Upconversion hollow nanospheres CeF_(3) co-doped with Yb^(3+) and Tm^(3+) for photocatalytic nitrogen fixation

作     者：Minghui Zhong Zhendong Wang Da Dai Baozhu Yang Shixiang Zuo Chao Yao Fengqin Wu Xiazhang Li Minghui Zhong;Zhendong Wang;Da Dai;Baozhu Yang;Shixiang Zuo;Chao Yao;Fengqin Wu;Xiazhang Li

作者机构：Advanced Catalysis and Green Manufacturing Collaborative Innovation CenterJiangsu Key Laboratory of Advanced Catalytic Materials and TechnologyChangzhou UniversityChangzhou 213164China W.M.Keck Center for Advanced Microscopy and MicroanalysisUniversity of DelawareNewarkDE19716USA 

出 版 物：《Journal of Rare Earths》 (稀土学报（英文版）)

年 卷 期：2022年第40卷第4期

页      面：586-594,I0003页

核心收录：

学科分类：081702[工学-化学工艺] 081704[工学-应用化学] 081705[工学-工业催化] 07[理学] 070304[理学-物理化学(含∶化学物理)] 08[工学] 0817[工学-化学工程与技术] 0703[理学-化学] 

基　　金：Project supported by the National Natural Science Foundation of China (51674043 51702026) 

主　　题：Rare earth CeF_(3) Hollow structure Upconversion Fluorine vacancy Photocatalytic nitrogen fixation 

摘      要：Solar driven nitrogen(N_(2))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 N_(2).In this work,hollow CeF_(3) nanospheres co-doped with activator Tm^(3+)and sensitizer Yb^(3+)(Yb^(3+):Tm^(3+):CeF_(3))were prepared by microwave hydrothermal *** product was employed as a catalyst for photo-driven N_(2) fixation by adjusting the molar ratio of Ce^(3+):Yb^(3+):Tm^(3+).Results show that the porous hollow structure enhances the light-harvesting by physical scattering and *** addition,heteroatom doping generates abundant fluorine vacancies(F_(V))which provide abundant active sites for adsorption and activation of N_(2).The sample with molar ratio of CeF_(3):Yb^(3+):Tm^(3+)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 NH_(4)+concentration achieves the highest value of 15.06μmol/(gcat∙h)under simulated sunlight while nearly 6.22μmol/(gcat∙h)under NIR *** study offers a promising and sustainable strategy for the fixation of atmospheric N_(2) using full-spectrum solar energy.