Sustainable Chemistry and Pharmacy最新文献_第2页

Water promoted lignin C–C bond cleavage in Bi4O5Br2@BiOBr heterojunction photocatalytic system 水促进Bi4O5Br2@BiOBr异质结光催化体系中木质素C-C键的裂解

IF 5.8 2区化学 Q2 CHEMISTRY, MULTIDISCIPLINARY

Sustainable Chemistry and Pharmacy

Pub Date : 2025-12-26 DOI: 10.1016/j.scp.2025.102305

Jie Xu , Zhuxue Duan , Chang Ge , Ge Zhao

Lignin is abundant in nature. Its high-value utilization is of great significance to promote green and sustainable development. Photocatalytic cleavage of lignin C–C bonds is an effective strategy to promote the value-added conversion of lignin. Unfortunately, due to the robustness of lignin C–C bonds and the complexity of its structure, the activity of photocatalysts for the cleavage of lignin C–C bonds still faces huge challenges. Herein, Bi₄O₅Br₂@BiOBr heterojunction photocatalyst was successfully synthesized by regulating the type of solvent. Moreover, the hydroxyl radical containing an oxygen atom and superoxide radical route were discovered to be effective in breaking lignin C–C bonds. A series of characterizations have demonstrated that the transfer of photogenerated carriers between Bi₄O₅Br₂ and BiOBr follows the Z-Scheme heterojunction pathway. Bi₄O₅Br₂@BiOBr also has excellent photogenerated carrier separation ability and a matching redox potential for lignin C–C bond cleavage. Under optimal conditions, the C–C bond cleavage selectivity in lignin models generally exceeds 90 %. H₂O in solvents plays an important role in photocatalytic reactions. It provides the required O and H atoms for breaking lignin C–C bonds, thus improving the lignin C–C bond cleavage. The photocatalytic mechanism confirmed that the cleavage process of lignin C–C bonds follows the C_β radical mechanism. This work provides a reference for the use of Bi-based photocatalysts to cleave the lignin C–C bonds.

木质素在自然界中是丰富的。其高价值利用对促进绿色可持续发展具有重要意义。光催化裂解木质素C-C键是促进木质素增值转化的有效策略。遗憾的是，由于木质素C-C键的坚固性和结构的复杂性，光催化剂裂解木质素C-C键的活性仍然面临着巨大的挑战。本文通过调节溶剂类型，成功合成了Bi4O5Br2@BiOBr异质结光催化剂。此外，还发现含有氧原子的羟基自由基和超氧自由基途径可以有效地破坏木质素的C-C键。一系列表征表明，光生载流子在Bi4O5Br2和BiOBr之间的转移遵循Z-Scheme异质结途径。Bi4O5Br2@BiOBr还具有优异的光生载流子分离能力和与木质素C-C键裂解相匹配的氧化还原电位。在最佳条件下，木质素模型的C-C键裂解选择性一般超过90%。溶剂中的H2O在光催化反应中起着重要的作用。它提供了破坏木质素C-C键所需的O和H原子，从而改善了木质素C-C键的裂解。光催化机制证实木质素C-C键的裂解过程遵循Cβ自由基机制。本研究为利用铋基光催化剂裂解木质素C-C键提供了参考。

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引用次数: 0

Development of ionic liquid saponification strategy based on synergistic extraction using N1923 and Cyanex272 for Sm/Co separation 基于N1923和Cyanex272协同萃取的离子液体皂化策略在Sm/Co分离中的应用

IF 5.8 2区化学 Q2 CHEMISTRY, MULTIDISCIPLINARY

Sustainable Chemistry and Pharmacy

Pub Date : 2025-12-25 DOI: 10.1016/j.scp.2025.102301

Haixia Zhang , Yun Gao , Hepeng Zhang , Peilin Lei , Tong Li , Sisi Chen , Xiaoqi Sun

