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The Z-scheme of 2D Structured BCN and Ti MOF Heterojunction High-Efficiency Photocatalytic Hydrogen Evolution 二维结构 BCN 和 Ti MOF 异质结的 Z 型高效光催化氢气发生器
IF 3.3 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-06-27 DOI: 10.1039/d4nj02339k
Cong Liu, Liuxue Zhang, Xuetong Xu, Jiaolong Qiao, Xu Jia, Fuying Wang, Xiulian Wang
Element doping and construction of heterojunction composites were the most common ways to enhance g-C3N4, which were very attractive in achieving high photocatalytic activity. In this study, 2D nanosheet structure BCN was obtained by doping B atom with graphite carbon nitride. Then, Ti MOF was loaded on BCN to obtain a Z-scheme heterojunction composite TBCN through the calcination. Under simulated sunlight, the photocatalytic hydrogen production rate of TBCN heterostructure was 1242 μmol h-1/g, which was 2.2 times than that of BCN and 9.34 times that of bulk graphitic carbon nitrogen-containing (GCN), respectively. The experimental results showed that the construction of Z-scheme heterojunction composite (TBCN) could effectively adjust the material band gap position, expanded the light absorption range, enhanced electron transfer and inhibited the electron-hole recombination, which were crucial for efficient photocatalysis. This study not only provided a strategy for constructing heterojunction composites in the field of g-C3N4 photocatalytic hydrogen evolution, but also deeply analyzed the electron migration direction and the reasons for enhancing carrier separation in the Z-type heterojunction scheme, which provided potential help for subsequent researchers.
元素掺杂和构建异质结复合材料是增强 g-C3N4 的最常见方法,这对实现高光催化活性非常有吸引力。本研究通过在氮化石墨碳中掺杂 B 原子获得了二维纳米片结构 BCN。然后,在 BCN 上负载 Ti MOF,通过煅烧得到 Z 型异质结复合 TBCN。在模拟阳光下,TBCN异质结构的光催化产氢率为1242 μmol h-1/g,分别是BCN的2.2倍和块状含石墨碳氮(GCN)的9.34倍。实验结果表明,构建 Z 型异质结复合材料(TBCN)可有效调整材料带隙位置、扩大光吸收范围、增强电子转移和抑制电子-空穴重组,这些对高效光催化至关重要。该研究不仅为g-C3N4光催化氢气进化领域异质结复合材料的构建提供了策略,而且深入分析了Z型异质结方案中电子迁移方向和载流子分离增强的原因,为后续研究人员提供了潜在的帮助。
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引用次数: 0
Synthesis of 2-fluorinated pyrazolo[1,5-a]pyridines via base- mediated [3+2] cycloaddition of N-aminopyridinium salts with gem-difluorostyrenes 通过碱介导的 N-氨基吡啶鎓盐与宝石二氟苯乙烯的 [3+2] 环加成反应合成 2-氟吡唑并[1,5-a]吡啶
IF 3.3 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-06-27 DOI: 10.1039/d4nj02150a
Yang Feng, Yuanyuan Wu, Zengjiang Yue, Ying Fu, Zhengyin Du
A method for the construction of 2-fluoropyrazolo[1,5-a]pyridines through base-promoted [3+2] cycloaddition of N-aminopyridinium salts with gem-difluorostyrenes has been established. A range of N-heterocycles with 2-fluorinated pyrazo[1,5-a]pyridines were efficiently obtained in moderate to good yields. The impact of different substituents on the reaction was discussed in detail. The protocol shows great potential for the synthesis of valuable fluorinated compounds by utilizing gem-difluorostyrenes as fluoride-containing building blocks.
