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  • 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.

  • Hongjin Li, Xiangyan Chen, Minghao Wu, Panpan Song, Xia Zhao
    Chinese Chemical Letters. 2022, 33(3): 1254-1258.

    In recent years, the strategy of inhibiting the interactions of p53 with murine double minute 2 (MDM2) and murine double minute X (MDMX) has been proved to be a promising approach for tumor therapy. However, the poor proteolytical stability and low intracellular delivery efficiency of peptide inhibitors limit their clinical application. Here, we designed and synthesized the bicyclic stapled peptides based on p53 by combining all-hydrocarbon stapling and lactam stapling strategies. We demonstrated that bicyclic stapled peptide p53-16 significantly improved α-helicity and proteolytic stability. Especially, p53-16 showed nanomolar binding affinity for MDM2 and MDMX. In addition, p53-16 could penetrate the cell membrane, and selectively inhibited the activity of tumor cells via activating p53 pathway in vitro. Our data suggest that p53-16 is a potential dual inhibitor of MDM2 and MDMX interactions. The bicyclic stapling strategy is a promising drug design strategy for protein–protein interactions inhibitors.

  • 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.

  • 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.

  • Chaoqun Wang, Ziqiang Deng, Hu Zhang, Rui Liu, Yi Lv
    Chinese Chemical Letters. 2022, 33(3): 1267-1270.

    Magnetic particles (MPs) are the most widely used commercialized engineering particles, which gained great success in various biological applications. Inspired by their intrinsic Fe isotope composition, we discovered a commercialized MPs-internal standard's novel function to realize the accurate quantification of biomolecules. The bioassay of carcinoembryonic antigen (CEA) was chosen as a modal system. The Fe isotope in MPs and Au isotope in report probes were simultaneously and sensitively detected by the elemental mass spectrometry. 197Au/57Fe isotopic ratios and CEA concentrations showed good linearity in the range of 0.6–300 ng/mL, with a detection limit of 0.09 ng/mL (3σ). The accuracy and precision of the proposed MPs-based immunoassay were greatly improved, by eliminating potential MPs loss during magnetic separation and absolute intensity fluctuations. Considering the exceptional availability and universality of commercialized MPs, the proposed method might open a new avenue for MPs' biological applications.

  • 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.

  • Wei Xiang, Mingjie Huang, Xiaohui Wu, Fugang Zhang, Dan Li, Tao Zhou
    Chinese Chemical Letters. 2022, 33(3): 1275-1278.

    This study has demonstrated an interesting amplification effect of magnetic field (MF) on the hydroxylamine (HA)-promoted zero valent iron (ZVI)/H2O2 Fenton-like system. Sulfamethoxazole (SMX) could be efficiently degraded at near neutral pH. Conditional parameters affecting the SMX degradation in the ZVI/H2O2/HA/MF system, e.g., pH and the dosages of ZVI, HA and H2O2, were investigated. Unlike the acid-favorable ZVI/H2O2 and ZVI/H2O2/HA systems, the MF-assisted system exhibited good performances even at pH up to 6.0 and highest degradation rate at pH of 5.0. •OH was still identified as the responsible oxidant. A mechanism involving the MF-enhanced heterogeneous-homogeneous iron cycle was proposed in the near-neutral ZVI/H2O2/HA system. Without MF, HA-induced reductive dissolution of the surface iron oxides occurred and thus leaded to homogeneous Fenton reactions. After the introduction of MF, the gradient magnetic field formed on the ZVI particles would induce the generation of concentration cells of Fe(Ⅱ) and local corrosion of iron. Large amounts of aqueous and bounded Fe(Ⅱ) catalyzed H2O2 to efficiently produce •OH, while HA maintained the surface and bulk cycles of Fe(Ⅱ)/Fe(Ⅲ). The result of study is expected to provide a green, energy-free method in improving the effectiveness of ZVI-based Fenton-like technologies at weak-acidic circumstances.

  • Xin Xu, Ganggang Li, Fenglian Zhang, Guoxia Jiang, Zhengping Hao
    Chinese Chemical Letters. 2022, 33(3): 1279-1282.

    H2S selective catalytic oxidation technology is a prospective way for the treatment of low concentration acid gas with simple process operation and low investment. However, undesirable results such as large formation of SO2 and catalyst deactivation inevitably occur, due to the temperature rise of fixed reaction bed caused by the exothermic reaction. Catalyst with high activity in wide operating temperature window, especially in high temperature range, is urgently needed. In this paper, a series of copper-substituted hexaaluminate catalysts (LaCux, x = 0, 0.5, 1, 1.5, 2, 2.5) were prepared and investigated for the H2S selective oxidation reaction at high temperature conditions (300-550℃). The LaCu1 catalyst exhibited excellent catalytic performance and great stability, which was attributed to the best reductive properties and proper pore structure. Besides, two facile deep processing paths were proposed to eliminate the remaining H2S and SO2 in the tail gas.

  • 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.

  • Dan Shao, Zekang Wang, Cuiping Zhang, Weijia Li, Hao Xu, Guoqiang Tan, Wei Yan
    Chinese Chemical Letters. 2022, 33(3): 1288-1292.

    Despite of the hazardous risk of Pb2+ leakage, lead dioxide has been attributed as a quasi-ideal anode material with high oxygen evolution potential, excellent conductivity, good stability and low cost in electrochemical oxidation wastewater treatment technique. In this study, a novel Ti/PbO2 anode was fabricated by embedding raw materials that are readily and cheaply available, i.e., hairs. The structure-activity relationship of the new electrode was firstly revealed by material and electrochemical characterizations. Then different levels of pollutants (azo dye, phenol and maleic acid) were used to investigate the electrochemical oxidation performance of the new electrode. Finally, the accelerated electrode lifetime and Pb2+ leakage tests were carried out. Results showed that the embedded hairs changed the preferential crystallographic orientation of PbO2 and decreased the grain size. Hairs introduced additional roughness and active sites, and decreased the electrode impedance, especially under 5 mg/cm2 of embedding amount. The removal efficiencies of different target pollutants were enhanced more or less by embedding appropriate amount of hairs, depending on the current density, but loading excessive hairs had a negative effect. The accumulation of intermediate products during phenol degradation was also changed by the hairs. The new electrode could undergo ~550 h of harsh electrolysis. It is also relieved that the Pb2+ leakage was found to be suppressed during this long-term electrolysis process.

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