Recovering samarium (Sm)/cobalt (Co) from waste samarium-cobalt (SmCo) magnets is of significance for both resource recycling and environmental concerns. In this study, we developed a greener and efficient strategy for Sm³⁺/Co²⁺ separation by employing a synergistic extraction system composed of Cyanex272 and N1923. When Cyanex272 and N1923 were mixed in an equimolar ratio, the synergistic extraction system had excellent extraction and separation performance, achieving a synergistic coefficient of 229.56 and a Sm³⁺/Co²⁺ separation factor of up to 6740.12. The effects of initial pH value, NaCl concentration, equilibrium time and temperature on Sm³⁺/Co²⁺ recovery were systematically investigated. The investigation using slope analysis method, FT-IR spectroscopy and ¹H NMR spectroscopy indicated that the mechanism of Sm³⁺ extraction by [N1923][Cyanex272] was ion association. Compared with conventional saponification with ammonia or NaOH, this article proposes for the first time an ionic liquid saponification strategy based on synergistic extraction between primary amine and acidic extractant. On the one hand, it can avoid a large amount of saponification wastewater. On the other hand, it does not require chemicals or energy consumption in the synthesis process of ionic liquid. [N1923][Cyanex272] demonstrates excellent reusability, phase stability and extraction efficiency over multiple cycles. These advantages fulfill key green chemistry principles and support a simplified, efficient, and greener approach for rare earth separation.

从废钐钴磁体中回收钐(Sm)/钴（Co）对资源回收和环境保护都具有重要意义。在这项研究中，我们开发了一种更绿色高效的Sm3+/Co2+分离策略，采用由Cyanex272和N1923组成的协同萃取体系。当Cyanex272和N1923以等摩尔比混合时，协同萃取体系具有良好的萃取分离性能，协同萃取系数达到229.56，Sm3+/Co2+分离系数高达6740.12。系统研究了初始pH值、NaCl浓度、平衡时间和温度对Sm3+/Co2+回收率的影响。采用斜率分析法、FT-IR光谱和1H NMR光谱研究表明，[N1923][Cyanex272]萃取Sm3+的机理为离子缔合。本文首次提出了一种基于伯胺与酸性萃取剂协同萃取的离子液体皂化策略。一方面可以避免大量皂化废水的产生。另一方面，它在离子液体的合成过程中不需要化学物质或能量消耗。[N1923][Cyanex272]在多个循环中表现出优异的可重用性、相稳定性和萃取效率。这些优势符合关键的绿色化学原理，并支持稀土分离的简化、高效和绿色的方法。

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引用次数: 0

Waste treatment with waste: Preparation of cold-bonded artificial lightweight aggregates by alkali activation synergized with coastal saline soil and multi-source solid wastes 废废处理：碱活化法与滨海盐渍土及多源固体废物协同制备冷粘结人工轻骨料

IF 5.8 2区化学 Q2 CHEMISTRY, MULTIDISCIPLINARY

Sustainable Chemistry and Pharmacy

Pub Date : 2025-12-24 DOI: 10.1016/j.scp.2025.102304

Rubin Han , Hongxiu Leng , Hui Luo , Wenbo Wu , Bukai Song , Yunrui Zhao , Bao-Jie He , Zhong-ling Zong

Soil salinization and the accumulation of industrial solid wastes are prominent environmental problems. To this end, artificial lightweight aggregates based on coastal chloride saline soil (CSS-LWA) was firstly fabricated by cold bonding method in this study, using Lianyungang coastal chloride saline soil (CSS), red mud (RM), and granulated blast furnace slag (GGBS) as the primary raw materials, with lime serving as the alkaline regulator and sodium silicate acting as the activator. To comprehensively examine the impact of process parameters on physical characteristics, microstructure, freeze-thaw resistance, heavy metal safety, and salinization improvement efficiency of CSS-LWA. Meanwhile, carbon emission accounting and cost calculation were carried out. The findings demonstrated that the optimal performance of CSS-LWA was achieved with a mixed composition of 47.5 % CSS, 12.5 % lime, 30 % RM, and 10 % GGBS, followed by steam curing at 70 °C for 24 h. Its cylinder compressive strength reached 8.53 MPa, with 1-h water absorption of 13.96 %, and bulk density of 824.30 kg/m³. Freeze-thaw (F-T) cycle test was carried out in accordance with GB/T 17431.2-2010, the optimal sample (X3-70 °C) was completely damaged after 19 cycles. All of heavy metal leaching concentrations were below the GB 5085.3–2007 limit values. Life Cycle Assessment (LCA) was performed to quantify only carbon emissions within the system boundary encompassing raw material acquisition, transportation, and production phases. The determined carbon emission per unit product of CSS-LWA was 208.8516 kg CO₂/t. This study provides technical references for the development of environmentally friendly construction aggregates in the context of circular economy.

