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Selective N-alkylation of amines with alcohols via hydrogen transfer catalyzed by copper complex in an ionic liquid media 离子液体介质中铜络合物通过氢转移催化胺与醇的选择性 N- 烷基化反应
Q2 Engineering Pub Date : 2024-01-17 DOI: 10.1016/j.ceja.2024.100585
N. Asharani , S. Shakeel Nawaz , S. Ranganatha , S. Supriya , Dileep Ramakrishna

A catalytic system containing a copper-Schiff base complex in ethyl methyl imidazolium hexafluoro phosphate [(EMIM)PF6] ionic liquid, where the ionic liquid was used as a solvent, was found to be very effective to catalyze the synthesis of benzazoles [i.e. imidazoles (C–N), thiazoles (C–S) and oxazoles (C–O)]. Substituted amines and alcohols reacted with each other in the given reaction conditions to give benzazoles. The reaction proceeded via a hydrogen transfer mechanism, which was proved by conducting series of reactions involving the conversion of aldehydes/ketones to corresponding primary and secondary alcohols. The reaction conditions were optimized with respect to catalyst concentration, best choice of the solvent, effect of different bases and the optimized chosen ones. It was found that the reaction required as low as 0.1 mol% of the catalyst and potassium carbonate as the base. Most interestingly the quantity of the products yielded the same when an equal ration of water: [EMIM]PF6 mixture was used as the solvent, same as when the ionic liquid alone was used as the solvent. A wide range of substituted alcohols and amines were tested and the products were formed within a short reaction time and comparatively good yields.

研究发现,在乙基甲基咪唑六氟磷酸盐[(EMIM)PF6]离子液体中含有铜-希夫碱络合物的催化体系(离子液体用作溶剂)对苯并唑[即咪唑(C-N)、噻唑(C-S)和噁唑(C-O)]的合成非常有效。在给定的反应条件下,被取代的胺和醇相互反应生成苯并唑。该反应通过氢转移机理进行,这一点已通过一系列涉及醛/酮转化为相应的伯醇和仲醇的反应得到证实。对反应条件进行了优化,包括催化剂浓度、溶剂的最佳选择、不同碱的影响以及所选碱的优化。结果发现,反应所需的催化剂和碱碳酸钾的浓度低至 0.1 摩尔%。最有趣的是,当水和[EMIM]PF6 混合物的比例相同时,生成物的数量也相同:[EMIM]PF6 混合物作为溶剂时,生成物的数量与单独使用离子液体作为溶剂时相同。对多种取代醇和胺进行了测试,在很短的反应时间内就生成了产物,而且产率相对较高。
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引用次数: 0
Performance optimization and carbon reduction effect of solid waste-based cementitious materials from iron and steel metallurgical slags and ammonia-soda residue 利用钢铁冶金渣和氨碱渣生产固体废弃物基胶凝材料的性能优化和减碳效果
Q2 Engineering Pub Date : 2024-01-11 DOI: 10.1016/j.ceja.2024.100584
Dong Xu , Jinglong Liu , Huihui Du , Bing Ma , Chang Tang , Wen Ni , Xiaofei Yan , Houhu Zhang

The utilization of solid waste as a resource is a beneficial approach to achieve pollution reduction and carbon reduction simultaneously. In this paper, we developed a quaternary solid waste-based cementitious materials (SWCMs) that can be used as a substitute for cement by utilizing four types of solid waste, namely ground granulated blast furnace slag (GGBS), steel slag (SS), ammonia-soda residue (ASR) and desulfurization gypsum (DG). The performance optimization and carbon emissions of SWCMs are investigated by response surface methodology and emission factor calculations. The results showed that a second-order polynomial model can accurately predict the compressive strength of mortar specimens of SWCMs, with prediction accuracies of 96.78 % and 87.17 % for compressive strengths at 3 days and 28 days, respectively. In terms of raw materials, DG content positively correlates with the compressive strength of the mortar containing SWCMs, moreover, ratios of GGBS to ASR of less than two or more than eight are beneficial. In addition, the production process of each ton of SWCMs emits 71.51 kg CO2, which is only 10 % of the production process of ordinary Portland cement. Overall, this work elucidates the influence of raw materials on the mechanical properties of quaternary SWCMs and quantifies their carbon reduction effects as a substitute for traditional cement, advancing the investigation and application of SWCMs in the realm of low-carbon materials.

