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“Super-heterojunctioned” thermoelectric polymers "超级热结 "热电聚合物
IF 9.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-09-30 DOI: 10.1016/j.cclet.2024.110523
Hanying Li , Wee-Liat Ong
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引用次数: 0
Boron cluster-based TADF emitter via through-space charge transfer enabling efficient orange-red electroluminescence
IF 9.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-09-30 DOI: 10.1016/j.cclet.2024.110520
Xiao Yu , Dongyue Cui , Mengmeng Wang , Zhaojin Wang , Mengzhu Wang , Deshuang Tu , Vladimir Bregadze , Changsheng Lu , Qiang Zhao , Runfeng Chen , Hong Yan
Thermally activated delayed fluorescence (TADF) materials driven by a through-space charge transfer (TSCT) mechanism have garnered wide interest. However, access of TSCT-TADF molecules with long-wavelength emission remains a formidable challenge. In this study, we introduce a novel V-type D-A-D-A' emitter, Trz-mCzCbCz, by using a carborane scaffold. This design strategically incorporates carbazole (Cz) and 2,4,6-triphenyl-1,3,5-triazine (Trz) as donor and acceptor moieties, respectively. Theoretical calculations alongside experimental validations affirm the typical TSCT-TADF characteristics of this luminogen. Owing to the unique structural and electronic attributes of carboranes, Trz-mCzCbCz exhibits an orange-red emission, markedly diverging from the traditional blue-to-green emissions observed in classical Cz and Trz-based TADF molecules. Moreover, bright emission in aggregates was observed for Trz-mCzCbCz with absolute photoluminescence quantum yield (PLQY) of up to 88.8 %. As such, we have successfully fabricated five organic light-emitting diodes (OLEDs) by utilizing Trz-mCzCbCz as the emitting layer. It is important to note that both the reverse intersystem crossing process and the TADF properties are profoundly influenced by host materials. The fabricated OLED devices reached a maximum external quantum efficiency (EQE) of 12.7 %, with an emission peak at 592 nm. This represents the highest recorded efficiency for TSCT-TADF OLEDs employing carborane derivatives as emitting layers.
{"title":"Boron cluster-based TADF emitter via through-space charge transfer enabling efficient orange-red electroluminescence","authors":"Xiao Yu ,&nbsp;Dongyue Cui ,&nbsp;Mengmeng Wang ,&nbsp;Zhaojin Wang ,&nbsp;Mengzhu Wang ,&nbsp;Deshuang Tu ,&nbsp;Vladimir Bregadze ,&nbsp;Changsheng Lu ,&nbsp;Qiang Zhao ,&nbsp;Runfeng Chen ,&nbsp;Hong Yan","doi":"10.1016/j.cclet.2024.110520","DOIUrl":"10.1016/j.cclet.2024.110520","url":null,"abstract":"<div><div>Thermally activated delayed fluorescence (TADF) materials driven by a through-space charge transfer (TSCT) mechanism have garnered wide interest. However, access of TSCT-TADF molecules with long-wavelength emission remains a formidable challenge. In this study, we introduce a novel V-type D-A-D-A' emitter, Trz-<em>m</em>CzCbCz, by using a carborane scaffold. This design strategically incorporates carbazole (Cz) and 2,4,6-triphenyl-1,3,5-triazine (Trz) as donor and acceptor moieties, respectively. Theoretical calculations alongside experimental validations affirm the typical TSCT-TADF characteristics of this luminogen. Owing to the unique structural and electronic attributes of carboranes, Trz-<em>m</em>CzCbCz exhibits an orange-red emission, markedly diverging from the traditional blue-to-green emissions observed in classical Cz and Trz-based TADF molecules. Moreover, bright emission in aggregates was observed for Trz-<em>m</em>CzCbCz with absolute photoluminescence quantum yield (PLQY) of up to 88.8 %. As such, we have successfully fabricated five organic light-emitting diodes (OLEDs) by utilizing Trz-<em>m</em>CzCbCz as the emitting layer. It is important to note that both the reverse intersystem crossing process and the TADF properties are profoundly influenced by host materials. The fabricated OLED devices reached a maximum external quantum efficiency (EQE) of 12.7 %, with an emission peak at 592 nm. This represents the highest recorded efficiency for TSCT-TADF OLEDs employing carborane derivatives as emitting layers.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 3","pages":"Article 110520"},"PeriodicalIF":9.4,"publicationDate":"2024-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143356836","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
New electrolyte concept: Compact ion-pair aggregate electrolyte
IF 9.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-09-27 DOI: 10.1016/j.cclet.2024.110512
