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IF 8.9 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-11-17 DOI: 10.1016/S1001-8417(25)01184-2
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引用次数: 0
Roadmap on sustainable materials and technologies 可持续材料和技术路线图
IF 8.9 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-11-14 DOI: 10.1016/j.cclet.2025.112116
Jing Guo , Chunhui Luo , Peng Li , Mao Ye , Zhihua Qiao , Yubo Wu , Huiqin Hu , Xubiao Luo , Liming Yang , Yulin Cai , Pengwei Li , Kai Zhu , Cheng Fu , Bing Yu , Yueying Chen , Shichang Wang , Ting Wang , Chongchong Qi , Zirou Liu , Dongmei Huang , Jianmin Ma
Sustainable development for our life is important task, which is driven by key materials and technologies. In this roadmap, we discuss three main aspects in addressing environmental questions, green chemical processes and energy challenges. They are included, such as gas treatment and separation, wastewater treatment, waste gas treatment, solid waste treatment, lithium extraction, hydrogen production, water splitting, CO2 reduction, photocatalytic clean technologies, plastic degradation, fuel cells, lithium batteries, sodium batteries, aqueous batteries, solid state batteries, metal air batteries and supercapacitors. Their status, challenges, progress and future perspectives are also discussed. We hope that this paper can give clear views on sustainable development in materials and technologies.
人类生活的可持续发展是一项重要任务,关键材料和关键技术是推动可持续发展的关键。在这个路线图中,我们讨论了解决环境问题、绿色化学过程和能源挑战的三个主要方面。它们包括,如气体处理和分离,废水处理,废气处理,固体废物处理,锂提取,制氢,水分解,二氧化碳还原,光催化清洁技术,塑料降解,燃料电池,锂电池,钠电池,水电池,固态电池,金属空气电池和超级电容器。讨论了它们的现状、挑战、进展和未来展望。我们希望本文能对材料和技术的可持续发展提出明确的看法。
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引用次数: 0
Entropy-stabilized nanoporous structures enable sintering-resistant Pt species 熵稳定的纳米孔结构使Pt物种具有抗烧结性
IF 8.9 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-11-14 DOI: 10.1016/j.cclet.2025.112114
Yunpeng Wang , Zhuxin Lyu , Yueming Sun, Yunqian Dai
Supported noble‐metal catalysts often suffer from nanoparticle sintering, resulting in rapid deactivation under high‐temperature conditions. We report hierarchically porous spinel type high-entropy oxide (S-HEO) nanofibers, (CrMnFeCoMg)3O4, as robust supports for Pt nanoparticles. The porous structure (38.5 m2/g) endows thermal stability, preserving porosity after 880 °C calcination. The porous Pt/S-HEO-500 exhibits exceptional sinter-resistance. Under 500 °C calcination, Pt exhibits only a 0.2 nm growth increment, owing to the physical confinement and strong metal–support interactions. For Pt/S-HEO-500, the T50 (50 % conversion temperature) for CO oxidation was merely 9 °C higher than that without calcination, with 100 % conversion retained over 100 h of steady-state operation. These findings position porous spinel HEO nanofibers as a versatile platform for designing sinter-resistant noble-metal catalysts in high-temperature applications.