土壤盐碱化和工业固体废物堆积是突出的环境问题。为此，本研究首次以连云港滨海氯盐土（CSS）、赤泥（RM）、粒状高炉渣（GGBS）为主要原料，以石灰为碱性调节剂，水玻璃为活化剂，采用冷粘接法制备了滨海氯盐土（CSS- lwa）人工轻质骨料。综合考察工艺参数对CSS-LWA的物理特性、微观结构、抗冻融性、重金属安全性和盐渍化改善效率的影响。同时进行碳排放核算和成本计算。结果表明：CSS- lwa的最佳性能为：CSS为47.5%，石灰为12.5%，RM为30%，GGBS为10%，70℃蒸汽养护24 h，柱压强度为8.53 MPa， 1 h吸水率为13.96%，容重为824.30 kg/m3。冻融（F-T）循环试验按照GB/T 17431.2-2010进行，最佳试样（X3-70℃）经过19次循环后完全破坏。重金属浸出浓度均低于GB 5085.3-2007限量值。生命周期评估（LCA）仅用于量化包括原材料获取、运输和生产阶段在内的系统边界内的碳排放。测定了CSS-LWA的单位产品碳排放量为208.8516 kg CO2/t。本研究为循环经济背景下环保建筑骨料的发展提供了技术参考。

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引用次数: 0

Circular valorization of engineering muck via low-carbon cementitious compositions: Synergistic hydration and life-cycle sustainability 通过低碳胶凝成分实现工程渣土的循环增值：协同水化和生命周期可持续性

IF 5.8 2区化学 Q2 CHEMISTRY, MULTIDISCIPLINARY

Sustainable Chemistry and Pharmacy

Pub Date : 2025-12-22 DOI: 10.1016/j.scp.2025.102303

Zhendong Yang , Wenbin Gao , Yijin Zhong , Chen Li , Wenting Li , Zhengwu Jiang

Engineering muck (EM), a massive byproduct of underground excavation, poses severe environmental and geotechnical challenges. In this study, a low-carbon and resource-efficient strategy is proposed to transform EM into stabilized earth-based construction materials (SECM) through optimized cementitious compositions. Three binder systems—plain cement, binary (cement-slag/fly ash), and ternary (cement-fly ash-limestone)—were systematically evaluated to clarify their effects on the mechanical, microstructural, and environmental behaviors of SECM by X-ray diffraction analysis, thermogravimetric analysis, scanning electron microscopy and carbon footprint assessment. The results reveal that slag substitution not only enhances long-term strength by 110–150 % but also reduces the carbon footprint by over 25 % compared with plain cement systems. The incorporation of limestone powder significantly improves early-age reactivity via filler and nucleation effects, while maintaining a low environmental impact. Microstructural and thermogravimetric analyses confirm that the synergistic hydration of cementitious phases and the formation of dense C–(A)–S–H gels underpin the strength development. Life-cycle-based evaluation demonstrates that the cement–slag system achieves the most favorable balance between performance and sustainability, reducing energy consumption and CO₂ emissions per unit compressive strength to 0.067 MJ MPa⁻¹ and 0.0074 kg CO₂-eq·MPa⁻¹, respectively. This work offers a novel pathway for the valorization of excavation waste and contributes to the design of next-generation low-carbon earth-based materials for sustainable urban development.

