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Regulating local electron transfer environment of covalent triazine frameworks through F, N co-modification towards optimized oxygen reduction reaction 通过 F、N 共修饰调节共价三嗪框架的局部电子转移环境,优化氧还原反应
IF 9.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-11 DOI: 10.1016/j.cclet.2024.110235
Quanyou Guo , Yue Yang , Tingting Hu, Hongqi Chu, Lijun Liao, Xuepeng Wang, Zhenzi Li, Liping Guo, Wei Zhou
The high conductivity of electrocatalyst can eliminate the Schottky energy barrier at the interface of heterogeneous phases during an electrocatalytic reaction and accelerate the rapid electron transfer to the catalytic active center. Therefore, the electronic conductivity is a vital parameter for oxygen reduction reaction (ORR). Covalent triazine frameworks (CTFs) have shown great potential application as electrocatalysts in ORR with a merit of the diverse building blocks. However, the intrinsic low conductivity and high impedance of CTFs could be significant setbacks in electrocatalytic application. Herein, CTFs were constructed by introducing F and N co-modification for efficient 2e ORR. Compared with the pristine CTF, the co-presence of F, N could increase the conductivity obviously by 1000-fold. As a result, F-N-CTF exhibits enhanced catalytic performance of H2O2 generation and selectivity towards reaction pathways. This work reveals the importance of conductivity optimization for CTFs and provides guidance for designing high conductivity non-metallic organic semiconductor catalysts for 2e ORR.
电催化剂的高电导率可以消除电催化反应过程中异相界面上的肖特基能垒,加速电子快速转移到催化活性中心。因此,电子电导率是氧还原反应(ORR)的一个重要参数。共价三嗪框架(CTFs)作为氧还原反应中的电催化剂具有巨大的应用潜力,其优点是结构单元多样。然而,CTF 固有的低电导率和高阻抗可能会成为电催化应用的重大障碍。本文通过引入 F 和 N 共修饰构建了 CTF,以实现高效的 2e- ORR。与原始 CTF 相比,F 和 N 的共存可使导电率明显提高 1000 倍。因此,F-N-CTF 在生成 H2O2 的催化性能和对反应途径的选择性方面都有所提高。这项工作揭示了 CTF 电导率优化的重要性,为设计用于 2e- ORR 的高电导率非金属有机半导体催化剂提供了指导。
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引用次数: 0
The advanced development of innovative photocatalytic coupling strategies for hydrogen production 用于制氢的创新光催化耦合战略的先进开发
IF 9.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-10 DOI: 10.1016/j.cclet.2024.110234
Yuehai Zhi , Chen Gu , Huachao Ji , Kang Chen , Wenqi Gao , Jianmei Chen , Dafeng Yan
Photocatalytic technology harnesses solar energy to facilitate chemical transformations, presenting significant potential in energy generation and environmental remediation. However, the conventional O2 evolution process is hindered by high reaction barriers and inefficiencies, which limit its widespread application. Therefore, exploring novel photocatalytic coupling strategies to replace water oxidation has become a key route to enhance the efficiency of H2 production. In this review, organic pollutants removal and the valorization of organics as substitutes for water oxidation coupling strategies for photocatalytic H2 production are comprehensively summarized. These strategies not only circumvent the high reaction barriers associated with O2 evolution to enhance the H2 production but also aid in the removing of organic pollutants or synthesis of value-added chemicals. We also present future research directions and underscore the significance of advanced catalyst design, in-depth analysis of reaction mechanisms, and systematic optimization strategies in realizing an efficient and sustainable photocatalytic process. This guidance is anticipated to provide theoretical and practical new insights for the future development of photocatalytic coupling reactions, fostering further explorations in the realm of renewable energy and environmental governance.
