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Ligninsulfonate-Derived Porous Sulfonated Carbon Using Templating Method for the Alkylation of Hemicellulose-Derived Furfurals to Biodiesel Precursors 使用模板法将木质素磺酸盐衍生的多孔磺化碳烷基化为生物柴油前体的半纤维素衍生糠醛
Pub Date : 2024-07-14 DOI: 10.1021/acssusresmgt.4c0020410.1021/acssusresmgt.4c00204
Shijie Fang, Yanchang Chu, Zhiting Gong, Rui Ma* and Le Yang*, 

This work provides a method to transform sodium lignosulfonate into sulfonated carbon materials through chemical activation using magnesium salt as a template instead of using conventional sulfonation agents, such as concentrated sulfuric acid or chlorosulfonic acid. Several magnesium salts, including magnesium nitrate, magnesium chloride, magnesium acetate, and magnesium citrate, are employed as activating templates for comparison, and magnesium nitrate turns out with the most abundant sulfonic acid group density of 1.35 mmol/g and highest specific surface area of 512 m2/g. Especially, the effect of magnesium salts during carbonization process on the structure evolution is explored using tandem thermogravimetric-mass spectrometry and reveals that magnesium nitrate prevents sulfur loss in the form of SO2, SO3, or H2S during carbonization, thus exhibiting the most abundant sulfonic acid group. These sulfonated carbon materials are tested in the alkylation reaction of furfural and 2-methylfuran to produce a C15 precursor of biodiesel, where the conversion of furfural and selectivity for 5,5-(furan-2-ylmethylene)bis(2-methylfuran) reach 90.2% and 87.2% at 70 °C for 6 h, respectively. This investigation underscores the efficient utilization of sulfonic acid functional groups inherent in sodium lignosulfonate to produce sulfonated carbon materials without the introduction of an exterior sulfur source and opens avenues for a broader application of lignosulfonates.

本研究提供了一种以镁盐为模板,而不是使用浓硫酸或氯磺酸等传统磺化剂,通过化学活化将木质素磺酸钠转化为磺化碳材料的方法。比较了硝酸镁、氯化镁、醋酸镁和柠檬酸镁等几种镁盐作为活化模板,结果发现硝酸镁的磺酸基密度最高,为 1.35 mmol/g,比表面积最大,为 512 m2/g。特别是利用串联热重-质谱法探讨了镁盐在碳化过程中对结构演变的影响,结果表明硝酸镁可防止硫以 SO2、SO3 或 H2S 的形式在碳化过程中流失,从而表现出最丰富的磺酸基团。这些磺化碳材料在糠醛和 2-甲基呋喃的烷基化反应中进行了测试,以生成生物柴油的 C15 前体,在 70 °C 下反应 6 小时,糠醛的转化率和 5,5-(呋喃-2-基亚基)双(2-甲基呋喃)的选择性分别达到 90.2% 和 87.2%。这项研究强调了木质素磺酸钠中固有的磺酸官能团在不引入外部硫源的情况下生产磺化碳材料的高效利用,并为木质素磺酸盐的更广泛应用开辟了途径。
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引用次数: 0
Ligninsulfonate-Derived Porous Sulfonated Carbon Using Templating Method for the Alkylation of Hemicellulose-Derived Furfurals to Biodiesel Precursors 使用模板法将木质素磺酸盐衍生的多孔磺化碳烷基化为生物柴油前体的半纤维素衍生糠醛
Pub Date : 2024-07-14 DOI: 10.1021/acssusresmgt.4c00204
Shijie Fang, Yanchang Chu, Zhiting Gong, Rui Ma, Le Yang
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引用次数: 0
Almond and Walnut Shell Activated Carbon for Methylene Blue Adsorption 用于吸附亚甲蓝的杏仁和核桃壳活性炭
Pub Date : 2024-07-13 DOI: 10.1021/acssusresmgt.4c00080
Z. McCaffrey, Lennard F. Torres, B. Chiou, W. Hart-Cooper, Colleen McMahan, W. Orts
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引用次数: 0
Almond and Walnut Shell Activated Carbon for Methylene Blue Adsorption 用于吸附亚甲蓝的杏仁和核桃壳活性炭
Pub Date : 2024-07-13 DOI: 10.1021/acssusresmgt.4c0008010.1021/acssusresmgt.4c00080
Zach McCaffrey*, Lennard F. Torres, Bor-Sen Chiou, William Hart-Cooper, Colleen McMahan and William J. Orts, 

