Site-specific surface tailoring for metal ion selectivity via under-coordinated structure engineering†,Nanoscale Horizons

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Site-specific surface tailoring for metal ion selectivity via under-coordinated structure engineering†
Nanoscale Horizons ( IF 8.0 ) Pub Date : 2018-07-25 00:00:00 , DOI: 10.1039/c8nh00094h
Li Yu _{1,

2,

3,

4,

5} , Gong Zhang _{6,

7,

8,

9} , Chunlei Liu _{1,

2,

3,

4,

5} , Huachun Lan _{6,

7,

8,

9} , Huijuan Liu _{1,

2,

3,

4,

5} , Jiuhui Qu _{1,

2,

3,

4,

5}

Affiliation

Coordinatively unsaturated atoms play an important role in structural and electronic tuning, while their effects on surface site tailoring for selective adsorption have not been well explored. We demonstrate a new concept based on elaborate tuning of the chemical states of lattice atoms to control the accessibility of different surface sites. The under-coordinated manganese structure developed herein not only benefits the formation of hydroxylated lateral edge sites for preferential complexation of lead (Pb) ions, but also favors a decrease in the proportions of metal-ion-nonspecific octahedral vacancy sites. On the basis of this strategy, a common core–shell structure was devised to further assemble highly exposed edge sites, achieving high selectivity coefficients (31.2–172.0) for Pb(II) against various metal cations. Even when these metal cations coexist at higher concentrations, the general specificity is still maintained, with further pH-enabled switchable sorption–desorption for adsorbent recyclability. Different from frequently reported specific ligand-induced selective systems, intrinsic structure modification as described herein will lead to a new paradigm for surface site tailoring that enables a versatile and tunable platform in environmental remediation, resource recovery and analyte sensing.

中文翻译：

通过不协调的结构工程进行针对金属离子选择性的特定位置表面修整†

配位不饱和原子在结构和电子调谐中起着重要作用，但尚未充分研究它们对选择性吸附的表面位点调节的影响。我们展示了一个基于精心调整晶格原子的化学状态来控制不同表面部位可及性的新概念。本文开发的配位不足的锰结构不仅有利于形成铅（Pb）离子优先络合的羟基化侧边位点，而且有利于降低金属离子非特异性八面体空位点的比例。在此策略的基础上，设计了一种通用的核-壳结构以进一步组装高度暴露的边缘位点，从而实现了对Pb（II）的高选择性系数（31.2–172.0））对抗各种金属阳离子。即使当这些金属阳离子以更高的浓度共存时，仍能保持一般的特异性，并具有进一步的pH值可转换的吸附-解吸功能，以实现吸附剂的可回收性。与经常报道的特异性配体诱导的选择性系统不同，本文所述的内在结构修饰将导致表面位点剪裁的新范式，该范式可在环境修复，资源回收和分析物感测中实现通用且可调节的平台。

更新日期：2018-07-25

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