Deng Guoqiang, Kang Xiangdong, Yang Yongqiang, Wang Lianzhou, Liu Gang
Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, 72 Wenhua Road, Shenyang 110016, China; School of Materials Science and Engineering, University of Science and Technology of China, 72 Wenhua Road, Shenyang 110016, China.
Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, 72 Wenhua Road, Shenyang 110016, China.
J Colloid Interface Sci. 2023 Nov;649:140-147. doi: 10.1016/j.jcis.2023.06.046. Epub 2023 Jun 10.
The limited visible-light-responsive photoactivities of most doped wide-bandgap photocatalysts with widened absorption range have long been the obstacles for the efficient conversion of solar energy to chemical energy by photocatalysis. The weak transport ability of visible-light-induced low-energy charge carriers, and numerous recombination centers arising from the energy-band modifiers along the transport path are two major factors responsible for such a mismatch. A potential solution is to shorten the transport path of photo-induced charges in well-modulated light absorbers with low-dimensional structure and the spatially concentrated dopants underneath their surfaces. As a proof of concept, skin B/N-doped red anatase TiO {001} nanoflakes with the absorption edge up to 675 nm were synthesized in this study. Experimental results revealed that boron dopants in the TiO nanoflakes from the hydrolysis of nanosized TiB played a crucial role in controlling nitrogen doping in the surface layer of the nanoflakes. As visible light excitation occurs at the surface layer, the photons can be sufficiently absorbed by the formed energy levels at the surface layers, and the photogenerated charge carriers can effectively migrate to the surface, thus leading to efficient visible-light-responsive photocatalytic oxygen evolution activity from water oxidation.
大多数具有拓宽吸收范围的掺杂宽带隙光催化剂的可见光响应光活性有限,长期以来一直是通过光催化将太阳能高效转化为化学能的障碍。可见光诱导的低能电荷载流子传输能力较弱,以及沿传输路径由能带改性剂产生的大量复合中心,是造成这种不匹配的两个主要因素。一个潜在的解决方案是在具有低维结构且表面下方有空间集中掺杂剂的良好调制光吸收体中缩短光生电荷的传输路径。作为概念验证,本研究合成了吸收边缘高达675nm的皮肤状B/N掺杂红色锐钛矿TiO{001}纳米片。实验结果表明,纳米尺寸的TiB水解产生的TiO纳米片中的硼掺杂剂在控制纳米片表面层的氮掺杂方面起着关键作用。由于可见光激发发生在表面层,光子可以被表面层形成的能级充分吸收,光生电荷载流子可以有效地迁移到表面,从而导致从水氧化中产生高效的可见光响应光催化析氧活性。