Co single-atom confined in N-doped hollow carbon sphere with superb stability for rapid degradation of organic pollutants
Co single-atom confined in N-doped hollow carbon sphere with superb stability for rapid degradation of organic pollutants
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Co单原子限制在氮掺杂空心碳球中，具有极好的稳定性，可快速降解有机污染物
DOI：
10.1016/j.cej.2022.139229
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发表时间：
2022-09
影响因子：
15.1
通讯作者：
Haijiao Xie
中科院分区：
文献类型：
--
作者：
Zhenyang Xu;Yimei Zhang;Fei Wang;Zhiying Li;Wenwen Gu;Yaxin Zhang;Haijiao Xie
单原子催化剂在水环境修复领域具有巨大的应用潜力。开发具有足够稳定性和优异催化性能的高效SAC是非常可取的，但仍然是一个巨大的挑战。本文通过将Co单原子引入到N掺杂的空心碳球（NHCS）中，制备了CoSA/NHCS催化剂，用于活化过一硫酸盐（PMS）去除双酚A（BPA）。实验和密度泛函理论（DFT）研究表明，Co-N4活性中心和电子转移机制的结合可以实现BPA的快速降解（1 min内降解98%）.通过计算BPA分子轨道和福井指数，预测了电子转移途径攻击BPA的主要活性位。通过LC-MS鉴定了BPA可能的降解中间体，并使用生态结构活性关系模型（ECOSAR）证明其无毒。在用于BPA降解反应的流通式装置中，在60 h后没有观察到催化剂失活，并且在100 h后仍然保持90%的去除效率，这进一步使其具有实际水环境修复的前景。
Single-atom catalysts (SACs), which have great potential in the field of water environmental remediation. Development of highly efficient SACs with sufficient stability and excellent catalytic performance was highly desirable, yet remains a huge challenge. Herein, a CoSA/NHCS catalyst was prepared by confining Co single-atom into the N-doped Hollow Carbon Sphere (NHCS) to activate peroxymonosulfate (PMS) for removing bisphenol A (BPA). Experimental and density functional theory (DFT) studies show that the combination of Co-N4active site and electron transfer mechanism could achieve rapid degradation of BPA (98 % within 1 min). The main active sites of BPA attacked by the electron transfer pathway were predicted by calculating BPA molecular orbitals and Fukui indices. The possible degradation intermediates of BPA were identified by LC-MS and demonstrated to be nontoxic using ecological structure activity relationship modeling (ECOSAR). In a flow-through device for BPA degradation reaction, no deactivation of the catalyst was seen after 60 h and still remained 90 % remove efficiency after 100 h, which further renders it promising for actual water environmental remediation.
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作者：
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影响因子：
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作者：
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通讯作者：
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