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Amine-Grafted Heterogeneous Catalysts from Waste for Diols Conversion into Cyclic Carbonates 从废弃物中提取胺接枝异相催化剂,用于将二元醇转化为环状碳酸盐
Pub Date : 2024-07-23 DOI: 10.1021/acssusresmgt.4c0013710.1021/acssusresmgt.4c00137
Adriano Parodi*, Myriam Merendino, Martina Vagnoni, Alessio Mezzi, Chiara Samorì and Paola Galletti, 

The valorization of cellulose- and starch-based wastes has been investigated through a two-step methodology, aiming at the synthesis of amine grafted chars tested as catalysts in the synthesis of cyclic carbonates from diols and dimethyl carbonate. Catalysts were prepared by subjecting the starting material to mild pyrolysis for obtaining biochars, followed by anchoring of 1,6-diamino-hexane on the surface of the char, performed in H2O. This protocol has been applied to three different pristine polysaccharides (starch, cellulose, and cellulose acetate) and wastes containing the same (post-use starch-based plastics, fir sawdust, and post-use cigarette filters). The success of the derivatization method was confirmed by XPS and elemental analyses. The obtained catalysts were effective and did not show any significant difference in terms of the catalytic activity. Broad investigation on the reaction scope has been conducted on several mono- and disubstituted, aliphatic, and aromatic 1,2-and 1,3-diols, giving carbonates in high yields and selectivity (up to 96% and 99%, respectively). Quantification of the active site density has also been performed, allowing the calculation of TONs, TOFs, and productivity values for each catalyst. The recyclability of the heterogeneous catalysts has also been proved, and characterization of the recycled materials confirmed this behaviour.

通过两步法研究了纤维素和淀粉基废弃物的价值化问题,目的是合成胺接枝炭,并将其作为从二醇和碳酸二甲酯合成环状碳酸盐的催化剂。在制备催化剂时,先对起始材料进行温和热解以获得生物炭,然后在 H2O 中将 1,6-二氨基己烷锚定在炭表面。该方案已应用于三种不同的原始多糖(淀粉、纤维素和醋酸纤维素)和含有相同多糖的废物(使用后的淀粉基塑料、杉木锯屑和使用后的香烟过滤嘴)。XPS 和元素分析证实了衍生化方法的成功。获得的催化剂是有效的,在催化活性方面没有任何显著差异。该催化剂对几种一元和二元、脂肪族和芳香族 1,2 和 1,3 二醇的反应范围进行了广泛的研究,得到了高产率和高选择性(分别高达 96% 和 99%)的碳酸盐。此外,还对活性位点密度进行了量化,从而计算出了每种催化剂的吨数、TOF 和生产率值。异相催化剂的可回收性也得到了证实,回收材料的表征也证实了这一特性。
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引用次数: 0
Sustainable Porous Heterogeneous Catalysts for the Conversion of Biomass into Renewable Energy Products 将生物质转化为可再生能源产品的可持续多孔异构催化剂
Pub Date : 2024-07-23 DOI: 10.1021/acssusresmgt.4c00190
Sujan Mondal, Santu Ruidas, S. Chongdar, Basudeb Saha, Asim Bhaumik
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引用次数: 0
Sustainable Porous Heterogeneous Catalysts for the Conversion of Biomass into Renewable Energy Products 将生物质转化为可再生能源产品的可持续多孔异构催化剂
Pub Date : 2024-07-23 DOI: 10.1021/acssusresmgt.4c0019010.1021/acssusresmgt.4c00190
Sujan Mondal, Santu Ruidas, Sayantan Chongdar, Basudeb Saha and Asim Bhaumik*, 

Bioenergy possesses the potential to alleviate our energy demands while maintaining renewability and carbon neutrality. The utilization of abundant biomass sources for bioenergy production presents a significant challenge. When considering chemical processes for conversion, the development of effective catalysts becomes imperative as they play a pivotal role in biomass-to-bioenergy/biofuel conversion. In such scenarios, heterogeneous nanoporous materials emerge as crucial components for facilitating catalytic conversion. This perspective provides a comprehensive summary of biomass, including its classification, valorization processes and applications along with recent advancements in various catalytic systems utilized for transforming biomass and its intermediates into renewable energy products. We delved into the diverse classes of heterogeneous catalysts, including metal-based, metal oxide-based, silica based, hybrid catalysts, and organic polymers, highlighting their unique structural and compositional features that influence catalytic activity and selectivity. Furthermore, we discussed the importance of pore structure, surface area, and active site accessibility in enhancing catalytic performance. By examining the advantages and limitations of different catalysts, we provide insights into the rational design and optimization of porous heterogeneous catalysts for efficient and sustainable bioenergy conversion. This perspective serves as a valuable resource for researchers and engineers in the field of renewable energy, seeking to develop innovative catalyst materials for biomass valorization.

