Chemistry Letters最新文献

英文中文

Theoretical Study on TiOOH Production over Au/TiO₂ Catalyst — Support Dependency of Propylene Oxide Production— Au/TiO2催化剂制备TiOOH的理论研究——环氧丙烷生产的载体依赖性

4区化学 Q3 CHEMISTRY, MULTIDISCIPLINARY

Chemistry Letters

Pub Date : 2023-10-07 DOI: 10.1246/cl.230367

Yasutaka Hamada, Yuki Mishima, Tomohisa Yonemori, Takashi Kawakami, Shusuke Yamanaka, Mitsutaka Okumura

Au supported anatase TiO2 enables the selective synthesis of propylene oxide from propylene using O2 and H2. However, this reaction does not proceed on Au supported rutile TiO2. The origin of this difference in the catalytic activity was examined using DFT calculations. DFT calculations revealed that the stability of the TiOOH active species was directly related to the product selectivity. Au supported anatase TiO2 enables the selective synthesis of propylene oxide from propylene using O2 and H2, while this reaction does not proceed on Au supported rutile TiO2. This difference of the catalytic activity was examined using DFT calculation. From the calculation results, it was found that the stability of TiOOH is directly related to the product selectivity.

Au负载锐钛矿TiO2使丙烯在O2和H2条件下选择性合成环氧丙烷成为可能。然而，在金负载的金红石型TiO2上不发生这种反应。使用DFT计算检查了催化活性差异的起源。DFT计算表明，TiOOH活性物质的稳定性与产物选择性直接相关。金负载型锐钛矿TiO2可以在O2和H2条件下选择性地从丙烯合成环氧丙烷，而金负载型金红石TiO2则不能进行此反应。这种催化活性的差异用DFT计算进行了检验。计算结果表明，TiOOH的稳定性与产物选择性直接相关。

引用次数: 0

Selective Self-Assembly of Gold Nanocrystals using Complementary Leucine Zipper Peptides 利用互补亮氨酸拉链肽选择性自组装金纳米晶体

4区化学 Q3 CHEMISTRY, MULTIDISCIPLINARY

Chemistry Letters

Pub Date : 2023-10-06 DOI: 10.1246/cl.230379

Issei Nakao, Kento Sumida, Mizuki Kitamatsu, Tetsuro Soejima

A heterodimeric leucine zipper (Lz)–based peptide hybrid was utilized as a molecular adhesive to bound two types of gold nanocrystals with different shapes. An acidic leucine zipper (LzE) and a basic leucine zipper (LzK) peptides with terminal cysteine are respectively adsorbed to the surface of spherical gold nanoparticles (LzE–Au NPs) and gold nanocubes (LzK–Au NCs). Transmission electron microscope (TEM) observation and visible (Vis) absorption spectroscopy were revealed that LzE–Au NPs and LzK–Au NCs are selectively self-assembled in water. The dynamic self-assembly behavior is also confirmed by in-situ fluorescence resonance energy transfer between fluorescence dyes connected to LzE and LzK peptides and other control experiments. Complementary acidic leucine zipper (LzE) and basic leucine zipper (LzK) peptides were successfully adsorbed to the surface of spherical gold nanoparticles (Au NPs) and gold nanocubes (Au NCs), respectively. Selective self-assembly of LzE–Au NPs and LzK–Au NCs was occurred by hydrophobic interaction between leucine residues and electrostatic interaction between K (Lys) and E (Glu) amino acids.

