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Unique compounds functionalized with three-membered cyclic structures 具有三元环结构的独特化合物
IF 7.6 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-06-16 DOI: 10.1016/j.gce.2025.06.005
Yuan Yao , Yingying Cao , Long Liu , Yanqiang Zhang
Three-membered cyclic compounds are a fascinating class of compounds: they have the maximum torsional and angular strain (sp3 hybridization but bond angles deviate from 109°28’), and possess unique physical and chemical properties. A lot of effort has been devoted to their synthesis and applications in recent years. This review provides an overview of various synthesis strategies for three-membered cyclic compounds, and summarizes the proposed reaction mechanisms and key issues such as structure-property relationships through specific examples. Meanwhile, the advantages and disadvantages of different synthesis strategies were discussed, including the recently developed electrochemical synthesis methods. Finally, the prospects and challenges for further scientific research and practical applications of three-membered cyclic compounds were emphasized. The summary of three-membered cyclic compounds is beneficial for the development and utilization of novel functionalized molecules.
三元环化合物是一类令人着迷的化合物:它们具有最大的扭转和角应变(sp3杂化,但键角偏离109°28′),并具有独特的物理和化学性质。近年来,人们对它们的合成和应用进行了大量的研究。本文综述了三元环类化合物的各种合成策略,并通过具体实例总结了所提出的反应机理和结构-性能关系等关键问题。同时,讨论了不同合成策略的优缺点,包括最近发展起来的电化学合成方法。最后,对三元环类化合物的进一步科学研究和实际应用提出了展望和挑战。对三元环类化合物的研究综述有助于开发和利用新型功能化分子。
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引用次数: 0
Molecular-level imaging of hydrogen-bonded organic frameworks by cryogenic low-dose electron microscopy 低温低剂量电子显微镜下氢键有机框架的分子水平成像
IF 7.6 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-06-08 DOI: 10.1016/j.gce.2025.06.004
Yikuan Liu , Yanbin Chen , Liwei Xia , Shuo Zhang, Zhangnan Zhong, Liwei Wang, Yujie Huang, Xinru Jiang, Mengru Bu, Qunfeng Zhang, Xiaonian Li, Yihan Zhu
The fundamental problems associated with structural inhomogeneities of hydrogen-bonded organic frameworks (HOFs), such as surface terminations and host-guest heterostructures that govern their functionalities and growth mechanisms, remain a critical gap in knowledge. This arises from the lack of advanced real-space structural characterization tools with molecular precision. By leveraging state-of-the-art cryogenic low-dose electron microscopy, this work overcomes the beam damage limitations of traditional techniques and elucidates the crystal structures, surface terminations, and host-guest structures of HOFs at molecular-level. Real-space observations confirm lateral crystal growth consistent with the terrace-ledge-kink (TLK) model, but deviate from the classical monomer-addition mechanism. Instead, we propose a nonclassical cooperative multisite monomer-addition mechanism, where simultaneous monomer addition at both framework and guest sites eventually drives crystal faceting.