通过碱促进 N-氨基吡啶鎓盐与二氟苯乙烯的 [3+2] 环加成,建立了一种构建 2-氟吡唑并[1,5-a]吡啶的方法。以中等至良好的产率高效地获得了一系列 N-杂环与 2-氟化吡唑并[1,5-a]吡啶。详细讨论了不同取代基对反应的影响。该方案显示了利用宝石-二氟苯乙烯作为含氟构建模块合成有价值的含氟化合物的巨大潜力。
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引用次数: 0
Promoting reducibility and activity of Cu by tuning oxygen defects on Ceria for selective electrochemical CO2 reduction to methane 通过调节氧化铈上的氧缺陷提高铜的还原性和活性,以选择性电化学方法将二氧化碳还原为甲烷
IF 3.3 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-06-27 DOI: 10.1039/d4nj01772b
Lingwei Yu, Ying Zhang, Leyi Zhou, Yaqi Wang, Xinru Ma, Zhangkun Hou, Hongchuan Zhang, Sai Xie, Zi-Feng Yan
Electrocatalytic reduction of CO2 (CO2RR) to valuable fuels or chemical feedstocks provides a potential pathway to reach carbon-neutral economy and address environmental issues. However, selectively reducing CO2 to methane with high energy density remains a big challenge. The synergistic effect of Cu/oxide active sites and substrate at the interface plays an important role in the catalytic performance. Herein, annealed cerium oxide nanorods (CeO2-x) loaded with Cu were synthesized and showed a high catalytic selectivity to methane. The faradaic efficiency of CH4 reached 52.7% at -1.8 V vs. RHE, in an H-type electrolytic cell. Detailed studies suggested that the enhanced performance of Cu-CeO2-x was attributed mainly to the reducibility of Cu species modulated by high concentration of oxygen vacancies on annealed CeO2-x, which stabilized highly efficient active sites for the electroreduction of CO2 to methane.
电催化还原二氧化碳(CO2RR),将其转化为有价值的燃料或化学原料,为实现碳中和经济和解决环境问题提供了一条潜在的途径。然而,选择性地将二氧化碳还原成高能量密度的甲烷仍然是一个巨大的挑战。铜/氧化物活性位点与底物在界面上的协同效应对催化性能起着重要作用。本文合成了负载铜的退火氧化铈纳米棒(CeO2-x),并显示出对甲烷的高催化选择性。在 H 型电解池中,当电压为 -1.8 V、相对于 RHE 时,CH4 的远催化效率达到 52.7%。详细研究表明,Cu-CeO2-x 性能的提高主要归因于退火 CeO2-x 上高浓度氧空位对 Cu 物种还原性的调节,从而稳定了 CO2 电还原成甲烷的高效活性位点。
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引用次数: 0
Morphology-controllable synthesis of rod-shaped CuO@Co3O4 derived from CuCo-MOF-74 for supercapacitors 由 CuCo-MOF-74 衍生的用于超级电容器的棒状 CuO@Co3O4 形态可控合成技术
IF 3.3 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-06-27 DOI: 10.1039/d4nj01863j
Bo Sun, Man Li, Lifeng Cheng, Qijian Li, Xiaowen Chen, Shengqi Wang, Wenhua Yan, Lei Wang, Fuxiang Wei, Qingliang Wang
Transition metal oxides (TMOs) have excellent electrochemical properties. However, they are commonly associated with short cycle lives, agglomeration, and lower electrical conductivity. To ameliorate these drawbacks, porous rod-shaped CuO@Co3O4 has been synthesized through calcination with optimized oxidation temperature by using CuCo-MOF-74 as a template. Due to the porous structure, the CuO@Co3O4 electrode significantly increases the contact area with the electrolyte and greatly improves the reaction kinetics. As a result, the CuO@Co3O4 electrode exhibits excellent electrochemical performance with a specific capacitance of 545.5 F g−1 at a current density of 1 A g−1. The capacitance retention at 10 A g−1 was 88.7% after 10 000 cycles. Furthermore, an asymmetric supercapacitor (SC) has been assembled with CuO@Co3O4 as the positive electrode and commercial reduced graphene oxide (RGO) as the negative electrode, and the device has exhibited an energy density of 38.2 W h kg−1 at a power density of 1268.3 W kg−1. Impressively, the capacitance retention remained 83.2% even after 10 000 cycles at a high current density of 10 A g−1. This performance has demonstrated the potential of CuO@Co3O4 as an anode material for SCs.