以异二聚亮氨酸拉链(Lz)肽杂化物为分子粘合剂，结合了两种不同形状的金纳米晶体。研究了带末端半胱氨酸的酸性亮氨酸拉链肽(LzE)和碱性亮氨酸拉链肽(LzK)分别吸附在球形金纳米粒子(LzE - au NPs)和金纳米立方(LzK - au NCs)表面。透射电镜(TEM)观察和可见(Vis)吸收光谱显示LzE-Au NPs和LzK-Au NCs在水中选择性自组装。通过LzE和LzK肽连接的荧光染料之间的原位荧光共振能量转移以及其他对照实验，也证实了动态自组装行为。互补酸性亮氨酸拉链肽(LzE)和碱性亮氨酸拉链肽(LzK)分别成功吸附在球形金纳米粒子(Au NPs)和金纳米立方(Au NCs)表面。LzE-Au NPs和LzK-Au NCs是通过亮氨酸残基之间的疏水相互作用和K (Lys)和E (Glu)氨基酸之间的静电相互作用选择性自组装的。

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引用次数: 0

A Novel Characteristic of a Water-soluble UV-B Absorber, 2-Phenylbenzimidazole-5-sulfonic Acid: Suppression of Riboflavin-sensitized Singlet Oxygen Generation 水溶性UV-B吸收剂2-苯基苯并咪唑-5-磺酸的新特性:抑制核黄素敏化的单线态氧生成

4区化学 Q3 CHEMISTRY, MULTIDISCIPLINARY

Chemistry Letters

Pub Date : 2023-10-05 DOI: 10.1246/cl.230330

Soichiro Hisanaga, Kazuyuki Miyazawa, Mikio Yagi, Azusa Kikuchi

2-Phenylbenzimidazole-5-sulfonic acid (PBSA) is a water-soluble UV-B absorber used in cosmetic sunscreens. Riboflavin (RF) is a water-soluble vitamin B2. RF is an efficient singlet oxygen photosensitizer. The effects of PBSA on RF-photosensitized singlet oxygen generation have been studied through measurements of transient absorption and time-resolved near-IR phosphorescence in phosphate buffer (pH 7.4). PBSA suppresses the RF-photosensitized singlet oxygen generation. The observed suppression can be ascribed to the quenching of the lowest excited triplet state of RF by PBSA. 2-Phenylbenzimidazole-5-sulfonic acid (PBSA) is a water-soluble UV-B absorber used in cosmetic sunscreens. Riboflavin (RF) is a water-soluble vitamin B2. RF is an efficient singlet oxygen photosensitizer. The effects of PBSA on RF-photosensitized singlet oxygen generation have been studied through measurements of transient absorption and time-resolved near-IR phosphorescence in phosphate buffer (pH 7.4). PBSA suppresses the RF-photosensitized singlet oxygen generation.

2-苯基苯并咪唑-5-磺酸(PBSA)是一种用于化妆品防晒霜的水溶性UV-B吸收剂。核黄素是一种水溶性维生素B2。RF是一种高效的单线态氧光敏剂。通过测量磷酸盐缓冲液(pH 7.4)的瞬态吸收和时间分辨近红外磷光，研究了PBSA对rf光敏单线态产氧的影响。PBSA抑制rf光敏单线态氧的生成。所观察到的抑制可以归因于PBSA对RF最低激发态的猝灭。2-苯基苯并咪唑-5-磺酸(PBSA)是一种用于化妆品防晒霜的水溶性UV-B吸收剂。核黄素是一种水溶性维生素B2。RF是一种高效的单线态氧光敏剂。通过测量磷酸盐缓冲液(pH 7.4)的瞬态吸收和时间分辨近红外磷光，研究了PBSA对rf光敏单线态产氧的影响。PBSA抑制rf光敏单线态氧的生成。

引用次数: 0

Au/Nb₂O₅-Catalyzed N-Formylation of Amines Utilizing High Selectivity to Formate Intermediate in CO₂ Hydrogenation Au/ nb2o5催化氨基n -甲酰化在CO2加氢反应中的高选择性

4区化学 Q3 CHEMISTRY, MULTIDISCIPLINARY

Chemistry Letters

Pub Date : 2023-10-05 DOI: 10.1246/cl.230365

Mitsuyo Hidaka, Mingyue Lin, Hiroki Yamakawa, Akihiro Nakayama, Toru Murayama, Tetsuya Shimada, Shinsuke Takagi, Tamao Ishida