与氢键有机框架(HOFs)结构不均质性相关的基本问题,如控制其功能和生长机制的表面末端和主客体异质结构,仍然是一个关键的知识缺口。这源于缺乏先进的具有分子精度的实空间结构表征工具。通过利用最先进的低温低剂量电子显微镜,这项工作克服了传统技术的光束损伤限制,并在分子水平上阐明了hof的晶体结构、表面末端和主客体结构。实空间观测证实了横向晶体生长符合梯田-边缘-扭结(TLK)模型,但偏离了经典的单体加成机制。相反,我们提出了一种非经典的合作多位点单体添加机制,其中在框架和客体位点同时添加单体最终驱动晶体饰面。
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引用次数: 0
Unlocking deep eutectic solvent knowledge through a large language model-driven framework and an interactive AI agent 通过大型语言模型驱动框架和交互式AI代理解锁深度共晶溶剂知识
IF 7.6 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-06-06 DOI: 10.1016/j.gce.2025.05.006
Xiting Peng , Yi Shen Tew , Kai Zhao , Chi Wang , Ren'ai Li , Shanying Hu , Xiaonan Wang
Artificial intelligence (AI) is playing an important role in advancing green chemical engineering, while the lack of data remains a primary challenge in many fields. Deep eutectic solvents (DESs) are a promising alternative to traditional organic solvents. However, the exploration of new DES formulations has long been constrained by trial-and-error research methods, a preference for familiar formulations, and a lack of easily accessible DES databases. This study proposes a framework driven by large language models (LLMs) for accurately and efficiently extracting data in the DES field, accelerating knowledge discovery. By coordinating LLMs and tools through predefined code paths, we extracted 34,027 data records and 9,215 unique DES formulations from 14,602 research articles, achieving an accuracy of over 90%, thereby creating a comprehensive domain knowledge base. An LLM-driven interactive agent has been deployed on an online platform, further facilitating access to this structured data and enabling researchers to overcome data limitations and accelerate the discovery of new DES formulations.
人工智能(AI)在推进绿色化学工程中发挥着重要作用,而缺乏数据仍然是许多领域的主要挑战。深共晶溶剂(DESs)是一种很有前途的有机溶剂替代品。然而,对新的DES配方的探索长期以来一直受到试错研究方法、对熟悉配方的偏好以及缺乏易于访问的DES数据库的限制。本研究提出了一个由大型语言模型(llm)驱动的框架,用于准确、高效地提取DES领域的数据,加速知识发现。通过协调llm和工具通过预定义的代码路径,我们从14,602篇研究文章中提取了34,027条数据记录和9,215个独特的DES公式,实现了90%以上的准确率,从而创建了一个全面的领域知识库。一个法学硕士驱动的交互式代理已经部署在一个在线平台上,进一步促进了对这些结构化数据的访问,使研究人员能够克服数据限制,加速发现新的DES配方。
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引用次数: 0
Aqueous polyamine-based deep eutectic solvent: balancing stability, CO2 absorption/desorption performance, and post-absorption viscosity 水聚胺基深共晶溶剂:平衡稳定性、CO2吸收/解吸性能和吸收后粘度
IF 7.6 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-06-05 DOI: 10.1016/j.gce.2025.06.001
Kaige Jia, Qiangbing Shi, Xiaoyan Ji
Deep eutectic solvents (DESs) have gained significant attention as potential absorbents for CO2 capture due to their tunable physicochemical properties and environmental sustainability. However, achieving a balance of thermal stability, absorption/desorption performance, and viscosity remains a critical challenge for industrial applications. To address this, a novel aqueous polyamine-based DES system was developed using an ionic liquid with high stabilityPzCl (piperazine chloride, P), as a hydrogen bond acceptor (HBA); a polyamine with multiple active sites, DETA (diethylenetriamine, D), as a hydrogen bond donor (HBD), and H2O as co-solvent. By systematically optimizing the molar ratio of PzCl to DETA, [PzCl][DETA] (PD) with a 1:5 molar ratio was identified as the optimal one based on the absorption capacity/rate, thermal stability, post-absorption viscosity, and desorption efficiency of its aqueous solution. Further investigation into the water content revealed that 30 wt% [PzCl][DETA] (1:5) effectively balanced the CO2 absorption capacity (0.168 g-CO2/g-absorbent) and desorption efficiency (54%), more outstanding than those of 30 wt% MEA (0.126 g-CO2/g-absorbent and 47%, respectively), and provided acceptable post-absorption viscosity (8.11 mPa·s), which was slightly higher than that of 30 wt% MEA (3.77 mPa·s) but lower than 10 mPa·s. These findings provide a scalable framework for designing sustainable absorbents that harmonize high performance with operational viability. This work bridges the gap between laboratory-scale innovations and industrial implementation in carbon capture technologies.
