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IF 7.5 3区 环境科学与生态学 Q2 ENERGY & FUELS Pub Date : 2025-10-29 DOI: 10.1016/S2588-9133(25)00085-7
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引用次数: 0
Design and synthesis of novel ionic liquids with unique structures and excellent catalytic activity for transesterification 具有独特结构和优异催化活性的新型离子液体的设计与合成
IF 7.5 3区 环境科学与生态学 Q2 ENERGY & FUELS Pub Date : 2025-09-01 DOI: 10.1016/j.crcon.2024.100264
Dan Wang , Zhentao Zhao , Yuxin Wang , Zhanguo Zhang , Jinggang Zhao , Peng Zheng , Guangwen Xu , Lei Shi
A series of novel ionic liquids (ILs) with near-neutrality, moderate nucleophilicity, and zwitterionic structure were synthesized using a one-step method. Notably, these ILs could be successfully synthesized by activating 1-methylimidazole with carbonate, carboxylic, and oxalate esters. The structures and properties of the synthesized ILs were qualitatively and quantitatively analyzed using Fourier-transform infrared spectroscopy, 1H/13C, nuclear magnetic resonance spectroscopy, thermogravimetry–mass spectrometry, and Hammett indicator. A mechanism was proposed for activating 1-methylimidazole, and the negative charge densities of the ILs were calculated. Considering MI-EC as an example, the best conditions for the synthesis of ILs were optimized reaction at 85 °C for 18 h, and the synthesis pathway was determined through density functional theory calculations. Herein, MI-EC exhibited excellent catalytic activity for transesterification reactions, and the corresponding ethylene carbonate (EC) conversion, dimethyl carbonate (DMC) yield, and turnover frequency (TOF) reached 50.4 %, 30.5 %, and 127.8 h−1, respectively, with a catalytic reaction of only 30 min. Furthermore, the mechanism underlying the transesterification reaction catalyzed by MI-EC was investigated. The catalytic activity and structure of MI-EC remained unchanged after six reuses, demonstrating its better stability. In addition, MI-EC displayed a wide range of substrate universality, such as carbonates, oxalates, and acetic esters. Thus, this study not only provides a theoretical and practical support foundation for designing and synthesizing ILs, but also provides a new perspective for preparing alkaline catalysts.
采用一步法合成了一系列具有近中性、中等亲核性和两性离子结构的新型离子液体。值得注意的是,这些il可以通过碳酸酯、羧酸酯和草酸酯活化1-甲基咪唑成功合成。采用傅里叶变换红外光谱、1H/13C、核磁共振光谱、热重质谱和Hammett指示剂对合成的ILs的结构和性质进行定性和定量分析。提出了1-甲基咪唑的活化机理,并计算了其负电荷密度。以MI-EC为例,优化了合成il的最佳条件,在85℃下反应18 h,通过密度泛函理论计算确定了合成途径。其中,MI-EC在酯交换反应中表现出优异的催化活性,相应的碳酸乙酯(EC)转化率、碳酸二甲酯(DMC)产率和周转频率(TOF)分别达到50.4%、30.5%和127.8 h−1,催化反应时间仅为30 min。进一步探讨了MI-EC催化酯交换反应的机理。6次重复使用后,MI-EC的催化活性和结构保持不变,表明其具有较好的稳定性。此外,MI-EC显示出广泛的底物普遍性,如碳酸盐,草酸盐和乙酸酯。因此,本研究不仅为设计和合成il提供了理论和实践支持基础,而且为制备碱性催化剂提供了新的视角。
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引用次数: 0
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IF 7.5 3区 环境科学与生态学 Q2 ENERGY & FUELS Pub Date : 2025-09-01 DOI: 10.1016/S2588-9133(25)00066-3
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引用次数: 0
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IF 6.4 3区 环境科学与生态学 Q2 ENERGY & FUELS Pub Date : 2025-06-01 DOI: 10.1016/S2588-9133(25)00051-1
