸铜（CuWO₄）具有合适的能带位置和较宽的光吸收范围，是一种很有前途的光电化学（PEC）水分解光阳极。然而，Cu固有的未填充的三维原子轨道充当天然的电子-空穴复合位点，显著限制了CuWO₄的PEC性能。

该文将具有完整原子轨道的Cs原子掺杂到CuWO₄中，以获得更好的体电荷分离能力。因此，在AM 1.5G照明下，Cs@CuWO₄与CuWO₄相比在1.23V vs RHE下的光电流密度从0.57增加到0.99 mA cm^-2，并且体积电荷转移效率从13.5%增加到19.3%。此外，态密度（DOS）计算进一步证明，Cs原子的引入有效地抑制了Cu3d轨道在费米能级的贡献。

该项工作为CuWO₄作为下一代PEC光阳极材料的发展提供了宝贵的参考。

附：英文原文

Title: Boosting bulk charge transport of CuWO4 photoanodes via Cs doping for solar water oxidation

Author: anonymous

Issue&Volume: 2023-12-15

Abstract: Copper tungstate (CuWO4) is a promising photoanode for photoelectrochemical (PEC) water splitting due to its appropriate energy band position and broad light absorption range. However, the inherent unfilled 3d atomic orbital of Cu acts as a natural electron-hole recombination site, significantly constraining the PEC performance of CuWO4. Herein, Cs atoms with complete atomic orbitals are doped into CuWO4 in order to obtain better bulk charge separation capability. As a result, the photocurrent of Cs@CuWO4 increased from 0.57 to 0.99 mA cm-2 compared to CuWO4 at 1.23 V vs. reversible hydrogen electrode (RHE) under AM 1.5G illumination, as well as the bulk charge transfer efficiencies rising from 13.5% to 19.3%. In addition, density of states (DOS) calculations further prove that the introduction of Cs atoms effectively suppresses the contribution of Cu 3d orbitals at the Fermi level. This work offers a valuable reference for the advancement of CuWO4 as the next-generation PEC photoanode material.

DOI: 10.1016/j.cjsc.2023.100207

Source: http://cjsc.ac.cn/cms/issues/542