过渡金属氧化物(TMO)具有优异的电化学特性。然而,它们通常具有循环寿命短、团聚和导电性较低等缺点。为了改善这些缺点,我们以 CuCo-MOF-74 为模板,在优化的氧化温度下通过煅烧合成了多孔棒状 CuO@Co3O4。由于具有多孔结构,CuO@Co3O4 电极大大增加了与电解质的接触面积,极大地改善了反应动力学。因此,CuO@Co3O4 电极表现出优异的电化学性能,在电流密度为 1 A g-1 时,比电容为 545.5 F g-1。在 10 A g-1 条件下,10 000 次循环后的电容保持率为 88.7%。此外,以 CuO@Co3O4 为正极、商用还原氧化石墨烯 (RGO) 为负极组装了一种不对称超级电容器 (SC),该器件在功率密度为 1268.3 W kg-1 时的能量密度为 38.2 W h kg-1。令人印象深刻的是,在 10 A g-1 的高电流密度下,即使经过 10 000 次循环,电容保持率仍高达 83.2%。这一性能证明了 CuO@Co3O4 作为 SC 负极材料的潜力。
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引用次数: 0
The synthesis of oligomers containing alternating C-glycosyl α-amino acids and proteinogenic α-amino acids 含有交替的 C-糖基 α-氨基酸和蛋白源 α-氨基酸的低聚物的合成
IF 3.3 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-06-26 DOI: 10.1039/d4nj02059f
Ivana Colić, Barbara Bogović, Ivanka Jerić
C-Glycosyl amino acids are a group of C-glycosides in which a carbohydrate molecule is attached to the side chain or backbone of the amino acid via a C–C bond. Despite the numerous methods that have been developed for their synthesis, the C-glycosyl α-amino acids and their oligomers are relatively unexplored. In this work, we presented a protocol for the synthesis of oligomers containing alternating C-glycosyl α-amino acids and proteinogenic α-amino acids. The methodology is based on the modification of α-acyloxyamides obtained from the Passerini reaction using α-D-galactopyranose- and α-L-sorbofuranose-derived aldehydes as C-glycosyl donors. The protocol enabled the synthesis of homo- and heterochiral tetramers, and homo- and heterovalent tetramers in very good yields.
C-糖基氨基酸是一组 C-糖苷,其中碳水化合物分子通过 C-C 键连接到氨基酸的侧链或骨架上。尽管合成 C-糖基 α-氨基酸的方法层出不穷,但对它们及其低聚物的研究却相对较少。在这项工作中,我们提出了一种交替合成含有 C-糖基 α-氨基酸和蛋白源 α-氨基酸的低聚物的方法。该方法基于使用源自 α-D 吡喃半乳糖和 α-L 呋喃山梨糖的醛作为 C-糖基供体,对 Passerini 反应中得到的 α-acyloxyamides 进行修饰。该方案能够以非常高的产率合成同手性和异手性四聚体以及同价和异价四聚体。
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引用次数: 0
Amphiphilic cyclodextrin derivatives with antibacterial activity: chemical mutation and structure–activity relationship 具有抗菌活性的两性环糊精衍生物:化学突变与结构-活性关系
IF 3.3 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-06-26 DOI: 10.1039/d4nj01874e
Hatsuo Yamamura, Ayame Kato, Eri Yamada, Hisato Kato, Takashi Katsu, Kazufumi Masuda, Kayo Osawa, Atsushi Miyagawa
The relationship between the membrane-disrupting antibacterial activities and the structures of cyclodextrin derivatives containing cationic and hydrophobic moieties was investigated.
