赵旭才,晋宇恒,郭思嘉,卫来,张丽丽,雷博程

• 1:伊犁师范大学物理科学与技术学院新疆凝聚态相变与微结构实验室
• 2:四川大学物理学院

摘要(Abstract)：

为提高NaTaO_3在可见光区的光谱响应范围，利用第一性原理方法研究了镧系金属(Ce、Pr、Nd、Sm、Eu)掺杂NaTaO_3体系，并对掺杂前后体系的晶体结构、形成能、电子结构以及光学性质进行了计算与分析。结果表明：掺杂体系均发生了晶格畸变，导致体系键布局发生变化，使体系内的正负电荷不再重合，从而在体系内产生了局域电势差，这有效阻碍了体系内部光生电子与空穴的复合，有利于提高NaTaO_3体系的光催化能力。在形成能的计算中发现NaTa_(0.875)Pr_(0.125)O_3的形成能最小，表明该体系最容易形成。掺杂体系的禁带宽度均减小，能级变密集。从态密度图中发现掺杂会加强原子轨道在费米能级的杂化程度，可以有效减少电子-空穴对的复合。从光学性质中发现Ce、Pr、Eu的掺入使NaTaO_3发生了红移，其中NaTa_(0.875)Pr_(0.125)O_3对可见光的响应范围最广，该体系有望成为新型高效的光催化剂材料。

关键词(KeyWords)： NaTaO_3;第一性原理;电子结构;光学性质;光催化

Abstract:

Keywords:

基金项目(Foundation): 伊犁师范大学科研项目(2022YSYB016);伊犁师范大学博士启动基金(2021YSBS009);; 新疆维吾尔自治区高校科技计划项目(XJEDU2021Y044);; 新疆维吾尔自治区重点实验室开放课题(2021D04015)