深共晶溶剂(DESs)由于其可调的物理化学性质和环境可持续性,作为二氧化碳捕获的潜在吸收剂受到了广泛的关注。然而,实现热稳定性、吸收/解吸性能和粘度的平衡仍然是工业应用的关键挑战。为了解决这一问题,研究人员开发了一种新型的基于聚胺的水基DES系统,该系统使用具有高稳定性的离子液体pzcl(氯化哌嗪,P)作为氢键受体(HBA);具有多个活性位点的多胺,DETA(二乙烯三胺,D)为氢键供体(HBD), H2O为助溶剂。通过对PzCl与DETA的摩尔比进行系统优化,通过对PzCl与DETA水溶液的吸附容量/速率、热稳定性、吸附后粘度和解吸效率的考察,确定了PzCl与DETA (PD)的摩尔比为1:5的最佳配比。进一步研究表明,30 wt% [PzCl][DETA](1:5)有效地平衡了CO2吸收能力(0.168 g-CO2/g-吸附剂)和解吸效率(54%),比30 wt% MEA (0.126 g-CO2/g-吸附剂和47%)更为突出,并提供了可接受的吸附后粘度(8.11 mPa·s),略高于30 wt% MEA (3.77 mPa·s),但低于10 mPa·s。这些发现为设计可持续吸收剂提供了一个可扩展的框架,以协调高性能和运营可行性。这项工作弥合了碳捕获技术在实验室规模创新和工业实施之间的差距。
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引用次数: 0
Stabilizing the cathode-electrolyte interphase for superior Li-ion batteries 稳定优质锂离子电池的阴极-电解质界面
IF 7.6 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-06-03 DOI: 10.1016/j.gce.2025.05.010
Yunze Zhang , Jian Wang
The cathode-electrolyte interphase (CEI) plays a pivotal role in determining the energy density and cycling stability of lithium-ion batteries. However, its complex formation mechanisms, dynamic evolution, and interplay with battery components pose significant challenges for a fundamental understanding and targeted regulation. While prior research has focused on modifying bulk electrolyte solvation structures and applying inert cathode coatings, this perspective analyzes the mechanisms of CEI formation and stabilization, with particular emphasis on cathode pre-interphase engineering, near-surface electric double-layer modulation, and functional coating design. Future research prospects are outlined, highlighting the advanced in situ characterization techniques with high spatiotemporal resolution to probe transient interfacial processes, along with innovative strategies for constructing CEI architectures.
阴极-电解质界面(CEI)对锂离子电池的能量密度和循环稳定性起着至关重要的作用。然而,其复杂的形成机制、动态演变以及与电池组件的相互作用为基本认识和有针对性的调控带来了重大挑战。虽然之前的研究主要集中在修改大块电解质溶剂化结构和应用惰性阴极涂层上,但本观点分析了CEI形成和稳定的机制,特别强调了阴极前界面工程,近表面双电层调制和功能涂层设计。展望了未来的研究前景,重点介绍了具有高时空分辨率的原位表征技术,以探测瞬态界面过程,以及构建CEI架构的创新策略。
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引用次数: 0
An internal circulation rotating packed bed for green chemical engineering: structure optimization of liquid lifter 绿色化工用内循环旋转填料床:提液器结构优化
IF 7.6 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-05-30 DOI: 10.1016/j.gce.2025.05.008
Zi-Lun Li , Liang Zheng , Li-Hua Wang , Yi-Qian Wei , Hai-Long Liao , Guang-Wen Chu , Yong Luo , Jian-Feng Chen
The internal circulation rotating packed beds (IN-RPBs) have been widely used in multiphase systems. However, its key component's liquid lifter suffers from the liquid lifting rate (QL), limiting the micro-mixing and mass transfer efficiency. In this study, the fluid motion inside the conventional lifter was theoretically analyzed. Based on the above theoretical analysis, a new impeller-equipped lifter was innovatively designed for the IN-RPB to enhance QL. Experiment results showed that QL was increased by 100% at 1400 r/min within the impeller-equipped lifter. Numerical simulations demonstrated that the flow field was altered in the impeller-equipped lifter, promoting the generation of vortices, thereby increasing the QL. Mass transfer experiments demonstrated that the structure optimization of the lifter led to a 60% increase in the gas-liquid volumetric mass transfer coefficient (kLa). This study provides a basis for the industrialization of the IN-RPB with an impeller-equipped lifter.
