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High sensitivity artificial synapses using printed high-transmittance ITO fibers for neuromorphic computing 利用印刷高透射率 ITO 纤维实现神经形态计算的高灵敏度人工突触
IF 9.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-05-20 DOI: 10.1016/j.cclet.2024.110030

Artificial synapses are essential building blocks for neuromorphic electronics. Here, solid polymer electrolyte-gated artificial synapses (EGASs) were fabricated using ITO fibers as channels, which possess an ultra-high sensitivity of 5 mV and a long-term memory time exceeding 3 min. Notably, digitally printed ITO-fiber arrays exhibit an ultra-high transmittance of approximately 99.67 %. Biological synaptic plasticity, such as excitatory postsynaptic current, paired-pulse facilitation, spike frequency-dependent plasticity, and synaptic potentiation and depression, were successfully mimicked using the EGASs. Based on the synaptic properties of the EGASs, an artificial neural network was constructed to perform supervised learning using the Fashion-MNIST dataset, achieving high pattern recognition rate (82.39 %) due to the linear and symmetric synaptic plasticity. This work provides insights into high-sensitivity artificial synapses for future neuromorphic computing.

人工突触是神经形态电子学的重要组成部分。在这里,我们利用 ITO 纤维作为通道,制造出了固体聚合物电解质门控人工突触(EGAS),它具有 5 mV 的超高灵敏度和超过 3 分钟的长期记忆时间。值得注意的是,数字印刷的 ITO 纤维阵列具有约 99.67% 的超高透射率。利用 EGAS 成功模拟了生物突触可塑性,如兴奋性突触后电流、成对脉冲促进、尖峰频率依赖性可塑性以及突触电位和抑制。根据 EGASs 的突触特性,构建了一个人工神经网络,利用时尚-MNIST 数据集进行监督学习,由于突触的线性和对称可塑性,实现了较高的模式识别率(82.39%)。这项工作为未来神经形态计算的高灵敏度人工突触提供了深入见解。
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引用次数: 0
Sonoafterglow luminescence for in vivo deep-tissue imaging 用于体内深层组织成像的声后辉发光技术
IF 9.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-05-18 DOI: 10.1016/j.cclet.2024.110026
Shihong Wu , Ronghui Zhou , Hang Zhao , Peng Wu
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引用次数: 0
A cucurbit[8]uril-based supramolecular phosphorescent assembly: Cell imaging and sensing of amino acids in aqueous solution 基于葫芦[8]脲的超分子磷光组件:细胞成像和水溶液中氨基酸的传感
IF 9.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-05-17 DOI: 10.1016/j.cclet.2024.110022

In recent years, host-guest interactions of macrocycles have emerged as a promising approach to effectively enhance pure organic room-temperature phosphorescence by inhibiting the nonradiative relaxation while isolating the effects of oxygen and water molecules. In this work, a supramolecular assembly Q[8]-BCPI was constructed by 6-bromoisoquinoline derivative (BCPI) and cucurbit[8]uril (Q[8]). The assembly produced intense green room temperature phosphorescence (RTP) emission and enabled supramolecular recognition and detection of l-tryptophan (L-Trp) and l-tyrosine (L-Tyr). Moreover, the Q[8]-BCPI assembly showed good biocompatibility and low biotoxicity, and had a good staining effect on HeLa cells.

近年来,通过抑制非辐射弛豫,同时隔离氧分子和水分子的影响,大环的主客体相互作用已成为有效增强纯有机物室温磷光的一种有前途的方法。在这项工作中,6-溴异喹啉衍生物(BCPI)和葫芦[8]脲(Q[8])构建了一种超分子组装体 Q[8]-BCPI。该组装体产生了强烈的绿色室温磷光(RTP)发射,并实现了对 l-色氨酸(L-Trp)和 l-酪氨酸(L-Tyr)的超分子识别和检测。此外,Q[8]-BCPI 组件具有良好的生物相容性和较低的生物毒性,对 HeLa 细胞具有良好的染色效果。
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引用次数: 0
Photocatalyst/metal-free sequential C–N/C–S bond formation: Synthesis of S-arylisothioureas via photoinduced EDA complex activation 光催化剂/无金属顺序 C-N/C-S 键形成:通过光诱导 EDA 复合物活化合成 S-芳基异硫脲类化合物
IF 9.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-05-17 DOI: 10.1016/j.cclet.2024.110024