光催化技术利用太阳能促进化学转化,在能源生产和环境修复方面具有巨大潜力。然而,传统的氧气进化过程受到高反应障碍和低效率的阻碍,限制了其广泛应用。因此,探索新型光催化耦合策略以取代水氧化已成为提高 H2 生产效率的关键途径。本综述全面总结了光催化制取 H2 的有机污染物去除和有机物价值化替代水氧化耦合策略。这些策略不仅规避了与氧气进化相关的高反应障碍,提高了 H2 产率,还有助于去除有机污染物或合成高附加值化学品。我们还介绍了未来的研究方向,并强调了先进催化剂设计、深入分析反应机理和系统优化策略对于实现高效、可持续光催化过程的重要意义。本指南有望为光催化偶联反应的未来发展提供理论和实践方面的新见解,促进可再生能源和环境治理领域的进一步探索。
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引用次数: 0
Linear polyurethanes with excellent comprehensive properties from poly(ethylene carbonate) diol 具有优异综合性能的聚碳酸乙二醇线型聚氨酯
IF 9.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-10 DOI: 10.1016/j.cclet.2024.110236
Xinyu Liu, Jialin Yang, Zonglin He, Jiaoyan Ai, Lina Song, Baohua Liu
The synthesis of polyurethanes (PUs) from the reaction of low molecular weight poly(ethylene carbonate) diol (PECD) is rarely investigated. This work reports a novel PU with excellent mechanical properties from the solution polymerization of 4,4′-diphenylmethane diisocyanate (MDI) with PECD that was derived from the copolymerization of carbon dioxide (CO2) and ethylene oxide (EO). The tensile strength, the elongation at break and 300 % constant tensile strength of the PECD-PU were up to 66 ± 2 MPa, 880 % ± 50 % and 13 MPa, respectively, higher than the control PUs from the reaction of MDI with commercial polyethers or polyesters. The PECD-PU with high CO2 carbonate content exhibited good solvent resistance and chemical stability. Of importance, the mechanical properties and chemical resistance of PECD-PU were significantly enhanced with the increasing content of CO2, i.e., the carbonate unit in PECD. This work provides comprehensive properties of PECD-derived PUs, indicating that PECD is a competitive precursor for the preparation of PU and has broad application prospects.
由低分子量聚(碳酸乙烯)二元醇(PECD)反应合成聚氨酯(PUs)的研究很少。这项工作报告了一种新型聚氨酯,它具有优异的机械性能,由 4,4′-二苯基甲烷二异氰酸酯(MDI)与 PECD 溶液聚合而成,PECD 由二氧化碳(CO2)和环氧乙烷(EO)共聚而成。PECD-PU 的拉伸强度、断裂伸长率和 300 % 恒定拉伸强度分别高达 66 ± 2 兆帕、880 % ± 50 % 和 13 兆帕,高于 MDI 与商用聚醚或聚酯反应生成的对照 PU。二氧化碳碳酸盐含量高的 PECD-PU 具有良好的耐溶剂性和化学稳定性。重要的是,PECD-PU 的机械性能和耐化学性随着 CO2(即 PECD 中的碳酸单元)含量的增加而显著提高。这项研究提供了 PECD 衍生聚氨酯的全面特性,表明 PECD 是制备聚氨酯的一种有竞争力的前驱体,具有广阔的应用前景。
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引用次数: 0
Methanol steam mediated corrosion engineering towards high-entropy NiFe layered double hydroxide for ultra-stable oxygen evolution 甲醇蒸汽介导的腐蚀工程,实现高熵镍铁层状双氢氧化物的超稳定氧进化
IF 9.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-10 DOI: 10.1016/j.cclet.2024.110232
Jinqiang Gao , Haifeng Yuan , Xinjuan Du , Feng Dong , Yu Zhou , Shengnan Na , Yanpeng Chen , Mingyu Hu , Mei Hong , Shihe Yang
Rational design of viable routes to obtain efficient and stable oxygen evolution reaction (OER) electrocatalysts remains challenging, especially under industrial conditions. Here, we provide a solvent-steam assisted corrosion engineering strategy to directly fabricate high-entropy NiFe-LDH with spatially resolved structural order. Ammonium fluoride in methanol steam enables the formation of nanosheets while Fe3+ effectively enhances their adhesion to the semi-sacrificial nickel-iron foam (NFF), thereby conjuring up a NiFe-LDH@NFF catalyst that exhibits remarkable adaptability to robust electrochemical activation yet with excellent stability. Comprehensive measurements reveal the in-situ formation of high-valance metal oxyhydroxide and the enhancement of adsorption-desorption process. Under the industrial condition (6 mol/L KOH, 60 °C), the NiFe-LDH@NFF exhibits excellent activity of 50 mA/cm2 at 1.55 V and high durability of over 120 h at 200 mA/cm2. We anticipate that the steam assisted strategy could promote the development of efficient non-precious electrocatalysts for hydrogen energy.