Jing Guo
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引用次数: 0
Efficient solution-processed near-infrared organic light-emitting diodes with a binary-mixed electron transport layer
IF 9.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-09-27 DOI: 10.1016/j.cclet.2024.110511
Haowen Shang , Yujie Yang , Bingjie Xue , Yikai Wang , Zhiyi Su , Wenlong Liu , Youzhi Wu , Xinjun Xu
A binary-mixed electron transport layer (ETL) has been reported for constructing solution-processable near-infrared organic light-emitting diodes (NIR OLEDs). Relative to the single-component ETL, the binary-mixed ETL composed of PDINN:TPBi can enhance the carrier transport capacity, reduce device impedance, and weaken fluorescence quenching of the emitting layer. By carefully selecting an appropriate luminescent material Y5 (a nonfullerene electron acceptor in organic solar cells) and precisely fine-tuning the molecular aggregation in active layer using a mixed solvent, the morphology is optimized and luminescence performance is enhanced, resulting in efficient NIR OLEDs with an emission peak at 890 nm. The experiment showcases a Y5-based near-infrared OLED with a maximum radiance of 34.9 W sr-1 m-2 and a maximum external quantum efficiency of 0.50%, which is among the highest values reported for non-doped fluorescent NIR OLEDs with an emission peak over 850 nm.
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引用次数: 0
Oxygen vacancies-rich molybdenum tungsten oxide nanowires as a highly active nitrogen fixation electrocatalyst 富氧空位钼钨氧化物纳米线作为高活性固氮电催化剂
IF 9.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-09-26 DOI: 10.1016/j.cclet.2024.110491
Jincheng Zhang , Mengjie Sun , Jiali Ren , Rui Zhang, Min Ma, Qingzhong Xue, Jian Tian
Herein, vacancy engineering is utilized reasonably to explore molybdenum tungsten oxide nanowires (W4MoO3 NWs) rich in O-vacancies as an advanced electrochemical nitrogen reduction reaction (eNRR) electrocatalyst, realizing further enhancement of NRR performance. In 0.1 mol/L Na2SO4, W4MoO3 NWs rich in O vacancies (CTAB-D-W4MoO3) achieve a large NH3 yield of 60.77 µg h-1 mg-1cat. at -0.70 V vs. RHE and a high faradaic efficiency of 56.42 % at -0.60 V, much superior to the W4MoO3 NWs deficient in oxygen vacancies (20.26 µg h-1 mg-1cat. and 17.1 % at -0.70 V vs. RHE). Meanwhile, W4MoO3 NWs rich in O-vacancies also show high electrochemical stability. Density functional theory (DFT) calculations present that O vacancies in CTAB-D-W4MoO3 reduce the energy barrier formed by the intermediate of *N-NH, facilitate the activation and further hydrogenation of *N-N, promote the NRR process, and improve NRR activity.
本文合理利用空位工程技术,探索将富含 O 空位的钼钨氧化物纳米线(W4MoO3 NWs)作为先进的电化学氮还原反应(eNRR)电催化剂,实现氮还原反应性能的进一步提高。在 0.1 mol/L Na2SO4 中,富含 O 空位的 W4MoO3 NWs(CTAB-D-W4MoO3)在 -0.70 V 对 RHE 时的 NH3 产率高达 60.77 µg h-1 mg-1cat.,在 -0.60 V 时的远化效率高达 56.42 %,远优于缺乏氧空位的 W4MoO3 NWs(在 -0.70 V 对 RHE 时的产率为 20.26 µg h-1 mg-1cat.)同时,富含氧空位的 W4MoO3 NWs 也表现出很高的电化学稳定性。密度泛函理论(DFT)计算表明,CTAB-D-W4MoO3 中的 O 空位降低了 *N-NH 中间体形成的能障,有利于 *N-N 的活化和进一步氢化,促进了 NRR 过程,提高了 NRR 活性。
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引用次数: 0
Polyvinyl alcohol fiber with enhanced strength and modulus and intense cyan fluorescence based on covalently functionalized graphene quantum dots 基于共价官能化石墨烯量子点的具有更高强度和模量以及更强青色荧光的聚乙烯醇纤维
IF 9.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-09-26 DOI: 10.1016/j.cclet.2024.110510
Manman Ou, Yunjian Zhu, Jiahao Liu, Zhaoxuan Liu, Jianjun Wang, Jun Sun, Chuanxiang Qin, Lixing Dai
In this study, we proposed a novel and efficient way to strengthen polyvinyl alcohol (PVA) fiber using graphene quantum dots (GQDs). PVA molecular chains were grafted onto the surface of GQDs through Friedel-Crafts alkylation reaction to obtain functionalized GQDs (f-GQDs), and PVA/f-GQDs composite fiber was successfully prepared by wet spinning and post-treatment. The tensile strength and Young's modulus of the composite fiber reached up to 1229.24 MPa and 35.36 GPa which were approximately twice and 4 times those of the pure PVA fiber, respectively. Moreover, the composite fiber was demonstrated excellent resistance to solvents. In addition, the PVA/f-GQDs composite fiber showed intense and uniform cyan fluorescence, meanwhile, it could maintain stable solid-state fluorescence in acid and alkali solutions and particularly after long-term immersion in water (1 month). This study proposes a promising route for obtaining high-performance conventional fibers with some new functions.
