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ACS Applied Polymer Materials · 2023 · IF 5

Dendritic Molecular Template Mediates and Directs Self-Assembly of Uniform Gold Nanoclusters to One-Pot Afford 3D-Supported Active Catalysts

Xiaoqiu Yao,Runxin Teng,Ming Jin,Decheng Wan

Uniform gold nanoclusters (AuNCs) are hardly available unless through abundant strong ligands (at the cost of low catalytic activity and narrow catalytic spectrum) or through well-defined (but expensive) templates, and it appears a tougher challenge for direct preparing supported and uniform AuNCs. Here, we show that with an amphiphilic and dendritic molecular template in hand, highly catalytically active, uniform, and supported AuNCs are one-pot achievable. Branched polyethylenimine (PEI) is modified with a few thioether groups and alkylated with hydrophobic acetyls and polystyrene chains to afford reverse micelle-like dendritic polymers. The structurally optimized dendritic polymer can act as a surfactant to mediate very stable water-in-oil high internal phase emulsion (HIPE) within a wide pH spectrum. Moreover, the dendritic polymer switches into the unimolecular state along the interface of the HIPE when pH is below 6, which is critical to the formation of uniform AuNCs. Experimentally, upon the transformation of HIPE into an open-cellular polyHIPE, the gold ions are simultaneously transformed into AuNCs. Direct preparation of the supported and uniform AuNCs (1.8 ± 0.2 nm) are feasible because the dendritic polymer can simultaneously act as a surfactant, a polymer ligand, and a unimolecular template. Meanwhile, the trace thioether groups in the PEI core reduce the size of AuNCs by enhancing nucleation of AuNCs since in the absence of thioether groups, larger particles are obtained. The supported AuNCs are catalytically active because they are stabilized by weak coligands. For the model reaction of the catalyzed reduction of 4-nitrophenol, the catalyst shows a turnover frequency of 112.5 h–1, which is very high. The catalyst is durable and well recyclable.

研究领域: 材料科学 · 催化化学 · 纳米技术
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TALANTA · 2025 · IF 6.1

An electrochemical quinine detection approach based on small molecule promoted split aptamer click ligation reaction

Xuan Luo,Susu Cui,Weiwei Yang,Yongsheng Yu

Quinine is a natural antimalarial drug that also serves as a food additive; however, excessive consumption can result in harmful side effects. Here, we propose a simple and cost-effective electrochemical strategy for quinine detection based on the small molecule-templated split aptamer click ligation (SMT-SpA-CLR), where the integrity of the aptamer is restored through the template-promoted proximity effect. We first investigate the effects of two splitting sites on the affinity of quinine aptamer and find that the loop of the stem with more Watson-Crick base pairs is more suitable for splitting, which can maintain the affinity to a great extent. The affinity of the Split 1 design ( K d  = 48 μM) is slightly reduced compared to the affinity of the parent aptamer. The stable quinine recognition and its sensitive detection are achieved by integrating the SMT-SpA-CLR with an electrochemical signal output. The linear response range for quinine detection is from 0.05 μM to 10 μM with a low detection limit of 25 nM (at S/N = 3). This strategy provides a novel ideal for the design of small molecule-templated split aptamer reaction and can potentially be expanded for detecting other small molecules and proteins.

研究领域: 生物化学 · 分析化学
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NEW JOURNAL OF CHEMISTRY · 2017 ·Vol. 41 ·期 10 ·3766-3772 · IF 3.269

Synthesis and properties enhancement of metal nanoclusters templated on a biological molecule/ionic liquids complex

