水稳定性过氧化物纳米管阵列在功能化聚氧化铝的诱导下增强了电荷载流子的传输,可用于高效光还原铀(VI)

IF 5.3 2区 材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY ACS Applied Nano Materials Pub Date : 2024-11-14 DOI:10.1039/d4qi02393e
Yan-Li Yang, Keke Guo, Xue Bai, Maochun Zhu, Siyue Wang, Shuxia Liu
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引用次数: 0

摘要

由于金属卤化物过氧化物(MHPs)具有优异的光电性能,因此构建基于 MHPs 的光催化剂是促进光催化还原铀(VI)的一种前景广阔的策略。然而,MHPs 在水中的不稳定性限制了其实际应用,这仍然是一个重大问题和挑战。在本文中,我们构建了一种由功能化 POMs 封装的基于包晶纳米管阵列的催化剂 (HMTA)3Pb2Br7@STA-PW12,该催化剂在搅拌条件下可在水中保持稳定 10 小时。值得注意的是,考虑到 POMs 的 "电子海绵 "特性,STA-PW12 作为电子传递介质,不仅由于长链 STA 的疏水性提高了催化剂在水中的稳定性,还有助于分离光生载流子,增强电荷从 (HMTA)3Pb2Br7 向 PW12 的转移,从而显著提高光催化活性。(HMTA)3Pb2Br7@STA-PW12 增强的电子载流子迁移率(μe)(1.1 cm2 V-1 s-1)和载流子扩散长度(245 nm)进一步说明了其有效的电荷载流子转移。DFT 计算进一步表明,电子从 (HMTA)3Pb2Br7 向 PW12 过渡,极大地抑制了光生载流子的重组,从而促进了电子转移。最后,合成的催化剂在光催化去除 U(VI)方面表现优异,在模拟阳光下 40 分钟后,U(VI)浓度为 40 ppm 时的去除率为 99.3%。
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Water-stable perovskite nanotube array with enhanced transport of charge carriers induced by functionalized polyoxometalate for highly-efficient photoreduction of uranium(VI)
Due to metal halide perovskites (MHPs) possess excellent optoelectronic performances, constructing MHPs based photocatalysts is a promising strategy to promote photocatalytic uranium(VI) reduction. However, instability of MHPs in water limits their practical application, which is still a major issue and challenge. In this article, we constructed a perovskite nanotube array-based catalyst encapsulated by functionalized POMs, (HMTA)3Pb2Br7@STA-PW12, which can maintain stability in water for 10 hours under stirring conditions. It is noteworthy that, considering the “electron-sponge” property of POMs, STA-PW12 acting as electronic transfer medium not only increases the stability of the catalyst in water due to the hydrophobic long-chain STA, but also contributes to the separation of photogenerated carriers and enhances charges transfer from (HMTA)3Pb2Br7 to PW12, which enhance the photocatalytic activity significantly. The enhanced electrons carrier mobility (μe) (1.1 cm2 V-1 s-1) and carrier diffusion length (245 nm) of (HMTA)3Pb2Br7@STA-PW12 further illustrate its effective charge carriers’ transfer. DFT calculations further indicate the transition of electrons from (HMTA)3Pb2Br7 to PW12, which greatly inhibits the recombination of photogenerated carriers, thereby advancing electron transfer. Finally, the synthesized catalyst exhibits an excellent performance in the photocatalytic removal of U(VI) with removal ratio of 99.3% in the U(VI) concentration of 40 ppm after 40 min under simulated sunlight.
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来源期刊
CiteScore
8.30
自引率
3.40%
发文量
1601
期刊介绍: ACS Applied Nano Materials is an interdisciplinary journal publishing original research covering all aspects of engineering, chemistry, physics and biology relevant to applications of nanomaterials. The journal is devoted to reports of new and original experimental and theoretical research of an applied nature that integrate knowledge in the areas of materials, engineering, physics, bioscience, and chemistry into important applications of nanomaterials.
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