工程渣土是地下开挖的大量副产品，对环境和岩土工程构成了严峻的挑战。本研究提出了一种低碳、资源高效的策略，通过优化胶凝成分，将EM转化为稳定的土基建筑材料（SECM）。通过x射线衍射分析、热重分析、扫描电镜和碳足迹评估，系统地评估了三种粘结剂体系——普通水泥、二元（水泥-矿渣/粉煤灰）和三元（水泥-粉煤灰-石灰石），以阐明它们对SECM的力学、微观结构和环境行为的影响。结果表明，与普通水泥体系相比，矿渣替代不仅可以提高长期强度110% ~ 150%，而且可以减少25%以上的碳足迹。石灰石粉的掺入通过填料和成核效应显著提高了早期反应性，同时保持了较低的环境影响。微观结构和热重分析证实，胶凝相的协同水化和致密的C - (A) - s - h凝胶的形成是强度发展的基础。基于全生命周期的评价表明，水泥-矿渣体系在性能和可持续性之间取得了最有利的平衡，单位抗压强度能耗和CO2排放量分别降低至0.067 MJ MPa−1和0.0074 kg CO2-eq·MPa−1。这项工作为挖掘废物的增值提供了一条新途径，并有助于为可持续城市发展设计下一代低碳土基材料。

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引用次数: 0

Sustainability of Analytical Methods Index (SAMI) as an SDG-based tool for chemical analysis 分析方法可持续性指数（SAMI）作为基于可持续发展目标的化学分析工具

IF 5.8 2区化学 Q2 CHEMISTRY, MULTIDISCIPLINARY

Sustainable Chemistry and Pharmacy

Pub Date : 2025-12-22 DOI: 10.1016/j.scp.2025.102294

Fotouh R. Mansour , Marcello Locatelli , Alaa Bedair

Sustainability in chemical analysis requires holistic evaluation tools that extend beyond environmental impact to encompass economic feasibility, social responsibility, and practical applicability. Current greenness metrics, while valuable, remain largely confined to ecological dimensions and do not explicitly align with the United Nations Sustainable Development Goals (SDGs). To bridge this gap, we introduce the Sustainability of Analytical Methods Index (SAMI), the first SDG-based framework (available at bit.ly/SAMI2026) for assessing analytical methods. SAMI employs a structured scoring system that quantifies positive and negative contributions across all 17 SDGs, supported by a color-coded visualization scheme for intuitive interpretation. Case studies demonstrate SAMI's ability to highlight strengths, limitations, and trade-offs of diverse analytical procedures, from conventional chromatographic methods to innovative low-cost, portable devices. Compared with existing greenness and practicality metrics, SAMI provides a more comprehensive, globally relevant perspective on the sustainability of analytical methods. By explicitly linking analytical practices to the SDGs, SAMI offers researchers, industry, and regulators a powerful tool to guide method selection, optimization, and innovation toward long-term sustainable development.

化学分析的可持续性需要全面的评估工具，超越环境影响，包括经济可行性、社会责任和实用性。目前的绿色指标虽然有价值，但仍主要局限于生态层面，与联合国可持续发展目标（sdg）没有明确的一致。为了弥补这一差距，我们引入了第一个基于可持续发展目标的框架——分析方法可持续性指数（SAMI）。ly/SAMI2026)用于评估分析方法。SAMI采用结构化评分系统，量化所有17个可持续发展目标的积极和消极贡献，并通过颜色编码的可视化方案提供直观解释。案例研究表明，SAMI有能力突出各种分析方法的优势、局限性和权衡，从传统的色谱方法到创新的低成本便携式设备。与现有的绿色和实用性指标相比，SAMI为分析方法的可持续性提供了更全面、全球相关的视角。通过明确地将分析实践与可持续发展目标联系起来，SAMI为研究人员、行业和监管机构提供了一个强大的工具，指导方法选择、优化和创新，以实现长期可持续发展。

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引用次数: 0

Choline chloride-carboxylic acid deep eutectic solvents for lead extraction from electronic waste: A green approach 氯化胆碱-羧酸深度共晶溶剂萃取电子废弃物中的铅：绿色途径