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引用次数: 0
Fluidized bed two-stage O2/steam gasification of agricultural biomass for low-tar syngas: An industrial-scale verification test 流化床两级O2/蒸汽气化农业生物质低焦油合成气:工业规模验证试验
IF 6.4 3区 环境科学与生态学 Q2 ENERGY & FUELS Pub Date : 2025-06-01 DOI: 10.1016/j.crcon.2025.100342
Chao Wang , Gang Song , Mengjuan Zhang , Kaixuan Yang , Zhenglin Wang , Xin Jia , Qingya Liu , Liguo Zhou , Zhennan Han , Shurong Wang , Jianguo Bian , Guangwen Xu
In the complete green synthesis technology chain, bio-syngas production remains the “first hurdle”. Especially, the “tar” problem in biomass gasification urgently needs to be solved. Recently, our team, in collaboration with Jinan Huangtai Gas Stove Co., Ltd., completed a 10,000-ton industrial test and technical verification of fluidized bed two-stage O2/steam gasification for production of syngas from biomass. The test results showed that the fluidized bed two-stage gasification was operated continuously and stably for over 110 h with various biomass feedstocks. Additionally, the lowest tar content in the produced gas reached 0.58 g/Nm3. The fly ash collected from the continuous test contained carbon of about 30 wt%. Thus, the technology was well proved for large-scale biomass gasification and production of syngas in terms of technical feasibility and operational stability.
在完整的绿色合成技术链中,生物合成气生产仍然是“第一关”。特别是生物质气化中的“焦油”问题亟待解决。最近,我们的团队与济南皇泰燃气炉有限公司合作,完成了流化床两级O2/蒸汽气化生产生物质合成气的万吨级工业试验和技术验证。试验结果表明,流化床两段气化在不同生物质原料下连续稳定运行110 h以上。采出气中最低焦油含量达到0.58 g/Nm3。从连续试验中收集的飞灰含碳量约为30%。因此,该技术在技术可行性和运行稳定性方面已经很好地证明了大规模生物质气化和合成气生产的技术可行性。
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引用次数: 0
Self-pillared hierarchical Silicalite-1 zeolites for enhanced Suzuki-Miyaura coupling reactions 增强Suzuki-Miyaura偶联反应的自柱状分层硅石-1沸石
IF 7.5 3区 环境科学与生态学 Q2 ENERGY & FUELS Pub Date : 2025-04-15 DOI: 10.1016/j.crcon.2025.100331
Xicheng Jia , Jianxin Liu , Yuming Zhang , Dahong Jiang
The Suzuki coupling reaction is a widely employed technique for the synthesis of biaryl compounds in various disciplines. This study introduces the development of a highly efficient and recyclable palladium-doped Silicalite-1 (S-1) catalyst featuring a hierarchical structure, which enhances the efficacy of Suzuki coupling reactions. By utilizing tetra-n-butylphosphonium hydroxide as a structure-directing agent and adjusting the molar ratios of ethanol and water in the synthetic precursor, we successfully produced a range of porous S-1 catalysts. These catalysts displayed a unique architecture characterized by interconnected thin pillars or lamellae. The catalyst’s remarkable specific activity facilitated rapid Suzuki coupling reactions, completing within just three hours under environmentally benign conditions. The Suzuki reaction mechanism was discussed, which involves an oxidative addition of bromobenzene to heterogeneous Pd, followed by metal exchange with phenyl boronic acid and completed by a reductive elimination. Comprehensive substrate screening, selectivity assessments, and recycling studies were also undertaken.