合理设计可行的路线以获得高效稳定的氧进化反应(OER)电催化剂仍然具有挑战性,尤其是在工业条件下。在此,我们提供了一种溶剂-蒸汽辅助腐蚀工程策略,可直接制造出具有空间分辨结构秩序的高熵镍铁合金-LDH。甲醇蒸汽中的氟化铵可促进纳米片的形成,而 Fe3+ 则可有效增强纳米片与半牺牲型镍铁泡沫(NFF)的粘附性,从而形成一种 NiFe-LDH@NFF 催化剂,该催化剂对强力电化学活化具有显著的适应性,同时还具有极佳的稳定性。综合测量结果表明,该催化剂在原位形成了高价金属氢氧化物,并增强了吸附-解吸过程。在工业条件(6 mol/L KOH,60 °C)下,NiFe-LDH@NFF 在 1.55 V 时的活性为 50 mA/cm2,在 200 mA/cm2 时的耐久性超过 120 小时。我们预计,蒸汽辅助策略可促进高效非贵金属氢能电催化剂的开发。
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引用次数: 0
Approved delivery strategies for biopharmaceuticals 已获批准的生物制药给药策略
IF 9.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-08 DOI: 10.1016/j.cclet.2024.110225
Makhloufi Zoulikha , Zhongjian Chen , Jun Wu , Wei He
In recent years, biopharmaceuticals have witnessed remarkable advancements, transforming the landscape of therapeutic interventions. Biopharmaceuticals encompassing therapeutics generated through cutting-edge biotechnological methods have shown promising therapeutic outcomes. However, their clinical success hinges significantly on overcoming drug delivery challenges related to stability, intracellular delivery, immunogenicity, and pharmacokinetic properties. Herein, we provide an overview of various marketed macromolecules, including nucleic acids, and immunotherapeutic agents such as cytokines and monoclonal antibodies, as well as other therapeutic peptides/proteins like enzymes, hormones, and coagulation factors. Our primary focus is on elucidating the delivery challenges associated with these macromolecules and highlighting the pivotal role played by drug delivery platforms in the development of currently marketed products, offering valuable insights for both scientific research and the pharmaceutical industry.
近年来,生物制药取得了显著进步,改变了治疗干预的格局。生物制药包括通过尖端生物技术方法产生的治疗药物,已显示出良好的治疗效果。然而,它们在临床上的成功在很大程度上取决于能否克服与稳定性、细胞内给药、免疫原性和药代动力学特性有关的给药难题。在此,我们将概述各种已上市的大分子,包括核酸、细胞因子和单克隆抗体等免疫治疗剂,以及酶、激素和凝血因子等其他治疗肽/蛋白。我们的主要重点是阐明与这些大分子相关的给药难题,并强调给药平台在目前上市产品的开发过程中发挥的关键作用,为科学研究和制药行业提供有价值的见解。
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引用次数: 0
Cross-section design of the flow channels in membrane electrode assembly electrolyzer for CO2 reduction reaction through numerical simulations 通过数值模拟设计用于二氧化碳还原反应的膜电极组件电解槽的流道截面
IF 9.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-06 DOI: 10.1016/j.cclet.2024.110204
Lili Zhang , Hui Gao , Gong Zhang , Yuning Dong , Kai Huang , Zifan Pang , Tuo Wang , Chunlei Pei , Peng Zhang , Jinlong Gong
Membrane electrode assembly (MEA) is widely considered to be the most promising type of electrolyzer for the practical application of electrochemical CO2 reduction reaction (CO2RR). In MEAs, a square-shaped cross-section in the flow channel is normally adopted, the configuration optimization of which could potentially enhance the performance of the electrolyzer. This paper describes the numerical simulation study on the impact of the flow-channel cross-section shapes in the MEA electrolyzer for CO2RR. The results show that wide flow channels with low heights are beneficial to the CO2RR by providing a uniform flow field of CO2, especially at high current densities. Moreover, the larger the electrolytic cell, the more significant the effect is. This study provides a theoretical basis for the design of high-performance MEA electrolyzers for CO2RR.