IF 5.8 2区化学 Q2 CHEMISTRY, MULTIDISCIPLINARY

Sustainable Chemistry and Pharmacy

Pub Date : 2025-12-22 DOI: 10.1016/j.scp.2025.102300

Floriatan Santos Costa , Luana Santos Moreira , Mateus Olivera Müller , Mario Henrique Gonzalez , Clarice D.B. Amaral

Waste printed circuit boards (WPCB), essential component of electronic devices, comprise a complex matrix of resins and metal alloys, and often contain toxic elements such as lead (Pb). The growing use and accumulation of WPCB has raised concerns due to their environmental impact. This study evaluated alternative and more sustainable solvents for Pb extraction from electronic waste (e-waste), with quantification by flame atomic absorption spectrometry (FAAS). Conventional acid-based extraction methods were adapted using diluted acids and deep eutectic solvents (DES) composed of choline chloride (ChCl) and carboxylic acids. The solvent composition, sample-to-solvent ratio, extraction time, and temperature were systematically optimized using experimental design. The ChCl-oxalic acid and ChCl-formic acid showed promising recoveries (from 95 % to 106 %) and relative standards deviations below 3.5 % under optimized conditions. Detection limits (<5.50 mg kg⁻¹) were adequate for the elevated Pb levels typically present in WPCBs. Overall, this study demonstrates that DES-based extractants offer a safe, efficient, and sustainable alternative to conventional methods for Pb extraction from electronic waste matrices, combining high analytical performance with reduced environmental and health risks.

废弃印刷电路板（WPCB）是电子设备的重要组成部分，由树脂和金属合金的复杂基体组成，通常含有铅（Pb）等有毒元素。由于对环境的影响，WPCB的使用和积累日益增加，引起了人们的关注。本研究通过火焰原子吸收光谱法（FAAS）对从电子废物中提取铅的替代溶剂和更可持续的溶剂进行了评估。传统的酸基提取方法采用稀释酸和由氯化胆碱（ChCl）和羧酸组成的深共晶溶剂（DES）。采用实验设计对溶剂组成、料液比、萃取时间、萃取温度进行了系统优化。在优化条件下，氯化草酸和氯化甲酸的回收率为95% ~ 106%，相对标准偏差小于3.5%。检测限（<5.50 mg kg - 1）对于wpcb中通常存在的铅水平升高是足够的。总体而言，本研究表明，基于des的萃取剂提供了一种安全、高效和可持续的方法，可替代传统的从电子废物基质中提取铅的方法，同时具有高分析性能，降低了环境和健康风险。

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引用次数: 0

Strength characteristics of South China coastal soft clay solidified by all solid waste geopolymer materials and its durability under dry/wet cycles of loading 华南沿海各类固体废弃物地聚合物固化软粘土强度特性及其干湿循环加载耐久性

IF 5.8 2区化学 Q2 CHEMISTRY, MULTIDISCIPLINARY

Sustainable Chemistry and Pharmacy

Pub Date : 2025-12-22 DOI: 10.1016/j.scp.2025.102298

Deluan Feng, Junsheng Zheng, Yanzhe Gu, Shihua Liang

Using cement and alkali-activated material with chemical activators to solidify coastal soft clay faces challenges of poor solidification effect and high economic cost. All solid waste geopolymer was synthesized with Ground Granulated Blast Furnace Slag (GGBS), calcium carbide residue (CCR) and desulfurized gypsum (DG) to solidify South China coastal soft clay. The optimal proportion of the geopolymer and the strength and durability of the solidified soft clay were investigated through unconfined compressive strength (UCS) tests and dry/wet cycle tests. The microscopic solidification mechanism of the solidified soft clay was interpreted through X-ray diffraction (XRD) test, Fourier transform infrared spectroscopy(FT-IR) test, thermogravimetric analysis (TGA) test and scanning electron microscopy (SEM) test. Moreover, the cost and sustainability analysis of the geopolymer for solidifying coastal soft clay was evaluated. The results show that: The optimal proportion of the geopolymer is GGBS:CCR:DG = 80:5:15; the 28 days UCS of the solidified soft clay reaches 5.79 MPa, which is 24.1 times that of its counterpart solidified by cement with the same content(20 %). The hydration gel and ettringite of the geopolymer can effectively cement the soft clay particles/aggregates, strengthen its microscopic structure, counteract the drying shrinkage during the seawater dry/wet cycle process, and mitigate the erosion and decomposition effects of Cl⁻, Mg²⁺ and SO₄²⁻ on the solidified soft clay, thereby improving its strength and durability. The energy consumption, carbon emissions and economic cost of the all solid waste geopolymer for solidifying coastal soft clay are reduced to 26.0 %, 7.5 % and 56.6 % of those of using cement, respectively.