Deformed orthorhombic niobium oxide-supported Au nanoparticles (Au/Nb2O5-DO) exhibited high catalytic activity for N-formylation of amines using CO2 and H2 compared to other Au/Nb2O5 catalysts having different crystalline structures. Au/Nb2O5-DO also showed high selectivity to methyl formate in CO2 hydrogenation. Nb2O5-DO possessed greater amount of acid sites than Au/Nb2O5-T (orthorhombic) and Au/Nb2O5-A (amorphous), which would be beneficial for the formate activation and amine adsorption. Deformed orthorhombic niobium oxide-supported Au nanoparticles (Au/Nb2O5-DO) exhibited high catalytic activity for N-formylation of amines using CO2 and H2 compared to other Au/Nb2O5 catalysts having different crystalline structures. Au/Nb2O5-DO also showed high selectivity to formate in CO2 hydrogenation. Nb2O5-DO possessed greater amount of acid sites than Au/Nb2O5-T (orthorhombic) and Au/Nb2O5-A (amorphous), which would be beneficial for the formate activation and amine adsorption.

与其他具有不同晶体结构的Au/Nb2O5催化剂相比，变形正交氧化铌负载的Au纳米颗粒(Au/Nb2O5- do)在CO2和H2催化n -甲酰化反应中表现出较高的催化活性。Au/Nb2O5-DO在CO2加氢过程中对甲酸甲酯也有较高的选择性。Nb2O5-DO比Au/Nb2O5-T(正晶型)和Au/Nb2O5-A(非晶型)具有更多的酸位，这有利于甲酸酯的活化和胺的吸附。与其他具有不同晶体结构的Au/Nb2O5催化剂相比，变形正交氧化铌负载的Au纳米颗粒(Au/Nb2O5- do)在CO2和H2催化n -甲酰化反应中表现出较高的催化活性。Au/Nb2O5-DO在CO2加氢反应中也表现出较高的选择性。Nb2O5-DO比Au/Nb2O5-T(正晶型)和Au/Nb2O5-A(非晶型)具有更多的酸位，这有利于甲酸酯的活化和胺的吸附。

引用次数: 0

Wrapping of Drug Assembly with Silica Layer and Confinement through Reversible Linkage with Copper(II) for Glutathione-Responsive Nanocapsule 谷胱甘肽响应纳米胶囊中硅层包裹药物组件和铜(II)可逆连接约束

4区化学 Q3 CHEMISTRY, MULTIDISCIPLINARY

Chemistry Letters

Pub Date : 2023-10-05 DOI: 10.1246/cl.230322

Hideki Matsune, Ryoya Yoshida, Ren Ikemizu, Koichiro Shiomori, Tsuyoshi Yamamoto, Masahiro Kishida

Colloidal nano-assembly containing doxorubicin (DOX) is prepared for the first time by co-precipitation with gluconate. The spherical assembly is wrapped with a porous silica layer via sol-gel process, and confined in the formed cage by treatment with copper(II) ions (Cu2+). The reversible linking of DOX with Cu2+ is allowed to suppress the leakage of DOX, but the quick release is turned on in response to glutathione (GSH). The synthesized stimulus-responsive nanocapsules are characterized, and examined in the release test with/without GSH and applied to living HeLa cells. Spherical molecular assembly containig doxorubicin (DOX) is prepared by co-precipitatinon of doxorubicin hydrochloride and sodium gluconate (NaGlc), and then wrapped with porous silica layer via sol-gel process. The permeation of Cu2+ is allowed to suppress the leaking of the contents due to the blocking of the microchannels in the surronding layer, but release DOX immediately in response to glutathione (GSH).