Wei Wang,Xiaolun Peng,Huayu Xiong,Wei Wen,Ting Bao,Xiuhua Zhang,Shengfu Wang

In this study, two biological template molecules and two common short-chain imidazolium ionic liquids with amphipathy were selected to synthesize four different types of metal nanoclusters (MNCs), which were templated on a biological molecule/imidazolium ionic liquids (ILs) complex with properties enhancement. The fluorescence intensity and stability of the MNCs were improved in different degrees via this simple and fast protocol. The fluorescence intensity of AgNCs was significantly enhanced primarily due to aggregation-induced emission (AIE), and it was attributed to the shrinking size and donation of delocalized electrons for other MNCs. Different template molecule must match with appropriate ILs to form a steady complex that stabilizes the MNCs. The stability of the MNCs was improved, especially for AuNCs, because biological molecule/imidazolium ILs complex was found to be an effective barrier in protecting the MNCs from quenching interactions. Compared to conventional cationic surfactant (sodium dodecyl sulfate, SDS), these imidazolium ILs exhibited superior properties enhancement of the nanomaterials. MNCs with excellent properties could be applied in bioanalysis, especially in fluorescence imaging in vitro, because of their undisturbed and durable optical signal.

研究领域: 材料科学 · 生物化学 · 纳米技术
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Advanced Composites and Hybrid Materials · 2025 ·Vol. 8 ·期 4 ·1-12 · IF 21.8

Molecular template engineering hierarchical porous Fe–N-C with tunable Fe3O4 particle size for efficient oxygen reduction reaction

Wang Lijuan,Shi Yaqin,Wang Yuan,Jia Chunijang,Hou Jie,Su Yizhen,Xu Ben Bin,Liao Zhijian,Zhu Linhua

Synergistic effect between M-N X sites and M X O Y particles in hierarchical porous M–N-C catalysts holds great promises in boosting oxygen reduction reaction (ORR). In this work, 1,4-dicyanobenzene was utilized as a molecular template to prepare the hierarchical porous Fe–N-C catalysts with size-tunable Fe 3 O 4 particles for enhanced ORR in Zn-air battery. The as-prepared Fe 3 O 4 #Fe–N/C DB0.1 owned a half-potential of 0.90 V vs RHE, exceeding that of commercial 20%Pt/C (E 1/2  = 0.82 V vs RHE), showing a maximum power density of 321 mW cm −2 in a homemade Zn-air battery. Density functional theory (DFT) calculations indicate that the electronic interaction between Fe 3 O 4 and Fe-N 4 sites enhances the adsorption energy of *OOH, effectively optimizing the energy barrier for *O formation, significantly reducing the limiting energy barrier. Such superior ORR activity in Fe 3 O 4 #Fe–N/C originated from the optimized hierarchical pores and synergistic effect between Fe-N X sites and Fe 3 O 4 particles. This work provides a new and facile template strategy for engineering hierarchical porous carbon-based materials to achieve highly efficient catalytic reactions.

研究领域: 材料科学 · 电化学 · 催化 · 纳米技术 · 能量存储与转换
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES · 2019 · IF 4.784

A porous collagen-carboxymethyl cellulose/hydroxyapatite composite for bone tissue engineering by bi-molecular template method

Xichan He,Keyong Tang,Xiumin Li,Fang Wang,Jie Liu,Fangfang Zou,Mengyuan Yang,Meixuan Li

Inspired by the mechanism of bone formation, a porous collagen-carboxymethyl cellulose/hydroxyapatite (Col-CMC/HA) composite was designed and fabricated using a biomimetic template of Col and CMC protein-polysaccharide bi-molecules. The morphology, composition and physical properties of Col-CMC/HA composites were characterized systematically. It was found that the nano-HA homogenously distributed on the surface of Col-CMC bi-templates while the composite presented 3D porous structure with pore size from 100 μm to 300 μm. The porosities of composites were located at the range of 71%–85%. Besides, the compressive strength of composites was highly depended on the ratio of Col to CMC in the organic template. The optimized composite in respect to physical properties showed a compressive strength as high as 7.06 MPa, quite close to that of natural bone. The high relative growth rate of wild-type mouse embryonic fibroblasts cells was found for the composite, indicating a good biocompatibility. The organic-inorganic composite also behaved good in collagenase resistance and could be biodegraded in 8 weeks, with about 50% of initial weight left at the ratio of Col to CMC of 1:9. The results demonstrated that the Col-CMC/HA composite by bi-molecular template method was a rational and safe method to prepare biomaterials with tunable properties.

研究领域: 生物材料 · 组织工程 · 材料科学 · 生物医学工程
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