负载型贵金属催化剂经常受到纳米颗粒烧结的影响,导致其在高温条件下快速失活。我们报告了分层多孔尖晶石型高熵氧化物(S-HEO)纳米纤维(crmnnfecomg)3O4作为Pt纳米颗粒的坚固支撑。多孔结构(38.5 m2/g)具有热稳定性,在880 °C煅烧后仍保持孔隙度。多孔Pt/S-HEO-500具有优异的抗烧结性能。在500 °C的煅烧条件下,由于物理限制和强金属-载体相互作用,Pt仅表现出0.2 nm的生长增量。对于Pt/S-HEO-500, CO氧化的T50(50 %转化温度)仅比未煅烧时高9 °C,在100 h的稳态运行中保持100 %的转化率。这些发现将多孔尖晶石HEO纳米纤维定位为设计高温应用中抗烧结贵金属催化剂的通用平台。
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引用次数: 0
Unraveling metabolic complexity of multi-payload PEG-irinotecan prodrug: A deconvolution-based LC-Q-TOF MS approach for preclinical pharmacokinetic characterization 揭示多载荷peg -伊立替康前药的代谢复杂性:基于反卷积的LC-Q-TOF质谱方法用于临床前药代动力学表征
IF 8.9 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-11-12 DOI: 10.1016/j.cclet.2025.112099
Shiwen Song , Mingyang Zhao , Xiangrong Song , Huaidong Yu , Xin Xu , Dong Sun , Jingkai Gu
PEGylation, the controlled covalent conjugation of polyethylene glycol to therapeutics, enhances therapeutic efficacy through optimized pharmacokinetics. However, to date no high-molecular-weight PEGylated small-molecule prodrugs have received regulatory approval. This technological gap can be partially attributed to the exponential proliferation of metabolic intermediates resulting from multi-payload conjugation strategies, which introduces unprecedented analytical complexities in metabolite profiling and pharmacokinetic characterization. To address this challenge, we developed a liquid chromatography-triple-quadrupole/time-of-flight mass spectrometry platform for PEG20k-(irinotecan)3, a Phase III clinical candidate. Our methodology employs payload stoichiometry-based chromatographic resolution for clustering isomeric PEG species. Complementarily, diagnostic product ions at m/z 699.83, 569.27, and 587.28 enable systematic differentiation between double-loaded, single-loaded, and released irinotecan payload. This approach successfully identifies eight metabolic clusters spanning from PEG-conjugates, cleaved PEG segments, and released small-molecule species. Its demonstrated capacity to deconvolute complex metabolic profiles—through payload-stoichiometry based chromatographic resolution coupled with diagnostic ion analysis—positions this workflow as an attractive tool for accelerating the development of PEGylated small-molecule therapeutics.
聚乙二醇化,控制共价偶联聚乙二醇到治疗剂,通过优化药代动力学提高治疗效果。然而,到目前为止,还没有高分子量聚乙二醇化的小分子前药获得监管部门的批准。这种技术差距可以部分归因于多载荷偶联策略导致的代谢中间体的指数增殖,这在代谢物分析和药代动力学表征中引入了前所未有的分析复杂性。为了应对这一挑战,我们开发了一种液相色谱-三重四极杆/飞行时间质谱分析平台,用于III期临床候选药物PEG20k-(伊立替康)3。我们的方法采用有效载荷化学计量为基础的聚类异构体聚乙二醇的色谱分辨率。此外,m/z 699.83、569.27和587.28的诊断产物离子可以系统地区分双载、单载和释放的伊立替康有效载荷。该方法成功地鉴定了8个代谢簇,包括PEG偶联物、裂解的PEG片段和释放的小分子物种。通过基于有效载荷化学计量学的色谱分辨率加上诊断离子分析,它证明了对复杂代谢谱进行反卷积的能力,这使得该工作流程成为加速聚乙二醇化小分子疗法开发的有吸引力的工具。
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引用次数: 0
Atomically dispersed Fe‑N4 sites on g‑C3N4 enable highly selective CO2‑to‑CO electrocatalysis g‑C3N4上原子分散的Fe‑N4位点实现了高选择性的CO2 - to - CO电催化
IF 8.9 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-11-11 DOI: 10.1016/j.cclet.2025.112096
Yongliang Ban , Meng Zhang , Jianya He , Chunfeng Shao , Zhongliao Wang , Wei Zhao , Kai Dai
The development of efficient and cost-effective non-precious-metal single-atom catalysts (SACs) is crucial for advancing the practical application of electrocatalytic CO2 reduction (CO2RR). However, identifying highly active metal atoms and designing catalysts with uniform active center structures remain significant challenges. To address this, we developed a generic pyrolysis method to synthesize a series of transition metal-based SACs with atomically dispersed metal anchored on carbon nitride support (M-C3N4, M = Fe, Ni, Cu). Benefiting from the unique electronic structure of the Fe-N4 sites supported on C3N4, the Fe-C3N4 catalyst demonstrated exceptional performance, achieving a CO Faradaic efficiency of 99.6 % and maintaining excellent stability. Theoretical calculations indicate that the Fe site exhibits a relatively stronger interaction with the *COOH intermediate, thereby helping to lower the energy barrier of the CO2 protonation process. This study provides valuable theoretical insights and practical synthesis strategies for designing high-performance non-precious-metal SACs for CO2RR.