Activated carbon (AC) from nutshells has the potential to be an economically attractive product. This study developed ACs from almond and walnut shells and compared their performance against two commercial ACs (Calgon Carbon Filtersorb 400 and Kuraray YP50) in adsorbing methylene blue (MB) at various concentrations. Activated carbons were generated from nutshell biochar using 2 levels of activation to investigate the effect of activation residence time on material properties including pore development and MB adsorption. Raw nutshells, nutshell biochars, and nutshell ACs were characterized using elemental (CHNSO) analysis, proximate analysis, thermogravimetric analysis, activation kinetics, Fourier transform infrared (FTIR), scanning electron microscopy (SEM), MB adsorption testing, Brunauer-Emmett-Teller (BET) surface area and pore size distribution, and linear regression analysis on incremental pore volume and methylene blue adsorption capacity. Results demonstrated that almond and walnut shells can be used to make activated carbon that has a similar or better methylene blue adsorption performance than the tested commercial carbons. Almond shell, walnut shell, and YP50 and Filtersorb 400 activated carbons showed MB adsorption capacities of 440, 358, 487, and 310 mg g–1, respectively. Physical activation using carbon dioxide led to enhanced micropore development, and specifically, greater volume of pores with widths between 8-18 Å led to higher MB adsorption capacity. Activated carbon manufactured from nutshells shows significant potential for wastewater applications as well as other applications requiring microporous carbon.

果壳活性炭(AC)有可能成为一种具有经济吸引力的产品。本研究从杏仁壳和核桃壳中提取活性炭,并与两种商用活性炭(Calgon Carbon Filtersorb 400 和 Kuraray YP50)比较了它们在不同浓度下吸附亚甲基蓝(MB)的性能。使用两种活化水平从果壳生物炭中生成活性炭,以研究活化停留时间对材料特性(包括孔隙发育和甲基溴吸附)的影响。使用元素(CHNSO)分析、近物分析、热重分析、活化动力学、傅里叶变换红外(FTIR)、扫描电子显微镜(SEM)、甲基溴吸附测试、布鲁诺-艾美特-泰勒(BET)表面积和孔径分布以及对孔隙增量和亚甲基蓝吸附能力的线性回归分析,对原始果壳、果壳生物炭和果壳活性炭进行了表征。结果表明,杏仁壳和核桃壳可用于制造活性炭,其亚甲基蓝吸附性能与测试的商用炭相似或更好。杏仁壳、核桃壳以及 YP50 和 Filtersorb 400 活性炭的甲基溴吸附容量分别为 440、358、487 和 310 毫克 g-1。使用二氧化碳进行物理活化可增强微孔发育,特别是宽度在 8-18 Å 之间的更大孔径可提高甲基溴的吸附能力。用果壳制造的活性炭在废水处理以及其他需要微孔碳的应用中显示出巨大的潜力。
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引用次数: 0
Meglumine Encapsulated CuI: A Green Heterogeneous Catalyst Derived from Low Value Biomass Meglumine to Access 1,2,3-Triazole Scaffolds 美姑明包裹的 CuI:一种从低价值生物质中提取的绿色异质催化剂 美姑明用于获取 1,2,3-三唑支架
Pub Date : 2024-07-12 DOI: 10.1021/acssusresmgt.4c00103
Manan S Patel, Jaydeepkumar N Parekh, Dipakkumar D Chudasama, Harsh C Patel, Manish Kumar Mishra, Jeebanjyoti Mohapatra, Kesur R. Ram
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引用次数: 0
Meglumine Encapsulated CuI: A Green Heterogeneous Catalyst Derived from Low Value Biomass Meglumine to Access 1,2,3-Triazole Scaffolds 美姑明包裹的 CuI:一种从低价值生物质中提取的绿色异质催化剂 美姑明用于获取 1,2,3-三唑支架
Pub Date : 2024-07-12 DOI: 10.1021/acssusresmgt.4c0010310.1021/acssusresmgt.4c00103
Manan S. Patel, Jaydeepkumar N. Parekh, Dipakkumar D. Chudasama, Harsh C. Patel, Manish Kumar Mishra, Jeebanjyoti Mohapatra and Kesur R. Ram*, 

In current state of the art, we report a solitary pot green tactic for the synthesis of task-specific CuI nanoparticles (NPs) encapsulated by eco-healthy low value biomass (LVBM) meglumine. The synthesized meglumine encapsulated CuI NPs (Meg-Cu) material was characterized by using various analytical tools, and it was found that CuI NPs (with <100 nm size) were encapsulated by meglumine molecules interacting with −NHMe and −OH functionalities of meglumine. Meg-Cu was utilized marvelously as a catalyst for the creation of 1,2,3-triazole scaffolds. The established protocol allowed the synthesis of 1,2,3-triazoles via both two- and three-component routes. Moreover, the protocol was efficiently used for the synthesis of 1,2,3-triazoles initiated from anilines via in-situ generation of aromatic azides. The catalyst was successfully recycled up to three times without a loss of catalytic activity. The structural integrity of the spent catalyst was investigated by FT-IR and TGA analysis. The present protocol embraces features like a short reaction time, wide substrate scope, environment-friendly reaction conditions, and good to excellent yields.