A photocatalyst-free visible-light-promoted three-component reaction of thianthrenium salts, isothiocyanates, and amines is presented, which affords a rapid and efficient approach to S-arylisothioureas under mild conditions. This developed method exhibits the advantages of readily available raw materials, broad substrate scope, good functional tolerance, and operational simplicity. It is worth mentioning that the byproduct thianthrene can be recycled in quantity, ultimately maximizing the atomic economy of the reaction and avoiding chemical waste. Mechanism investigations support the strategy involving a photoinduced EDA complex.

本文介绍了一种无光催化剂可见光促进的噻吩鎓盐、异硫氰酸盐和胺的三组分反应,它提供了一种在温和条件下快速高效地制备 S-芳基异硫脲的方法。该方法具有原料易得、底物范围广、功能耐受性好和操作简单等优点。值得一提的是,副产品噻蒽可以大量回收利用,最终最大限度地提高了反应的原子经济性,避免了化学废物的产生。机理研究支持涉及光诱导 EDA 复合物的策略。
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引用次数: 0
20 nm-ultra-thin fluorosiloxane interphase layer enables dendrite-free, fast-charging, and flexible aqueous zinc metal batteries 20 纳米超薄氟硅氧烷相间层实现了无枝晶、快速充电和灵活的水性锌金属电池
IF 9.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-05-17 DOI: 10.1016/j.cclet.2024.110025

Dendrite growth of zinc (Zn) anode at high current density severely affects the fast-charging performance of aqueous zinc metal batteries (AZMBs). While interfacial modification strategies can optimize Zn performance, challenges such as complicated preparation processes, excessive layer thicknesses, and high voltage hysteresis should be addressed. Herein, we utilize a cost-effective liquid fluorosiloxane, (3,3,3-trifluoropropyl)trimethoxysilane, for scalable modification of Zn foil via drop-casting at room temperature, resulting in an ultra-thin interphase layer of only 20 nm. The Si-O-Zn bonds formed between fluorosiloxane and Zn ensure interfacial stability, and the Si-O-Si bonds between fluorosiloxane molecules help to homogenize the electric field distribution. Additionally, the abundant highly electronegative fluorine atoms on the anode surface act as zincophilic sites, promoting the uniform deposition of Zn2+. Thus, the modified Zn foil (SiFO-Zn) exhibits excellent dendrite suppression, reduced voltage hysteresis, and prolonged cycle life at ultra-high current density (40 mA/cm2), achieving a cumulative areal capacity of 12.9 Ah/cm2. Further, the full cell assembled with 10 μm-thick SiFO-Zn anode and MnO2 cathode achieves 2600 cycles at 5 A/g with minimal capacity degradation, and a large-size (22.5 cm−2) pouch cell powers the light-emitting diode even after reverse bending, demonstrating the potential of AZMBs for fast-charging flexible devices.