开发高效、经济的非贵金属单原子催化剂对于推进电催化CO2还原(CO2RR)的实际应用至关重要。然而,鉴定高活性金属原子和设计具有均匀活性中心结构的催化剂仍然是一个重大挑战。为了解决这个问题,我们开发了一种通用的热解方法来合成一系列过渡金属基SACs,这些SACs将原子分散的金属锚定在氮化碳载体上(M- c3n4, M = Fe, Ni, Cu)。得益于C3N4上Fe-N4位独特的电子结构,Fe-C3N4催化剂表现出优异的性能,CO法拉第效率达到99.6 %,并保持了优异的稳定性。理论计算表明,Fe位点与*COOH中间体的相互作用相对较强,从而有助于降低CO2质子化过程的能垒。该研究为设计高性能的CO2RR非贵金属sac提供了有价值的理论见解和实用的合成策略。
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引用次数: 0
Rise of colloidal silver bismuth sulfide nanocrystals solar cells 胶体硫化银铋纳米晶太阳能电池的兴起
IF 8.9 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-11-04 DOI: 10.1016/j.cclet.2025.112054
Yongqiang Ji , Donglin Jia , Fan Xu , Zhengwei Li , Lin Zhang , Le Li , Hengwei Qiu
In recent years, AgBiS2 nanocrystals (NCs) have emerged as a research hotspot in the field of solar cells due to their excellent optoelectronic properties and environmentally friendly characteristics. Although the theoretical power conversion efficiency (PCE) of AgBiS2 NC solar cells can reach up to 26%, the current best device only achieved a PCE of 10.84%. Such an enormous efficiency gap is primarily caused by the complex surface defects, severe carrier recombination, and undesirable energy-level mismatches. Therefore, this review comprehensively summarizes recent advancements in AgBiS2 NCs, including their crystal structures, optoelectronic properties, synthesis methods, ligand engineering, and device optimization. By fine-tuning synthesis conditions (e.g., temperature, precursor ratios) and employing ligand exchange strategies (solid-state/liquid-state), significant improvements in material performance have been realized. Furthermore, device structure optimization (e.g., transport layer selection, interface modification) and energy-level alignment engineering have further enhanced efficiency. Despite decent stabilities of AgBiS2 NCs, several challenges such as large-area uniformity and long-term device durability remain unraveled, which may be the major obstacles for their further commercialization. Future advancements in defect control, the development of novel ligands, and encapsulation technologies are expected to expand the applications of AgBiS2 NCs in flexible electronics, aerospace, and wearable devices.
近年来,AgBiS2纳米晶体(NCs)因其优异的光电性能和环保特性成为太阳能电池领域的研究热点。虽然AgBiS2 NC太阳能电池的理论功率转换效率(PCE)可以达到26%,但目前最好的器件的PCE仅达到10.84%。这种巨大的效率差距主要是由复杂的表面缺陷、严重的载流子复合和不理想的能级不匹配造成的。因此,本文综述了AgBiS2纳米材料的晶体结构、光电性能、合成方法、配体工程和器件优化等方面的最新进展。通过微调合成条件(如温度、前驱体比例)和采用配体交换策略(固态/液态),实现了材料性能的显著改善。此外,器件结构优化(如传输层选择、接口修改)和能级对齐工程进一步提高了效率。尽管AgBiS2 NCs具有良好的稳定性,但诸如大面积均匀性和长期设备耐用性等几个挑战仍未解决,这可能是其进一步商业化的主要障碍。未来在缺陷控制、新型配体和封装技术方面的进步有望扩大AgBiS2 NCs在柔性电子、航空航天和可穿戴设备中的应用。
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引用次数: 0
Metal-organic framework materials for encapsulation, release and delivery of essential oils: Engineering strategies and challenges 用于精油封装、释放和输送的金属有机框架材料:工程策略和挑战
IF 8.9 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-11-01 DOI: 10.1016/j.cclet.2025.112049
Junfeng Huang , Hongxin Chen , Yan Liao , Xiaowen Zhang , Zengzhu Zhang , Xiaoyu Su , Zihong Xie , Biao Li , Baode Shen , Pengfei Yue
