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  • Yanxia Wang, Jianping Sheng, Xiaoli Zhao, Ye He, Fan Dong, Yanjuan Sun
    Chinese Chemical Letters. 2023, 34(6): 107967-.

    The NO gas is easily oxidized to form toxic by-products (NO2) during the oxidation process, which are adsorbed on the catalyst surface and inhibit the subsequent reaction. For photocatalytic NO removal, a significant challenge is to achieve catalytic stability while maintaining high conversion efficiency. Here, we fabricated a (BiO)2CO3/β-Bi2O3 heterostructure that enables efficient charge transfer and promotes the NO removal. We propose that the catalytic stability depends on the heterojunction structure, which is able to generate interfacial charge transfer channels. In addition, we further introduce graphene quantum dots on the heterojunction structure, which further strengthens the interfacial charge transfer dynamics and finally realizes that the NO2 byproduct could gain electrons and convert to the final product (nitrite or nitrate). This composite structure not only exhibits high activity for NO removal but also maintains long-term stability under visible light.

  • Xiangguo Meng, Siju Bi, Shixin Jin, Kai Wu, Shanchao Wu, Lei Shao, Pierre-Antoine Bonnet, Chunquan Sheng
    Chinese Chemical Letters. 2023, 34(6): 108096-.

    A novel route of enzalutamide was developed in five steps. Starting from 4-amino-2-(trifluoromethyl)benzonitrile (7) and Boc-2-aminoisobutyric acid (16), condensation, deprotection, Ullmann coupling, cyclization and amination provided enzalutamide in 41.0% total yield. This route avoids the using of toxic chemical, unstable intermediate and high-risk reaction. It is a potential efficient and economical procedure for industrialization.

  • Qiuyun Li, Kelu Yan, Yannan Zhu, Gang Qi, Yining Wang, Wen-Juan Hao, Bo Jiang
    Chinese Chemical Letters. 2023, 34(6): 108014-.

    A new Rh(Ⅲ)-catalyzed aldehydic C-H activation/[4 + 3] annulation cascade of N-sulfonyl-2-aminobenzaldehydes with gem-difluorocyclopropenes is reported for the first time, and used to produce a range of hitherto unreported precedented β-monofluorinated benzo[b]azepin-5-ones with good yields and complete regioselectivity. This approach features a broad substrate scope, good functional group tolerance, and high regioselectivity, which may include Rh(Ⅲ)-catalyzed aldehydic C−H activation, tandem site-/regioselective insertion, defluorinated ring-scission, and 1, 2-elimination.

  • Weikang Hu, Ming Yang, Qingyun Yan, Jiahui Ji, Yan Bao, Jinlong Zhang, Mingyang Xing
    Chinese Chemical Letters. 2023, 34(6): 108109-.

    Heterogeneous Fenton has been widely used in the disposal of organic pollutants, however, slow regeneration of Fe(Ⅱ) remains limitation for its practical application of long-term treatment. Herein, we come up with a novel Fe-based heterogeneous Fenton catalyst named as FeSxOy-X (X is the ratio of ethylene glycol to N, N-dimethylformamide). With the help of the abundant defect electrons in Sulfur vacancies, Fe(Ⅱ) regeneration on the surface of FeSxOy-1:1 was accelerated, resulting in a stable proportion of Fe(Ⅱ) on the surface, which maintained continuously stable generation of hydroxyl radical (OH) and singlet oxygen (1O2). Thus, without any organic reagents or cocatalysts, FeSxOy-1:1 based Fenton system achieved effective long-term degradation of 560 mg/L quinoline within only 7 days, which was evidently better than reported FeS and SV-FeS2 (SV: Sulfur vacancy). The system had excellent adaptability to water quality and the COD removal rate of biochemical wastewater was as high as 79.8%.

  • Tiantian Wang, Yu Zhou, Hao Zheng, Tao Shen, Dongmei Wang, Jinlan Zhang
    Chinese Chemical Letters. 2023, 34(6): 107887-.