采用葡萄糖酸盐共沉淀法首次制备了含有多柔比星(DOX)的胶体纳米组件。通过溶胶-凝胶法将球形组件包裹在多孔二氧化硅层中，并通过铜(II)离子(Cu2+)处理将其限制在形成的笼中。DOX与Cu2+的可逆连接可以抑制DOX的泄漏，但在谷胱甘肽(GSH)的作用下会开启快速释放。对合成的刺激反应纳米胶囊进行了表征，并在加/不加谷胱甘肽的释放试验中进行了检测，并将其应用于活HeLa细胞。以盐酸阿霉素和葡萄糖酸钠(NaGlc)共沉淀法制备了含阿霉素(DOX)的球形分子组装体，并通过溶胶-凝胶法制备多孔二氧化硅层。Cu2+的渗透被允许抑制由于周围层的微通道阻塞的内容物的泄漏，但立即释放DOX响应谷胱甘肽(GSH)。

引用次数: 0

Stabilization of DNA-encapsulating Droplets through Negative Charge at the Droplet Interface 通过液滴界面负电荷稳定dna包封液滴

4区化学 Q3 CHEMISTRY, MULTIDISCIPLINARY

Chemistry Letters

Pub Date : 2023-10-05 DOI: 10.1246/cl.230294

Mayu Shono, Fumika Fujita, Kenichi Yoshikawa, Akihisa Shioi

It was found that stable cell-sized droplets entrapping DNA molecules are spontaneously generated through micro segregation. To clarify the mechanism, we performed measurements of the electrification by adapting a polymer solution with polyethylene glycol/dextran. We determined the Donnan potential for macroscopic phase segregation in both the presence and absence of DNA, together with the measurements of Zeta potentials of the microphase solution with number of small droplets. We confirmed that the droplets entrapping DNA are negatively charged. Stable cell-sized droplets entrapping DNA are spontaneously generated through micro segregation of polyethylene glycol/dextran solution. To clarify the mechanism, we determined the Donnan potential for macroscopic phase segregation in both with and without DNA, together with the Zeta potential measurements of the microphase solution with number of small droplets. We confirmed that the DNA-encapsulating droplets are negatively charged.

研究发现，细胞大小的稳定液滴包裹DNA分子是通过微分离自发产生的。为了阐明其机理，我们通过采用聚乙二醇/葡聚糖聚合物溶液进行了通电测量。我们确定了存在和不存在DNA时宏观相分离的Donnan电位，以及微相溶液中小液滴数量的Zeta电位的测量。我们证实了包裹DNA的液滴是带负电荷的。通过聚乙二醇/右旋糖酐溶液的微分离，自发地产生了包裹DNA的稳定细胞大小的液滴。为了阐明这一机制，我们测定了含DNA和不含DNA的宏观相分离的Donnan电位，以及含有小液滴的微相溶液的Zeta电位。我们确认包裹dna的液滴带负电荷。

引用次数: 0

Machine Learning Accelerated Discovery of Subnanoparticles for Electrocatalytic Hydrogen Evolution

4区化学 Q3 CHEMISTRY, MULTIDISCIPLINARY

Chemistry Letters

Pub Date : 2023-10-05 DOI: 10.1246/cl.230310

Quan Zou, Akiyoshi Kuzume, Masataka Yoshida, Takane Imaoka, Kimihisa Yamamoto

Metal and alloy subnanoparticles (SNPs) have been anticipated to be a class of promising catalysts because of their fundamental difference from nanoparticles (NPs). In general, the interaction among the surface and bulk atoms of SNPs is significant due to the higher degree of alloying in SNPs than that in NPs counterparts. This study compared the SNPs and NPs concerning their electrocatalytic activities of hydrogen evolution reaction (HER) to understand the essential difference between alloy SNPs and NPs by using machine learning. Phase segregation does not occur on multimetallic subnanoparticles (SNPs), but easily occurs on nanoparticles (NPs), which led to the homogeneously alloying of SNPs and unpredictable phase segregation of NPs. Because of this distinct behavior between SNPs and NPs, the HER activity of SNPs should be easier to predict than NPs. Therefore, machine learning was applied to accelerate the discovery of SNPs.

