Pub Date : 2024-05-20DOI: 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。
{"title":"High sensitivity artificial synapses using printed high-transmittance ITO fibers for neuromorphic computing","authors":"","doi":"10.1016/j.cclet.2024.110030","DOIUrl":"10.1016/j.cclet.2024.110030","url":null,"abstract":"<div><p>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.</p></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":null,"pages":null},"PeriodicalIF":9.4,"publicationDate":"2024-05-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141137030","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}
Pub Date : 2024-05-18DOI: 10.1016/j.cclet.2024.110026
Shihong Wu , Ronghui Zhou , Hang Zhao , Peng Wu
{"title":"Sonoafterglow luminescence for in vivo deep-tissue imaging","authors":"Shihong Wu , Ronghui Zhou , Hang Zhao , Peng Wu","doi":"10.1016/j.cclet.2024.110026","DOIUrl":"10.1016/j.cclet.2024.110026","url":null,"abstract":"","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":null,"pages":null},"PeriodicalIF":9.4,"publicationDate":"2024-05-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141138678","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}
Pub Date : 2024-05-17DOI: 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。
{"title":"A cucurbit[8]uril-based supramolecular phosphorescent assembly: Cell imaging and sensing of amino acids in aqueous solution","authors":"","doi":"10.1016/j.cclet.2024.110022","DOIUrl":"10.1016/j.cclet.2024.110022","url":null,"abstract":"<div><p>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 <span>l</span>-tryptophan (L-Trp) and <span>l</span>-tyrosine (L-Tyr). Moreover, the Q[8]-BCPI assembly showed good biocompatibility and low biotoxicity, and had a good staining effect on HeLa cells.</p></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":null,"pages":null},"PeriodicalIF":9.4,"publicationDate":"2024-05-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141035510","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}
Pub Date : 2024-05-17DOI: 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.
{"title":"Photocatalyst/metal-free sequential C–N/C–S bond formation: Synthesis of S-arylisothioureas via photoinduced EDA complex activation","authors":"","doi":"10.1016/j.cclet.2024.110024","DOIUrl":"10.1016/j.cclet.2024.110024","url":null,"abstract":"<div><p>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 <em>S</em>-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.</p></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":null,"pages":null},"PeriodicalIF":9.4,"publicationDate":"2024-05-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141053805","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}
Pub Date : 2024-05-17DOI: 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.
{"title":"20 nm-ultra-thin fluorosiloxane interphase layer enables dendrite-free, fast-charging, and flexible aqueous zinc metal batteries","authors":"","doi":"10.1016/j.cclet.2024.110025","DOIUrl":"10.1016/j.cclet.2024.110025","url":null,"abstract":"<div><p>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 <em>via</em> 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 Zn<sup>2+</sup>. 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/cm<sup>2</sup>), achieving a cumulative areal capacity of 12.9 Ah/cm<sup>2</sup>. Further, the full cell assembled with 10 μm-thick SiFO-Zn anode and MnO<sub>2</sub> cathode achieves 2600 cycles at 5 A/g with minimal capacity degradation, and a large-size (22.5 cm<sup>−2</sup>) pouch cell powers the light-emitting diode even after reverse bending, demonstrating the potential of AZMBs for fast-charging flexible devices.</p></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":null,"pages":null},"PeriodicalIF":9.4,"publicationDate":"2024-05-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141042735","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}
Pub Date : 2024-05-16DOI: 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。
{"title":"Selenium nanoparticles enhance the chemotherapeutic efficacy of pemetrexed against non-small cell lung cancer","authors":"","doi":"10.1016/j.cclet.2024.110018","DOIUrl":"10.1016/j.cclet.2024.110018","url":null,"abstract":"<div><p>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 <em>in vitro</em>. 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.</p></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":null,"pages":null},"PeriodicalIF":9.4,"publicationDate":"2024-05-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141029580","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}
Pub Date : 2024-05-16DOI: 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.
{"title":"Imaging polarity changes in pneumonia and lung cancer using a lipid droplet-targeted near-infrared fluorescent probe","authors":"","doi":"10.1016/j.cclet.2024.110020","DOIUrl":"10.1016/j.cclet.2024.110020","url":null,"abstract":"<div><p>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 <strong>BFZ</strong> 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 <strong>BFZ</strong> 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.</p></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":null,"pages":null},"PeriodicalIF":9.4,"publicationDate":"2024-05-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141055712","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}
Pub Date : 2024-05-14DOI: 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.
{"title":"CoSe2 nanowire array enabled highly efficient electrocatalytic reduction of nitrate for ammonia synthesis","authors":"","doi":"10.1016/j.cclet.2024.110005","DOIUrl":"10.1016/j.cclet.2024.110005","url":null,"abstract":"<div><p>The electrocatalytic reduction of nitrate (NO<sub>3</sub><sup>–</sup>) not only facilitates the environmentally sustainable production of ammonia (NH<sub>3</sub>) but also purifies water by removing NO<sub>3</sub><sup>–</sup>, thereby transforming waste into valuable resources. The process of converting NO<sub>3</sub><sup>–</sup> to NH<sub>3</sub> is complex, involving eight electron transfers and multiple intermediates, making the choice of electrocatalyst critical. In this study, we report a cobalt selenide (CoSe<sub>2</sub>) nanowire array on carbon cloth (CoSe<sub>2</sub>/CC) as an effective electrocatalyst for the NO<sub>3</sub><sup>–</sup> to NH<sub>3</sub> conversion. In an alkaline medium with 0.1 mol/L NO<sub>3</sub><sup>–</sup>, CoSe<sub>2</sub>/CC demonstrates exceptional NH<sub>3</sub> Faradaic efficiency of 97.6 % and a high NH<sub>3</sub> yield of 517.7 µmol h<sup>–1</sup> cm<sup>–2</sup> at –0.6 V <em>versus</em> the reversible hydrogen electrode. Furthermore, insights into the reaction mechanism of CoSe<sub>2</sub> in the electrocatalytic NO<sub>3</sub><sup>–</sup> reduction are elucidated through density functional theory calculations.</p></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":null,"pages":null},"PeriodicalIF":9.4,"publicationDate":"2024-05-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141044342","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}
Pub Date : 2024-05-14DOI: 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.
{"title":"Interface engineering of 2D NiFe LDH/NiFeS heterostructure for highly efficient 5-hydroxymethylfurfural electrooxidation","authors":"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","doi":"10.1016/j.cclet.2024.110011","DOIUrl":"10.1016/j.cclet.2024.110011","url":null,"abstract":"<div><p>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 <em>via</em> 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) <em>via in-situ</em> 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 <em>via</em> 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.</p></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":null,"pages":null},"PeriodicalIF":9.4,"publicationDate":"2024-05-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141025589","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}
Pub Date : 2024-05-10DOI: 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.
{"title":"Encapsulating Si particles in multiple carbon shells with pore-rich for constructing free-standing anodes of lithium storage","authors":"","doi":"10.1016/j.cclet.2024.109990","DOIUrl":"10.1016/j.cclet.2024.109990","url":null,"abstract":"<div><p>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.</p></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":null,"pages":null},"PeriodicalIF":9.4,"publicationDate":"2024-05-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141046209","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}