生物能源具有缓解我们的能源需求,同时保持可再生性和碳中和的潜力。利用丰富的生物质资源生产生物能源是一项重大挑战。在考虑化学转化过程时,开发有效的催化剂势在必行,因为催化剂在生物质到生物能源/生物燃料的转化过程中发挥着关键作用。在这种情况下,异质纳米多孔材料成为促进催化转化的关键成分。本视角对生物质进行了全面总结,包括生物质的分类、价值化过程和应用,以及用于将生物质及其中间产物转化为可再生能源产品的各种催化系统的最新进展。我们深入探讨了各类异质催化剂,包括金属基、金属氧化物基、硅基、混合催化剂和有机聚合物,重点介绍了影响催化活性和选择性的独特结构和组成特征。此外,我们还讨论了孔隙结构、表面积和活性位点可及性对提高催化性能的重要性。通过研究不同催化剂的优势和局限性,我们深入了解了如何合理设计和优化多孔异质催化剂,以实现高效、可持续的生物能源转化。这一视角为可再生能源领域的研究人员和工程师提供了宝贵的资源,帮助他们开发创新的催化剂材料,实现生物质的价值化。
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引用次数: 0
Amine-Grafted Heterogeneous Catalysts from Waste for Diols Conversion into Cyclic Carbonates 从废弃物中提取胺接枝异相催化剂,用于将二元醇转化为环状碳酸盐
Pub Date : 2024-07-23 DOI: 10.1021/acssusresmgt.4c00137
Adriano Parodi, Myriam Merendino, Martina Vagnoni, Alessio Mezzi, C. Samorì, Paola Galletti
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引用次数: 0
Unlocking the Potential: Algal Biomass Cultivation and Growth Kinetics Using Tanning Process Water 释放潜能:利用制革工艺水培养藻类生物质和生长动力学
Pub Date : 2024-07-22 DOI: 10.1021/acssusresmgt.4c00050
Mahesh Kumar Gagrai
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引用次数: 0
Unlocking the Potential: Algal Biomass Cultivation and Growth Kinetics Using Tanning Process Water 释放潜能:利用制革工艺水培养藻类生物质和生长动力学
Pub Date : 2024-07-22 DOI: 10.1021/acssusresmgt.4c0005010.1021/acssusresmgt.4c00050
Mahesh Kumar Gagrai*, 

A basic kinetic model has been applied to microalgae to predict the growth parameters in Zarrouk Media composition (ZMC) and precipitated chrome tanning effluent (PCTE). The model was fitted with the experimental data of Spirulina cultivation to estimate growth parameters: nutrient adsorption constant (Ka) (h–1), nutrient desorption constant (Kd) (h–1), rate of respiration (rRc)(h–1), efficiency of bio-synthesis (β) (g g–1), respiration rate (h–1)(rRc), rate of maximum photosynthesis (pmax) (h–1), coefficient for light-absorption (α) (m2 g–1), photon efficiency (g.μmol–1 photons–1) (φm), etc. The model suggests a higher nutrient adsorption rate in ZMC (0.75 h–1) as compared to PCTE (1.40 × 10–2 h–1). The rate of respiration of Spirulina decreased due to cultivation in PCTE from 5.36 × 10–3 to 1.91 × 10–3 h–1. The biosynthetic efficiency of Spirulina decreased from 8.72 to 2.002 due to cultivation in PCTE media. The maximum photosynthetic rate h–1 was slightly higher in ZMC as compared to PCTE media. The model parameter values were lower for Spirulina in PCTE than those in ZMC. Spirulina’s cell density was lower in PCTE compared to ZMC, as the doubling time was increased from 9.97 h–1 to 31.47 h–1. Moreover, the optimum pH for growth was also shifted from 9.5 to 10.5. The higher dose of PCTE (Cl > 2.96 × 103 mg L–1) restricted cell growth. Adding Cr(III) in ZMC has a higher impact on cell growth than Cr(VI). The model parameters with Cr(III) and Cr(VI) also showed a decrease in values except rRc and β have higher values for Cr(VI) as compared to Cr(III) added ZMC due to the non-interaction of Cr(VI) with algae. The model-predicted cell growth rates closely align with experimental results, with deviations within an ±7% margin. The addition of heavy metals to ZMC disrupts nutrient interactions and transport mechanisms during Spirulina cell growth.