采用水泥和碱活化材料加化学活化剂固化滨海软粘土，面临固化效果差、经济成本高的挑战。以矿渣（GGBS）、电石渣（CCR）和脱硫石膏（DG）为原料，合成了全固体废物地聚合物，用于固化华南沿海软粘土。通过无侧限抗压强度（UCS）试验和干湿循环试验，研究了地聚合物的最佳配比和固化软粘土的强度和耐久性。通过x射线衍射（XRD）测试、傅里叶变换红外光谱（FT-IR）测试、热重分析（TGA）测试和扫描电镜（SEM）测试，对固化软粘土的微观凝固机理进行了解释。此外，还对海岸软粘土固化用地聚合物的成本和可持续性进行了评价。结果表明：地质聚合物的最佳配比为GGBS:CCR:DG = 80:5:15；软粘土固化后的28天单抗强度达到5.79 MPa，是同等掺量（20%）水泥固化软粘土的24.1倍。地聚合物的水化凝胶和钙矾石能有效胶结软粘土颗粒/集合体，强化其微观结构，抵消海水干湿循环过程中的干燥收缩，减轻Cl−、Mg2+和SO42−对固化软粘土的侵蚀和分解作用，从而提高软粘土的强度和耐久性。全固废地聚合物固化滨海软粘土的能耗、碳排放和经济成本分别降低到水泥的26.0%、7.5%和56.6%。

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引用次数: 0

Multifunctional modification of bio–based polyamide 56 fabric via luteolin for durable colouristic, antioxidant, antibacterial and UV protective properties 木犀草素对生物基聚酰胺56织物的多功能改性，具有持久的显色、抗氧化、抗菌和防紫外线性能

IF 5.8 2区化学 Q2 CHEMISTRY, MULTIDISCIPLINARY

Sustainable Chemistry and Pharmacy

Pub Date : 2025-12-19 DOI: 10.1016/j.scp.2025.102295

Xue Zhang , Miaoyan Li , Xin Zhang , Xueni Hou , Xiangrong Wang

Natural extracts, characterized by their superior biocompatibility and multifunctionality, have demonstrated remarkable potential in fields such as antibacterial, antioxidant and ultraviolet (UV) protection. However, at present, natural extracts are facing a key bottleneck in functional finishing—poor washing durability. In this study, luteolin, a natural extract, was chosen to treat bio-based Polyamide 56 (PA56) fabrics. The findings indicated that the fabric dyed with luteolin not only achieved good coloration but also exhibited outstanding multi-functional properties: the ultraviolet protection factor (UPF) value reached 205, the ABTS radical cation (ABTS^•+) scavenging rate was 99 %, and the antibacterial rates against Escherichia coli (E. coli) and Staphylococcus aureus (S. aureus) were 70 % and 95 %, respectively. To further enhance the color fastness and functional durability, this study introduced metal ions. Through the coordination reaction between luteolin, metal ions and PA56, the color fastness was successfully raised to level 4 or above, and the durability of functionalities was significantly improved. After 10 washing cycles, the UPF value of the fabric remained at 155, the ABTS^•+ scavenging rate exceeded 60 %, and the antibacterial rate against S. aureus remained at 75 %. This study proposed and verified a sustainable and coordinated strategy based on coordination chemistry, systematically addressing the durability issue of natural functional finishing agents.

