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首页> 外文期刊>Journal of Materials Chemistry, A. Materials for energy and sustainability >Boosting the photoreduction activity of Cr(vi) in metal-organic frameworks by photosensitiser incorporation and framework ionization
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Boosting the photoreduction activity of Cr(vi) in metal-organic frameworks by photosensitiser incorporation and framework ionization

机译：通过光敏仪掺入和框架电离，促进Cr（vi）在金属有机框架中的拍摄活动

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摘要

It is mandatory to decontaminate Cr(vi) species from water streams due to their high toxicity. The photoreduction of hazardous Cr(vi) to nontoxic Cr(iii) is a very promising approach to control Cr(vi) pollution. Although some MOFs and their composites have been employed as photocatalysts to reduce toxic Cr(vi), their catalytic activities are always limited by inefficient visible light absorption and inferior Cr(vi) adsorption performances. Herein, cationic Ru-UiO-dmbpy(1) that is decorated with a high density of cationic charges and also embedded with catalytically competent and visible light harvesting moieties (i.e.Ru(bpy)(3)) was successfully synthesized by a sequential mix-and-match and ionization process. The presence of Ru(bpy)(3)moieties makes Ru-UiO-dmbpy(1) an excellent visible-light harvester, extending the absorption edge from 420 nm for pristine UiO-bpy to about 780 nm for Ru-UiO-bpy/Ru-UiO-dmbpy(1). Driven by ion exchange, Ru-UiO-dmbpy(1) shows a large adsorption rate constant (k(2)) of 1.33 x 10(-2)g mg(-1)min(-1)in the adsorption of Cr2O72-, which is 8.26 times that of pristine UiO-bpy and 6.27 times that of the non-ionization counterpart Ru-UiO-bpy(1) under the same adsorption conditions. The equilibrium Cr(2)O(7)(2-)uptake capacity of Ru-UiO-dmbpy(1) reaches 101.8 mg g(-1), which is about 1.98 and 1.81 times that of UiO-bpy and Ru-UiO-bpy(1), respectively. With an efficient visible light absorption ability and superior Cr(vi) adsorption performance, Ru-UiO-dmbpy(1) shows a reaction rate constant (k(1)) of 0.011 min(-1)in the photoreduction of Cr(vi) without any sacrificial agents under visible light illumination, which is much larger than those of pristine UiO-bpy (0.003 min(-1)) and its non-ionization counterpart Ru-UiO-bpy(1) (0.007 min(-1)) under the same conditions. The result unambiguously demonstrates that the Cr(vi) photoreduction activity could be largely enhanced by photosensitiser introduction and framework ionization. To further evaluate the catalytic performance of Ru-UiO-dmbpy(1), Cr(vi) reduction was also investigated in the presence of various sacrificial agents. Remarkably, a high Cr(vi) photoreduction rate of 6.4 mg(Cr(VI))g(catalyst)(-1)min(-1)was obtained when benzyl alcohol was used as a sacrificial agent, which is a record value among those reported for MOF-based photocatalysts.
机译：由于它们的高毒性，因此必须从水流中净化Cr（VI）物种。危险Cr（VI）对无毒Cr（III）的捕捉是一种非常有希望的控制Cr（VI）污染的方法。尽管已经使用一些MOF和它们的复合材料作为光催化剂来减少毒性Cr（VI），但它们的催化活性始终受到低效的可见光吸收和下克（VI）吸附性能的限制。这里，用阳离子电荷高密度装饰的阳离子Ru-UIO-DMBPY（1）并通过顺序混合成功地合成了催化态度和可见光收集部分（IERU（BPY）（3）） - 和匹配和电离过程。 Ru（BPY）（3）部分的存在使Ru-Uio-DMBPY（1）优异的可见光收割机，将吸收边缘从420nm延伸到ru-uio-bpy的原始UIO-BPY到约780nm / Ru-uio-dmbpy（1）。由离子交换驱动，Ru-UIO-DMBPY（1）显示了CR2O72的吸附中1.33×10（-2）g mg（-1）min（-1）的大吸附速率（K（2）） - ，这是在相同吸附条件下的原始UIO-BPY的8.26倍，并且在相同的吸附条件下的非电离对应ru-uio-bpy（1）的6.27倍。 Ru-UIO-DMBPY（1）的平衡Cr（2）O（2）（2-）摄取能力达到101.8mg g（-1），约为uio-bpy和ru-uio的1.98和1.81倍-bpy（1）分别。具有高效的可见光吸收能力和优异的Cr（VI）吸附性能，Ru-UIO-DMBPY（1）显示CR（VI）的光触耗0.011 min（-1）的反应速率常数（k（1））在可见光照明下没有任何牺牲剂，这远远大于原始UIO-BPY（0.003分钟（-1））及其非电离对应ru-uio-bpe（1）（0.007 min（-1））在相同的条件下。结果明确地证明了Cr（VI）光电通过光电介绍和骨架电离可以大大提高Cr（VI）光电活性。为了进一步评价Ru-UIO-DMBPY（1）的催化性能，还在各种牺牲剂的存在下研究了Cr（VI）。值得注意的是，当苄醇用作牺牲剂时，获得6.4mg（Cr（vi））g（ - 1）min（-1）的高Cr（vi）光电率（cr（vi））（ - 1）min（-1），这是一个记录值那些报道了基于MOF的光催化剂。

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  • 作者

    Zheng He-Qi; He Xing-Hao; Zeng Yong-Nian; Qiu Wei-Hua; Chen Jin; Cao Gao-Juan; Lin Rong-Guang; Lin Zu-Jin; Chen Banglin;

  • 作者单位

    Fujian Agr &

    Forestry Univ Coll Life Sci Dept Appl Chem Fuzhou 350002 Peoples R China;

    Fujian Agr &

    Forestry Univ Coll Life Sci Dept Appl Chem Fuzhou 350002 Peoples R China;

    Fujian Agr &

    Forestry Univ Coll Life Sci Dept Appl Chem Fuzhou 350002 Peoples R China;

    Fujian Agr &

    Forestry Univ Coll Life Sci Dept Appl Chem Fuzhou 350002 Peoples R China;

    Fujian Agr &

    Forestry Univ Coll Life Sci Dept Appl Chem Fuzhou 350002 Peoples R China;

    Fujian Agr &

    Forestry Univ Coll Life Sci Dept Appl Chem Fuzhou 350002 Peoples R China;

    Fujian Agr &

    Forestry Univ Coll Life Sci Dept Appl Chem Fuzhou 350002 Peoples R China;

    Fujian Agr &

    Forestry Univ Coll Life Sci Dept Appl Chem Fuzhou 350002 Peoples R China;

    Univ Texas San Antonio Dept Chem One UTSA Circle San Antonio TX 78249 USA;

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  • 正文语种 eng
  • 中图分类 工程材料学;
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