内循环旋转填料床(in - rpbs)在多相系统中得到了广泛应用。然而,其关键部件升液器受升液率(QL)的影响,限制了微混合和传质效率。本文从理论上分析了传统提升机内部的流体运动。在上述理论分析的基础上,为IN-RPB创新设计了一种新的叶轮式提升器来提高QL,实验结果表明,在1400 r/min时,叶轮式提升器内的QL提高了100%。数值模拟结果表明,叶轮式升力器内的流场发生了改变,促进了涡流的产生,从而提高了QL。传质实验结果表明,结构优化后的升力器气液体积传质系数(kLa)提高了60%。本研究为叶轮式提升机IN-RPB的工业化生产提供了依据。
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引用次数: 0
OFC: Outside Front Cover OFC:外封面
IF 9.1 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-05-23 DOI: 10.1016/S2666-9528(25)00023-8
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引用次数: 0
Outside Back Cover 外封底
IF 9.1 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-05-23 DOI: 10.1016/S2666-9528(25)00032-9
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引用次数: 0
A perspective on transforming fats, oil, and grease (FOG) into hydrogen: insights on steam reforming catalysts and the case study of Hong Kong using techno-economic analysis and life cycle assessment 将油脂转化为氢气的展望:蒸汽重整催化剂的见解及以香港为例,运用科技经济分析及生命周期评估
IF 7.6 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-05-16 DOI: 10.1016/j.gce.2025.05.002
Ariel Riofrio , Miguel A. Bañares , Zhenlei Zhang , Xiangping Zhang , King Lun Yeung
The increasing demand for sustainable energy has intensified interest in hydrogen production from renewable sources. Although catalytic steam reforming of methane and other feedstocks has been extensively investigated, research on utilizing fats, oils, and grease (FOG) remains limited and dispersed. This study offers a comprehensive analysis of steam reforming catalysts for FOG conversion, concentrating on nickel-based, noble metal, and metal oxide-supported catalysts initially developed for methane, waste cooking oil, and glycerol. Catalyst performance is assessed in terms of activity, stability, cost, and environmental impact, addressing sustainable catalyst design and recycling principles. FOG management strategies are also explored, with a particular emphasis on Hong Kong, where FOG interception is crucial due to infrastructure constraints. Unlike cities where food waste is ground and flushed through extensive sewer systems, Hong Kong necessitates localized FOG removal to prevent costly blockages and environmental harm. A techno-economic analysis demonstrated the feasibility of producing H2 at a selling price as low as USD 3/kg H2, with a carbon capture potential of 0.40 kg CO2-eq/kg H2. Life cycle assessment (LCA) further confirmed environmental benefits, indicating the potential to capture 0.14 kg CO2 per kg of FOG processed. Additionally, the study identifies opportunities for cost reduction through more efficient FOG acquisition and valorization, which can enhance carbon savings and economic viability. Overall, this work underscores the potential of FOG as a renewable feedstock and delineates key research directions for catalyst development and integrated waste-to-hydrogen systems.
