Green Chemical Engineering最新文献

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IF 7.6 Q1 ENGINEERING, CHEMICAL

Green Chemical Engineering

Pub Date : 2025-12-24 DOI: 10.1016/S2666-9528(25)00099-8

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IF 7.6 Q1 ENGINEERING, CHEMICAL

Green Chemical Engineering

Pub Date : 2025-12-24 DOI: 10.1016/S2666-9528(25)00107-4

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IF 7.6 Q1 ENGINEERING, CHEMICAL

Green Chemical Engineering

Pub Date : 2025-10-31 DOI: 10.1016/S2666-9528(25)00090-1

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IF 7.6 Q1 ENGINEERING, CHEMICAL

Green Chemical Engineering

Pub Date : 2025-10-31 DOI: 10.1016/S2666-9528(25)00081-0

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IF 7.6 Q1 ENGINEERING, CHEMICAL

Green Chemical Engineering

Pub Date : 2025-08-30 DOI: 10.1016/S2666-9528(25)00064-0

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IF 7.6 Q1 ENGINEERING, CHEMICAL

Green Chemical Engineering

Pub Date : 2025-08-30 DOI: 10.1016/S2666-9528(25)00072-X

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Integrated alkaline and deep eutectic solvent-based green strategy for lignin fractionation and thermochemical valorization 木质素分馏和热化学增值的碱性和深共晶溶剂型综合绿色策略

IF 7.6 Q1 ENGINEERING, CHEMICAL

Green Chemical Engineering

Pub Date : 2025-07-09 DOI: 10.1016/j.gce.2025.07.004

Penghui Li , Shubin Wu , Honghong Wang , Yuliang He

In this work, an efficient and green strategy for selective extraction and high-value utilization of lignin was proposed. Most of the hemicellulose in the feedstock was first removed by alkaline pretreatment to create a favorable structural environment for subsequent lignin dissolution. Subsequently, an acid-alcohol deep eutectic solvent (DES) system based on FeCl₃-ethylene glycol (FeCl₃-EG) was developed to achieve efficient and selective lignin dissolution. The results of characterization by Fourier transform infrared (FT-IR) spectroscopy, X-ray diffraction (XRD), and Brunauer-Emmett-Teller (BET) showed that the lignin was removed significantly after the treatment, the cellulose structure was preserved, and the crystallinity and specific surface area were increased to 73.46% and 2.764 m²/g, respectively. The highest delignification rate of 96.53% was achieved when EG:FeCl₃ = 1:0.3. Gas chromatography-mass spectrometry (GC-MS) detected a variety of low molecular phenolic products. In-situ Raman spectroscopy revealed the dynamic process of lignin dissolution from the cell wall. The regenerated lignin was systematically characterized by FTIR, thermogravimetry (TG), elemental analysis, and two-dimensional heteronuclear single quantum coherence-nuclear magnetic resonance (2D HSQC-NMR), and it was found that as the FeCl₃ content in DES increased, the β-O-4 content decreased, and the thermal stability of lignin increased. The pyrolysis properties were further analyzed by in-situ infrared (IR) spectroscopy, pyrolysis gas chromatography-mass spectrometry (Py GC-MS), and U-tube device, which showed that the regenerated lignin pyrolysis products had a high yield of the liquid phase and good phenol selectivity (40.94%), which demonstrated good selectivity and application prospects. This study provides a theoretical basis and process reference for the green extraction of lignin and its platform compound conversion.

本文提出了一种高效、绿色的木质素选择性提取和高价值利用策略。原料中的大部分半纤维素首先通过碱性预处理去除，为随后的木质素溶解创造有利的结构环境。随后，开发了一种基于fecl3 -乙二醇（FeCl3-EG）的酸醇深度共晶溶剂（DES）体系，以实现高效、选择性的木质素溶解。傅里叶变换红外光谱（FT-IR）、x射线衍射（XRD）、BET （bruauer - emmet - teller）表征结果表明，处理后木质素被明显去除，纤维素结构保持不变，结晶度和比表面积分别提高到73.46%和2.764 m2/g。当EG:FeCl3 = 1:0.3时，脱木质素率最高，达96.53%。气相色谱-质谱联用技术（GC-MS）检测了多种低分子酚类产物。原位拉曼光谱揭示了木质素从细胞壁溶解的动态过程。利用FTIR、热重（TG）、元素分析和二维异核单量子相干核磁共振（2D HSQC-NMR）对再生木质素进行了系统表征，发现随着DES中FeCl3含量的增加，β-O-4含量降低，木质素的热稳定性提高。通过原位红外光谱（IR）、热解气相色谱-质谱（Py GC-MS）和u型管装置对其热解特性进行分析，结果表明再生木质素热解产物液相收率高，苯酚选择性好（40.94%），具有良好的选择性和应用前景。本研究为木质素的绿色提取及其平台化合物转化提供了理论依据和工艺参考。