铃木偶联反应是合成联芳基化合物的一种广泛应用的技术。本研究介绍了一种高效、可回收的掺杂钯硅-1 (S-1)催化剂的开发,该催化剂具有层次化结构,提高了铃木偶联反应的效率。利用四正丁基氢氧化磷作为结构导向剂,调节前驱体中乙醇和水的摩尔比,成功制备了一系列多孔S-1催化剂。这些催化剂表现出独特的结构特征,即相互连接的薄柱或薄片。催化剂显著的比活性促进了快速的铃木偶联反应,在无害环境的条件下,仅需3小时即可完成。讨论了溴苯氧化加成非均相钯,与苯硼酸进行金属交换,并通过还原消除完成的铃木反应机理。还进行了全面的底物筛选、选择性评估和回收研究。
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引用次数: 0
Enhanced performance of gasification by blending coal into biomass in a fluidized bed two-stage system 在流化床两级系统中混合煤与生物质提高气化性能
IF 7.5 3区 环境科学与生态学 Q2 ENERGY & FUELS Pub Date : 2025-04-15 DOI: 10.1016/j.crcon.2025.100333
Chao Wang , Hanyang Li , Mengjuan Zhang , Zhenglin Wang , Zhennan Han , Xin Jia , Gang Song , Kaixuan Yang , Guoqing Guan , Guangwen Xu
Biomass, blended with a small amount of coal, was fed into a fluidized bed two-stage gasifier to produce low-tar H2-rich gas through O2-rich gasification. The blended coal improved the energy density of biomass fuel and also worked as the bed material. For the fluidized bed two-stage gasification, large char particles of biomass and coal tend to accumulate at the bottom of the gasifier (a riser) to form a carbon-rich reaction zone there. Then, the O2 coming from the bottom of the gasifier mainly reacts with such char, consequently suppressing its interaction with the gases including H2 from pyrolyzer. Using O2-rich air with an ER of 0.35 and at gasification temperatures of about 890 °C, gasifying biomass blending 10 wt% coal produced gas containing 13.3 vol% CO, 20.1 vol% CO2, 4.3 vol% CH4, and 9.8 vol% H2, giving an LHV of 4.9 MJ/Nm3d. Tar content in the produced gas gradually decreased with time, and over the last 6 h the measured content was 0.012 g/Nm3d. Steady operation was well achieved, showing the performance without ash agglomeration for the O2-rich gasification of biomass.
将生物质与少量煤混合,送入流化床两段气化炉,通过富o2气化生产低焦油富h2气。混合煤提高了生物质燃料的能量密度,也可作为床料。对于流化床两段气化,生物质和煤的大炭颗粒倾向于积聚在气化炉底部(提升管),在那里形成富碳反应区。然后,来自气化炉底部的O2主要与这种焦炭反应,从而抑制其与热解器产生的H2等气体的相互作用。使用ER为0.35的富o2空气,在890°C的气化温度下,气化生物质混合10 wt%煤产生的含有13.3 vol% CO, 20.1 vol% CO2, 4.3 vol% CH4和9.8 vol% H2的气体,LHV为4.9 MJ/Nm3d。采出气中焦油含量随时间逐渐降低,最后6 h测得含量为0.012 g/Nm3d。稳定运行效果良好,显示了富氧生物质气化无灰结块的性能。
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引用次数: 0
Adsorption of heavy metals from water using teak-based carbon material through graft copolymerization 柚木基碳材料接枝共聚对水中重金属的吸附研究
IF 7.5 3区 环境科学与生态学 Q2 ENERGY & FUELS Pub Date : 2025-04-10 DOI: 10.1016/j.crcon.2025.100332
Jin-Wei Zhang , Nguyen Duy Hai , Muhammad Al Kholif , Huan-Ping Chao
This study presents the development of carbonaceous adsorbents derived from teak wood waste for the removal of heavy metals, such as lead (Pb2+), copper (Cu2+), and cadmium (Cd2+) from aqueous solutions. The adsorbents − hydrochar (TH), biochar (TB), and activated carbon (TAC) − were synthesized through thermal and chemical activation processes and further enhanced by graft copolymerization using acrylic acid. Comprehensive characterizations, including SEM, EDS, XPS, BET, and FTIR, revealed that grafting significantly increased surface functional groups (COOH and OH), thereby improving adsorption capacities. Adsorption isotherms followed the Langmuir model, indicating a chemisorption mechanism dominated by ion exchange and complexation. Post-grafting, maximum adsorption capacities for Pb2+ increased from 116 mg/g (TH) to 294 mg/g (THG), Cu2+ from 84 mg/g (TH) to 164 mg/g (THG), and Cd2+ from 106 mg/g (TH) to 170 mg/g (THG). The study concludes that grafted teak-based materials hold high potential as cost-effective and efficient adsorbents for water purification applications, contributing to sustainable waste management and environmental protection.