Essential oils (EOs) are widely present in aromatic plants and possess a wide range of significant pharmacological activities such as antibacterial, antioxidant and anti-tumor properties. They have broad application prospects in medical care, food, agriculture and other fields. However, their poor stability poses substantial challenges that significantly hinder their development and practical application. Metal-organic framework materials (MOFs), characterized by highly controllable structures, large specific surface areas, and stimuli-responsive release properties, have been extensively utilized in various fields such as drug delivery and food preservation. Due to their capacity to encapsulate and deliver EOs, MOFs have garnered considerable attention. In this review, we systematically summarize the structural features, types, and characteristics of MOFs, as well as the recent advancements in their application for controlled EO release. Furthermore, we focus on discussing engineering strategies aimed at enhancing the encapsulation, release, and delivery of EOs using MOFs. Finally, we briefly outline the existing challenges in the delivery of EOs using MOFs and present well-reasoned insights into prospective directions for future research.
精油广泛存在于芳香植物中,具有抗菌、抗氧化、抗肿瘤等药理活性。在医疗、食品、农业等领域有着广阔的应用前景。然而,它们的稳定性差带来了重大挑战,严重阻碍了它们的发展和实际应用。金属-有机骨架材料(MOFs)具有结构高度可控、比表面积大、刺激响应释放等特点,在药物递送、食品保鲜等领域得到了广泛的应用。由于它们封装和交付EOs的能力,mof已经引起了相当大的关注。本文系统地综述了MOFs的结构特点、类型和特点,以及其在可控EO释放中的应用进展。此外,我们将重点讨论旨在增强使用mof的EOs的封装、发布和交付的工程策略。最后,我们简要概述了使用mof提供EOs的现有挑战,并对未来研究的预期方向提出了合理的见解。
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引用次数: 0
Dovetail joint strategy for constructing giant multi-propeller supramolecular architectures 巨型多螺旋桨超分子结构的燕尾连接策略
IF 8.9 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-10-31 DOI: 10.1016/j.cclet.2025.112051
He Zhao , Qiangqiang Dong , Fengxue Liu , Ning Wang , Lijun Wang , Mingzhao Chen , Zhilong Jiang , Die Liu , Jun Wang , Pingshan Wang , Yiming Li
The structural principles of traditional Chinese mortise-and-tenon joints have inspired breakthroughs in supramolecular engineering. Nevertheless, substantial challenges remain in constructing nanoscale supramolecular architectures with precisely controlled giant dimensions. Herein, we report a precision-guided synthetic strategy for constructing giant 2D and 3D supramolecular architectures with rhomboidal motifs, which was achieved through a dovetail joint strategy. Initial assembly of bis-mortise ligand L1 with dovetail tenon ligand L2 in the presence of Cd2+ ions yielded the fundamental bis-rhombic supramolecule R1. Subsequent structural elaboration of the dovetail tenon motif enabled the development of multitopic ligands L3 and L4, which facilitated the construction of expanded architectures of the giant bis-propeller supramolecule R2 and tris-propeller supramolecule R3. The synthesized supramolecules R1–R3 were fully characterized multidimensional NMR spectroscopy, electrospray ionization mass spectrometry (ESI-MS), traveling wave ion mobility mass spectrometry (TWIM-MS), transmission electron microscopy (TEM), and atomic force microscopy (AFM). This work develops an innovative dovetail-joint assembly strategy for constructing rigid giant supramolecular architectures, establishing a new paradigm for precision engineering of complex 3D molecular systems.