金属和合金亚纳米颗粒(SNPs)由于其与纳米颗粒(NPs)的根本区别而被认为是一类很有前途的催化剂。一般来说，SNPs的表面原子和体原子之间的相互作用是显著的，因为SNPs的合金化程度高于NPs。本研究通过比较SNPs和NPs在析氢反应(HER)中的电催化活性，通过机器学习了解合金SNPs和NPs的本质区别。多金属亚纳米粒子(SNPs)表面不发生相偏析，但在纳米粒子(NPs)表面容易发生相偏析，导致SNPs的合金化均质化和NPs的相偏析不可预测。由于SNPs和NPs之间的这种不同行为，SNPs的HER活性应该比NPs更容易预测。因此，机器学习被用于加速snp的发现。

引用次数: 0

Indications for echocardiography and confirmation rates of cardiovascular diseases: experience of a specialist cardiac outpatient clinic in Kumasi, Ghana. 超声心动图检查的适应症和心血管疾病的确诊率：加纳库马西心脏病专科门诊的经验。

IF 0.9 4区化学 Q3 CHEMISTRY, MULTIDISCIPLINARY

Chemistry Letters

Pub Date : 2023-10-01 DOI: 10.4103/aam.aam_151_22

Yaw Amo Wiafe, Emmanuel Acheamfour-Akowuah, Isaac Kofi Owusu

Background: Transthoracic echocardiography is a very helpful noninvasive cardiovascular imaging technique for the diagnosis and risk stratification in the management of patients with cardiovascular diseases. We aimed to review the clinical indications for transthoracic echocardiography and the confirmation rate of cardiovascular diseases by echocardiography at a specialist cardiac clinic in Ghana.

Methods: Using a cross-sectional study design, the echocardiography reports of all patients above the age of 15 who were assessed at the clinic were analyzed. Data on patient demographics, clinical history, clinical indication for echocardiography, and the echocardiographic findings were analyzed using version 25.0 of the Statistical Package for Social Sciences (SPSS).

Results: A total of 594 participants were studied. The age range of participants was 15-96 years, with a mean (± standard deviation) age of 53.72 (± 17.25) years. There were more females (50.17%) than males (49.83%). Most (54.21%) of the participants had echocardiography for cardiac evaluation. Other indications included hypertension/hypertensive heart disease (HHD) (n = 131; 22.06%), heart failure (n = 69; 11.62%), chest pains (n = 12; 2.02%), and valvular heart disease (VHD) (n = 11; 1.85%). Three hundred and eight-nine (70.30%) of the participants had their clinical diagnoses confirmed by echocardiography; echocardiographic confirmation rates for heart failure, VHD, and HHD were 92.75%, 90.91%, and 88.54%, respectively.

Conclusion: Echocardiography showed high confirmation rates for our patients with heart failure, VHD, and HHD. Prompt usage of this noninvasive cardiovascular imaging for the initial evaluation of patients with cardiovascular diseases is highly recommended.

背景：经胸超声心动图是一种非常有用的无创心血管成像技术，有助于心血管疾病患者的诊断和风险分层管理。我们的目的是回顾经胸超声心动图的临床适应症以及加纳一家心脏专科诊所的超声心动图心血管疾病确诊率：方法：采用横断面研究设计，分析了在该诊所接受评估的所有 15 岁以上患者的超声心动图报告。使用 25.0 版社会科学统计软件包（SPSS）分析了患者人口统计学、临床病史、超声心动图检查的临床指征和超声心动图检查结果等数据：共有 594 人接受了研究。参与者的年龄范围为 15-96 岁，平均年龄（± 标准差）为 53.72（± 17.25）岁。女性（50.17%）多于男性（49.83%）。大多数参与者（54.21%）进行超声心动图检查是为了评估心脏情况。其他适应症包括高血压/高血压性心脏病（HHD）（131 人；22.06%）、心力衰竭（69 人；11.62%）、胸痛（12 人；2.02%）和瓣膜性心脏病（VHD）（11 人；1.85%）。389名参与者（70.30%）的临床诊断由超声心动图确诊；心衰、VHD和HHD的超声心动图确诊率分别为92.75%、90.91%和88.54%：结论：超声心动图对心衰、VHD 和 HHD 患者的确诊率很高。强烈建议在对心血管疾病患者进行初步评估时及时使用这种无创心血管成像技术。