    Schisandrin A is a natural dibenzocyclooctene lignan with potent neuroprotective activity. However, the specific mechanisms or direct target proteins have not been clarified up to now. In this study, we designed and synthesized the probes of schisandrin A with photoreactive diazirine and clickable alkyne to identify its direct target in SH-SY5Y cells by employing activity-based protein profiling (ABPP) technique. Ykt6 was prominent among the 13 proteins obtained with high confidence and we confirmed Ykt6 as the direct target of schisandrin A by CETSA, IF, SPR and knockdown assay. Functionally, schisandrin A protected the cells against the injury induced by glutamate by regulating autophagy via Ykt6. This discovery may provide a novel therapeutic option for various neuronal cell damage-mediated diseases.

  • Teng Zhou, Xiaohan He, Juncheng Zhao, Liuyong Shi, Liping Wen
    Chinese Chemical Letters. 2023, 34(6): 107667-.

    Nanopore detection is a hot issue in current research. One of the challenges is how to slow down the transport velocity of nanoparticles in nanopores. In this paper, we propose a functional group modified nanopore. That means a polyelectrolyte brush layer is grafted on the surface of the nanopore to change the surface charge properties. The existing studies generally set the charge density of the brush layer to a fixed value. On the contrary, in this paper, we consider an essential property of the brush layer: the volume charge density is adjustable with pH. Thus, the charge property of the brush layer will change with the local H+ concentration. Based on this, we established a mathematical model to study the transport of nanoparticles in polyelectrolyte brush layer modified nanopores. We found that pH can effectively adjust the charge density and even the polarity of the brush layer. A larger pH can reduce the transport velocity of nanoparticles and improve the blockade degree of ion current. The grafting density does not change the polarity of the brush charge. The larger the grafting density, the greater the charge density of the brush layer, and the blockade degree of ion current is also more obvious. The polyelectrolyte brush layer modified nanopores in this paper can effectively reduce the nanoparticle transport velocity and retain the essential ion current characteristics, such as ion current blockade and enhancement.

  • Xianqiang Huang, Weilong Cui, Sen Liu, Gang Liu, Yalin Zhang, Zhihao Zhang, Guodong Shen, Zhen Li, Jianyong Wang, Yifa Chen
    Chinese Chemical Letters. 2023, 34(6): 107692-.

    One-step assembly of organic-ligand modified Pd-Keggin-POMs has been rarely reported, so as for their applications in catalytic benzothiadiazole generation and derived cell-imaging probing. Herein, three Pd-Keggin-POMs (compounds 13) have been successfully synthesized via a one-step assembly strategy. Thus-obtained Pd-Keggin-POMs with well-defined structures and heterogeneous properties enable highly efficient catalytic benzothiadiazole generation. Specifically, compound 3 showed outstanding catalytic activities in Suzuki-Miyaura coupling reactions for the generation of benzothiadiazole derivatives (yields, 90%-97%) and was represented as one of the best catalysts reported to date. Consequently, the obtained benzothiadiazoles were used as the bio-probe for tracking lipid droplets in living-cells and exhibited large Stokes shifts (130 nm), low cytotoxicity and good targeting, which could be also applied to mark the distribution of LDs in living HeLa cells. Systematic investigations clearly decipher the functions of Pd-Keggin-POMs toward finding novel bio-probe materials, highlighting a new insight into the generation of sustainable materials in life-science.

  • Xiaoyang Du, Qian Zhang, Zeyu He, Hui Lin, Gang Yang, Zhenhua Chen, Caijun Zheng, Silu Tao
    Chinese Chemical Letters. 2023, 34(6): 107641-.