锌(Zn)阳极在高电流密度下的枝晶生长严重影响了锌金属水电池(AZMB)的快速充电性能。虽然界面改性策略可以优化锌的性能,但仍需解决制备工艺复杂、层厚度过大和高压滞后等难题。在本文中,我们利用一种具有成本效益的液态氟硅氧烷--(3,3,3-三氟丙基)三甲氧基硅烷,在室温下通过滴注法对 Zn 箔进行了可扩展的改性,从而形成了仅 20 纳米的超薄相间层。氟硅氧烷和 Zn 之间形成的 Si-O-Zn 键确保了界面稳定性,氟硅氧烷分子之间的 Si-O-Si 键有助于均匀电场分布。此外,阳极表面丰富的高电负性氟原子可作为亲锌位点,促进 Zn2+ 的均匀沉积。因此,改性锌箔(SiFO-Zn)在超高电流密度(40 mA/cm2)条件下表现出卓越的枝晶抑制能力,降低了电压滞后,延长了循环寿命,实现了 12.9 Ah/cm2 的累积面积容量。此外,由 10 μm 厚的 SiFO-Zn 阳极和 MnO2 阴极组装而成的全电池在 5 A/g 的条件下可循环使用 2600 次,且容量衰减极小;即使在反向弯曲后,大尺寸(22.5 cm-2)袋状电池也能为发光二极管供电,这证明了 AZMB 在柔性设备快速充电方面的潜力。
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引用次数: 0
Selenium nanoparticles enhance the chemotherapeutic efficacy of pemetrexed against non-small cell lung cancer 硒纳米粒子增强培美曲塞对非小细胞肺癌的化疗效果
IF 9.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-05-16 DOI: 10.1016/j.cclet.2024.110018

Selenium (Se) plays an important role in the development and treatment of lung cancer, yet its specific mechanisms remain elusive. Lower Se level in serum was noted in lung cancer patients compared to normal controls. Therefore, developing effective therapeutic adjuvants containing Se might benefit the treatment of lung cancer patients. This study aimed to investigate the association between Se and the chemotherapeutic efficacy of lung cancer. Lentinan-modified selenium nanoparticles (LET-SeNPs) were created to develop and verify the effectiveness of Se containing adjuvant applied with pemetrexed on lung cancer cells. A synergistic effect was observed between LET-SeNPs and pemetrexed in vitro. The combination of LET-SeNPs and pemetrexed could induce reactive oxygen species overproduction, mitochondrial dysfunction and DNA damage, ultimately leading to cancer cell apoptosis. It is implied that LET-SeNPs might be a promising sensitizer to pemetrexed chemotherapy and could potentially enhance chemotherapy efficiency in non-small cell lung cancer.

硒(Se)在肺癌的发展和治疗中发挥着重要作用,但其具体机制仍难以捉摸。与正常对照组相比,肺癌患者血清中的硒含量较低。因此,开发有效的含 Se 辅助治疗剂可能对肺癌患者的治疗有益。本研究旨在探讨 Se 与肺癌化疗疗效之间的关系。研究人员制作了龙胆素修饰的硒纳米粒子(LET-SeNPs),以开发和验证含Se的辅助剂与培美曲塞一起应用对肺癌细胞的疗效。在体外实验中,LET-SeNPs 与培美曲塞之间产生了协同效应。LET-SeNPs 与培美曲塞的结合可诱导活性氧过量产生、线粒体功能障碍和 DNA 损伤,最终导致癌细胞凋亡。这意味着 LET-SeNPs 可能是培美曲塞化疗的增敏剂,并有可能提高非小细胞肺癌的化疗效率。
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引用次数: 0
Imaging polarity changes in pneumonia and lung cancer using a lipid droplet-targeted near-infrared fluorescent probe 利用脂滴靶向近红外荧光探针成像肺炎和肺癌的极性变化
IF 9.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-05-16 DOI: 10.1016/j.cclet.2024.110020