在这项研究中,我们提出了一种利用石墨烯量子点(GQDs)增强聚乙烯醇(PVA)纤维的新型高效方法。通过 Friedel-Crafts 烷基化反应将 PVA 分子链接枝到 GQDs 表面,得到功能化 GQDs(f-GQDs),并通过湿法纺丝和后处理成功制备了 PVA/f-GQDs 复合纤维。复合纤维的拉伸强度和杨氏模量分别达到 1229.24 MPa 和 35.36 GPa,约为纯 PVA 纤维的 2 倍和 4 倍。此外,复合纤维还具有优异的耐溶剂性。此外,PVA/f-GQDs 复合纤维显示出强烈而均匀的青色荧光,同时在酸碱溶液中,尤其是在水中长期浸泡(1 个月)后,仍能保持稳定的固态荧光。这项研究为获得具有某些新功能的高性能传统纤维提供了一条可行的途径。
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引用次数: 0
Engineered iron-based metal-organic frameworks nanoplatforms for cancer theranostics: A mini review 用于癌症治疗的铁基金属有机框架纳米平台:微型综述
IF 9.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-09-25 DOI: 10.1016/j.cclet.2024.110501
Yunlong Li , Xinyu Zhang , Shuang Liu , Chunsheng Li , Qiang Wang , Jin Ye , Yong Lu , Jiating Xu
Up to now, numerous emerging methods of cancer treatment including chemodynamic therapy, photothermal therapy, photodynamic therapy, sonodynamic therapy, immunotherapy and chemotherapy have rapidly entered a new stage of development. However, the single treatment mode is often constrained by the complex tumor microenvironment. Recently, the nanomaterials and nanomedicine have emerged as promising avenues to overcome the limitation in cancer theranostics. Especially, metal-organic frameworks (MOFs) have gained considerable interests in cancer therapy because of their customizable morphologies, easy functionalization, large specific surface area, and good biocompatibility. Among these MOFs, iron-based MOFs (Fe-MOFs) are particularly promising for cancer treatment due to their properties as nano-photosensitizers, peroxidase-like activity, bioimaging contrast capabilities, and biodegradability. Utilizing their structural regularity and synthetic tunability, Fe-MOFs can be engineered to incorporate organic molecules or other inorganic nanoparticles, thereby creating multifunctional nanoplatforms for single or combined theranostic modes. Herein, the minireview focuses on the recent advancements of the Fe-MOFs-based nanoplatforms for self-enhanced imaging and treatment at tumor sites. Furthermore, the clinical research development of Fe-MOFs-based nanoplatforms is discussed, addressing key challenges and innovations for the future. Our review aims to provide novice researchers with a foundational understanding of advanced cancer theranostic modes and promote their clinical applications through the modification of Fe-MOFs.