将基本动力学模型应用于微藻类,以预测扎鲁克培养基成分(ZMC)和沉淀铬鞣废水(PCTE)中的生长参数。该模型与螺旋藻培养的实验数据进行了拟合,以估算生长参数:养分吸附常数(Ka)(h-1)、养分解吸常数(Kd)(h-1)、呼吸速率(rRc)(h-1)、生物合成效率(β)(g g-1)、呼吸速率(h-1)(rRc)、最大光合速率(pmax)(h-1)、光吸收系数(α)(m2 g-1)、光子效率(g.μmol-1光子-1)(φm)等。模型表明,与 PCTE(1.40 × 10-2 h-1)相比,ZMC(0.75 h-1)的养分吸附率更高。螺旋藻在 PCTE 中的呼吸速率从 5.36 × 10-3 h-1 降至 1.91 × 10-3 h-1。螺旋藻在 PCTE 培养基中的生物合成效率从 8.72 降至 2.002。与 PCTE 培养基相比,ZMC 培养基的最大光合速率略高。螺旋藻在 PCTE 培养基中的模型参数值低于在 ZMC 培养基中的模型参数值。与 ZMC 相比,螺旋藻在 PCTE 中的细胞密度较低,倍增时间从 9.97 h-1 增加到 31.47 h-1。此外,生长的最佳 pH 值也从 9.5 变为 10.5。较高剂量的 PCTE(Cl- > 2.96 × 103 mg L-1)限制了细胞的生长。与六价铬相比,在 ZMC 中添加三价铬对细胞生长的影响更大。铬(III)和铬(VI)的模型参数值也有所下降,但与添加铬(III)的 ZMC 相比,铬(VI)的 rRc 和 β 值更高,这是因为铬(VI)与藻类没有相互作用。模型预测的细胞生长率与实验结果非常吻合,偏差在 ±7% 的范围内。在 ZMC 中添加重金属会破坏螺旋藻细胞生长过程中的营养相互作用和运输机制。
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引用次数: 0
Pyrometallurgical Approach to Extracting Valuable Metals from a Combination of Diverse Li-Ion Batteries’ Black Mass 从多种锂离子电池黑质中提取有价金属的高温冶金方法
Pub Date : 2024-07-21 DOI: 10.1021/acssusresmgt.4c0011710.1021/acssusresmgt.4c00117
Safoura Babanejad*, Hesham Ahmed, Charlotte Andersson and Elsayed Mousa, 

Li-ion batteries (LIBs) are widely used nowadays. Because of their limited lifetimes and resource constraints in manufacturing them, it is essential to develop effective recycling routes to recover their valuable elements. This study focuses on the pyrometallurgical recycling of black mass (BM) from a mixture of different LIBs. In this study, the high-temperature behavior of two types of mixed BM is initially examined. Subsequently, the effect of mechanical activation on the BM reduction kinetics is investigated. Finally, hematite is added to the BM to first be reduced by the excess graphite in the BM and second to form an Fe-based alloy containing Co and Ni. This study demonstrates that mechanical activation does not necessarily affect the kinetics of BM high-temperature behavior. Furthermore, it demonstrates that alloy-making by the addition of hematite is a successful method to simultaneously utilize the graphite in the BM and recover Co and Ni, regardless of the LIB type.

When the sustainability in pyrometallurgical recycling of Li-ion batteries was enhanced, precious metals were recovered through an in situ alloy-making process, with an attempt to decrease CO2 emissions.

锂离子电池(LIB)如今已被广泛使用。由于锂离子电池的寿命有限,且在制造过程中存在资源限制,因此必须开发有效的回收途径,以回收其有价值的元素。本研究的重点是对不同 LIB 混合物中的黑质(BM)进行高温冶金回收。本研究首先考察了两种混合黑质的高温行为。随后,研究了机械活化对黑质还原动力学的影响。最后,赤铁矿被添加到 BM 中,首先被 BM 中多余的石墨还原,其次形成含有 Co 和 Ni 的铁基合金。这项研究表明,机械活化并不一定会影响 BM 的高温行为动力学。此外,它还证明了通过添加赤铁矿来制造合金是一种成功的方法,可以同时利用锂离子电池中的石墨并回收钴和镍,而不受锂离子电池类型的影响。为了提高锂离子电池高温冶金回收的可持续性,我们通过原位合金制造工艺来回收贵金属,以减少二氧化碳的排放。
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引用次数: 0
Pyrometallurgical Approach to Extracting Valuable Metals from a Combination of Diverse Li-Ion Batteries’ Black Mass 从多种锂离子电池黑质中提取有价金属的高温冶金方法
Pub Date : 2024-07-21 DOI: 10.1021/acssusresmgt.4c00117
Safoura Babanejad, Hesham Ahmed, Charlotte Andersson, Elsayed Mousa
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引用次数: 0
Green Reduction of Waste-Battery-Derived Graphene Oxide by Jute Leaves and Its Application for the Removal of Tetracyclines from Aqueous Media 黄麻叶绿色还原废电池衍生的氧化石墨烯及其在去除水介质中的四环素方面的应用
Pub Date : 2024-07-20 DOI: 10.1021/acssusresmgt.4c00181
Md. Humayun Kabir, Md. Sanwar Hossain, Mohammad Mahfujur Rahman, Md. Ashrafuzzaman, Mehedi Hasan, Md. Yeasin Pabel, Dipa Islam, Muhammad Shahriar Bashar, Tania Faruque, Sabina Yasmin
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引用次数: 0
Green Reduction of Waste-Battery-Derived Graphene Oxide by Jute Leaves and Its Application for the Removal of Tetracyclines from Aqueous Media 黄麻叶绿色还原废电池衍生的氧化石墨烯及其在去除水介质中的四环素方面的应用
Pub Date : 2024-07-20 DOI: 10.1021/acssusresmgt.4c0018110.1021/acssusresmgt.4c00181
Md. Humayun Kabir*, Md. Sanwar Hossain, Mohammad Mahfujur Rahman, Md. Ashrafuzzaman, Mehedi Hasan, Md. Yeasin Pabel, Dipa Islam, Muhammad Shahriar Bashar, Tania Faruque and Sabina Yasmin*, 