As the main organ of gas exchange, the lungs are susceptible to various exogenous attacks, and pneumonia is one of the major inflammatory diseases that threaten human health. Generally, pneumonia is a disease that occurs in the alveoli and respiratory bronchioles induced by pathogens and further causes local and systemic inflammatory responses. The development of pneumonia can bring various serious complications, including lung abscess, sepsis, meningitis, brain damage and hearing loss. Over the past few decades, the mortality rate of pneumonia patients has remained high. While lung cancer is another lung-related malignant tumors worldwide, with a low 5 year survival rate. Exploring the mechanisms of their occurrence and interaction between pneumonia and lung cancer is a challenging and meaningful task. The abnormalities of lipid droplets (LDs) polarity have been found strongly accompanied by many diseases, especially cancer, inflammation, and metabolic diseases. However, their exact role is not yet clear. Hence, it is significant to develop a novel detection method to observe the polarity changes of LDs, which would help to reveal the development process of diseases pneumonia and lung cancer. In this work, a new polarity-sensitive LDs-targeted near-infrared probe BFZ up to 712 nm was designed, according to the intramolecular charge transfer mechanism, which displayed high fluorescence intensity in low polarity while showing decreased fluorescence intensity in high-polarity conditions with a significant redshift. The BFZ was successfully applied to the change of LDs polarity in lipopolysaccharide (LPS)-stimulated A549 cells, and a mouse model of lung inflammation. It also tells the polarity differences between normal and tumor cells and between normal and tumor tissues. Moreover, the correlations between pneumonia and polarity changes were observed through the imaging experiments, which may provide an insightful method for the early diagnosis of pneumonia and lung cancer.

作为气体交换的主要器官,肺容易受到各种外源性侵袭,而肺炎则是威胁人类健康的主要炎症性疾病之一。一般来说,肺炎是由病原体诱发发生在肺泡和呼吸支气管,并进一步引起局部和全身炎症反应的疾病。肺炎的发生会带来各种严重的并发症,包括肺脓肿、败血症、脑膜炎、脑损伤和听力丧失。过去几十年来,肺炎患者的死亡率一直居高不下。而肺癌是世界上另一种与肺有关的恶性肿瘤,5 年生存率很低。探索肺炎和肺癌的发生和相互作用机制是一项具有挑战性和意义的任务。脂滴极性异常已被发现与多种疾病密切相关,尤其是癌症、炎症和代谢性疾病。然而,它们的确切作用尚不明确。因此,开发一种新型检测方法来观察脂滴极性的变化意义重大,这将有助于揭示肺炎和肺癌等疾病的发展过程。本研究根据分子内电荷转移机制,设计了一种对极性敏感的新型 LDs 靶向近红外探针 BFZ,其波长可达 712 nm,在低极性条件下表现出较高的荧光强度,而在高极性条件下荧光强度下降,并有明显的红移。BFZ 成功应用于脂多糖(LPS)刺激的 A549 细胞和小鼠肺部炎症模型中 LDs 极性的变化。它还揭示了正常细胞与肿瘤细胞、正常组织与肿瘤组织之间的极性差异。此外,通过成像实验还观察到肺炎与极性变化之间的相关性,这可能为肺炎和肺癌的早期诊断提供一种有启发性的方法。
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引用次数: 0
CoSe2 nanowire array enabled highly efficient electrocatalytic reduction of nitrate for ammonia synthesis CoSe2 纳米线阵列可高效电催化硝酸盐还原合成氨
IF 9.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-05-14 DOI: 10.1016/j.cclet.2024.110005

The electrocatalytic reduction of nitrate (NO3) not only facilitates the environmentally sustainable production of ammonia (NH3) but also purifies water by removing NO3, thereby transforming waste into valuable resources. The process of converting NO3 to NH3 is complex, involving eight electron transfers and multiple intermediates, making the choice of electrocatalyst critical. In this study, we report a cobalt selenide (CoSe2) nanowire array on carbon cloth (CoSe2/CC) as an effective electrocatalyst for the NO3 to NH3 conversion. In an alkaline medium with 0.1 mol/L NO3, CoSe2/CC demonstrates exceptional NH3 Faradaic efficiency of 97.6 % and a high NH3 yield of 517.7 µmol h–1 cm–2 at –0.6 V versus the reversible hydrogen electrode. Furthermore, insights into the reaction mechanism of CoSe2 in the electrocatalytic NO3 reduction are elucidated through density functional theory calculations.