对可持续能源日益增长的需求增强了人们对可再生能源制氢的兴趣。尽管甲烷和其他原料的催化蒸汽重整已经得到了广泛的研究,但利用脂肪、油和油脂(FOG)的研究仍然有限且分散。本研究提供了FOG转化的蒸汽重整催化剂的综合分析,集中在镍基、贵金属和金属氧化物支持的催化剂上,最初是为甲烷、废食用油和甘油开发的。催化剂性能从活性、稳定性、成本和环境影响等方面进行评估,解决可持续催化剂设计和回收原则。此外,还探讨了光纤陀螺管理策略,特别强调香港,由于基础设施的限制,光纤陀螺拦截至关重要。不同于城市的食物垃圾被碾碎并通过广泛的下水道系统冲走,香港需要局部清除雾雾,以防止代价高昂的堵塞和环境危害。一项技术经济分析表明,以低至3美元/千克H2的价格生产氢气是可行的,每千克H2的碳捕集潜力为0.40千克二氧化碳当量。生命周期评估(LCA)进一步证实了环境效益,表明每处理1千克雾可捕获0.14千克二氧化碳。此外,该研究还确定了通过更有效的FOG获取和定价来降低成本的机会,这可以提高碳节约和经济可行性。总的来说,这项工作强调了FOG作为可再生原料的潜力,并描绘了催化剂开发和综合废物制氢系统的关键研究方向。
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引用次数: 0
Smooth pore surface in zeolites for krypton capture under humid conditions 在潮湿条件下,沸石的光滑孔表面用于氪捕获
IF 7.6 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-05-10 DOI: 10.1016/j.gce.2025.04.005
Yongheng Ren , Xiaohua Liu , Genggeng Dai , Lu Zhang , Hongwei Chen , Pengcheng Yang , Ye Li , Xinyue Yu , Yang Chen , Xiufeng Shi , Peng Lin , Jiangfeng Yang , Jinping Li , Libo Li
Efficient trace radioactive krypton isotopes (85Kr) capture from air under humid conditions is a critical challenge for nuclear safety and environmental protection. Commercial zeolites suffer from low Kr/N2 selectivity due to cation-induced interactions that strengthen nitrogen (N2) adsorption, while their hydrophilicity triggers severe water competition. Herein, we proposed utilizing the smooth pore surface in pure-silica zeolites to weaken the N2 adsorption and mitigate water competition. The pure silica ZSM-11 exhibited significant Kr/N2 selectivity (4.8) and Kr uptake of 12.8 cm3/g at 298 K and 1 bar, superior to the commercial zeolites. Its intersecting ten-membered ring (10-MR) channels facilitated optimal Kr interactions and distribution, as corroborated by Grand Canonical Monte Carlo (GCMC) simulations, which revealed preferential multisite Kr···O interactions with significantly higher Kr densities than N2. Dynamic breakthrough experiments demonstrated that pure silica zeolites, particularly ZSM-11, achieved superior Kr capturing performance and cycling stability under humid conditions (relative humidity (RH) = 72.6%), realizing a leap from ppm levels to high purity (> 80%) Kr. This work demonstrated the rational design of pore surface and topologies in zeolite for inert gases capture provided an effective technological route for radioactive krypton isotopes separation under humid conditions.
在潮湿条件下从空气中有效捕获痕量放射性氪同位素(85Kr)是核安全和环境保护的关键挑战。由于阳离子诱导的相互作用加强了氮(N2)的吸附,商业沸石的Kr/N2选择性较低,而它们的亲水性引发了严重的水竞争。在此,我们提出利用纯硅沸石的光滑孔表面来减弱N2吸附和缓解水竞争。纯二氧化硅ZSM-11在298 K和1 bar条件下具有显著的Kr/N2选择性(4.8)和Kr吸收量(12.8 cm3/g),优于工业沸石。其交叉的十元环(10-MR)通道促进了最佳的Kr相互作用和分布,正如大规范蒙特卡罗(GCMC)模拟所证实的那样,显示出Kr密度显著高于N2的优先多位点Kr···O相互作用。动态突破实验表明,纯硅沸石,特别是ZSM-11,在潮湿条件下(相对湿度(RH) = 72.6%)具有优越的Kr捕获性能和循环稳定性,实现了从ppm水平到高纯度(> 80%) Kr的飞跃。该工作证明了沸石中用于惰性气体捕获的孔表面和拓扑结构的合理设计为放射性氪同位素在潮湿条件下分离提供了有效的技术途径。
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引用次数: 0
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Green Chemical Engineering
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