天然提取物具有良好的生物相容性和多功能性，在抗菌、抗氧化和防紫外线等领域显示出巨大的潜力。然而，目前天然提取物在功能性整理方面面临着一个关键的瓶颈——洗涤耐久性差。在这项研究中，选择天然提取物木犀草素处理生物基聚酰胺56 （PA56）织物。结果表明，木草素染色织物不仅着色效果好，而且具有良好的多功能性：紫外线防护因子（UPF）值达205，ABTS自由基阳离子（ABTS•+）清除率达99%，对大肠杆菌（E. coli）和金黄色葡萄球菌（S. aureus）的抑菌率分别为70%和95%。为了进一步提高色牢度和功能耐久性，本研究引入了金属离子。通过木犀草素与金属离子与PA56的配位反应，成功地将色牢度提高到4级以上，并显著提高了功能的耐久性。洗涤10次后，织物的UPF值保持在155，ABTS•+清除率超过60%，对金黄色葡萄球菌的抗菌率保持在75%。本研究提出并验证了一种基于配位化学的可持续协调策略，系统地解决了天然功能性整理剂的耐久性问题。

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引用次数: 0

Design of alkali-activated MSWI fly ash-based cementitious materials under carbonation curing: Mechanical properties, heavy metal solidification, and mechanisms 碳酸化固化下碱活化MSWI粉煤灰基胶凝材料的设计：力学性能、重金属固化及机理

IF 5.8 2区化学 Q2 CHEMISTRY, MULTIDISCIPLINARY

Sustainable Chemistry and Pharmacy

Pub Date : 2025-12-19 DOI: 10.1016/j.scp.2025.102299

An Sai , Wang Baomin , Chen Wenxiu , Fan Chengcheng

Municipal solid waste incineration fly ash contains a large number of harmful heavy metals (HMs), which need to be properly handled. This study innovatively proposes a method for efficiently solidifying HMs through the synergistic effect of high-pressure and high-concentration carbonation curing technology and alkali-activated materials (AAMs). A new type of eco-friendly alkali-activated material was prepared via orthogonal experiments. The microstructure and chemical composition changes of AAMs under carbonation were analyzed in depth, and the mechanism by which carbonation affects the solidification/stabilization (S/S) of HMs was revealed. Results showed that although carbonation reduced the compressive strength of AAMs (with a maximum reduction rate of 52.6 %), it significantly improved the S/S effect of HMs, and the solidified body showed good stability in terms of strength at 180d of curing. The maximum reduction rates of leaching concentrations of Cd, Cu, Pb, and Zn were 48.1 %, 56.5 %, 61.6 %, and 51.9 %, respectively. Microscopic analysis showed that carbonation curing promoted the formation of C₄AH₁₃, xonotlite, and Friedel's salt. These hydration products enhance the S/S of HMs mainly through ion exchange, surface complexation, adsorption, and precipitation. Compared with traditional cement S/S methods and non-carbonated alkali-activated systems, this method achieves a 15 %–20 % higher heavy metal (Cd, Cu, Pb, Zn) immobilization rate. These results indicate the potential application of carbonation curing technology in the field of AAMs. This study not only advances research on the synergy between carbonation curing and AAMs, but also contributes to the coordinated development of hazardous solid waste treatment and environmental protection.

城市生活垃圾焚烧飞灰中含有大量有害重金属，需要妥善处理。本研究创新性地提出了一种利用高压高浓度碳化固化技术与碱活化材料（AAMs）协同作用高效固化HMs的方法。通过正交实验制备了一种新型环保型碱活性材料。深入分析了碳化作用下aam的显微组织和化学成分变化，揭示了碳化作用影响aam凝固/稳定化（S/S）的机理。结果表明，碳化虽然降低了AAMs的抗压强度（最大降低率为52.6%），但显著提高了HMs的S/S效应，固化体在固化180d时表现出良好的强度稳定性。Cd、Cu、Pb和Zn的浸出浓度最大还原率分别为48.1%、56.5%、61.6%和51.9%。显微分析表明，碳化固化促进了C4AH13、硅钙石和弗里德尔盐的形成。这些水化产物主要通过离子交换、表面络合、吸附和沉淀来提高HMs的S/S。与传统水泥S/S法和非碳酸碱活化体系相比，该方法的重金属（Cd、Cu、Pb、Zn）固定化率提高了15% - 20%。这些结果表明了碳化固化技术在aam领域的潜在应用前景。本研究不仅推进了碳酸化固化与AAMs协同作用的研究，也有助于危险固体废物处理与环境保护的协调发展。

