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  • Feng Wu, Xuemin Kong, Yixuan Liu, Shuli Wang, Zhong Chen, Xu Hou
    Chinese Chemical Letters. 2024, 35(8): 109754-.

    The isolation of circulating tumor cells (CTCs) from complex biological samples is of paramount significance for advancing cancer diagnosis, prognosis, and treatment. However, the low concentration of CTCs and nonspecific adhesion of white blood cells (WBCs) present challenges that hinder the efficiency and purity of captured CTCs. Microfluidic-based strategies utilize precise fluid control at the micron level to incorporate specific micro/nanostructures or recognition molecules, enabling effective CTCs separation. Moreover, by employing surface modification designs that exhibit exceptional anti-adhesion properties against WBCs, the purity of isolated CTCs can be further enhanced. This review offers an in-depth exploration of recent advancements, challenges, and opportunities associated with microfluidic-based CTCs isolation from biological samples. Firstly, we will comprehensively introduce the microfluidic-based strategies for achieving high-efficiency CTCs isolation, which includes the morphological design of microchannels for physical force-based CTCs isolation and the specific modification of microchannel surfaces for affinity-based CTCs isolation. Subsequently, a review of recent research advances in microfluidic-based high-purity CTCs isolation is presented, focusing on strategies that decrease the nonspecific adhesion of WBCs through surface micro-/nanostructure construction or chemical and biological modification. Finally, we will summarize the article by providing the prospective opportunities and challenges for the future development of microfluidic-based CTCs isolation.

  • Xiaohong Wen, Mei Yang, Lie Li, Mingmin Huang, Wei Cui, Suping Li, Haiyan Chen, Chen Li, Qiuping Guo
    Chinese Chemical Letters. 2024, 35(8): 109291-.

    Intracellular ATP is an emerging biomarker for cancer early diagnosis because it is a key messenger for regulating the proliferation and migration of cancer cells. However, the conventional ATP biosensing strategy is often limited by the undesired on-target off-tumor interference. Here, we reported a novel strategy to design enzymatically controlled DNA tetrahedron nanoprobes (En-DT) for biosensing and imaging ATP in tumor cells. The En-DT was designed via rational engineering of structure-switching aptamers with the incorporation of an enzyme-activatable site and further conjugation on the DNA tetrahedron. The En-DT could be catalytically activated by apurinic/apyrimidinic endonuclease 1 (APE1) in cancer cells, but they did not respond to ATP in normal cells, thereby enabling cancer-specific ATP biosensing and imaging in vitro and in vivo with improved tumor specificity. This strategy would facilitate the precise detection of a broad range of biomarker in tumors and may promote the development of smart probes for cancer diagnosis.

  • Jing-Jing Zhang, Lujun Lou, Rui Lv, Jiahui Chen, Yinlong Li, Guangwei Wu, Lingchao Cai, Steven H. Liang, Zhen Chen
    Chinese Chemical Letters. 2024, 35(8): 109342-.

    As a powerful noninvasive imaging technology, positron emission tomography (PET) has been playing an important role in disease theranostics and drug discovery. The successful application of PET relies on not only the biological properties of PET tracers but also the availability of facile and efficient radiochemical reactions to enable practical production and widespread use of PET tracers. Most recently, photochemistry is emerging as a novel, mild and efficient approach to generating PET agents. In this review, we focus on the recent advances in newly developed photocatalytic radiochemical reactions, innovation on automated photochemical radiosynthesis modules, as well as implementation in late-stage radiolabeling and radiopharmaceutical synthesis for PET imaging. We believe that this review will inspire the development of more promising radiolabeling protocols for the preparation of clinically useful PET agents.

  • Ruilong Geng, Lingzi Peng, Chang Guo
    Chinese Chemical Letters. 2024, 35(8): 109433-.

    The dynamic kinetic asymmetric transformation of racemic propargylic ammonium salts with prochiral aldimine esters through a stereodivergent propargylation is catalyzed by dual nickel and copper catalysis. Thus, a diverse range of optically active α-quaternary amino esters were produced via CN bond cleavage with high reaction efficiency and stereoselectivity (up to > 99% ee). By selection of the appropriate pairwise combination of catalyst configurational isomers, all four possible stereoisomers of the corresponding propargylation products are obtained in high yields with excellent regio-, diastereo-, and enantioselectivities.

  • Yuchen Wang, Yaoyu Liu, Xiongfei Huang, Guanjie He, Kai Yan
    Chinese Chemical Letters. 2024, 35(8): 109301-.

    Metal-nanocluster materials have gradually become a promising electrode candidate for supercapacitor application. The high-efficient and rational architecture of these metal-nanocluster electrode materials with satisfied supercapacitive performance are full of challenges. Herein, Fe-nanocluster anchored porous carbon (FAPC) nanosheets were constructed through a facile and low-cost impregnation-activation strategy. Various characterization methods documented that FAPC nanosheets possessed a mesopore-dominated structure with large surface area and abundant Fe-N4 active sites, which are crucial for supercapacitive energy storage. The optimal FAPC electrode exhibited a high specific capacitance of 378 F/g at a specific current of 1 A/g and an excellent rate capability (271 F/g at 10 A/g), which are comparable or even superior to that of most reported carbon candidates. Furthermore, the FAPC-based device achieved a desired specific energy of 14.8 Wh/kg at a specific power of 700 W/kg. This work opens a new avenue to design metal-nanocluster materials for high-performance biomass waste-based supercapacitors.

