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  • Sheng Yu, Yaqi Wang, Sobhan Chatterjee, Feng Liang, Fei Zhu, Haibing Li
    Chinese Chemical Letters. 2021, 32(1): 179-183.

    Chirality is a fascinating and essential feature of life and highly associated with many significant pharmaceutical, chemical, and biological processes. The construction of chiral recognition platform is a hot research topic and challenging assignment. Herein, we report an electrochemical method by differential pulse voltammetry (DPV) for the enantioselective recognition of chiral drug propranolol (R/S-PPL) through a nanochannel platform based on the N-acetyl-L-cysteine functionalized Pillar[5]arenes derivative NALC-P5 and the porous polycarbonate membrane. The chiral discrimination depends on the difference in the supramolecular host-guest interaction between the chiral NALC-P5 and the R/S-PPL. The transmission rate of the R/S-PPL can be regulated in the nanochannel and we can achieve the selective transport of the chiral drugs. This simple electrochemical technique has potential applications as a general platform for the recognition of chiral molecules.

  • Wenjuan Yang, Yating Zhu, Junjun Li, Zheng Chen, Farhat Nosheen, Qitao Zhang, Zhicheng Zhang
    Chinese Chemical Letters. 2021, 32(1): 286-290.

    The conversion of chemical feedstock materials into high value-added products accompanied with dehydrogenation is of great value in the chemical industry. However, the catalytic dehydrogenation reaction is inhibited by a limited number of expensive noble metal catalysts and lacks understanding of dehydrogenation mechanism. Here, we report the use of heterogeneous non-noble metal iron nanoparticles (NPs) incorporated mesoporous nitrogen-doped carbon to investigate the dehydrogenation mechanism based on experiment observation and density functional theory (DFT) method. Fe NPs catalyst displays excellent performance in the dehydrogenation of 1, 2, 3, 4-tetrahydroquinoline (THQ) with 100% selectivity and 100% conversion for 10-12 h at room temperature. The calculated adsorption energy implies that THQ prefers to adsorb on Fe NPs as compared with absence of Fe NPs. What is more, the energy barrier of transition state is relatively low, illustrating the dehydrogenation is feasible. This work provides an atomic scale mechanism guidance for the catalytic dehydrogenation reaction and points out the direction for the design of new catalysts.

  • Juan Li, Wanling Li, Yan Rao, Feng Shi, Suhua Yu, Huizhen Yang, Lingfeng Min, Zhanjun Yang
    Chinese Chemical Letters. 2021, 32(1): 150-153.

    3D highly ordered silver nanoparticles (AgNPs) coated silica photonic crystal beads (Ag/SPCBs) were prepared and exploited as a novel surface enhanced Raman scattering (SERS) substrate. The monodisperse and size-controlled SPCBs were prepared via self-assembly of silica nanoparticles process using a simple microfluidic device. Then the Ag/SPCBs were easily obtained by in situ growth of AgNPs onto the NH2-modified SPCBs. Field emitting scanning electron microscopy (SEM) and energy dispersive X-ray spectrometry (EDX) were used to characterize the Ag/SPCBs. The effect of silica nanoparticle size and AgNO3 concentration on the SERS performance of the resultant Ag/SPCBs substrate were discussed in detail. The results indicate that the Ag/SPCBs have highest SERS signals when silica nanoparticle size is 250 nm and AgNO3 concentration is 0.8 mg/mL. Using malachite green (MG) as model analyte, the Ag/SPCBs substrate displayed a high sensitivity and a wide linear range for MG. The well-designed Ag/SPCBs show high uniformity and excellent reproducibility, and can be used as an effective SERS substrate for sensitive assay application.

  • Hao Wang, Xiuli Wang, Rong-Mei Kong, Lian Xia, Fengli Qu
    Chinese Chemical Letters. 2021, 32(1): 198-202.

    In this research, a hydroxyl group functionalized metal-organic framework (MOF), UiO-66-(OH)2, was synthesized as a "on-off-on" fluorescent switching nanoprobe for highly sensitive and selective detection of Fe3+, ascorbic acid (AA) and acid phosphatase (ACP). UiO-66-(OH)2 emits yellow-green light under ultraviolet light, when Fe3+ was added, Fe3+ was chelated with hydroxyl group, the electrons in the excited state S1 of the MOF transferred to the half-filled 3d orbits of Fe3+, resulting in fluorescence quenching because of the nonradiative electron/hole recombination annihilation. AA could reduce Fe3+ to Fe2+, which can destroy the electron transfer between UiO-66-(OH)2 and Fe3+ after AA adding, resulted in nonoccurrence of the nonradiative electron transfer, leading to the recovery of UiO-66-(OH)2 fluorescence intensity. The probe can also be used to detect ACP based on the enzymolysis of 2-phospho-L-ascorbic acid (AAP) to produce AA. Benefitting from the hydroxyl group and the characteristics of UiO-66, including the high porosity and large surface area, the developed UiO-66-(OH)2 showed extensive advantages as a fluorescent probe for detection of multi-component, such as high sensitivity and selectivity, colorimetric detection, fast response kinetics and easy to operate, economical and secure. This is the first time to use active group functionalized MOFs as a multi-component sensor for these three substances detection.

  • Yang Zhou, Yanqiang Li, Qingran Ding, Youchao Liu, Yangxin Chen, Xitao Liu, Xiaoying Huang, Lina Li, Sangen Zhao, Junhua Luo
    Chinese Chemical Letters. 2021, 32(1): 263-265.