研究了膜破坏抗菌活性与含有阳离子和疏水分子的环糊精衍生物结构之间的关系。
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引用次数: 0
Ixora coccinea flowers derived green luminescent carbon quantum dots for Fe3+ recognition and preparation of Pd nanoparticles for the Suzuki- Miyaura coupling and cyanation process 用于识别 Fe3+ 的 Ixora coccinea 花衍生绿色发光碳量子点以及制备用于铃木-宫浦偶联和氰化过程的 Pd 纳米粒子
IF 3.3 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-06-26 DOI: 10.1039/d4nj02217c
Kulathu Iyer Sathiyanarayanan, Namrata Priyadarshini Hota
The solvothermal method of producing spherically shaped and highly fluorescent tiny shaped (~3 nm) nitrogen-doped carbon quantum dots (NCQDs) with high quantum yield (43%) from Ixora coccinea flowers and o-Phenylenediamine has been approached sustainably. Since this NCQD exhibits excitation-dependent fluorescence activity, it was used to detect the Fe3+ ion selectively in real-time with human blood serum because it is a component of human blood. The Limit of Detection (LOD) of NCQD was found to be 60nM. We also synthesized palladium nanoparticles utilizing NCQDs without additional reducing or stabilizing agents because these quantum dots serve as both. Numerous characterization techniques were used to characterize the nanoparticle, and all the characterizations showed the presence of NCQD which stabilizes the nanoparticle. Palladium nanoparticles' small size (4 nm) and large surface area (35.77 m2/g) enable them to exhibit strong catalytic activity in Suzuki-Miyaura coupling and cyanation processes. It is obvious that synthetic palladium nanoparticles and NCQD have a variety of uses in the field of catalysis and sensing respectively.
我们采用溶热法从 Ixora coccinea 花和邻苯二胺中制备出了高量子产率(43%)的球形高荧光微小形状(约 3 nm)氮掺杂碳量子点(NCQDs)。由于这种 NCQD 具有依赖激发的荧光活性,因此它被用来实时选择性地检测人体血清中的 Fe3+ 离子,因为它是人体血液的一种成分。结果发现,NCQD 的检测限(LOD)为 60nM。我们还利用 NCQD 合成了钯纳米粒子,无需额外的还原剂或稳定剂,因为这些量子点同时具有还原剂和稳定剂的作用。我们使用了大量的表征技术对纳米粒子进行表征,所有表征结果都表明,NCQD 的存在稳定了纳米粒子。钯纳米粒子尺寸小(4 nm),比表面积大(35.77 m2/g),因此在铃木-米亚乌拉偶联和氰化过程中具有很强的催化活性。显然,合成的钯纳米粒子和 NCQD 分别在催化和传感领域具有多种用途。
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引用次数: 0
Nanoconstruction of curcuminoid boron difluoride dyes with aggregation-induced emission for high-light fluorescence imaging of malignant tumor 具有聚集诱导发射的姜黄二氟化硼染料的纳米结构,用于恶性肿瘤的高亮荧光成像
IF 3.3 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-06-26 DOI: 10.1039/d4nj01682c
Ziwei Zhao, Susu Yan, Yanan Li
Curcuminoid boron difluoride dyes have garnered significant attention in the realm of bioimaging, primarily due to their excellent photophysicochemical properties. However, the strong hydrophobicity limits their optimal near-infrared (NIR) fluorescence emission, and the synthesis process is complicated. In this study, Curc-TPA, a curcuminoid boron difluoride derivative with high fluorescence quantum yield, was simply synthesized and surprisingly exhibited aggregation-induced NIR emission in dimethyl sulfoxide/water mixture. The compound self-assembled into stable and homogeneous nanoparticles through hydrophobic interaction with amphiphilic polymer 1,2-distearoyl-sn-glycero-3-phosphoethanolamine-poly(ethylene glycol), which showed enhanced aggregation-induced emission (AIE) capacity in the NIR region. The nanoparticles specifically enriched at the tumor site due to enhanced penetration and retention effect and exhibited bright fluorescence imaging in vitro and in vivo. Notably, they showed satisfactory hematological compatibility and unobservable cellular and histological toxicity. Therefore, it is of promising clinical significance in the AIE-enhanced NIR fluorescence imaging-visualized precise diagnosis of cancer.