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引用次数: 0

A multiscale investigation combining thermodynamic modeling and molecular dynamics study on CO2 capture with [N1111][Triz]-H2O solvent [N1111][Triz]-H2O溶剂捕集CO2的热力学模型与分子动力学研究

IF 7.6 Q1 ENGINEERING, CHEMICAL

Green Chemical Engineering

Pub Date : 2025-07-01 DOI: 10.1016/j.gce.2025.06.008

Haichuan Yin , Yan Xu , Xiaochun Zhang , Xu Wang , Peng Yang , Guoxiong Zhan , Yinge Bai , Zhenlei Zhang , Xiangping Zhang

The urgent need to mitigate anthropogenic CO₂ emissions has driven the development of energy-efficient carbon capture systems. This study investigated a [N₁₁₁₁][Triz]-H₂O hybrid solvent for CO₂ capture using integrated experimental and computational approaches. A multiscale methodology combining thermodynamic analysis, phase equilibrium measurements, and molecular dynamics (MD) simulations was employed to elucidate the absorption mechanisms and the composition-property relationships. The thermodynamic analysis, incorporating Henry's law, the non-random two-liquid (NRTL) model for activity coefficients, the Redlich-Kwong equation, and reaction equilibrium constraints, accurately predicted the gas-liquid equilibrium (GLE) behavior, achieving an R² of 99.1% and an average absolute relative deviation (AARD) of 7.76%. The [N₁₁₁₁][Triz]-H₂O hybrid solvent exhibits exceptional CO₂ absorption performance, with a capacity of 0.25 mol/mol (at 313.15 K and 0.025 MPa for w_IL = 80%), attributed to synergistic physical-chemical interactions. MD simulations reveal the dynamic CO₂ absorption process in [N₁₁₁₁][Triz]-H₂O hybrid solvents: CO₂ molecules preferentially accumulate at the gas-liquid interface before gradually diffusing into the bulk phase. Increasing the [N₁₁₁₁][Triz] content enhances CO₂ absorption capacity by providing more interaction sites, while water modulates interfacial behavior and diffusion kinetics. This research provides in-depth insights into the absorption behaviors of [N₁₁₁₁][Triz]-H₂O hybrid solvents for CO₂, offering theoretical support for the development of efficient CO₂ capture solvents and highlighting its potential for industrial implementation.

减少人为二氧化碳排放的迫切需要推动了节能碳捕获系统的发展。本研究采用实验与计算相结合的方法研究了[N1111][Triz]-H2O混合溶剂对CO2的捕集效果。采用热力学分析、相平衡测量和分子动力学（MD）模拟相结合的多尺度方法来阐明吸收机理和组成-性质关系。热力学分析结合亨利定律、活度系数非随机双液（NRTL）模型、Redlich-Kwong方程和反应平衡约束，准确预测了气液平衡（GLE）行为，R2为99.1%，平均绝对相对偏差（AARD）为7.76%。[N1111][Triz]-H2O混合溶剂表现出优异的CO2吸收性能，在313.15 K和0.025 MPa （wIL = 80%）条件下，由于物理化学相互作用的协同作用，其CO2吸收容量为0.25 mol/mol。MD模拟揭示了CO2在[N1111][Triz]-H2O混合溶剂中的动态吸收过程：CO2分子优先在气液界面积聚，然后逐渐扩散到体相。增加[N1111][Triz]含量通过提供更多的相互作用位点来提高CO2的吸收能力，而水调节界面行为和扩散动力学。本研究深入了解了[N1111][Triz]-H2O混合溶剂对CO2的吸收行为，为开发高效的CO2捕集溶剂提供了理论支持，并突出了其工业应用潜力。

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引用次数: 0

Sustainable hybrid photo/electro-enzyme systems for CO2 conversion 可持续的光/电-酶混合系统用于二氧化碳转化

IF 7.6 Q1 ENGINEERING, CHEMICAL

Green Chemical Engineering

Pub Date : 2025-06-21 DOI: 10.1016/j.gce.2025.06.006

Wanrong Dong , Jinde Cai , Qimei Sun , Likun Luan , Xiuling Ji , Shaojuan Zeng , Yuhong Huang

