Upconversion hollow nanospheres CeF3 co-doped with Yb3+and Tm3+for photocatalytic nitrogen fixation

• 作者: Minghui Zhong Zhendong Wang Da Dai Baozhu Yang Shixiang Zuo Chao Yao Fengqin Wu Xiazhang Li
• 来源期刊: 稀土学报（英文版）
• 年，卷（期）: 2022,（4）
• 所属期刊栏目: RARE EARTH CATALYSIS
• 页码范围: 586-594
• 页数: 9页
• 语种: 英文

摘要

Solar driven nitrogen(N2)fixation to synthesize ammonia is a potential alternative for the traditional Haber-Bosch approach to meeting industrial demand,but is largely hampered by the difficulties in the harvesting of solar energy and activating inert N2.In this work,hollow CeF3 nanospheres co-doped with activator Tm3+and sensitizer Yb3+(Yb3+∶Tm3+∶CeF3)were prepared by microwave hydrothermal method.The product was employed as a catalyst for photo-driven N2 fixation by adjusting the molar ratio of Ce3+∶Yb3+∶Tm3+.Results show that the porous hollow structure enhances the light-harvesting by physical scattering and reflection.In addition,heteroatom doping generates abundant fluorine vacancies(Fv)which provide abundant active sites for adsorption and activation of N2.The sample with molar ratio of CeF3∶Yb3+∶Tm3+at 178∶20∶2 demonstrates the highest utilization of solar energy attributed to the strongest upconversion capability of near-infrared(NIR)light to visible and ultraviolet(UV)light,and the NH4+concentration achieves the highest value of 15.06 μmol/(gcat·h)under simulated sunlight while nearly 6.22 μmol/(gcat·h)under NIR light.Current study offers a promising and sustainable strategy for the fixation of atmospheric N2 using full-spectrum solar energy.