本研究介绍了从柚木废料中提取的碳质吸附剂的开发,用于去除水溶液中的重金属,如铅(Pb2+),铜(Cu2+)和镉(Cd2+)。通过热活化法和化学活化法合成了氢炭(TH)、生物炭(TB)和活性炭(TAC),并通过丙烯酸接枝共聚进一步增强了吸附剂的性能。SEM、EDS、XPS、BET和FTIR等综合表征表明,接枝能显著增加表面官能团(COOH和OH),从而提高吸附能力。吸附等温线符合Langmuir模型,表明化学吸附机制以离子交换和络合为主。接枝后,Pb2+的最大吸附量从116 mg/g (THG)增加到294 mg/g (THG), Cu2+从84 mg/g (THG)增加到164 mg/g (THG), Cd2+从106 mg/g (TH)增加到170 mg/g (THG)。该研究得出结论,接枝柚木基材料在水净化应用中具有很高的成本效益和高效吸附剂的潜力,有助于可持续的废物管理和环境保护。
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引用次数: 0
Bio-based papers from seaweed and coconut fiber: sustainable materials for a greener future 海藻和椰子纤维制成的生物基纸:绿色未来的可持续材料
IF 7.5 3区 环境科学与生态学 Q2 ENERGY & FUELS Pub Date : 2025-04-03 DOI: 10.1016/j.crcon.2025.100329
Nida Khan , K. Sudhakar , R. Mamat
The paper industry’s reliance on deforestation for wood pulp has raised environmental concerns and led to fluctuating prices. This study explores the potential of seaweed (Sargassum wightii) and coconut waste, abundant in Malaysia, as sustainable alternatives for biopaper production. These materials offer a promising solution to mitigate deforestation, address waste issues, and promote sustainable manufacturing. Three biopaper samples were fabricated using 100 % seaweed, 100 % coconut fiber, and a 50/50 blend of seaweed and coconut fiber. The blending of seaweed and coconut fiber allows for customising biopaper properties, such as density and flexibility, making it suitable for a broader range of applications. To characterise these biopapers, scanning electron microscopy (SEM), thermogravimetric analysis (TGA), Fourier-transform infrared spectroscopy (FTIR), and X-ray diffraction (XRD) were employed. Additionally, the grammage (GSM) of each biopaper was determined to compare it with traditional wood pulp-based paper to explore its potential applications. FTIR analysis revealed a wide peak between 3343.47 cm−1 and 3355.75 cm−1 in all samples, confirming the existence of O–H bonds often observed in alcohols. TGA examination at 900 °C demonstrated considerable char production, with the seaweed-based bio paper yielding the most char (26.6 %), followed by the coconut-based paper (15.17 %) and the seaweed-coconut mix (13.49 %). The XRD examination indicates that the structure is largely amorphous, with broad peaks in the 2θ range of 11° to 23°. Water absorption test showed that all biopaper samples were hydrophilic; absorption rates for seaweed-based biopaper were 128 g/m2, coconut-based biopaper was 580 g/m2, and the mix of seaweed and coconut was 446 g/m2. High biodegradability was demonstrated by soil burial tests, which indicated weight reductions of 23 %, 57 %, and 64 % for the blended biopaper, seaweed, and coconut after 14 days, respectively. These results highlight Sargassum wightii’s potential as a sustainable biopaper material. When mixed with coconut fiber waste, it can increase density and broaden its possible applications, providing a viable alternative to wood-based papers while also encouraging environmental sustainability.