莪术二氟化硼染料在生物成像领域备受关注,这主要是因为它们具有出色的光物理化学特性。然而,强烈的疏水性限制了其最佳的近红外(NIR)荧光发射,而且合成过程复杂。本研究简单合成了具有高荧光量子产率的姜黄二氟化硼衍生物 Curc-TPA,并在二甲亚砜/水混合物中令人惊讶地表现出聚集诱导的近红外发射。该化合物通过与两性聚合物 1,2-二硬脂酰-sn-甘油-3-磷乙醇胺-聚乙二醇的疏水作用自组装成稳定、均质的纳米颗粒,在近红外区域显示出更强的聚集诱导发射(AIE)能力。由于穿透和滞留效应增强,这些纳米粒子在肿瘤部位特异性富集,并在体外和体内显示出明亮的荧光成像。值得注意的是,它们显示出令人满意的血液学相容性和不可观察到的细胞和组织学毒性。因此,AIE 增强近红外荧光成像可视化精确诊断癌症具有重要的临床意义。
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引用次数: 0
Effect of cis/trans isomerization on the photochromic performance of triphenylethylene 顺式/反式异构化对三苯乙烯光致变色性能的影响
IF 3.3 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-06-26 DOI: 10.1039/d4nj02060j
Zhuocheng Li, hao Cui, suhang Xu, Zihang Zhang, Zuoqin Liang, Changqing Ye, Xiaomei Wang
Revealing the structure-property relationships is crucial for promoting the development of photochromic materials and achieving the desired function in practical applications. Herein, a series of triphenylethylene photochromic materials (TP, TP-F, TP-Cl and TP-Br) have been synthesized and their photochromic properties were investigated. Monohalogenated TP-F, TP-Cl and TP-Br display obvious photochromic behaviors in solution, solid state and polymer film. It is found that the halogen atoms with weak electron withdrawing ability can dramatically enhance the photocolorabilities of triphenylethylene. Moreover, TP-Cl and TP-Br exhibit different fatigue processes from TP-F. The further characterization reveals that the key factor leading to the diverse photochromic properties is cis/trans isomerization of triphenylethylene. The coloration of triphenylethylene mainly comes from the photo-triggered cyclization of cis-isomers. The initial attenuation of TP-Cl and TP-Br under UV irradiation is mainly caused by cis-trans photoisomerization, rather than the oxygen-involved photooxidation reactions. Based on the controllable “turn-on” and “turn-off” photobehaviors, TP-Cl and TP-Br were applied in the photoswitchable patterns, showing enhanced signal-to-background ratio.
揭示结构-性能关系对于促进光致变色材料的发展以及在实际应用中实现所需的功能至关重要。本文合成了一系列三苯乙烯光致变色材料(TP、TP-F、TP-Cl 和 TP-Br),并研究了它们的光致变色性能。单卤化 TP-F、TP-Cl 和 TP-Br 在溶液、固态和聚合物薄膜中均表现出明显的光致变色行为。研究发现,取电子能力较弱的卤素原子能显著增强三苯乙烯的光致变色能力。此外,TP-Cl 和 TP-Br 表现出与 TP-F 不同的疲劳过程。进一步的特性分析表明,导致三苯基乙烷具有不同光致变色特性的关键因素是三苯基乙烷的顺/反异构化。三苯乙烯的着色主要来自光触发的顺式异构体环化。在紫外线照射下,TP-Cl 和 TP-Br 的初始衰减主要是由顺式-反式光异构化引起的,而不是氧参与的光氧化反应。基于可控的 "开启 "和 "关闭 "光行为,TP-Cl 和 TP-Br 被应用于光电开关模式,显示出更高的信噪比。
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引用次数: 0
Correction: Exploring high-energy and low-sensitivity energetic compounds based on experiments and DFT studies 更正:基于实验和 DFT 研究探索高能量和低灵敏度高能化合物
IF 3.3 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-06-26 DOI: 10.1039/d4nj90088j
Caijin Lei, Qiaoli Li, Shenshen Li, Hongwei Yang, Jijun Xiao, Guangbin Cheng
Correction for ‘Exploring high-energy and low-sensitivity energetic compounds based on experiments and DFT studies’ by Qiaoli Li et al., New J. Chem., 2023, 47, 19523–19528, https://doi.org/10.1039/D3NJ03514J.
对李巧丽等 "基于实验和 DFT 研究的高能低敏高能化合物探索 "的更正,《新化学杂志》,2023 年,47 期,19523-19528,https://doi.org/10.1039/D3NJ03514J。
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引用次数: 0
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