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一种用于电化学过程中从水中选择性去除铬酸根的杂化金属-有机骨架-还原氧化石墨烯纳米材料。

A Hybrid Metal-Organic Framework-Reduced Graphene Oxide Nanomaterial for Selective Removal of Chromate from Water in an Electrochemical Process.

机构信息

Department of Civil and Environmental Engineering, Rice University, MS 319, 6100 Main Street, Houston 77005, United States.

NSF Nanosystems Engineering Research Center Nanotechnology-Enabled Water Treatment, Rice University, MS 6398, 6100 Main Street, Houston 77005, United States.

出版信息

Environ Sci Technol. 2020 Oct 20;54(20):13322-13332. doi: 10.1021/acs.est.0c04703. Epub 2020 Oct 8.

Abstract

Hexavalent chromium Cr(VI) is a highly toxic groundwater contaminant. In this study, we demonstrate a selective electrochemical process tailored for removal of Cr(VI) using a hybrid MOF@rGO nanomaterial synthesized by growth of a nanocrystalline, mixed ligand octahedral metal-organic framework with cobalt metal centers, [Co(btec)(bipy)(DMF)] (Co-MOF), on the surface of reduced graphene oxide (rGO). The rGO provides the electric conductivity necessary for an electrode, while the Co-MOF endows highly selective adsorption sites for CrO. When used as an anode in the treatment cycles, the MOF@rGO electrode exhibits strong selectivity for adsorption of CrO over competing anions including Cl, SO, and As(III) and achieves charge efficiency (CE) >100% due to the strong physisorption of CrO by Co-MOF; both electro- and physisorption capacities are regenerated with the reversal of the applied voltage, when highly toxic Cr(VI) is reduced to less toxic reduced Cr species and subsequently released into brine. This approach allows easy regeneration of the nonconducting Co-MOF without any chemical addition while simultaneously transforming Cr(VI), inspiring a novel electrochemical method for highly selective degradation of toxic contaminants using tailor-designed electrodes with high affinity adsorbents.

摘要

六价铬 Cr(VI) 是一种剧毒的地下水污染物。在本研究中,我们展示了一种选择性电化学过程,该过程使用混合 MOF@rGO 纳米材料通过在还原氧化石墨烯 (rGO) 表面生长具有钴金属中心的纳米晶、混合配体八面体金属-有机骨架来定制,用于去除 Cr(VI)。rGO 提供了电极所需的导电性,而 Co-MOF 赋予了高度选择性的 CrO 吸附位点。当用作处理循环中的阳极时,MOF@rGO 电极对 CrO 的吸附表现出很强的选择性,超过了包括 Cl、SO 和 As(III) 在内的竞争阴离子,并由于 Co-MOF 对 CrO 的强物理吸附而实现了电荷效率 (CE) >100%;当施加的电压反转时,电和物理吸附容量都得到了再生,此时剧毒的 Cr(VI) 被还原为毒性较低的还原 Cr 物种,并随后释放到盐水中。这种方法允许在不添加任何化学物质的情况下轻松再生不导电的 Co-MOF,同时将 Cr(VI) 转化为具有高亲和力吸附剂的定制电极,从而为高度选择性降解有毒污染物提供了一种新颖的电化学方法。

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