造纸业依赖砍伐森林生产木浆,这引起了人们对环境的担忧,并导致价格波动。本研究探索了马来西亚丰富的海藻(马尾藻)和椰子废料作为生物纸生产的可持续替代品的潜力。这些材料为减轻森林砍伐、解决废物问题和促进可持续制造业提供了一个有希望的解决方案。用100%海藻、100%椰子纤维和50/50海藻和椰子纤维混合制备了三种生物纸样品。海藻和椰子纤维的混合可以定制生物纸的特性,如密度和灵活性,使其适用于更广泛的应用。利用扫描电子显微镜(SEM)、热重分析(TGA)、傅里叶变换红外光谱(FTIR)和x射线衍射(XRD)对这些生物膜进行了表征。此外,确定了每种生物纸的克重(GSM),并将其与传统木浆基纸进行比较,以探索其潜在的应用前景。FTIR分析显示,在所有样品中,3343.47 cm−1和3355.75 cm−1之间有一个宽峰,证实了醇中常见的O-H键的存在。900°C时的TGA测试显示出相当大的碳产量,其中以海藻为基础的生物纸的碳产量最高(26.6%),其次是椰子纸(15.17%)和海藻-椰子混合物(13.49%)。XRD分析表明,该材料在11°~ 23°的2θ范围内具有较宽的峰,结构基本呈非晶态。吸水试验表明,所有生物纸样品均具有亲水性;海藻基生物纸的吸收率为128 g/m2,椰子基生物纸的吸收率为580 g/m2,海藻和椰子的混合吸收率为446 g/m2。土壤掩埋试验表明,高生物降解性表明,混合生物纸、海藻和椰子在14天后分别减轻了23%、57%和64%的重量。这些结果突出了马尾藻作为可持续生物纸材料的潜力。当与椰子纤维废物混合时,它可以增加密度并扩大其可能的应用范围,为木基纸提供可行的替代品,同时也鼓励环境的可持续性。
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引用次数: 0
Progressive adaptation of microalgae consortium to elevated carbon dioxide coupled with enhanced production of essential fatty acids 微藻联合体对高浓度二氧化碳的逐步适应以及必需脂肪酸的增强生产
IF 7.5 3区 环境科学与生态学 Q2 ENERGY & FUELS Pub Date : 2025-04-02 DOI: 10.1016/j.crcon.2025.100330
Alston Bernard D’Souza , Atiqur Rahaman , Khandaker Asif Ahmed , Elena Adaschewski , Dieter Hanelt , Abdelfatah Abomohra
This study investigated the possible adaptation of a microalgae consortium to elevated carbon dioxide (CO2) concentrations reaching up to 50 % v/v in a lab-scale photobioreactor (PBR). Results showed a significant reduction in the growth rate of the consortium with increasing CO2 supplementation, from 1.327 d-1 in the initial culture without CO2 supplementation to 0.369 d-1 at 50 % CO2. At the lowest applied CO2 supplementation of 10%, the growth rate was 0.735 d-1. Interestingly, supplementation of 40% CO2 in the final run showed insignificant difference in the growth rate of the consortium compared to that at 10% CO2. Microbial community analysis revealed a shift towards bacterial genera that enhance the microalgal growth, while some algal genera (mainly Tetradesmus and Chlorella) became more dominant under CO2 enrichment. Compared to the initial consortium, the proportion of polyunsaturated fatty acids (PUFAs) increased from 36.2% to 58.1% under 40% CO2, mainly due to the increase in the proportion of essential fatty acids (EFAs) such as alpha-linolenic acid (ALA) and linoleic acid (LA). Under 40% CO2 supplementation, an increase in cell size was observed, despite a reduction in cell number. This study highlights the potential of microalgae consortia to adapt to high CO2 levels, leading to a dominance of certain algal genera. This adaptation improves the production of EFAs, thereby contributing to both environmental sustainability and industrial applications.