在目前的技术水平下,我们报道了用生态健康的低值生物质(LVBM)巨鲁胺合成任务特异性CuI纳米粒子(NPs)的单锅绿色方法。利用各种分析工具对合成的巨鲁明封装 CuI NPs(Meg-Cu)材料进行了表征,发现 CuI NPs(大小为 100 nm)被巨鲁明分子与巨鲁明的 -NHMe 和 -OH 官能相互作用而封装。镁铜作为催化剂被用于创造 1,2,3-三唑支架,效果奇佳。所建立的方案允许通过双组分和三组分路线合成 1,2,3-三唑。此外,该方案还可通过原位生成芳香叠氮化物,有效地用于合成由苯胺引发的 1,2,3-三唑。催化剂可成功循环使用三次,且不会丧失催化活性。通过傅立叶变换红外光谱和热重分析研究了废催化剂的结构完整性。本方案具有反应时间短、底物范围广、反应条件对环境友好、产率高至优等特点。
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引用次数: 0
Persea Americana Leaf Extract-Derived Nanohybrids: A Sustainable and Green Approach for Rapid Photocatalytic Degradation of Organic Contaminants in Water 美洲鲈鱼叶提取物衍生纳米混合体:快速光催化降解水中有机污染物的可持续绿色方法
Pub Date : 2024-07-12 DOI: 10.1021/acssusresmgt.4c00118
Sandeep Kumar Singh, Sankeerthana Avasarala, Mahima S, Suryasarathi Bose
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引用次数: 0
Ultrasound Induced Enhancement of Biological Gas-to-Liquid Process for Methanol Synthesis from Methane Using Methylotuvimicrobium buryatense 5GB1C 超声波诱导增强生物气液分离工艺,利用埋地甲霉 5GB1C 从甲烷中合成甲醇
Pub Date : 2024-07-12 DOI: 10.1021/acssusresmgt.4c00116
Aradhana Priyadarsini, K. Khaire, Aditya Singh Chauhan, Sachin Kumar, L. Barbora, Subhrangsu Sundar Maitra, V. S. Moholkar
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引用次数: 0
Fabrication of Thermoplastic Poly(ether-ester) Elastomers with High Melting Temperature and Elasticity from Bio-based 2,5-Furandicarboxylic Acid 用生物基 2,5-呋喃二甲酸制造具有高熔点和弹性的热塑性聚醚酯弹性体
Pub Date : 2024-07-12 DOI: 10.1021/acssusresmgt.4c0014110.1021/acssusresmgt.4c00141
Tao Yang, Fei Liu*, Ruixue Gao, Xiaoqin Zhang*, Jiaxi Li, Jinggang Wang* and Jin Zhu, 

Even though current research on bio-based poly(ester-ether) elastomers (TPEEs) has expanded to include applications, only odd TPEEs with outstanding melting temperatures have been reported thus far. This is due to certain features, like desirable elastic properties and high melting temperature, which are still challenging to obtain without the utilization of petroleum-based monomers. In order to prepare bio-based TPEE with both high thermal resistance and elastic recovery, furan-based poly(1,4-cyclohexanedimethylene furandicarboxylate)-poly(tetramethylene glycol) multiblock copolymers (PCFTMG2k) were synthesized in this work. These copolymers had weight fractions of soft segments PTMG (ωPTMG) ranging from 30 to 80% while maintaining Mn of the soft segments at 2 kg/mol. Indeed, while PTMG segments are found to delay substantially the crystallization of the PCF within the copolymers, the results show that TPEEs with both elastic properties and high melting temperatures can be successfully prepared by introducing soft segments with relatively good crystallization ability and controlling the content of soft segments. Moreover, the crystallization behavior of the copolymers was investigated, from which it was found that the copolymers transformed from a non-cocrystallization state to an isodimorphic state as the content of soft segments increased. More importantly, PCFTMG2k-80, containing 80 wt % of the PTMG segment, showed a shape recovery rate as high as 84.9% during the first cyclic test at 200% strain and Tm up to 198°C at a high PTMG concentration, which is higher than those of almost all the TPA-based TPEEs. This PCFTMG2k bio-based TPEE will occupy an important position in the future market of high melting temperature thermoplastic elastomers.