硝酸盐(NO3-)的电催化还原不仅有助于以环境可持续的方式生产氨气(NH3),还能通过去除 NO3- 净化水质,从而变废为宝。将 NO3- 转化为 NH3 的过程非常复杂,涉及 8 次电子转移和多个中间产物,因此选择电催化剂至关重要。在本研究中,我们报告了一种碳布上的硒化钴(CoSe2)纳米线阵列(CoSe2/CC),它是将 NO3- 转化为 NH3 的有效电催化剂。在含有 0.1 mol/L NO3- 的碱性介质中,CoSe2/CC 与可逆氢电极相比,在 -0.6 V 电压下的 NH3 法拉效率高达 97.6 %,NH3 产率高达 517.7 µmol h-1 cm-2。此外,还通过密度泛函理论计算阐明了 CoSe2 在电催化还原 NO3- 过程中的反应机理。
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引用次数: 0
Interface engineering of 2D NiFe LDH/NiFeS heterostructure for highly efficient 5-hydroxymethylfurfural electrooxidation 用于高效 5-hydroxymethylfurfural 电氧化的二维 NiFe LDH/NiFeS 异质结构的界面工程设计
IF 9.4 1区 化学 Q1 Chemistry Pub Date : 2024-05-14 DOI: 10.1016/j.cclet.2024.110011
Lili Wang , Ya Yan , Rulin Li , Xujie Han , Jiahui Li , Ting Ran , Jialu Li , Baichuan Xiong , Xiaorong Song , Zhaohui Yin , Hong Wang , Qingjun Zhu , Bowen Cheng , Zhen Yin

The electrochemical oxidation of 5-hydroxymethylfurfural (HMF) to valuable chemicals is an efficient way to upgrade biomass molecules and replace traditional catalytic synthesis. It is crucial to develop efficient and low-cost earth-abundant electrocatalysts to enhance catalytic performance of HMF oxidation. Herein, a new type of two-dimensional (2D) hybrid arrays consisting of NiFe layered double hydroxides (LDH) nanosheets and bimetallic sulfide (NiFeS) is constructed via interface engineering for efficient electrocatalytic oxidation of HMF to 2,5-furandicarboxylic acid (FDCA). The preparation process of 2D NiFe LDH/NiFeS with ultrathin heterostructure involves in anchoring a Co-based metal-organic framework (Co MOF) as template onto the carbon cloth (CC) via in-situ growth, formation of NiFe LDH on the surface of Co MOF and subsequent partial sulfidation. The electrocatalyst of NiFe LDH/NiFeS exhibits outstanding performance towards HMF oxidation, about 98.5% yield for FDCA and 97.2% Faraday efficiency (FE) in the alkaline electrolyte with 10 mmol/L HMF, as well as excellent stability retaining 90.1% FE for FDCA after six cycles test. Moreover, even at an HMF concentration of 100 mmol/L, the yield and FE for FDCA remain high at 83.6% and 93.6%, respectively. These findings highlight that 2D heterostructure containing abundant interfaces between NiFe LDH nanosheets and NiFeS can enhance the intrinsic activity of LDH and thus promote the oxidation reaction kinetics. Additionally, the synergistic effect of the bimetallic NiFe compounds also improved the selectivity of HMF conversion to FDCA. Our present work demonstrates that constructing 2D ultrathin heterostructure of NiFe LDH/NiFeS is a facile strategy via interface engineering to enhance the intrinsic activity of LDH electrocatalysts, which would open new avenues toward low-cost and advanced 2D nanocatalysts for sustainable energy conversion and electrochemical valorization of biomass derivatives.