本研究探讨了微藻联合体在实验室规模光生物反应器(PBR)中对二氧化碳(CO2)浓度升高达到50% v/v的可能适应性。结果表明,随着CO2添加量的增加,该联合体的生长速率显著降低,从初始培养时不添加CO2的1.327 d-1降至50% CO2时的0.369 d-1。最低CO2添加量为10%时,生长速率为0.735 d-1。有趣的是,在最后一次运行中补充40%的二氧化碳与10%的二氧化碳相比,联合体的生长速度没有显著差异。微生物群落分析显示,在CO2富集条件下,微藻的生长向有利于微藻生长的细菌属转移,而一些藻类属(主要是四角藻和小球藻)则变得更占优势。与初始财团相比,在40% CO2下,多不饱和脂肪酸(PUFAs)的比例从36.2%增加到58.1%,主要是由于必需脂肪酸(EFAs)如α -亚麻酸(ALA)和亚油酸(LA)的比例增加。在补充40%二氧化碳的情况下,观察到细胞大小增加,尽管细胞数量减少。这项研究强调了微藻联合体适应高二氧化碳水平的潜力,导致某些藻类属的优势。这种适应改进了EFAs的生产,从而促进了环境可持续性和工业应用。
{"title":"Progressive adaptation of microalgae consortium to elevated carbon dioxide coupled with enhanced production of essential fatty acids","authors":"Alston Bernard D’Souza ,&nbsp;Atiqur Rahaman ,&nbsp;Khandaker Asif Ahmed ,&nbsp;Elena Adaschewski ,&nbsp;Dieter Hanelt ,&nbsp;Abdelfatah Abomohra","doi":"10.1016/j.crcon.2025.100330","DOIUrl":"10.1016/j.crcon.2025.100330","url":null,"abstract":"<div><div>This study investigated the possible adaptation of a microalgae consortium to elevated carbon dioxide (CO<sub>2</sub>) concentrations reaching up to 50 % <em>v/v</em> in a lab-scale photobioreactor (PBR). Results showed a significant reduction in the growth rate of the consortium with increasing CO<sub>2</sub> supplementation, from 1.327 d<sup>-1</sup> in the initial culture without CO<sub>2</sub> supplementation to 0.369 d<sup>-1</sup> at 50 % CO<sub>2</sub>. At the lowest applied CO<sub>2</sub> supplementation of 10%, the growth rate was 0.735 d<sup>-1</sup>. Interestingly, supplementation of 40% CO<sub>2</sub> in the final run showed insignificant difference in the growth rate of the consortium compared to that at 10% CO<sub>2</sub>. Microbial community analysis revealed a shift towards bacterial genera that enhance the microalgal growth, while some algal genera (mainly <em>Tetradesmus</em> and <em>Chlorella</em>) became more dominant under CO<sub>2</sub> enrichment. Compared to the initial consortium, the proportion of polyunsaturated fatty acids (PUFAs) increased from 36.2% to 58.1% under 40% CO<sub>2</sub>, mainly due to the increase in the proportion of essential fatty acids (EFAs) such as alpha-linolenic acid (ALA) and linoleic acid (LA). Under 40% CO<sub>2</sub> supplementation, an increase in cell size was observed, despite a reduction in cell number. This study highlights the potential of microalgae consortia to adapt to high CO<sub>2</sub> levels, leading to a dominance of certain algal genera. This adaptation improves the production of EFAs, thereby contributing to both environmental sustainability and industrial applications.</div></div>","PeriodicalId":52958,"journal":{"name":"Carbon Resources Conversion","volume":"8 4","pages":"Article 100330"},"PeriodicalIF":7.5,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145160394","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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Carbon Resources Conversion
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