作者(Author): 赵旭才,晋宇恒,郭思嘉,卫来,张丽丽,雷博程

DOI: 10.14106/j.cnki.1001-2028.2023.1482

参考文献(References)：

• [1] Meng N C,Jin B,Chow C,et al.Recent developments in photocatalytic water treatment technology:A review [J].Water Research,2010,44(10):2997-3027.
• [2] Lorna J M,Wan R W D,Mohammad B K.An overview of photocells and photoreactors for photoelectrochemical water splitting [J].International Journal of Hydrogen Energy,2010,35(11):5233-5244.
• [3] Fujishima A,Honda K.Electrochemical photolysis of water at a semiconductor electrode [J].Nature,1972,238(5358):37-38.
• [4] Sayama K,Arakawa H.Effect of Na2CO3 addition on photocatalytic decomposition of liquid water over various semiconductor catalysis [J].Journal of Photochemistry and Photobiology A:Chemistry,1994,77(2):243-247.
• [5] Huang H,Yang C,Wang M,et al.Enhancement of the optical absorption of carbon group elements doped ZnS in the visible light range [J].Renewable Energy,2018,117:22-27.
• [6] Zhao S,Zhang Y,Wang Y,et al.Ionic liquid-assisted synthesis of Br-modified g-C3N4 semiconductors with high surface area and highly porous structure for photoredox water splitting [J].Journal of Power Sources,2017,370:106-113.
• [7] Castelli I E,Landis D D,Thygesen K S,et al.New cubic perovskites for one- and two-photon water splitting using the computational materials repository [J].Energy & Environmental Science,2012,5(10):9034-9043.
• [8] Zhang M,Liu G,Zhang D,et al.Facile fabrication of NaTaO3 film and its photoelectric properties [J].Journal of Alloys and Compounds,2014,602:322-325.
• [9] Kato H,Kudo A.Water splitting into H2 and O2 on alkali tantalate photocatalysts ATaO3 (A=Li,Na,and K) [J].The Journal of Physical Chemistry B,2001,105(19):4285-4292.
• [10] Kato H,Kudo A.Highly efficient decomposition of pure water into H2 and O2 over NaTaO3 photocatalysts [J].Catalysis Letters,1999,58(2/3):153-155.
• [11] Lee Y,Watanabe T,Takata T,et al.Hydrothermal synthesis of fine NaTaO3 powder as a highly efficient photocatalyst for overall water splitting [J].Bulletin of the Chemical Society of Japan,2007,80(2):423-428.
• [12] Liu D,Wei C,Xue B,et al.Synthesis and photocatalytic activity of N-doped NaTaO3 compounds calcined at low temperature [J].Journal of Hazardous Materials,2010,182(1):50-54.
• [13] Han Y X,Yang C L,Sun Y T,et al.The novel optical properties of CdS caused by concentration of impurity Co [J].Journal of Alloys and Compounds,2014,585:503-509.
• [14] Liu J,Wang L,Liu J,et al.DFT study on electronic structures and optical absorption properties of C,S cation- doped SrTiO3 [J].Open Physics,2009,7(4):762-767.
• [15] Huang H C,Yang C L,Wang M S,et al.Enhanced photocatalytic performance of anatase TiO2 substitutionally co-doped with La and N [J].Solar Energy Materials and Solar Cells,2017,170:233-238.
• [16] Sudrajat H,Hartuti S.Easily separable N-doped ZnO microspheres with high photocatalytic activity under visible light [J].Materials Research Bulletin,2018,102:319-323.
• [17] Akihide I,Hideki K,Akihiko K.The effect of alkaline earth metal ion dopants on photocatalytic water splitting by NaTaO3powder [J].ChemSusChem,2009,2(9):873-877.
• [18] Liu Y L,Yang C L,Wang M S,et al.Te-doped perovskite NaTaO3 as a promising photocatalytic material for hydrogen production from water splitting driven by visible light [J].Materials Research Bulletin,2018,107(12):125-131.
• [19] 马磊，刘晨曦，潘多桥，等.Se和Cd掺杂GaN电子结构与光学性质的第一性原理研究 [J].电子元件与材料，2022,41(2):149-156.
• [20] 赵志峰，王海芳，张天玑，等.La-C共掺ZnO的电子结构和光学性质的第一性原理研究 [J].电子元件与材料，2021,40(2):131-136.
• [21] Liu Y,Wang H,Chen D,et al.Achieving thermally stable and anti-hydrolytic Sr2Si5N8∶Eu2+ phosphor via a nanoscale carbon deposition strategy [J].Ceramics International,2021,47(3):3244-3251.
• [22] Liu Y,Hu J,Ju L,et al.Hydrophobic surface modification toward highly stable K2SiF6∶Mn4+ phosphor for white light-emitting diodes [J].Ceramics International,2020,46(7):8811-8818.
• [23] Yang X,Xing X,Liu Y,et al.A new thermal degradation mechanism of red Sr2Si5N8∶Eu phosphor:From the view of microstructural evolution [J].Optical Materials,2021,121:111506.
• [24] Jana P,Mata Montero C,Pizarro P,et al.Photocatalytic hydrogen production in the water/methanol system using Pt/RE∶NaTaO3 (RE=Y,La,Ce,Yb) catalysts [J].International Journal of Hydrogen Energy,2014,39(10):5283-5290.
• [25] Segall M D,Lindan P J D,Probert M J,et al.First-principles simulation:Ideas,illustrations and the CASTEP code [J].Journal of Physics Condensed Matter,2002,14(11):2717-2744.
• [26] Perdew J P,Burke K,Ernzerhof M.Generalized gradient approximation made simple [J].Physical Review Letters,1996,77(18):3865-3868.
• [27] Chadi D J,Cohen M L.Special points in the brillouin zone [J].Physical Review B,1973,8(12):5747-5753.
• [28] Xu J,Xue D,Yan C.Chemical synthesis of NaTaO3 powder at low-temperature [J].Materials Letters,2005,59(23):2920-2922.
• [29] Bezares I,Del Campo A,Herrasti P,et al.A simple aqueous electrochemical method to synthesize TiO2 nanoparticles [J].Physical Chemistry Chemical Physics,2015,17(43):29319-29326.
• [30] Fang Y,Cheng D,Niu M,et al.Tailoring the electronic and optical properties of rutile TiO2 by (Nb + Sb,C) codoping from DFT + U calculations [J].Chemical Physics Letters,2013,567:34-38.
• [31] Segall M D,Pickard C J,Shah R,et al.Population analysis in plane wave electronic structure calculations [J].Molecular Physics,1996,89(2):571-577.
• [32] 张丽丽，夏桐，刘桂安，等.第一性原理方法研究N-Pr共掺杂ZnO的电子结构和光学性质 [J].物理学报，2019,68(1):245-253.