In recent years, contamination of aquatic ecosystems by antibiotics, especially tetracyclines (TCs), has become a significant concern. In this study, we have synthesized reduced graphene oxide (GrGO) using jute leaf extract as a green reducing and stabilizing agent for the reduction of graphene oxide (GO). The GO itself was synthesized from graphite derived from waste dry-cell batteries, making the process simple and cost-effective. We aimed to explore its potential as an adsorbent for the rapid and efficient removal of TCs from aqueous media. Characterization of GO and GrGO was carried out using FTIR, FESEM, EDX, and XRD techniques, revealing the successful reduction of GO to GrGO. The adsorption of TCs by GrGO was performed in a batch of experiments to assess the effect of adsorbent (GrGO) dose, solution pH, contact time, and temperature to find out the optimal condition of adsorption. The quantitative analysis of TCs before and after adsorption was conducted by using liquid chromatography–mass spectrometry (LC-MS/MS). Under optimal conditions, 98% of tetracycline (TEC), 97% of oxytetracycline (OTC), and 97% of chlortetracycline (CTC) were successfully removed from aqueous solutions. The adsorption isotherm of TCs onto GrGO fit well with the Freundlich isotherm model, while the kinetic data were best described by the pseudo-second-order model. The maximum adsorption capacity (qm) of GrGO for TEC, OTC, and CTC were found to be 22.85, 18.53, and 22.23 mg/g, respectively. Notably, the GrGO adsorbent demonstrated the ability to be reused effectively. Thermodynamic studies confirmed that the adsorption process is spontaneous and endothermic. The rapid and effective removal of these TCs was primarily governed by electrostatic and nonbonding interactions on the surface of GrGO. The findings indicate that green-synthesized GrGO is an effective and promising low-cost adsorbent for the removal of TCs from aqueous solutions.

近年来,抗生素,尤其是四环素(TCs)对水生生态系统的污染已成为人们关注的焦点。在这项研究中,我们利用黄麻叶提取物作为还原氧化石墨烯(GO)的绿色还原剂和稳定剂,合成了还原氧化石墨烯(GrGO)。GO 本身是从废弃干电池中提取的石墨合成的,因此工艺简单、成本效益高。我们的目的是探索其作为吸附剂的潜力,以快速有效地去除水介质中的三氯甲烷。我们使用傅立叶变换红外光谱(FTIR)、有限电子显微镜(FESEM)、电子衍射X和X射线衍射(XRD)技术对GO和GrGO进行了表征,结果表明GO成功地还原成了GrGO。通过批量实验评估了吸附剂(GrGO)剂量、溶液 pH 值、接触时间和温度对 TCs 的吸附效果,从而找出了最佳的吸附条件。采用液相色谱-质谱法(LC-MS/MS)对吸附前后的三氯乙酸进行了定量分析。在最佳条件下,水溶液中 98% 的四环素(TEC)、97% 的土霉素(OTC)和 97% 的金霉素(CTC)被成功去除。TC 在 GrGO 上的吸附等温线与 Freundlich 等温线模型非常吻合,而动力学数据则用伪二阶模型进行了最佳描述。GrGO 对 TEC、OTC 和 CTC 的最大吸附容量(qm)分别为 22.85、18.53 和 22.23 mg/g。值得注意的是,GrGO 吸附剂具有有效重复使用的能力。热力学研究证实,吸附过程是自发和内热的。GrGO 表面的静电和非键相互作用是快速有效去除这些三氯甲烷的主要原因。研究结果表明,绿色合成的 GrGO 是一种有效且有前景的低成本吸附剂,可用于去除水溶液中的三氯甲烷。
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引用次数: 0
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ACS Sustainable Resource Management
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