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  • Xiaofei Wang, Xuezhen Lin, Huijuan Qiu, Jianda Xie, Zhengyu Lu, Yusong Wang, Weitai Wu
    Chinese Chemical Letters. 2022, 33(3): 1445-1449.

    Here, we report a finding on light-mediated CO2-responsiveness. It is found on the microgels that are made of side-chain type metallopolymers containing metalla-aromatics. Turbidity and laser light scattering studies on dilute aqueous dispersion of these microgels in dark indicate high CO2-responsivity, but poor reversibility upon N2 purge, which can be improved by exposing to light. This light-mediated CO2-responsiveness can be elucidated by the loss of aromaticity from initial photoexcitation and concurrent formation of a less reactive, antiaromatic excited state of relatively low CO2 binding affinity, and by subsequent relief of antiaromaticity that can enhance the CO2 removal. The finding is also checked by CO2 uptake-release experiments on the microgels, which enables both CO2 capture of high capacity and CO2 removal of good reversibility under a mild condition, allowing effective and reversible response to dilute CO2.

  • Yu Liu, Xiaowei Zhang, Lisha Lu, Jun Ye, Jianlin Wang, Xiaomin Li, Xuedong Bai, Wenlong Wang
    Chinese Chemical Letters. 2022, 33(3): 1271-1274.

    The ability of plasmonic nanostructures to efficiently harvest light energy and generate energetic hot carriers makes them promising materials for utilization in photocatalytic water spitting. Apart from the traditional Au and Ag based plasmonic photocatalysts, more recently the noble–metal–free alternative plasmonic materials have attracted ever–increasing interest. Here we report the first use of plasmonic zirconium nitride (ZrN) nanoparticles as a promising photocatalyst for water splitting. Highly crystalline ZrN nanoparticles with sizes dominating at 30–50 nm were synthesized that exhibit intense visible and near–infrared absorption due to localized surface plasmon resonance (LSPR). Without utilizing any noble metal cocatalysts such as Pt, the plasmonic ZrN nanoparticles alone showed stable photocatalytic activity for H2 evolution in aqueous solution with methanol as sacrificial electron donor. The addition of a cobalt oxide (CoOx) cocatalyst can facilitate the separation of photogenerated charge carriers and further improve the photocatalytic activity. The optimized CoOx modified ZrN photocatalyst was observed not only to activate the O2 evolution reaction with presence of electron acceptor, but also to drive overall water splitting for the simultaneous H2 and O2 evolution in the absence of any sacrificial agents.

  • Danni Guo, Lixia Zhao, Hui Zhang
    Chinese Chemical Letters. 2022, 33(3): 1263-1266.

    Fabrication of multifunctional nanoplatform to in situ monitor Fenton reaction is of vital importance to probe the underlying reaction process and design high-performance catalyst. Herein, a hybrid catalyst comprising of single-crystalline Au nanoparticles (SC Au NPs) on reduced graphene oxide (RGO) sheet was prepared, which not only exhibited an excellent 1O2 mediated Fenton-like catalytic activity in promoting rhodamine 6G (R6G) degradation by activating H2O2, but also displayed a sensitive surface-enhanced Raman spectroscopy (SERS) detection performance to R6G with a linear response range from 1.0 × 10-8 mol/L to 1.0 × 10-5 mol/L thus providing a powerful and versatile nanoplatform for in situ SERS monitoring Fenton-like catalytic reaction. The integration of catalytic and SERS activities into a single nanostructure are expected to provide great potentials for practical applications in environmental catalysis.

  • Yan Song, Ran Wang, Xiuyuan Li, Baiqi Shao, Hongpeng You, Chaozheng He
    Chinese Chemical Letters. 2022, 33(3): 1283-1287.

    Exploiting efficient and recyclable photocatalysts is a vital matter for environmental purification. Herein, cerium vanadate (CeVO4) sub-microspheres and silver nanowire (AgNW)@CeVO4 with core-shell architecture as photocatalysts are rationally constructed by hydrothermal approach. The AgNW@CeVO4 photocatalyst obtained by depositing CeVO4 on the surface of Ag NWs possess one dimensional continuous structure, which expand the optical absorption range and reduce the band gap of CeVO4 photocatalyst. Moreover, the resultant AgNW@CeVO4 photocatalyst demonstrates superior photocatalytic performance in the degradation of rhodamine B, methylene blue, and 4-nitrophenol pollutants upon solar light irradiation, compared with pure CeVO4. The excellent photocatalytic activity can be ascribed to the introduction of Ag NWs, which afford rapid charge transport channels and reservoir for the electrons in the AgNW@CeVO4 heterostructure to promote separation of electron–hole pairs. The first-principles investigations reveal increase of adsorption energy of oxygen molecules on the CeVO4 surface with the presence of Ag. Meanwhile, Ag NWs can further improve the photocatalytic efficiency of the AgNW@CeVO4 based on the plasmonic effect. More importantly, the good structural stability and recyclability of AgNW@CeVO4 are observed due to the strong synergistic effect, which ensures long-term usability of photocatalyst and great promise in water purification. This work can offer valuable reference into designs and construction of Ce-based heterojunction photocatalysts for environmental remediation.

  • Wendong Zhang, Yun Wang, Yi Wang, Yi Liang, Fan Dong
    Chinese Chemical Letters. 2022, 33(3): 1259-1262.