    Two fluoride sulfates, K2Mn3(SO4)3F2·4H2O (I) and Rb2Mn3(SO4)3F2·2H2O (Π) are obtained by water solution method. Single-crystal X-ray diffraction analysis indicated that they crystallize in space groups of Cmc21. Their structures feature a pseudo-KTP structure consisting of interconnecting [Mn3(SO4)3F2(H2O)2] layers, which are further packing along the a axis with alkali metal cations balancing the charges. The structure relationships between the two compounds are discussed. Second-harmonic generation measurements manifest that I and Π have similar second-harmonic generation responses of about 0.2 and 0.25 times that of KH2PO4.

  • Chenghao Hou, Lijing Liu, Siyang Meng, Yue Wu, Meiran Xie, Yongkui Shan, Pingang He, Pengfei Sun, Xiaojuan Liao
    Chinese Chemical Letters. 2021, 32(1): 214-217.

    Integrating silica with organic nanoparticles can generate unique properties. Here pillar[5]arene/silica hybrid vesicles were constructed based on the amphiphilic and rigid properties of pillararenes, as well as the catalytic hydrolysis of tetraethoxysilane. Such vesicles exhibited the high strength of silica and unique molecular recognition of pillararenes, both of which could tune the pH-triggered release behavior. Furthermore, a rhodamine B derivative with hexyl group (RhB-C6) was synthesized, which can form a complex with the pillar[5]arene. Based on the host-guest interaction and high strength of silica, the hybrid vesicles could load more RhB-C6 and the rhodamine B was released more slowly compared with the organic vesicles.

  • Ge Yang, Chao Zhu, Liping Zhao, Linsen Li, Yuanyu Huang, Yukui Zhang, Feng Qu
    Chinese Chemical Letters. 2021, 32(1): 218-220.

    Selection of aptamers with high affinity and good specificity requires multiple rounds of alternating steps of separation and PCR amplification. Herein, we proposed a novel high-efficiency aptamers picking strategy: One-round pressure controllable selection (OPCS). OPCS integrates four types of screening superiority, high-efficiency separation, one-round selection and PCR amplification, synchronous negative selection and targets competition. The controllable screening pressure can be achieved through two approaches, balanced competition by the regulation of protein concentration, and dominant competition by introducing a predatory protein with high concentration. In OPCS process, two proteins were co-incubated with one ssDNA library, and each protein bound its favorable sequences specifically and formed protein-ssDNA complex respectively. Meanwhile, one protein could supply/suffer the picking pressure of affinity and specificity to/from another, which eliminated weakly bound or unbound sequences for each other. Two complexes could be separated and collected conveniently, and aptamers for two proteins obtained synchronously with high affinity and good specificity. This strategy not only provides a more effective way for aptamers selection, but shows great potential in other ligands or drugs selection.

  • Guanglei Li, Dan Wen
    Chinese Chemical Letters. 2021, 32(1): 221-228.

    The metabolic disorder of glucose in human body will cause diseases such as diabetes and hyperglycemia. Hence the determination of glucose content is very important in clinic diagnosing. In recent years, researchers have proposed various non-invasive wearable sensors for rapid and real-time glucose monitoring from human body fluids. Unlike those reviews which discussed performances, detection environments or substrates of the wearable glucose sensor, this review focuses on the sensing nanomaterials since they are the key elements of most wearable glucose sensors. The sensing nanomaterials such as carbon, metals, and conductive polymers are summarized in detail. And also the structural characteristics of different sensing nanomaterials and the corresponding wearable glucose sensors are highlighted. Finally, we prospect the future development requirements of sensing nanomaterials for wearable glucose sensors. This review would give some insights to the further development of wearable glucose sensors and the modern medical treatment.

  • Qishun Liu, Yufen Lv, Ruisheng Liu, Xiaohui Zhao, Jiawen Wang, Wei Wei
    Chinese Chemical Letters. 2021, 32(1): 136-139.

    A convenient and regioselective sulfonylation/cyclization of 1,6-enynes with arylazo sulfones has been developed to access a series of sulfonylated γ-butyrolactams. The present reaction could be efficiently conducted under catalyst- and additive-free conditions, in which C—S and C—C bonds were selectively constructed in one-pot procedure.

  • Hongwei Zhao, Yanqiu Zhang, Li Lixiang, Xin Geng, Haiming Yang, Weimin Zhou, Chengguo Sun, Baigang An
    Chinese Chemical Letters. 2021, 32(1): 140-145.

    Both nitrogen-doping feature and pore structure are critical factors for developing nitrogen-doped carbons based catalysts with a high performance toward oxygen reduction reaction (ORR). Herein, a simple one-step CVD of acetylene and acetonitrile vapor method using silanized SBA-15 as a template has been developed to synthesize an ordered porous carbon (OPC) with dual nitrogen-doped interfaces. The optimized sample as prepared with the CVD of 4 h at 750 ℃ contains two types of ordered mesopores that one type is the ordered cylindrical pores inheriting from the pores of SBA-15 and has a pore width of 4.0~5.0 nm, the other type is the ordered quasi-hexagonal pores with a width of 3.0~4.0 nm produced by etching the pore walls of SBA-15. These two types of pores whose pore walls are built by the nitrogen doped carbon layers resulted by the CVD and thus it actually makes the dual nitrogen-doped interfaced OPC (DN-OPC). Meanwhile, DN-OPC contains a few of micropores and a large SSA of 1430 m2/g. This dual-ordered pores and dual nitrogen-doped interfaces cannot only facilitate mass transport but also utilize the active sites of DN-OPC for ORR. Therefore, as metal-free ORR catalyst, DN-OPC exhibits a good activity close to commercial Pt/C catalyst, and an excellent durability and methanol tolerance.

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