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引用次数: 0

Efficient synthesis of 1,6-hexanediamine via aqueous-phase reductive amination over bifunctional Ru–Co/α-Al2O3 catalyst 双功能Ru-Co /α-Al2O3催化剂上水相还原胺化高效合成1,6-己二胺

IF 5.8 2区化学 Q2 CHEMISTRY, MULTIDISCIPLINARY

Sustainable Chemistry and Pharmacy

Pub Date : 2025-12-19 DOI: 10.1016/j.scp.2025.102297

Bao Guo , Xinxiao Wu , Fang Li , Wenjing Tang , Wei Xue , Jianhua Lv

This study presents a sustainable synthesis strategy based on renewable resources, utilizing biomass-derived 1,6-hexanediol (HDO) and aqueous ammonia as feedstocks for the efficient aqueous-phase reductive amination to produce 1,6-hexanediamine (HMDA). Under mild reaction conditions (175 °C, 5.5 h), the Ru–Co/α-Al₂O₃ catalyst, through its electron-rich microenvironment and the electronic synergistic effects of the Ru–Co bimetallic system, effectively promotes both the dehydrogenation of HDO and selective amination. Systematic characterizations reveal that the introduction of Co significantly alters the particle size and electronic structure of Ru, promotes the formation of Ru–Co alloys, and enhances the hydrogen spillover effect. Notably, the Ru^δ+ species facilitate the formation of the intermediate 6-amino-1-hexanol (AHO) with a maximum selectivity of 57.3 %. The electron-rich Ru interface further improves the adsorption and activation of AHO, achieving a maximum HMDA selectivity of 25.2 %. CO-DRIFTS analysis confirms that the electron density of the Ru sites is significantly increased, optimizing the catalytic interface and enhancing the adsorption and activation of intermediates. Density functional theory (DFT) calculations show that the Ru–Co alloy interface increases the electron density at Ru sites, effectively lowering the activation energy for key steps, such as the initial dehydrogenation of HDO, thereby accelerating the transformation of intermediates and promoting the efficient formation of HMDA. This strategy offers an innovative green synthetic pathway for the valorization of biomass-derived oxygenated compounds.

本研究提出了一种基于可再生资源的可持续合成策略，利用生物质衍生的1,6-己二醇（HDO）和水氨作为原料，进行高效的水相还原胺化反应，生产1,6-己二胺（HMDA）。在温和反应条件下（175℃，5.5 h）， Ru-Co /α-Al2O3催化剂通过其富电子微环境和Ru-Co双金属体系的电子协同效应，有效促进HDO脱氢和选择性胺化反应。系统表征表明，Co的引入显著改变了Ru的粒径和电子结构，促进了Ru - Co合金的形成，并增强了氢溢出效应。值得注意的是，Ruδ+物种促进中间产物6-氨基-1-己醇（ho）的形成，最大选择性为57.3%。富电子Ru界面进一步提高了ho的吸附和活化能力，HMDA的最大选择性达到25.2%。CO-DRIFTS分析证实，Ru位点的电子密度显著增加，优化了催化界面，增强了中间体的吸附和活化。密度泛函理论（DFT）计算表明，Ru - co合金界面增加了Ru位点的电子密度，有效降低了HDO初始脱氢等关键步骤的活化能，从而加速了中间体的转化，促进了HMDA的有效形成。这种策略为生物质衍生的含氧化合物的增值提供了一种创新的绿色合成途径。

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