中国传统榫卯连接的结构原理激发了超分子工程的突破。然而,构建具有精确控制的巨大尺寸的纳米级超分子结构仍然存在重大挑战。在此,我们报告了一种精确制导的合成策略,用于构建具有菱形基序的巨型二维和三维超分子结构,该策略通过燕尾连接策略实现。在Cd2+离子存在下,双榫配体L1与燕尾榫配体L2的初始组装产生了基本的双斜方超分子R1。随后对燕尾榫基序的结构细化使多主题配体L3和L4的发展成为可能,从而促进了巨型双螺旋桨超分子R2和三螺旋桨超分子R3的扩展结构的构建。对合成的超分子R1-R3进行了多维核磁共振谱、电喷雾电离质谱(ESI-MS)、行波离子迁移率质谱(TWIM-MS)、透射电子显微镜(TEM)和原子力显微镜(AFM)等表征。本工作开发了一种用于构建刚性巨型超分子结构的创新燕尾连接装配策略,为复杂3D分子系统的精密工程建立了新的范例。
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引用次数: 0
Lithium-bond chemistry enlightens 600 Wh/kg solid-state batteries 锂键化学启发600 Wh/kg固态电池
IF 8.9 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-10-30 DOI: 10.1016/j.cclet.2025.112045
Hong-Li Long, Hong-Jie Peng
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引用次数: 0
Rigid urea-based structures drive analysis of chiral amino acids 刚性脲基结构驱动手性氨基酸的分析
IF 8.9 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-10-30 DOI: 10.1016/j.cclet.2025.112039
Yanhui Zhong , Peisi Xie , Chengyi Xie , Lei Guo , Weiwei Chen , Shuyi Wang , Xiaoxiao Wang , Fuyue Wang , Zian Lin , Gongke Li , Zongwei Cai
Chiral amino acids (AAs) serve as essential building blocks of proteins and play vital physiological roles in living organisms. To achieve accurate, rapid, and high-throughput analysis of chiral AAs, this work proposed a methylbenzyl isocyanate (MBIC) derivatization strategy coupled with ultra-high performance liquid chromatography-mass spectrometry or trapped ion mobility spectrometry-mass spectrometry. The integration of a chiral carbon atom with a rigid urea-based structure can significantly enhance the separation of chiral MBIC-labeled AA enantiomers. This phenomenon can be attributed to the labeled l-AAs allow the carboxyl group to form intramolecular hydrogen bonds with the amino group in the rigid urea-based structure, whereas labeled d-AAs are unable to form such bonds. The method based on MBIC derivatization coupled with ultra-performance liquid chromatography-tandem mass spectrometry achieved simultaneous separation of 19 pairs of chiral AAs using only a C18 column within 30 min, enabling quantitatively detect twelve types of chiral AAs in the serum of healthy humans and Parkinson's patients. The distribution of twenty-four chiral AAs is observed in mouse brain using MBIC labeling-based matrix-assisted laser desorption/ionization-trapped ion mobility spectrometry-mass spectrometry imaging without prior separation. Our work elucidates the principles governing the separation of chiral AAs using derivatization methods, providing valuable guidance for the separation of chiral compounds.
手性氨基酸(AAs)作为蛋白质的基本组成部分,在生物体中起着重要的生理作用。为了实现准确、快速、高通量的手性原子吸收光谱分析,本研究提出了异氰酸甲酯(MBIC)衍生化策略与超高性能液相色谱-质谱或捕获离子迁移率谱-质谱联用。手性碳原子与刚性脲基结构的整合可以显著增强mbic标记的手性AA对映体的分离。这一现象可归因于标记的l- aa允许羧基与刚性脲基结构中的氨基形成分子内氢键,而标记的d- aa则不能形成这种键。基于MBIC衍生化-超高效液相色谱-串联质谱联用的方法在30 min内仅用C18色谱柱即可同时分离19对手性原子吸收剂,可定量检测健康人及帕金森病患者血清中的12种手性原子吸收剂。采用基于MBIC标记的基质辅助激光解吸/电离捕获离子迁移谱-质谱成像技术,在不预先分离的情况下,观察了24种手性原子吸收剂在小鼠脑内的分布。本研究阐明了衍生化方法分离手性原子吸收剂的原理,为手性化合物的分离提供了有价值的指导。
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引用次数: 0
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Chinese Chemical Letters
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