将固体废弃物作为一种资源加以利用,是同时实现污染减排和碳减排的有益方法。本文利用磨细高炉矿渣(GGBS)、钢渣(SS)、氨碱渣(ASR)和脱硫石膏(DG)四种固体废弃物,开发了一种可替代水泥的四元固体废弃物基胶凝材料(SWCMs)。通过响应面方法和排放因子计算,研究了 SWCM 的性能优化和碳排放。结果表明,二阶多项式模型可准确预测 SWCMs 砂浆试样的抗压强度,3 天和 28 天抗压强度的预测准确率分别为 96.78 % 和 87.17 %。在原材料方面,DG 含量与含有 SWCMs 的砂浆抗压强度呈正相关,而且 GGBS 与 ASR 的比率小于 2 或大于 8 都是有益的。此外,每吨 SWCMs 的生产过程会排放 71.51 千克二氧化碳,仅为普通硅酸盐水泥生产过程的 10%。总之,这项研究阐明了原材料对四元全硅酸盐水泥力学性能的影响,并量化了其作为传统水泥替代品的减碳效果,推动了全硅酸盐水泥在低碳材料领域的研究和应用。
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引用次数: 0
Exploring the Potential of Rare Earth Doped Carbon Dots: Concepts and Applications 探索掺稀土碳点的潜力:概念与应用
Q2 Engineering Pub Date : 2024-01-06 DOI: 10.1016/j.ceja.2024.100583
Juliana De Gregori da Rocha, Maria Alice Prado Cechinel, Larissa Fátima Rocha, Humberto Gracher Riella, Natan Padoin, Cíntia Soares

Carbon dots (CDs) are nanostructures containing mainly carbon atoms and abundant functional groups. With remarkable and adjustable physicochemical properties, CDs have excellent hydrophilicity, photoluminescence (PL), biocompatibility, and low toxicity. Although the numerous advantages make CDs a research target for synthesizing advanced materials, some limitations are pertinent and must be corrected. Rare earth elements (RE) are excellent candidates for doping CDs, obtaining hybrid materials called RE-CDs to optimize luminescence properties, applicability, and quantum yields. Hybrids allow the combination of the advantageous characteristics of both CDs and RE, drastically improving their luminous and magneto-optical imaging performance and opening the door to numerous practical and technological applications. To date, no studies in the literature have provided in-depth analyses of the methods used to prepare RE-CDs, the characterization techniques used, the challenges, and a critical analysis of what could be improved in the synthesis by proposing practical solutions. To fill this gap, this review initially presents a detailed survey of CDs and RE separately. Subsequently, RE-CDs hybrid materials are addressed, as well as their obtainment, commonly used characterizations, and recent applications, from analyte detection to their functionality in medical nanodevices. Finally, criticisms and suggestions for future work are also discussed to inspire new research and discoveries about the technological potential of hybrid materials derived from the doping of RE-CDs.

碳点(CD)是一种主要含有碳原子和丰富官能团的纳米结构。碳点具有显著的可调理化特性,具有良好的亲水性、光致发光性(PL)、生物相容性和低毒性。虽然 CD 具有众多优点,是合成先进材料的研究目标,但也存在一些局限性,必须加以纠正。稀土元素(RE)是掺杂 CD 的绝佳候选元素,可获得称为 RE-CD 的混合材料,从而优化发光特性、适用性和量子产率。杂化材料结合了光盘和稀土元素的优势特性,大大提高了发光和磁光成像性能,为众多实际应用和技术应用打开了大门。迄今为止,还没有任何文献对制备 RE-CDs 的方法、所用表征技术、面临的挑战进行深入分析,并通过提出实用的解决方案对合成中可改进之处进行批判性分析。为了填补这一空白,本综述首先对 CD 和 RE 分别进行了详细的调查。随后,论述了 RE-CDs 混合材料,以及它们的获得、常用表征方法和最新应用,从分析物检测到它们在医疗纳米设备中的功能。最后,还讨论了对未来工作的批评和建议,以激发对掺杂 RE-CDs 衍生的混合材料技术潜力的新研究和新发现。
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引用次数: 0
Recovery of NixMnyCoz(OH)2 and Li2CO3 from spent Li-ionB cathode leachates using non-Na precipitant-based chemical precipitation for sustainable recycling 利用基于非钠沉淀剂的化学沉淀法从废锂离子电池阴极浸出液中回收 NixMnyCoz(OH)2 和 Li2CO3,实现可持续循环利用
Q2 Engineering Pub Date : 2023-12-30 DOI: 10.1016/j.ceja.2023.100582
Tendai Tawonezvi , Dorcas Zide , Myalelo Nomnqa , Mandisa Madondo , Leslie Petrik , Bernard Jan Bladergroen

