School of Chemistry and Chemical Engineering, Jiangxi University of Science and Technology, Ganzhou 341000, China.
School of Chemical Engineering, Guangdong University of Petrochemical Technology, Maoming 525000, China.
Molecules. 2023 Mar 7;28(6):2435. doi: 10.3390/molecules28062435.
The green and clean sunlight-driven catalytic conversion of CO into high-value-added chemicals can simultaneously solve the greenhouse effect and energy problems. The controllable preparation of semiconductor catalyst materials and the study of refined structures are of great significance for the in-depth understanding of solar-energy-conversion technology. In this study, we prepared nitrogen-doped NiO semiconductors using a one-pot molten-salt method. The research shows that the molten-salt system made NiO change from p-type to n-type. In addition, nitrogen doping enhanced the adsorption of CO on NiO and increased the separation of photogenerated carriers on the NiO. It synergistically optimized the CO-reduction system and achieved highly active and selective CO photoreduction. The CO yield on the optimal nitrogen-doped photocatalyst was 235 μmol·g·h (selectivity 98%), which was 16.8 times that of the p-type NiO and 2.4 times that of the n-type NiO. This can be attributed to the fact that the nitrogen doping enhanced the oxygen vacancies of the NiOs and their ability to adsorb and activate CO molecules. Photoelectrochemical characterization also confirmed that the nitrogen-doped NiO had excellent electron -transfer and separation properties. This study provides a reference for improving NiO-based semiconductors for photocatalytic CO reduction.
阳光驱动的绿色清洁催化转化 CO 为高附加值化学品，可以同时解决温室效应和能源问题。半导体催化剂材料的可控制备和精细结构的研究，对于深入了解太阳能转化技术具有重要意义。本研究采用一步熔融盐法制备了氮掺杂 NiO 半导体。研究表明，熔融盐体系使 NiO 从 p 型转变为 n 型。此外，氮掺杂增强了 CO 在 NiO 上的吸附，并增加了 NiO 上光生载流子的分离。它协同优化了 CO 还原体系，实现了高效和选择性的 CO 光还原。最佳氮掺杂光催化剂上的 CO 产率为 235 μmol·g·h（选择性 98%），是 p 型 NiO 的 16.8 倍，是 n 型 NiO 的 2.4 倍。这归因于氮掺杂增强了 NiO 的氧空位及其对 CO 分子的吸附和活化能力。光电化学表征也证实了氮掺杂 NiO 具有优异的电子转移和分离性能。本研究为改善基于 NiO 的半导体用于光催化 CO 还原提供了参考。
