School of Chemistry and Chemical Engineering, Jiangsu University, Zhenjiang 212013, P. R. China.
School of Materials Science and Engineering, Jiangsu University, Zhenjiang 212013, Jiangsu, PR China.
Inorg Chem. 2023 Feb 6;62(5):2394-2403. doi: 10.1021/acs.inorgchem.2c04208. Epub 2023 Jan 23.
Photoelectrochemical nitrate reduction reaction (PEC NIRR) could convert the harmful pollutant nitrate (NO) to high-value-added ammonia (NH) under mild conditions. However, the catalysts are currently hindered by the low catalytic activity and slow kinetics. Here, we reported a heterostructure composed of CeO and BiVO, and the "frustrated Lewis pairs (FLPs)" concept was introduced for understanding the role of Lewis acids and Lewis bases on PEC NIRR. The electron density difference maps indicated that FLPs were significantly active for the adsorption and activation of NO. Furthermore, carbon (C) improved the carrier transport ability and kinetics, contributing to the NH yield of 21.81 μg h cm. The conversion process of NO to NH was tracked by NO and NO isotopic labeling. Therefore, this study demonstrated the potential of CeO-C/BiVO for efficient PEC NIRR and provided a unique mechanism for the adsorption and activation of NO over FLPs.
光电化学硝酸盐还原反应（PEC NIRR）可以在温和条件下将有害污染物硝酸盐（NO）转化为高附加值的氨（NH）。然而，目前催化剂受到催化活性低和动力学缓慢的限制。在这里，我们报道了一种由 CeO 和 BiVO 组成的异质结构，并引入了“受阻路易斯对（FLPs）”概念来理解路易斯酸和路易斯碱在 PEC NIRR 中的作用。电子密度差图表明，FLPs 对 NO 的吸附和活化具有显著的活性。此外，碳（C）提高了载流子输运能力和动力学，有助于 NH 的产率达到 21.81 μg h cm。通过 NO 和 NO 同位素标记跟踪了 NO 到 NH 的转化过程。因此，本研究证明了 CeO-C/BiVO 用于高效 PEC NIRR 的潜力，并为 FLPs 上 NO 的吸附和活化提供了独特的机制。