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引用次数: 0

Antibacterial rattle-type polypyrrole-silver nanocomposite particles synthesized by aqueous chemical oxidative dispersion polymerization 水化学氧化分散聚合法制备抗菌响尾蛇型聚吡咯-银纳米复合粒子

4区化学 Q3 CHEMISTRY, MULTIDISCIPLINARY

Chemistry Letters

Pub Date : 2023-09-30 DOI: 10.1246/cl.230318

Nattawut Rodtuk, Kazusa Takeuchi, Tomoyasu Hirai, Yoshinobu Nakamura, Warayuth Sajomsang, Preeyaporn Chaiyasat, Amorn Chaiyasat, Syuji Fujii

Rattle-type polypyrrole-silver nanocomposite particles were synthesized by aqueous chemical oxidative dispersion polymerization in one step and one pot manner and were characterized in terms of particle size, morphology and chemical composition. The resulting nanocomposite particles could function as an antibacterial agent against Staphylococcus aureus and Escherichia coli. Rattle-type polypyrrole-silver nanocomposite particles were synthesized by aqueous chemical oxidative dispersion polymerization in one step and one pot manner and were characterized in terms of particle size, morphology and chemical composition. The resulting nanocomposite particles could function as an antibacterial agent against Staphylococcus aureus and Escherichia coli.

采用一步一锅水相化学氧化分散聚合法制备了响尾蛇型聚吡咯-银纳米复合粒子，并对其粒径、形貌和化学成分进行了表征。所制备的纳米复合颗粒具有抗金黄色葡萄球菌和大肠杆菌的抗菌作用。采用一步一锅水相化学氧化分散聚合法制备了响尾蛇型聚吡咯-银纳米复合粒子，并对其粒径、形貌和化学成分进行了表征。所制备的纳米复合颗粒具有抗金黄色葡萄球菌和大肠杆菌的抗菌作用。

引用次数: 0

The Effect of Mixed Ligands on the Polymerization Rate of SET-LRP in Aqueous Solution 混合配体对SET-LRP水溶液聚合速率的影响

4区化学 Q3 CHEMISTRY, MULTIDISCIPLINARY

Chemistry Letters

Pub Date : 2023-09-29 DOI: 10.1246/cl.230355

Xiaojing Feng, Wenxia Yuan

The mixed-ligand effect is investigated in single electron transfer-living radical polymerization (SET-LRP) of OEOMA in aqueous solution for the first time. Mediated by equimolar of tris(2-aminoethyl)amine (TREN) and tris(dimethylaminoethyl)amine (Me6-TREN), SET-LRP exhibits the highest polymerization rate while maintains living characteristics. The higher concentration of self-assembled micellar particles formed by amphiphilic initiator and monomer in aqueous solution under the influence of mixed ligands may be considered as one of factors for the mixed-ligand effect. A mixed-ligand effect is observed at 1:1 molar combination of tris(2-dimethylaminoethyl)amine (Me6-TREN) with tris(2-aminoethyl)amine (TREN) during Cu(0) wire-catalyzed single-electron transfer-living radical polymerization (SET-LRP) of OEOMA initiated with PEG-derived initiator in aqueous solution. A higher concentration of self-assembled micellar particles of monomer (or initiator) is proposed as one of the reasons for the mixed-ligand effect.

首次研究了水溶液中OEOMA的单电子转移-活自由基聚合(SET-LRP)的混合配体效应。由三(2-氨基乙基)胺(TREN)和三(二甲氨基乙基)胺(Me6-TREN)等摩尔分子介导的SET-LRP在保持活性特性的同时具有最高的聚合速率。两亲性引发剂和单体在混合配体作用下在水溶液中形成的自组装胶束粒子浓度较高，可以认为是混合配体效应的因素之一。在铜(0)线催化peg引发OEOMA的单电子转移-活性自由基聚合(et - lrp)过程中，三(2-二甲氨基乙基)胺(Me6-TREN)与三(2-氨基乙基)胺(TREN)在水溶液中以1:1摩尔组合时观察到混合配体效应。单体(或引发剂)的自组装胶束粒子浓度较高是混合配体效应的原因之一。

引用次数: 0

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