Carbon dioxide (CO₂), as an abundant and renewable carbon feedstock, holds immense potential for sustainable biomanufacturing. However, natural carbon fixation pathways, such as the Calvin-Benson-Bassham (CBB) cycle and the reverse tricarboxylic acid (rTCA) cycle, suffer from intrinsic limitations, including low catalytic efficiency, high adenosine triphosphate (ATP) consumption, and oxygen sensitivity. Recent advances in synthetic biology and metabolic engineering have pioneered artificial pathways (e.g., the crotonyl-CoA/ethylmalonyl-CoA/hydroxybutyryl-CoA (CETCH) cycle) that bypass central metabolism, achieving higher fixation rates with reduced ATP consumption. Concurrently, photocatalytic and electrocatalytic systems have emerged as complementary strategies to address cofactor dependency and CO₂ activation thermodynamic barriers. This review summarizes breakthroughs in (i) rational design for CO₂ conversion pathway optimization, (ii) photocatalysis, and (iii) electrocatalysis for CO₂ activation and cofactor regeneration. By integrating these disciplines, synergistic systems achieve unprecedented efficiency in converting CO₂ to Cn compounds (e.g., ethanol, glyoxylate, sugar, and starch) and establish a foundation for scalable carbon-negative biotechnologies. However, challenges remain, including enzyme denaturation under operational stresses, inefficiencies in multi-enzyme cascades due to kinetic mismatches, and the need for sustainable metrics to ensure net-negative carbon footprints. Future research should prioritize material innovation, CO₂ assimilation system integration, and optimization to unlock higher efficiency CO₂ conversion, aligning with global decarbonization goals while producing high-value chemicals.

二氧化碳作为一种丰富的可再生碳原料，在可持续生物制造中具有巨大的潜力。然而，自然的碳固定途径，如Calvin-Benson-Bassham （CBB）循环和反三羧酸（rTCA）循环，存在固有的局限性，包括催化效率低、三磷酸腺苷（ATP）消耗高、氧敏感性高。合成生物学和代谢工程的最新进展开创了绕过中枢代谢的人工途径（例如，巴丁酰辅酶a /乙基丙二酰辅酶a /羟丁基辅酶a （CETCH）循环），在减少ATP消耗的同时实现更高的固定率。同时，光催化和电催化系统已经成为解决辅因子依赖和二氧化碳激活热力学障碍的互补策略。本文综述了在CO2转化途径优化的合理设计、CO2活化与辅因子再生的光催化、CO2活化与辅因子再生的电催化等方面的突破。通过整合这些学科，协同系统在将二氧化碳转化为Cn化合物（如乙醇、乙醛酸盐、糖和淀粉）方面实现了前所未有的效率，并为可扩展的负碳生物技术奠定了基础。然而，挑战仍然存在，包括操作压力下的酶变性，由于动力学不匹配导致的多酶级联效率低下，以及需要可持续的指标来确保净负碳足迹。未来的研究应优先考虑材料创新、二氧化碳同化系统集成和优化，以解锁更高效率的二氧化碳转化，与全球脱碳目标保持一致，同时生产高价值化学品。

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引用次数: 0

The investigation of the reaction mechanism of CO2 in HMDA/DEEA and EAE/1DMA2P aqueous solution systems CO2在HMDA/DEEA和EAE/1DMA2P水溶液体系中的反应机理研究

IF 7.6 Q1 ENGINEERING, CHEMICAL

Green Chemical Engineering

Pub Date : 2025-06-16 DOI: 10.1016/j.gce.2025.06.003

Can Lv, Yimin Deng, Dongfang Zhao, Miyi Li, Helei Liu

Revealing the reaction mechanism of CO₂ absorption by mixed amine solutions can provide theoretical guidance for establishing complex kinetic models. This study investigated the CO₂ capture mechanisms of blended amine systems, specifically 1,6-hexamethyl diamine (HMDA)-N,N-diethylethanolamine (DEEA) and 2-(ethylamino)ethanol (EAE)-1-dimethylamino-2-propanol (1DMA2P), utilizing ¹³C nuclear magnetic resonance (NMR) spectroscopy and quantum mechanical calculations. The ¹³C NMR analysis identified the formation and conversion of species during CO₂ absorption, while quantum calculations elucidated the reaction energetics. The results indicate that tertiary amines (DEEA or 1DMA2P) facilitate CO₂ absorption by promoting the desorption of protonated primary amines (HMDA or EAE), thereby enhancing the absorption rate. This research provides insights into the role of tertiary amines in blended systems, guiding the development of efficient and low-energy amine solvents for CO₂ capture.

揭示混合胺溶液吸收CO2的反应机理，可为建立复杂动力学模型提供理论指导。本研究利用13C核磁共振（NMR）和量子力学计算研究了混合胺体系，特别是1,6-六甲二胺(HMDA)- n， n -二乙基乙醇胺（DEEA）和2-（乙胺）乙醇(EAE)-1-二甲氨基-2-丙醇（1DMA2P）的CO2捕获机制。13C核磁共振分析确定了CO2吸收过程中物质的形成和转化，量子计算阐明了反应的能量学。结果表明，叔胺（DEEA或1DMA2P）通过促进质子化伯胺（HMDA或EAE）的解吸来促进CO2的吸收，从而提高吸收率。本研究提供了对叔胺在混合体系中的作用的见解，指导了用于CO2捕获的高效和低能量胺溶剂的开发。

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