尽管目前对生物基聚(酯-醚)弹性体(TPEEs)的研究已扩展到各种应用领域,但迄今为止,仅有少数几种具有出色熔融温度的 TPEEs 被报道过。这是因为某些特性,如理想的弹性性能和高熔点,在不使用石油基单体的情况下仍很难获得。为了制备具有高耐热性和弹性恢复能力的生物基 TPEE,本研究合成了呋喃基聚(1,4-环己烷二甲基呋喃二甲酸酯)-聚(四甘醇)多嵌段共聚物(PCFTMG2k)。这些共聚物的软段 PTMG 重量分数(ωPTMG)从 30% 到 80% 不等,同时软段的锰含量保持在 2 kg/mol。结果表明,通过引入结晶能力相对较好的软段并控制软段的含量,可以成功制备出既具有弹性特性又具有较高熔化温度的 TPEE。此外,还研究了共聚物的结晶行为,发现随着软段含量的增加,共聚物会从非结晶态转变为同晶态。更重要的是,含有 80 wt % PTMG 段的 PCFTMG2k-80 在 PTMG 浓度较高的情况下,在 200% 应变和高达 198°C 的温度下进行第一次循环测试时,形状恢复率高达 84.9%,高于几乎所有基于 TPA 的 TPEE。这种 PCFTMG2k 生物基热塑性弹性体将在未来的高熔点热塑性弹性体市场中占据重要地位。
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引用次数: 0
Ultrasound Induced Enhancement of Biological Gas-to-Liquid Process for Methanol Synthesis from Methane Using Methylotuvimicrobium buryatense 5GB1C 超声波诱导增强生物气液分离工艺,利用埋地甲霉 5GB1C 从甲烷中合成甲醇
Pub Date : 2024-07-12 DOI: 10.1021/acssusresmgt.4c0011610.1021/acssusresmgt.4c00116
Aradhana Priyadarsini, Kaustubh Chandrakant Khaire, Aditya Singh Chauhan, Sachin Kumar, Lepakshi Barbora, Subhrangsu Sundar Maitra and Vijayanand S. Moholkar*, 

Methanol is a potential alternate liquid transportation fuel. Conventional processes for methanol production from methane are energy-intensive. Microbial conversion of methane to methanol (Biological Gas-To-Liquid process) is a potential eco-friendly alternative. In this study, we have reported the intensification of methane fermentation to methanol (24 h batch mode) by Methylotuvimicrobium buryatense 5GB1C using 33 kHz sonication. The fermentation process was optimized for the sonication treatment time and duty cycle. A maximum titer of 20 mM (127.5 mg methanol/g dry cell weight biomass) was obtained in a 10 h sonication treatment at a 10% duty cycle, which was ∼57% higher than in control experiments. A mechanistic study of this result using pmoA gene expression (measured using qRT-PCR) and total protein analysis (sodium dodecyl sulfate-polyacrylamide gel electrophoresis (SDS-PAGE)) revealed that the overexpression of the pmoA gene (therefore, pmoCAB operon) led to the overexpression of the particulate methane monooxygenase (pMMO) enzyme in the metabolic pathway of M. buryatense resulting in the production of pMMO in higher quantities than that in control experiments. The ultimate manifestation of these phenomena was faster enzyme kinetics and high methanol yield.

甲醇是一种潜在的替代液体运输燃料。利用甲烷生产甲醇的传统工艺是能源密集型的。用微生物将甲烷转化为甲醇(生物气液工艺)是一种潜在的生态友好型替代方法。在这项研究中,我们报告了利用 33 kHz 超声波强化 Methylotuvimicrobium buryatense 5GB1C 将甲烷发酵为甲醇(24 小时批处理模式)的情况。发酵过程中对超声处理时间和占空比进行了优化。在占空比为 10%的情况下,超声处理 10 小时后,获得的最大滴度为 20 毫摩尔(127.5 毫克甲醇/克细胞干重生物质),比对照实验高出 57%。利用 pmoA 基因表达(使用 qRT-PCR 测量)和总蛋白分析(十二烷基硫酸钠-聚丙烯酰胺凝胶电泳(SDS-PAGE))对这一结果进行的机理研究表明,pmoA 基因(因此是 pmoCAB 操作子)的过度表达导致了埋囊菌代谢途径中的微粒甲烷单加氧酶(pMMO)的过度表达,从而产生了甲醇。buryatense 的代谢途径中的微粒甲烷单加氧酶(pMMO)过度表达,导致 pMMO 的产生量高于对照实验。这些现象的最终表现是酶动力学更快,甲醇产量更高。
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