将 5-hydroxymethylfurfural (HMF) 电化学氧化为有价值的化学品是提升生物质分子等级和取代传统催化合成的有效方法。开发高效、低成本的富土电催化剂以提高 HMF 氧化的催化性能至关重要。本文通过界面工程构建了一种由镍铁层双氢氧化物(LDH)纳米片和双金属硫化物(NiFeS)组成的新型二维(2D)混合阵列,用于将 HMF 高效电催化氧化为 2,5-呋喃二甲酸(FDCA)。具有超薄异质结构的二维 NiFe LDH/NiFeS 的制备过程包括:通过原位生长将 Co 基金属有机框架(Co MOF)作为模板锚定在碳布(CC)上,在 Co MOF 表面形成 NiFe LDH,然后进行部分硫化。NiFe LDH/NiFeS 电催化剂在 HMF 氧化方面表现出卓越的性能,在 10 mmol/L HMF 的碱性电解液中,FDCA 收率约为 98.5%,法拉第效率(FE)约为 97.2%。此外,即使 HMF 浓度为 100 mmol/L,FDCA 的产率和 FE 仍然很高,分别为 83.6% 和 93.6%。这些发现突出表明,镍铁合金 LDH 纳米片与镍铁合金之间含有丰富界面的二维异质结构可以提高 LDH 的内在活性,从而促进氧化反应动力学。此外,双金属镍铁化合物的协同效应还提高了 HMF 转化为 FDCA 的选择性。我们目前的工作表明,通过界面工程构建镍铁合金 LDH/NiFeS 二维超薄异质结构是提高 LDH 电催化剂内在活性的一种简便策略,这将为低成本、先进的二维纳米催化剂开辟新的途径,从而实现可持续能源转换和生物质衍生物的电化学增值。
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引用次数: 0
Encapsulating Si particles in multiple carbon shells with pore-rich for constructing free-standing anodes of lithium storage 在富含孔隙的多层碳壳中封装硅颗粒,以构建独立的锂储能阳极
IF 9.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-05-10 DOI: 10.1016/j.cclet.2024.109990

Silicon based (Si-based) materials are considered to be the most promising anode materials for lithium-ion batteries (LIBs) due to their high specific capacity. However, the issues of poor electrical conductivity and volume expansion during cycling have not been effectively addressed. The optimum remedy is to select specific materials to establish an exceptional conductive and volume buffer structure to assist the Si materials to develop its excellent lithium storage properties. Here, Si particles were encapsulated into porous carbon fibers containing ultrafine Co particles (CP) to obtained Si-x@CP-y film. Among them, the addition of Si particles and the void structure was precisely regulated to achieve a superior electrode with a high specific capacity. Subsequently, the two-dimensional conductive material reduced graphene oxide (rGO) nanosheets were further incorporated to obtain Si-2@CP-2@rGO films with core@multi-shell structure. The final electrode was equipped with one-, two-, and three-dimensional electronic pathways to allow rapid electron transport, and featured with multi-layer buffer structure and reserved pores that could effectively mitigate volume changes. As expected, the free-standing Si-2@CP-2@rGO electrode delivered a high specific capacity of 1221.2 mAh/g after 100 cycles at 0.1 A/g in a half cell, and the assembled full cell showed 249.0 mAh/g after 200 cycles at 0.2 A/g, which fulfilled the lightweight requirement for new energy storage devices.

硅基(Si-based)材料因其高比容量而被认为是最有前途的锂离子电池(LIB)负极材料。然而,导电性差和循环过程中体积膨胀的问题尚未得到有效解决。最佳的补救措施是选择特定的材料来建立特殊的导电性和体积缓冲结构,以帮助硅材料发展其优异的锂存储特性。本文将硅颗粒封装到含有超细钴颗粒(CP)的多孔碳纤维中,从而获得了 Si-x@CP-y 薄膜。其中,通过精确调节硅颗粒的添加量和空隙结构,获得了具有高比容量的优异电极。随后,进一步加入二维导电材料还原氧化石墨烯(rGO)纳米片,得到具有核@多壳结构的 Si-2@CP-2@rGO 薄膜。最终电极具有一维、二维和三维电子通路,可实现快速电子传输,并具有多层缓冲结构和预留孔隙,可有效减缓体积变化。正如预期的那样,独立的 Si-2@CP-2@rGO 电极在 0.1 A/g 条件下循环 100 次后,半电池的比容量达到了 1221.2 mAh/g,组装后的全电池在 0.2 A/g 条件下循环 200 次后,比容量达到了 249.0 mAh/g,满足了新型储能设备的轻量化要求。
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引用次数: 0
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Chinese Chemical Letters
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