Gu Meng, Liu Dong, Ding Tao, Liu Xiaokang, Chen Tao, Shen Xinyi, Yao Tao
National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei 230029, P. R. China.
Dalton Trans. 2021 May 14;50(18):6076-6082. doi: 10.1039/d1dt00385b. Epub 2021 Apr 23.
ZrO is one of the most stable metal oxides which is applicable to various chemical reactions in harsh environments. However, the photocatalytic performance of ZrO is relatively poor due to the negligible use of the solar spectrum caused by the wide bandgap (E = 5.3 eV). Here, we report plasmon enhanced Au nanoparticles decorated onto ZrO through a facile tannic acid-reduction method. The Au/ZrO heterojunctions exhibited efficient and stable photocatalytic activity of reducing CO into main CO and CH, at the rates of 25.6 μmol g h and 5.1 μmol g h at most, respectively, approximately 6-fold enhanced compared to the pristine ZrO, under simulated solar light. The reduction rates could also be improved over 10-fold under visible light when Au nanoparticles were loaded onto ZrO. UV-Vis diffuse reflectance spectra confirmed the enhanced visible-light absorption of Au/ZrO caused by localized surface plasmon resonance (LSPR). Electrochemical impedance spectra (EIS) and photocurrent tests proved the more efficient charge transport and electron-hole separation of Au/ZrO heterojunctions. This study demonstrates an effective strategy of LSPR effects to improve the photocatalytic performances of semiconductors.
ZrO是最稳定的金属氧化物之一，适用于恶劣环境中的各种化学反应。然而，由于宽带隙（E = 5.3 eV）导致对太阳光谱的利用率可忽略不计，ZrO的光催化性能相对较差。在此，我们报道了通过一种简便的单宁酸还原法将等离子体增强的金纳米颗粒装饰在ZrO上。Au/ZrO异质结在模拟太阳光下表现出高效且稳定的光催化活性，将CO还原为主要产物CO和CH，速率分别最高可达25.6 μmol g⁻¹ h⁻¹和5.1 μmol g⁻¹ h⁻¹，与原始ZrO相比提高了约6倍。当金纳米颗粒负载在ZrO上时，在可见光下还原速率也可提高10倍以上。紫外-可见漫反射光谱证实了由局域表面等离子体共振（LSPR）引起的Au/ZrO对可见光吸收的增强。电化学阻抗谱（EIS）和光电流测试证明了Au/ZrO异质结具有更高效的电荷传输和电子-空穴分离。这项研究展示了一种利用LSPR效应提高半导体光催化性能的有效策略。