迄今为止,包括化学动力疗法、光热疗法、光动力疗法、声动力疗法、免疫疗法和化疗在内的众多新兴癌症治疗方法已迅速进入新的发展阶段。然而,单一的治疗模式往往受制于复杂的肿瘤微环境。近来,纳米材料和纳米医学的出现为克服肿瘤治疗学的局限性提供了很好的途径。特别是金属有机框架(MOFs),由于其形态可定制、易于功能化、比表面积大、生物相容性好等特点,在癌症治疗中获得了极大的关注。在这些 MOFs 中,铁基 MOFs(Fe-MOFs)因其具有纳米光敏剂、过氧化物酶样活性、生物成像对比能力和生物可降解性等特性,在癌症治疗中尤其具有广阔的前景。利用其结构的规则性和合成可调性,Fe-MOFs 可与有机分子或其他无机纳米粒子结合,从而创造出单一或组合治疗模式的多功能纳米平台。在此,小编将重点介绍基于 Fe-MOFs 的纳米平台在肿瘤部位自我增强成像和治疗方面的最新进展。此外,还讨论了基于 Fe-MOFs 的纳米平台的临床研究发展,探讨了未来的主要挑战和创新。我们的综述旨在让新手研究人员对先进的癌症治疗模式有一个基础性的了解,并通过对 Fe-MOFs 的改性促进其临床应用。
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引用次数: 0
High-temperature-stable RRAMs with well-defined thermal effect mechanisms enable by engineering of robust 2D <100>-oriented organic-inorganic hybrid perovskites
IF 9.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-09-24 DOI: 10.1016/j.cclet.2024.110495
Weihong Ding, Kaiyue Song, Xianglong Li, Xiaoxia Sun
The exploitation of organic-inorganic hybrid perovskites (OIHPs) as active layer materials for typical sandwich-structured resistive memories has attracted widespread interest due to the property of low power consumption and fast switching. However, the inherent thermal instability of perovskites limits the application of OIHPs-based resistive memories under extreme conditions, while the influence of thermal effects on their resistance change characteristics remains unclear. Herein, a novel 2D <100>-oriented high-temperature resistant OIHP [(BIZ-H)2(PbBr4)]n (BIZ = benzimidazole) is prepared as an active layer material to fabricate FTO/[(BIZ-H)2(PbBr4)]n/Ag resistive memory with excellent thermal reproducibility and stability up to 120 °C. The increase in temperature leads to a decrease in the PbBr6 octahedral distortion in the crystal structure, an increase in hydrogen bonding between the (BIZ-H)+ cation and the (PbBr4)n2n- layer, and a shortening of the spacing of the inorganic layers, which is found to result in the creation and predominance of thermally activated traps with increasing temperature. This work provides a new direction for the next generation of OIHPs-based resistive memories with high-temperature tolerance.
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引用次数: 0
Efficient synthesis of nano high-entropy compounds for advanced oxygen evolution reaction
IF 9.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-09-24 DOI: 10.1016/j.cclet.2024.110498
Genxiang Wang , Linfeng Fan , Peng Wang , Junfeng Wang , Fen Qiao , Zhenhai Wen
Developing efficient electrocatalysts for oxygen evolution reaction (OER) is imperative to enhance the overall efficiency of electrolysis systems and rechargeable metal-air batteries operating in aqueous solutions. High-entropy materials, featured with their distinctive multi-component properties, have found extensive application as catalysts in electrochemical energy storage and conversion devices. However, synthesizing nanostructured high-entropy compounds under mild conditions poses a significant challenge due to the difficulty in overcoming the immiscibility of multiple metallic constituents. In this context, the current study focuses on the synthesis of an array of nano-sized high entropy sulfides tailored for OER via a facile precursor pyrolysis method at low temperature. The representative compound, FeCoNiCuMnSx, demonstrates remarkable OER performance, achieving a current density of 10 mA/cm2 at an overpotential of merely 220 mV and excellent stability with constant electrolysis at 100 mA/cm2 for over 400 h. The in-situ formed metal (oxy)hydroxide has been confirmed as the real active sites and its exceptional performance can be primarily attributed to the synergistic effects arising from its multiple components. Furthermore, the synthetic methodology presented here is versatile and can be extended to the preparation of high entropy phosphides, which also present favorable OER performance. This research not only introduces promising non-noble electrocatalysts for OER but also offers a facile approach to expand the family of nano high-entropy materials, contributing significantly to the field of electrochemical energy conversion.