The interest in recycling spent lithium-ion batteries (Li-ionB) has surged due to the rising demand for valuable metals (e.g., Co, Ni, Li and Mn) and concerns about environmental repercussions emanating from conventional battery waste disposal. Conventional precipitation-based hydrometallurgy recycling processes utilise Na-based or metal-based precipitants. The Na, from Na-based precipitants, is present in high concentrations in the process effluent since they are not recovered during the recycling process. The Na-rich effluent cannot be discarded since it doesn't meet environmental regulations as per the U.S. Environmental Protection Agency (EPA) (2023) therefore creating a storage and disposal problem. It is therefore imperative to utilise non-Na-based precipitants to eliminate the effluent disposal problem. This paper focuses on the recovery of NixCoyMnz(OH)2 and Li2CO3, main precursors for Li-ionB cathode production, from a typical spent Li-ionB cathode (NMC 532) using non-Na precipitant-based chemical precipitation. This study reports NixCoyMnz(OH)2 and Li2CO3 recovery from spent Li-ionBs for closed-loop Li-ionB cathode recycling through an integrated hydrometallurgy and chemical precipitation process. Through the utilisation of leachate solutions comprising 2 M H2SO4 + 6 vol.% H2O2, and a 75 g/L S/L ratio and conducting leaching for 120 min at a temperature of 60 °C and IS of 350 rpm, the recovery efficiency of 98.1 % for Li, 97.1 % for Co, 96.1 % for Ni, and 95.7 % for Mn. The pH of the NMC leachate was initially adjusted to 5 to precipitate Fe, Al and Cu impurities. Thereafter, active metal species (Ni, Mn and Co) were precipitated at a pH of 13 as Ni0.5Co0.2Mn0.3(OH)2 composite microparticles by adding LiOH precipitant. Thereafter, the Li-rich resultant liquor was further used to recover the Li by adding 3.4 mol of CO2 bubbled at 0.068 mol (CO2)/L.min and 40 °C for 45 min. The Li2CO3 precipitates were separated from the suspension through filtration followed by washing using deionised water and hot air drying. The reaction time is 45 mins, and the agitation speed is 150 rpm. Through this multi-stage precipitation process, >98 % of Ni, Co, Mn and > 91 % of Li can be recovered in the form of Ni0.5Mn0.3Co0.2OH2 and Li2CO3 respectively. The process exhibits great potential for recovery of valuable materials from spent Li-ionBs. The recovered Ni0.5Co0.2Mn0.3(OH)2 and Li2CO3 materials will be used as precursors in the anhydrous NMC cathode production process.