膜电极组件(MEA)被广泛认为是电化学二氧化碳还原反应(CO2RR)实际应用中最有前途的电解槽类型。在 MEA 中,流道通常采用方形截面,对其进行配置优化有可能提高电解槽的性能。本文介绍了针对 CO2RR 的 MEA 电解槽中流道横截面形状影响的数值模拟研究。结果表明,高度较低的宽流道可提供均匀的二氧化碳流场,从而有利于 CO2RR,尤其是在电流密度较高的情况下。此外,电解槽越大,效果越显著。这项研究为设计用于 CO2RR 的高性能 MEA 电解槽提供了理论依据。
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引用次数: 0
Recent progress in the biomedical application of PEDOT:PSS hydrogels PEDOT:PSS 水凝胶生物医学应用的最新进展
IF 9.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-06 DOI: 10.1016/j.cclet.2024.109810
Binhan Zhao , Zheng Li , Lan Zheng , Zhichao Ye , Yuyang Yuan , Shanshan Zhang , Bo Liang , Tianyu Li

Bioelectronics have gained substantial research attention owing to their potential applications in health monitoring and diagnose, and greatly promoted the development of biomedicine. Recently, poly(3,4-ethylenedioxythiophene):polystyrene sulfonate (PEDOT:PSS) hydrogels have arose as a promising candidate for the next-generation bioelectronic interface due to its high-conductivity, versatility, flexibility and biocompatibility. In this review, we highlight the recent advances of PEDOT:PSS hydrogels, including the gelation methods and modification strategies, and summarize their wide applications in different type of sensors and tissue engineering in detail. We expect that this work will provide valuable information regarding the functionalizations and applications of PEDOT:PSS hydrogels.

生物电子学因其在健康监测和诊断方面的潜在应用而备受研究关注,并极大地推动了生物医学的发展。最近,聚(3,4-亚乙二氧基噻吩):聚苯乙烯磺酸盐(PEDOT:PSS)水凝胶因其高导电性、多功能性、柔韧性和生物相容性而成为下一代生物电子界面的理想候选材料。在这篇综述中,我们重点介绍了 PEDOT:PSS 水凝胶的最新进展,包括凝胶化方法和改性策略,并详细总结了它们在不同类型传感器和组织工程中的广泛应用。我们希望这项工作能为 PEDOT:PSS 水凝胶的功能化和应用提供有价值的信息。
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引用次数: 0
Persistent luminescence encoding for rapid and accurate oral-derived bacteria identification 用于快速准确识别口腔细菌的持续发光编码技术
IF 9.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-06 DOI: 10.1016/j.cclet.2024.110223
Chaohui Zheng , Jing Xi , Shiyi Long , Tianpei He , Rui Zhao , Xinyuan Luo , Na Chen , Quan Yuan
The dysbiosis of oral microbiota contributes to diseases such as periodontitis and certain cancers by triggering the host inflammatory response. Developing methods for the immediate and sensitive identification of oral microorganism is crucial for the rapid diagnosis and early interventions of associated diseases. Traditional methods for microbial detection primarily include the plate culturing, polymerase chain reaction and enzyme-linked immunosorbent assay, which are either time-consuming or laborious. Herein, we reported a persistent luminescence-encoded multiple-channel optical sensing array and achieved the rapid and accurate identification of oral-derived microorganisms. Our results demonstrate that electrostatic attractions and hydrophobic-hydrophobic interactions dominate the binding of the persistent luminescent nanoprobes to oral microorganisms and the microbial identification process can be finished within 30 min. Specifically, a total of 7 oral-derived microorganisms demonstrate their own response patterns and were differentiated by linear discriminant analysis (LDA) with the accuracy up to 100 % both in the solution and artificial saliva samples. Moreover, the persistent luminescence encoded array sensor could also discern the microorganism mixtures with the accuracy up to 100 %. The proposed persistent luminescence encoding sensor arrays in this work might offer new ideas for rapid and accurate oral-derived microorganism detection, and provide new ways for disease diagnosis associated with microbial metabolism.
