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Hydrolytically stable citrate capped Fe3O4@UiO-66-NH2 MOF: A hetero-structure composite with enhanced activity towards Cr (VI) adsorption and photocatalytic H2 evolution
Journal of Colloid and Interface Science ( IF 9.4 ) Pub Date : 2021-08-09 , DOI: 10.1016/j.jcis.2021.08.031
Suraj Prakash Tripathy 1 , Satyabrata Subudhi 1 , Snehaprava Das 1 , Malay Kumar Ghosh 2 , Mira Das 3 , Raghunath Acharya 4 , Rashmi Acharya 1 , Kulamani Parida 1
Affiliation  

Design and facile fabrication of a magnetically separable hetero-structure photocatalyst as well as an adsorbent having dual green benefits towards energy conversion and pollutant remediation are quite indispensable in the current scenario. In this regard, a composite of citrate capped Fe3O4 and UiO-66-NH2 has been designed to remediate Cr (VI) by adsorption and harvest photons from visible light for clean energy (H2) conversion. The material was prepared by the union of citrate capped Fe3O4 (CCM) and versatile aqueous stable Zr-based MOF (UiO-66-NH2) through in-situ solvothermal method. The composite of CCM with MOF (MU-2) was studied through sophisticated analysis techniques; PXRD, FT-IR, BET, UV–Visible DRS, PL, TG, HRTEM and XPS etc. to reveal the inherent characteristics of the material. BET surface analysis revealed high specific surface area (572.13 m2 g−1) of MU-2 in comparison to its pristine MOF. Furthermore, the dual function composite MU-2′s VSM studies showed that its magnetic saturation is 3.07 emu g−1 that is suitable for magnetic separation after desired reaction from aqueous media. The Cr (VI) sorption studies revealed that the composite adsorbent (MU-2) showed maximum monolayer adsorption capacity (Qm) of 743 mg g−1 which followed pseudo second order kinetics. Moreover, the sorption thermodynamics revealed that the process was spontaneous and endothermic in nature. In addition to it, the synthesized composite material displayed enhanced activity towards photocatalytic H2 evolution with a maximum evolution rate of 417 µmole h−1 with an apparent conversion efficiency (ACE) of 3.12 %. Typically, MU-2 displays high adsorptions of Cr (VI) as well as some extent of Cr (VI) reduction owning to its populous active sites and free carboxylate groups respectively. Moreover, the synergistic effect of CCM and UNH in the composite resulted in Z scheme mediated charge transfer mechanism that showed enhanced H2 photo-evolution rates. Hence, MU-2 can be readily utilized as magnetically retrievable dual function composite for Cr (VI) adsorption and photocatalytic H2 evolution.



中文翻译:

水解稳定的柠檬酸盐封端 Fe3O4@UiO-66-NH2 MOF:一种对 Cr (VI) 吸附和光催化析氢具有增强活性的异质结构复合材料

在当前情况下,设计和轻松制造可磁分离的异质结构光催化剂以及对能量转换和污染物修复具有双重绿色效益的吸附剂是必不可少的。在这方面,柠檬酸盐封端的 Fe 3 O 4和 UiO-66-NH 2的复合材料已被设计为通过吸附和收集可见光中的光子来修复 Cr (VI) 以实现清洁能源 (H 2 ) 转化。该材料由柠檬酸盐封端的 Fe 3 O 4 (CCM) 和多功能水性稳定 Zr 基 MOF (UiO-66-NH 2) 通过原位溶剂热法。通过复杂的分析技术研究了 CCM 与 MOF (MU-2) 的复合材料;PXRD、FT-IR、BET、UV-Visible DRS、PL、TG、HRTEM 和 XPS 等,以揭示材料的固有特性。BET 表面分析显示与其原始 MOF 相比,MU-2具有高比表面积 (572.13 m 2 g -1 )。此外,双功能复合材料MU-2的VSM研究表明,其磁饱和度为3.07 emu g -1,适合在与水介质发生所需反应后进行磁分离。Cr (VI) 吸附研究表明,复合吸附剂 (MU-2) 的最大单层吸附容量 (Q m ) 为 743 mg g -1遵循伪二级动力学。此外,吸附热力学表明该过程本质上是自发和吸热的。除了它,将合成的复合材料显示的增强的活性朝光催化ħ 2演变为417微摩尔小时的最大释放速率-1用的3.12%的表观转换效率(ACE)。通常,MU-2 表现出对 Cr (VI) 的高吸附以及一定程度的 Cr (VI) 还原,这分别归功于其大量的活性位点和游离羧酸盐基团。此外,复合材料中 CCM 和 UNH 的协同作用导致 Z 方案介导的电荷转移机制,显示出增强的 H 2光进化率。因此,MU-2 可以很容易地用作磁性可回收的双功能复合材料,用于 Cr (VI) 吸附和光催化 H 2析出。

更新日期:2021-08-13
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