{"title":"Efficient synthesis of nano high-entropy compounds for advanced oxygen evolution reaction","authors":"Genxiang Wang ,&nbsp;Linfeng Fan ,&nbsp;Peng Wang ,&nbsp;Junfeng Wang ,&nbsp;Fen Qiao ,&nbsp;Zhenhai Wen","doi":"10.1016/j.cclet.2024.110498","DOIUrl":"10.1016/j.cclet.2024.110498","url":null,"abstract":"<div><div>Developing efficient electrocatalysts for oxygen evolution reaction (OER) is imperative to enhance the overall efficiency of electrolysis systems and rechargeable metal-air batteries operating in aqueous solutions. High-entropy materials, featured with their distinctive multi-component properties, have found extensive application as catalysts in electrochemical energy storage and conversion devices. However, synthesizing nanostructured high-entropy compounds under mild conditions poses a significant challenge due to the difficulty in overcoming the immiscibility of multiple metallic constituents. In this context, the current study focuses on the synthesis of an array of nano-sized high entropy sulfides tailored for OER <em>via</em> a facile precursor pyrolysis method at low temperature. The representative compound, FeCoNiCuMnS<sub>x</sub>, demonstrates remarkable OER performance, achieving a current density of 10 mA/cm<sup>2</sup> at an overpotential of merely 220 mV and excellent stability with constant electrolysis at 100 mA/cm<sup>2</sup> for over 400 h. The <em>in-situ</em> formed metal (oxy)hydroxide has been confirmed as the real active sites and its exceptional performance can be primarily attributed to the synergistic effects arising from its multiple components. Furthermore, the synthetic methodology presented here is versatile and can be extended to the preparation of high entropy phosphides, which also present favorable OER performance. This research not only introduces promising non-noble electrocatalysts for OER but also offers a facile approach to expand the family of nano high-entropy materials, contributing significantly to the field of electrochemical energy conversion.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 4","pages":"Article 110498"},"PeriodicalIF":9.4,"publicationDate":"2024-09-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143098704","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
High quantum yield yellow emission carbon dots for the construction of blue light blocking films 用于构建蓝光阻挡薄膜的高量子产率黄色发射碳点
IF 9.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-09-24 DOI: 10.1016/j.cclet.2024.110497
Liwen Wang , Boyang Wang , Siyu Lu , Shubo Lv , Xiaoli Qu
White light illumination is essential in daily life, however, the substantial amount of blue light it contains can damage human eyes. Therefore, it is important to block this high-energy blue light to protect visual health. In this study, yellow-emitting carbon dots (CDs) with a quantum yield exceeding 94 % were synthesized using citric acid and urea. These CDs effectively absorb blue light. By incorporating them into polystyrene, multiple films termed CDs-based blue light blocking films (CBFs) were developed, each offering different levels of blue light absorption. These CBFs exhibited excellent transparency and efficient blue light filtering capabilities. This study highlights the potential of high quantum yield CDs, which specifically absorb blue light, as foundational materials for developing light-blocking solutions against high-energy short-wavelength light.
白光照明在日常生活中必不可少,但其中含有的大量蓝光会对人眼造成伤害。因此,阻挡这种高能蓝光以保护视力健康非常重要。本研究利用柠檬酸和尿素合成了量子产率超过 94% 的黄色发光碳点(CD)。这些碳点能有效吸收蓝光。通过将它们与聚苯乙烯结合,开发出了多种薄膜,称为基于 CD 的蓝光阻隔薄膜(CBF),每种薄膜都具有不同程度的蓝光吸收能力。这些 CBF 具有出色的透明度和高效的蓝光过滤能力。这项研究凸显了高量子产率 CD(专门吸收蓝光)作为开发阻挡高能短波光解决方案的基础材料的潜力。
{"title":"High quantum yield yellow emission carbon dots for the construction of blue light blocking films","authors":"Liwen Wang ,&nbsp;Boyang Wang ,&nbsp;Siyu Lu ,&nbsp;Shubo Lv ,&nbsp;Xiaoli Qu","doi":"10.1016/j.cclet.2024.110497","DOIUrl":"10.1016/j.cclet.2024.110497","url":null,"abstract":"<div><div>White light illumination is essential in daily life, however, the substantial amount of blue light it contains can damage human eyes. Therefore, it is important to block this high-energy blue light to protect visual health. In this study, yellow-emitting carbon dots (CDs) with a quantum yield exceeding 94 % were synthesized using citric acid and urea. These CDs effectively absorb blue light. By incorporating them into polystyrene, multiple films termed CDs-based blue light blocking films (CBFs) were developed, each offering different levels of blue light absorption. These CBFs exhibited excellent transparency and efficient blue light filtering capabilities. This study highlights the potential of high quantum yield CDs, which specifically absorb blue light, as foundational materials for developing light-blocking solutions against high-energy short-wavelength light.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 2","pages":"Article 110497"},"PeriodicalIF":9.4,"publicationDate":"2024-09-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142699636","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
期刊
Chinese Chemical Letters
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