摘要
在“碳达峰、碳中和”背景下,太阳能驱动的半导体光催化技术被认为是解决能源危机和环境问题的有效方法之一.开发高效的半导体光催化材料是半导体光催化技术发展的重中之重.在众多半导体光催化材料中,TiO_(2)因其无毒性、光化学稳定性良好和价格低廉等优点,在光催化领域备受关注.然而,单一TiO_(2)较低的光生载流子的分离和转移效率是制约其进一步应用的关键问题.通过负载助催化剂可以提供更多的活性位点、增强光吸收以及提高光生载流子的分离和转移效率,被认为是提高光催化活性的有效策略.本文利用静电自组装策略和光还原法成功地将双助催化剂Ti_(3)C_(2)纳米片和Ag纳米颗粒修饰在分层花状TiO_(2)微球表面,构筑了Ag/Ti_(3)C_(2)/TiO_(2)复合光催化材料,并考察其光催化产氢性能.Zeta电位测试结果表明,带有相反表面电荷的分层花状TiO_(2)微球和Ti_(3)C_(2)纳米片可以通过静电作用构筑稳定的Ti_(3)C_(2)/TiO_(2)复合光催化材料.同时,基于Ti_(3)C_(2)/TiO_(2)复合材料的光催化性能,在光照条件下Ag+可被还原为Ag而被固定在Ti_(3)C_(2)/TiO_(2)复合材料表面.通过X射线粉末衍射、拉曼光谱、扫描电子显微镜和透射电子显微镜等证明成功制备了Ag/Ti_(3)C_(2)/TiO_(2)复合光催化材料.此外,X射线光电子能谱也证明了复合材料中存在光生电子的分离和转移过程.接触角测试结果表明,构筑的Ag/Ti_(3)C_(2)/TiO_(2)复合材料具有较好的亲水性,可以更好地吸附水分子以保证还原反应的进行.紫外-可见漫反射光谱测试结果表明,Ti_(3)C_(2)和Ag助催化剂的引入提高了材料的光吸收能力.荧光光谱、时间分辨荧光光谱、光电流密度和电化学阻抗等测试结果表明,Ag/Ti_(3)C_(2)/TiO_(2)复合材料具有较好的光生载流子分离和转移效率以及更长的光生载流子寿命.另外,线性扫描伏安测试证明了Ag/Ti_(3)C_(2)/
Solar‐powered semiconductor photocatalysis is considered a powerful strategy for addressing environmental pollution and energy crisis.Nevertheless,the separation and transfer abilities of photogenerated photocatalysts remain unsatisfactory.Herein,dual Ti_(3)C_(2)nanosheets/Ag co‐catalysts synergistically decorated hierarchical flower‐like TiO_(2 )microspheres for boosting photocatalytic H_(2) production were fabricated by electrostatic self‐assembly and subsequent photoreduction procedures.The optimal Ag/Ti_(3)C_(2)/TiO_(2 )composite demonstrated an excellent photocatalytic H_(2)‐production rate of 1024.72μmol g^(−1)h^(−1)under simulated solar irradiation,achieving nearly 40,2.3,and 1.8 folds with respect to that obtained on pristine TiO2,optimized Ti_(3)C_(2)/TiO_(2 )composite,and Ag/TiO_(2 )composite,respectively.The considerably improved photocatalytic H_(2)‐production activity is associated with the synergistic effect of the hierarchical flower‐like structure of TiO2,excellent electrical conductivity of Ti_(3)C_(2),and surface plasmon resonance effect of Ag,which enhances the light absorption capacity and promotes the separation and transfer of photogenerated carriers.This study provides insight into the design of high‐efficiency photocatalysts with dual co‐catalysts for solar H_(2) production.
作者
刘德法
孙彬
白硕杰
高婷婷
周国伟
Defa Liu;Bin Sun;Shuojie Bai;Tingting Gao;Guowei Zhou(Key Laboratory of Fine Chemicals in Universities of Shandong,Jinan Engineering Laboratory for Multi‐scale Functional Materials,School of Chemistry and Chemical Engineering,Qilu University of Technology(Shandong Academy of Sciences),Jinan 250353,Shandong,China)
基金
国家自然科学基金(52202102,51972180)
山东省自然科学基金(ZR2019BB030,ZR2021ZD27,ZR2020ME082)
山东省高等学校青年创新团队发展计划(2021KJ056)
烟台先进材料与绿色制造山东省实验室开放基金(AMGM2023F13,AMGM2021F05)
山东省大学生创新创业训练计划(S202210431016)
济南市高校院所创新团队(2018GXRC006)
齐鲁工业大学科教产融合试点工程项目(2022PY062).
关键词
分层花状TiO_(2)微球
双助催化剂
光催化
协同效应
产氢
Hierarchical flower‐like TiO2
microsphere
Dual co‐catalysts
Photocatalysis
Synergistic effect
H_(2) production