    The domain purity, material crystallinity and distribution at the interface between the active layer and the transport layer have an important impact on the performance of organic solar cells (OSCs) and organic photodetectors (OPDs), while this focal issue has received less attention in previous studies. From this perspective, a new method to simultaneously enhance the performance of OSC and OPD is proposed, namely, using a sequential deposition method to first construct a compact stacking structure of dual-donor (D18-Cl:PTO2) eutectic in the donor layer, and then induce the ordered deposition of the acceptor (Y6). Compared with the conventional bulk heterojunction (BHJ), the active layer realized by this method not only improves the crystallinity and stacking order of the constituent material on the surface of the transport layer, but also regulates a good vertical distribution, which is conducive to improving the charge transport and extraction efficiency, reducing the leakage current, and enhancing the stability of the device. As a result, the OSC device based on the D18-Cl:PTO2/Y6 structure achieves a power conversion efficiency of up to 17.65% and good light-degradation stability, which is much better than that of BHJ-based OSC (PCE of 16.37%). For the OPD, the dark current at reverse bias is reduced by more than an order of magnitude, and the maximum responsivity is improved to 0.52 A/W through the optimization of the donor phase at the interface. Moreover, the strategy does not require additional post-processing compared to the BHJ preparation, which reduces the device construction cost and process complexity, providing an effective way for developing high-performance organic optoelectronic devices.

  • Jing Wu, Lei Yang, Xin Liu, Beibei Xiao, Zhimin Ao
    Chinese Chemical Letters. 2023, 34(6): 107659-.

    The electrochemical nitrogen reduction reaction (NRR) for the ammonia production under ambient conditions is regarded as a sustainable alternative to the industrial Haber–Bosch process. However, the electrocatalytic systems that efficiently catalyze nitrogen reduction remain elusive. In the work, the nitrogen reduction activity of the transition metal decorated bismuthene TM@Bis is fully investigated by means of density functional theory calculations. Our results demonstrate that W@Bis delivers the best efficiency, wherein the potential-determining step is located at the last protonation step of *NH2 + H+ + e → *NH3 via the distal mechanism with the limiting potential UL of 0.26 V. Furthermore, the dopants of Re and Os are also promising candidates for experimental synthesis due to its good selectivity, in despite of the slightly higher UL of NRR with the value of 0.55 V. However, the candidates of Ti, V, Nb and Mo delivered the relative lower UL of 0.35, 0.37, 0.41 and 0.43 V might be suffered from the side hydrogen evolution reaction. More interestingly, a volcano curve is established between UL and valence electrons of metal elements wherein W with 4 electrons in d band located at the summit. Such phenomenon originates from the underlying acceptance-back donation mechanism. Therefore, our work provides a fundament understanding for the material design for nitrogen reduction electrocatalysis.

  • Zhijie Zhao, Xiao Fan, Shuoxuan Wang, Xiaoning Jin, Junjie Li, Yuping Wei, Yong Wang
    Chinese Chemical Letters. 2023, 34(6): 107892-.

    Conductive hydrogels have shown great prospects as wearable flexible sensors. Nevertheless, it is still a challenge to construct hydrogel-based sensor with great mechanical strength and high strain sensitivity. Herein, an ion-conducting hydrogel was fabricated by introducing gelatin-dialdehyde β-cyclodextrin (Gel-DACD) into polyvinyl alcohol-borax (PVA-borax) hydrogel network. Natural Gel-DACD network acted as mechanical deformation force through non-covalent cross-linking to endow the polyvinyl alcohol-borax/gelatin-dialdehyde β-cyclodextrin hydrogel (PGBCDH) with excellent mechanical stress (1.35 MPa), stretchability (400%), toughness (1.84 MJ/m3) and great fatigue resistance (200% strain for 100 cycles). Surprisingly, PGBCDH displayed good conductivity of 0.31 S/m after adding DACD to hydrogel network. As sensor, it showed rapid response (168 ms), high strain sensitivity (gage factor (GF) = 8.57 in the strain range of 200%-250%) and reliable sensing stability (100% strain for 200 cycles). Importantly, PGBCDH-based sensor can accurately monitor complex body movements (knee, elbow, wrist and finger joints) and large-scale subtle movements (speech, swallow, breath and facial expressions). Thus, PGBCDH shows great potential for human monitoring with high precision.

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