钛缺陷的未掺杂锐钛矿型 TiO2 具有 p 型导电性、室温铁磁性和卓越的光催化性能,Journal of the American Chemical Society

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钛缺陷的未掺杂锐钛矿型 TiO2 具有 p 型导电性、室温铁磁性和卓越的光催化性能
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2015-02-18 , DOI: 10.1021/ja512047k
Songbo Wang _{1,

2} , Lun Pan _{1,

2} , Jia-Jia Song _{1,

2} , Wenbo Mi ₃ , Ji-Jun Zou _{1,

2} , Li Wang _{1,

2} , Xiangwen Zhang _{1,

2}

Affiliation

缺陷对于化学和物理应用中的金属氧化物至关重要。与经常研究的氧空位相比，n型未掺杂金属氧化物中的工程金属空位仍然是一个巨大的挑战，并且很少报道金属空位对理化性质的影响。在这里，我们使用最重要和研究最广泛的半导体锐钛矿 TiO2，证明金属空位 (VTi) 可以很容易地引入未掺杂的氧化物中，并且 VTi 的存在导致了许多新的理化性质。使用钛酸四丁酯在乙醇-甘油混合物中的溶剂热处理然后热煅烧合成锐钛矿TiO.905O2。电池晶格参数的实验测量和 DFT 计算表明，非化学计量是由 VTi 而非氧间隙的存在引起的。VTi 的存在改变了 TiO2 的电荷密度和价带边缘，并且在室温下在 g = 1.998 处出现了未报告的强 EPR 信号。与普通的 n 型和非铁磁性 TiO2 相反，Ti 缺陷的 TiO2 显示出固有的 p 型导电性，具有高电荷迁移率，室温铁磁性强于 Co 掺杂的 TiO2 纳米晶。此外，Ti 缺陷的 TiO2 在 H2 生成（4.4 倍）和有机物降解（苯酚的 7.0 倍）方面表现出比普通 TiO2 更好的光催化性能，这是由于在体中和半导体/电解质界面上更有效的电荷分离和转移. 有金属缺陷的未掺杂氧化物代表了一种独特的材料；这项工作证明了以简单可靠的方式制造这种材料的可能性，从而为化学和物理设备中的多功能材料提供了新的机会。

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Titanium-Defected Undoped Anatase TiO2with p-Type Conductivity, Room-Temperature Ferromagnetism, and Remarkable Photocatalytic Performance

Defects are critically important for metal oxides in chemical and physical applications. Compared with the often studied oxygen vacancies, engineering metal vacancies in n-type undoped metal oxides is still a great challenge, and the effect of metal vacancies on the physiochemical properties is seldom reported. Here, using anatase TiO2, the most important and widely studied semiconductor, we demonstrate that metal vacancies (VTi) can be introduced in undoped oxides easily, and the presence of VTi results in many novel physiochemical properties. Anatase Ti0.905O2 was synthesized using solvothermal treatment of tetrabutyl titanate in an ethanol-glycerol mixture and then thermal calcination. Experimental measurements and DFT calculations on cell lattice parameters show the unstoichiometry is caused by the presence of VTi rather than oxygen interstitials. The presence of VTi changes the charge density and valence band edge of TiO2, and an unreported strong EPR signal at g = 1.998 presents under room temperature. Contrary to normal n-type and nonferromagnetic TiO2, Ti-defected TiO2 shows inherent p-type conductivity with high charge mobility, and room-temperature ferromagnetism stronger than Co-doped TiO2 nanocrystalline. Moreover, Ti-defected TiO2 shows much better photocatalytic performance than normal TiO2 in H2 generation (4.4-fold) and organics degradation (7.0-fold for phenol), owing to the more efficient charge separation and transfer in bulk and at semiconductor/electrolyte interface. Metal-defected undoped oxides represent a unique material; this work demonstrates the possibility to fabricate such material in easy and reliable way and thus provides new opportunities for multifunctional materials in chemical and physical devices.

更新日期：2015-02-18

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