In-situ construction of different Lewis acids in hyper-cross-linked polymer as water-resistant adsorbent for efficient Hg0 removal

IF 4.1 3区 医学 Q2 BIOCHEMISTRY & MOLECULAR BIOLOGY
Yifan Xu , Xinyu Wu , Limin Liu , Yueqing Xu , Cheng Chen , Yi Wang , Cheng Zhang , Xiaoshuo Liu , Chengyan Li , Houhu Zhang
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Abstract

Hyper-cross-linked polymers (HCP) are regarded as promising materials for limiting gaseous Hg0 emissions. However, the protracted synthesis period and the complicated post-modification process hinder practical use in gaseous pollution control. Herein, a facile in-situ catalytic method for converting waste plastic into Lewis acid-embedded HCP is proposed to overcome these drawbacks. Various Lewis acids could serve as catalysts for HCP skeleton formation as well as Hg0-affinitive species. The resulting HCP-Metal samples exhibited high demercuration (De-Hg) ability (∼100% in 120 min) and excellent water resistance (10% H2O), greatly surpassing those of state-of-the-art adsorbents. Experiments and theoretical calculations confirmed that Hg0 bonding configurations include Hg0 over Cl-monodentate, Cl-bridged sites and metal-top sites. The closer energy level of electron donor orbital for FeCl3/CuCl2 corresponds to excellent De-Hg performance. This exploration of the use of different Lewis acids in the in-situ catalytic process offers promising applications in environmental remediation and energy storage.

Abstract Image

在超交联聚合物中原位构建不同的路易斯酸作为防水吸附剂,实现高效除汞
超交联聚合物(HCP)被认为是限制气态 Hg0 排放的理想材料。然而,漫长的合成周期和复杂的后改性过程阻碍了其在气态污染控制中的实际应用。本文提出了一种将废塑料转化为路易斯酸嵌入式 HCP 的简便原位催化方法,以克服这些缺点。各种路易斯酸可作为 HCP 骨架形成的催化剂,也可作为 Hg0 亲和剂。所得到的 HCP-Metal 样品具有很高的脱汞(De-Hg)能力(120 分钟内脱汞∼100%)和出色的耐水性(10% H2O),大大超过了最先进的吸附剂。实验和理论计算证实,Hg0 的成键构型包括 Hg0 与 Cl 单价位点、Cl 桥接位点和金属顶位点的成键构型。FeCl3/CuCl2 的电子供体轨道能级较近,因此具有出色的除汞性能。在原位催化过程中使用不同路易斯酸的这一探索为环境修复和能量存储提供了广阔的应用前景。
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来源期刊
ACS Chemical Neuroscience
ACS Chemical Neuroscience BIOCHEMISTRY & MOLECULAR BIOLOGY-CHEMISTRY, MEDICINAL
CiteScore
9.20
自引率
4.00%
发文量
323
审稿时长
1 months
期刊介绍: ACS Chemical Neuroscience publishes high-quality research articles and reviews that showcase chemical, quantitative biological, biophysical and bioengineering approaches to the understanding of the nervous system and to the development of new treatments for neurological disorders. Research in the journal focuses on aspects of chemical neurobiology and bio-neurochemistry such as the following: Neurotransmitters and receptors Neuropharmaceuticals and therapeutics Neural development—Plasticity, and degeneration Chemical, physical, and computational methods in neuroscience Neuronal diseases—basis, detection, and treatment Mechanism of aging, learning, memory and behavior Pain and sensory processing Neurotoxins Neuroscience-inspired bioengineering Development of methods in chemical neurobiology Neuroimaging agents and technologies Animal models for central nervous system diseases Behavioral research
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