口腔微生物菌群失调会引发宿主炎症反应,从而导致牙周炎和某些癌症等疾病。开发即时灵敏地识别口腔微生物的方法对于快速诊断和早期干预相关疾病至关重要。传统的微生物检测方法主要包括平板培养、聚合酶链反应和酶联免疫吸附试验,这些方法费时费力。在此,我们报告了一种持久发光编码多通道光学传感阵列,并实现了对口腔微生物的快速准确识别。我们的研究结果表明,静电吸引和疏水-疏水相互作用主导了持久性发光纳米微生物与口腔微生物的结合,微生物鉴定过程可在 30 分钟内完成。具体来说,共有 7 种口腔微生物展示了各自的反应模式,并通过线性判别分析(LDA)对溶液和人工唾液样本进行了区分,准确率高达 100%。此外,持久发光编码阵列传感器还能辨别微生物混合物,准确率高达 100%。这项工作中提出的持久性发光编码传感器阵列可能会为快速、准确地检测口腔微生物提供新的思路,并为与微生物代谢相关的疾病诊断提供新的方法。
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引用次数: 0
A portable and versatile fluorescent platform for high-throughput screening of toxic phosgene, diethyl chlorophosphate and volatile acyl chlorides 用于高通量筛选有毒光气、氯磷酸二乙酯和挥发性酰基氯的便携式多功能荧光平台
IF 9.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-06 DOI: 10.1016/j.cclet.2024.110222
Beitong Zhu , Xiaorui Yang , Lirong Jiang , Tianhong Chen , Shuangfei Wang , Lintao Zeng
Highly toxic phosgene, diethyl chlorophosphate (DCP) and volatile acyl chlorides endanger our life and public security. To achieve facile sensing and discrimination of multiple target analytes, herein, we presented a single fluorescent probe (BDP-CHD) for high-throughput screening of phosgene, DCP and volatile acyl chlorides. The probe underwent a covalent cascade reaction with phosgene to form boron dipyrromethene (BODIPY) with bright green fluorescence. By contrast, DCP, diphosgene and acyl chlorides can covalently assembled with the probe, giving rise to strong blue fluorescence. The probe has demonstrated high-throughput detection capability, high sensitivity, fast response (within 3 s) and parts per trillion (ppt) level detection limit. Furthermore, a portable platform based on BDP-CHD was constructed, which has achieved high-throughput discrimination of 16 analytes through linear discriminant analysis (LDA). Moreover, a smartphone adaptable RGB recognition pattern was established for the quantitative detection of multi-analytes. Therefore, this portable fluorescence sensing platform can serve as a versatile tool for rapid and high-throughput detection of toxic phosgene, DCP and volatile acyl chlorides. The proposed “one for more” strategy simplifies multi-target discrimination procedures and holds great promise for various sensing applications.
剧毒光气、氯磷酸二乙酯(DCP)和挥发性酰基氯危及我们的生命和公共安全。为了实现对多种目标分析物的简便感知和鉴别,我们在本文中提出了一种单一荧光探针(BDP-CHD),用于高通量筛选光气、氯磷酸二乙酯和挥发性酰基氯。该探针与光气发生共价级联反应,生成具有亮绿色荧光的硼二吡咯并烯(BODIPY)。相比之下,二氯丙烷、二光气和酰基氯可以与探针共价结合,产生强烈的蓝色荧光。该探针具有高通量检测能力、高灵敏度、快速反应(3 秒内)和万亿分之一(ppt)级检测限。此外,还构建了一个基于 BDP-CHD 的便携式平台,通过线性判别分析(LDA)实现了对 16 种分析物的高通量判别。此外,还建立了一种可适应智能手机的 RGB 识别模式,用于定量检测多种分析物。因此,这种便携式荧光传感平台可作为一种多功能工具,用于快速、高通量检测有毒光气、二氯丙醇和挥发性酰基氯。所提出的 "以一当十 "策略简化了多目标判别程序,在各种传感应用中大有可为。
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引用次数: 0
Highly robust supramolecular polymer networks crosslinked by metallacycles 金属环交联的高稳健性超分子聚合物网络
IF 9.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-04 DOI: 10.1016/j.cclet.2024.110208
Xiaoman Dang , Zhiying Wu , Tangxin Xiao , Zhouyu Wang , Leyong Wang
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引用次数: 0
期刊
Chinese Chemical Letters
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