    A novel SrSn(OH)6 photocatalyst with large plate and particle size were synthesized via a facile chemical precipitation method. The photocatalytic activity of the SrSn(OH)6 was evaluated by the removal of NO at ppb level under UV light irradiation. Based on the ESR measurements, SrSn(OH)6 photocatalyst was found to have the ability to generate the main active species of O2•−, OH and 1O2 during the photocatalytic process. Moreover, SrSn(OH)6 photocatalyst not only exhibits high photocatalytic activity for NO removal (79.6%), but also has good stability after five cycles. The in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) was used to investigate the NOx transfer pathway and the intermediate products distribution during the adsorption and photocatalytic NO oxidation process. The present work not only provides an efficient material for air pollutants purification at room temperature but also in-depth understanding of the mechanism involved in the photocatalytic NO removal process.

  • Hedong Qi, Yuwei Xu, Pin Hu, Chi Yao, Dayong Yang
    Chinese Chemical Letters. 2022, 33(3): 1131-1140.

    As a biologically active macromolecule, deoxyribonucleic acid (DNA) has the advantages of sequence programmability and structure controllability and can accurately transmit sequence information to specific biological functions. Facing the complex internal microenvironment and heterogeneity in tumor treatment, the construction and applications of DNA-based nanomaterials have become a focus point of research. In particular, the hybridization of DNA molecules with other materials endows DNA-based nanomaterials with multiple functions such as targeting, stimulus responsiveness and regulations of biological activities, making DNA nanostructures great potential in the treatment of major human diseases. In this review, the construction and characteristics of DNA-based nanomaterials are introduced. Then, the functions and applications of DNA-based nanomaterials in the delivery of chemotherapy drugs and gene drugs, stimulus-responsive release and regulation of cell homeostasis are reviewed. Finally, the future development and challenges of DNA-based nanomaterials are prospected. We envision that DNA-based nanomaterials can enrich the nanomaterial system by rational design and synthesis and address the growing demands on biological and biomedical applications in the real world.

  • Xiaohu Zhang, Lixiao Han, Hao Chen, Shengyao Wang
    Chinese Chemical Letters. 2022, 33(3): 1117-1130.

    Considering the significant importance in both ecological and environmental fields, converting nitrogen oxide (NOx, especially NO) into value-added NH3 or harmless N2 lies in the core of research over the past decades. Exploring catalyst for related gas molecular activation and highly efficient reaction systems operated under low temperature or even mild conditions are the key issues. Enormous efforts have been devoted to NO removal by utilizing various driving forces, such as thermal, electrical or solar energy, which shine light on the way to achieve satisfying conversion efficiency. Herein, we will review the state-of-the-art catalysts for NO removal driven by the above-mentioned energies, including a comprehensive introduction and discussion on the pathway and mechanism of each reaction, and the recent achievements of catalysts on each aspect. Particularly, the progress of NO removal by environmentally friendly photocatalysis and electrocatalysis methods will be highlighted. The challenges and opportunities in the future research on the current topic will be discussed as well.

  • Dao-Qing Dong, Jing-Cheng Song, Shao-Hui Yang, Qi-Xue Qin, Zu-Li Wang, En-Xuan Zhang, Yuan-Yuan Sun, Qing-Qing Han, Shan Yue
    Chinese Chemical Letters. 2022, 33(3): 1199-1206.

    Oximes derivatives have been vastly used in organic synthesis. In this review, C(sp3)−H bond functionalization of oximes derivatives via iminyl radical induced 1, 5−hydrogen atom transfer was discussed. According to the different type of products, this review was divided into three parts: (1) C(sp3)−H bond functionalization for C−C bond formation. (2) C(sp3)−H bond functionalization for C−N bond formation. (3) C(sp3)−H bond functionalization for C−S, C−F bond formation.

  • Tesfaye Tebeka Simur, Tian Ye, You-Jie Yu, Feng-Lian Zhang, Yi-Feng Wang
    Chinese Chemical Letters. 2022, 33(3): 1193-1198.

    Selective functionalization of C–F bonds in trifluoromethyl groups has recently received a growing interest, as it offers atom- and step-economic pathways to access highly valuable mono- and difluoroalkyl-substituted organic molecules using simple and inexpensive trifluoromethyl sources as the starting materials. In this regard, impressive progress has been made on the defluorinative functionalization reactions that proceed via radical intermediates. Nevertheless, it is still a great challenge to precisely control the defluorination process, due to the continuous decrease of the C–F bond strength after the replacement of one or two fluorine atoms with various functionalities. This review article is aimed to provide a brief overview of recently reported methods used to functionalize C–F bonds of CF3 groups via radical intermediates. An emphasis is placed on the discussion of mechanistic aspects and synthetic applications

  • Wenjie Zhou, Zhe Hu, Jinxin Wei, Hanqing Dai, Yuanyuan Chen, Siyu Liu, Zhongtao Duan, Fengxian Xie, Wanlu Zhang, Ruiqian Guo
    Chinese Chemical Letters. 2022, 33(3): 1245-1253.

    Quantum dots-hydrogel composites are promising new materials that have attracted extensive attention due to their incomparable biocompatibility and acceptable biodegradability, leading to enormous potential applications for various fields. This review summarizes the recent advances in quantum dots-hydrogel composites with a focus on synthesis methods, including hydrogel gelation in quantum dots (QDs) solution, embedding prepared QDs into hydrogels after gelation, forming QDs in situ within the preformed gel and cross-linking via QDs to form hydrogels. In particularly, biomedical applications as bioimaging, biosensing and drug delivery are also reviewed, followed by a discussion on the inherent challenges of design optimization, biocompatibility and bimodal applications and the prospect of the future development. These results will guide the development of quantum dots-hydrogel composites and provide critical insights to inspire researchers in future.

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