  • Yue Zhang, Xiaoya Fan, Xun He, Tingyu Yan, Yongchao Yao, Dongdong Zheng, Jingxiang Zhao, Qinghai Cai, Qian Liu, Luming Li, Wei Chu, Shengjun Sun, Xuping Sun
    Chinese Chemical Letters. 2024, 35(8): 109806-.

    Electrocatalytic synthesis of urea through CN bond formation, converting carbon dioxide (CO2) and nitrate (NO3), presents a promising, less energy-intensive alternative to industrial urea production process. In this communication, we report the application of Mo2C nanosheets-decorated carbon sheets (Mo2C/C) as a highly efficient electrocatalyst for facilitating CN coupling in ambient urea electrosynthesis. In CO2-saturated 0.2 mol/L Na2SO4 solution containing 0.05 mol/L NO3, the Mo2C/C catalyst achieves an impressive urea yield of 579.13 µg h–1 mg–1 with high Faradaic efficiency of 44.80% at –0.5 V versus the reversible hydrogen electrode. Further theoretical calculations reveal that the multiple Mo active sites enhance the formation of *CO and *NH2 intermediates and facilitate their CN coupling. This research propels the use of Mo2C-based electrodes in electrocatalysis and accentuates the capabilities of binary metal-based catalysts in CN coupling reactions.

  • Zhirong Yang, Shan Wang, Ming Jiang, Gengchen Li, Long Li, Fangzhi Peng, Zhihui Shao
    Chinese Chemical Letters. 2024, 35(8): 109518-.

    The development of low-cost, earth-abundant and environmentally benign transition metal catalysts, which can catalyze multiple different types of asymmetric reactions, is an important objective in modern asymmetric catalysis. Herein we demonstrate that a chiral Ni/P-Phos catalyst achieves three types of asymmetric reactions: allenylic substitution of racemic allenic ethers, 1,4-hydroalkylation of prochiral 1,3-enynes and double alkylation of newly designed enynyl ether reagents. Three methods complement each other and produce various axially chiral allene derivatives bearing a pyrazolidine-3,5-dione unit, which is widely present in drugs and biologically active molecules with versatile pharmacological activities.

  • Jiqing Liu, Qi Dang, Liting Wang, Dejin Wang, Liang Tang
    Chinese Chemical Letters. 2024, 35(8): 109277-.

    The advancement of energy storage technology has paved the way for the application of electrochemical processes in achieving low-carbon and precise environmental pollution reduction. Electrodes play a crucial role in efficiently removing organic pollutants and heavy metals. To implement electrochemical pollution control technology in practical engineering, flexible electrode preparation is vital. This review highlights recent progress in flexible electrode research, focusing on the selection and structural design of flexible electrode materials. It summarizes the latest advancements in current collectors, active materials, and preparation methods to enhance conductivity, flexibility, and cycle stability. The application of flexible electrodes in water pollution control is categorized into three aspects: Organic pollutants, inorganic pollutants, and composite pollutants. Finally, the challenges and research requirements for enhancing electrode flexibility in environmental governance are discussed, along with prospects for their future applications.

  • Zhenhao Wang, Yuliang Tang, Ruyu Li, Shuai Tian, Yu Tang, Dehai Li
    Chinese Chemical Letters. 2024, 35(7): 109247-.

    Described here is a divergent, biosynthetically inspired synthesis of cochlearol B and ganocin A. Key steps of the synthesis include the chromene unit construction through a biomimetic acid-catalyzed [4 + 2] ring cyclization. A photochemical [2 + 2] cycloaddition was featured to construct the cyclobutane core of cochlearol B. Different skeletal rearrangements of cochlearol B afforded ganocin A, that one of them was Lewis acid mediated epoxide rearrangement and another was DDQ induced cyclobutane formed tetrahydrofuran ring. The described syntheses not only achieved these natural products in an efficient manner, but also provided insight into the biosynthetic relationship between the two different skeletons.

  • Li Lin, Song-Lin Tian, Zhen-Yu Hu, Yu Zhang, Li-Min Chang, Jia-Jun Wang, Wan-Qiang Liu, Qing-Shuang Wang, Fang Wang
    Chinese Chemical Letters. 2024, 35(7): 109802-.

    A solid electrolyte interphase (SEI) with a robust mechanical property and a high ionic conductivity is imperative for high-performance zinc metal batteries. However, it is difficult to form such a SEI directly from an electrolyte. In this work, a molecular crowding effect is based on the introduction of Zn(OTF)2 and Zn(ClO4)2 to 2 mol/L ZnSO4 electrolytes. Simulations and experiments indicate that the Zn(OTF)2 and Zn(ClO4)2 not only create a molecularly crowded electrolyte environment to promote the interaction of Zn2+and OTF, but also participate in the reduction to construct a robust and high ionic-conductive SEI, thus promoting metal zinc deposition to the (002) crystal surface. With this molecular crowding electrolyte, a high current density of 1 mA/cm2 can be obtained by assembling symmetric batteries with Zn as the anode for over 1000 h. And in a temperature environment of −10 ℃, a current density of 1 mA/cm2 can be obtained by assembling symmetric batteries with Zn for over 200 h. Zn//Bi2S3/VS4@C cells achieve a CE rate of up to 99.81% over 1000 cycles. Hence, the utilization of a molecular crowding electrolyte is deemed a highly effective approach to fabricating a sophisticated SEI for a zinc anode.

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