由于对有价金属(如钴、镍、锂和锰)的需求不断增加,以及人们对传统电池废物处理方式造成的环境影响的担忧,人们对回收利用废旧锂离子电池(Li-ionB)的兴趣急剧增加。传统的基于沉淀的湿法冶金回收工艺利用 Na 基沉淀剂或金属基沉淀剂。由于在回收过程中无法回收 Na 基沉淀剂中的 Na,因此 Na 在工艺废水中的浓度很高。由于富含 Na 的废水不符合美国环境保护局(EPA)(2023 年)的环保规定,因此无法丢弃,这就造成了储存和处理问题。因此,当务之急是利用非 Na 基沉淀剂来解决废水处理问题。本文重点介绍了使用非 Na 沉淀剂化学沉淀法从典型的废锂离子电池阴极(NMC 532)中回收 NixCoyMnz(OH)2 和 Li2CO3 的情况,这两种物质是生产锂离子电池阴极的主要前体。本研究报告通过综合水冶和化学沉淀工艺,从废锂离子电池中回收 NixCoyMnz(OH)2 和 Li2CO3,用于闭环锂离子电池阴极循环利用。通过利用由 2 M H2SO4 + 6 vol.% H2O2 和 75 g/L S/L 比率组成的浸出液,并在温度为 60 °C 和 IS 为 350 rpm 的条件下浸出 120 分钟,锂的回收率达到 98.1%,钴的回收率达到 97.1%,镍的回收率达到 96.1%,锰的回收率达到 95.7%。最初将 NMC 浸出液的 pH 值调至 5,以沉淀铁、铝和铜杂质。然后,加入 LiOH 沉淀剂,在 pH 值为 13 时沉淀出活性金属物种(镍、锰和钴),形成 Ni0.5Co0.2Mn0.3(OH)2 复合微粒。之后,在富含锂的液体中加入 3.4 mol CO2,以 0.068 mol (CO2)/L.min 和 40 °C 的温度鼓泡 45 分钟,进一步回收锂。通过过滤从悬浮液中分离出 Li2CO3 沉淀,然后使用去离子水进行洗涤,并进行热空气干燥。反应时间为 45 分钟,搅拌速度为 150 rpm。通过这种多级沉淀过程,可分别以 Ni0.5Mn0.3Co0.2OH2 和 Li2CO3 的形式回收 98% 的镍、钴、锰和 91% 的锂。该工艺展示了从废锂离子电池中回收有价值材料的巨大潜力。回收的 Ni0.5Co0.2Mn0.3(OH)2 和 Li2CO3 材料将用作无水 NMC 阴极生产工艺的前驱体。
{"title":"Recovery of NixMnyCoz(OH)2 and Li2CO3 from spent Li-ionB cathode leachates using non-Na precipitant-based chemical precipitation for sustainable recycling","authors":"Tendai Tawonezvi ,&nbsp;Dorcas Zide ,&nbsp;Myalelo Nomnqa ,&nbsp;Mandisa Madondo ,&nbsp;Leslie Petrik ,&nbsp;Bernard Jan Bladergroen","doi":"10.1016/j.ceja.2023.100582","DOIUrl":"https://doi.org/10.1016/j.ceja.2023.100582","url":null,"abstract":"<div><p>The interest in recycling spent lithium-ion batteries (Li-ionB) has surged due to the rising demand for valuable metals (e.g., Co, Ni, Li and Mn) and concerns about environmental repercussions emanating from conventional battery waste disposal. Conventional precipitation-based hydrometallurgy recycling processes utilise Na-based or metal-based precipitants. The Na, from Na-based precipitants, is present in high concentrations in the process effluent since they are not recovered during the recycling process. The Na-rich effluent cannot be discarded since it doesn't meet environmental regulations as per the U.S. Environmental Protection Agency (EPA) (2023) therefore creating a storage and disposal problem. It is therefore imperative to utilise non-Na-based precipitants to eliminate the effluent disposal problem. This paper focuses on the recovery of Ni<sub>x</sub>Co<sub>y</sub>Mn<sub>z</sub>(OH)<sub>2</sub> and Li<sub>2</sub>CO<sub>3</sub>, main precursors for Li-ionB cathode production, from a typical spent Li-ionB cathode (NMC 532) using non-Na precipitant-based chemical precipitation. This study reports Ni<sub>x</sub>Co<sub>y</sub>Mn<sub>z</sub>(OH)<sub>2</sub> and Li<sub>2</sub>CO<sub>3</sub> recovery from spent Li-ionBs for closed-loop Li-ionB cathode recycling through an integrated hydrometallurgy and chemical precipitation process. Through the utilisation of leachate solutions comprising 2 M H<sub>2</sub>SO<sub>4</sub> + 6 vol.% H<sub>2</sub>O<sub>2</sub>, and a 75 g/L S/L ratio and conducting leaching for 120 min at a temperature of 60 °C and IS of 350 rpm, the recovery efficiency of 98.1 % for Li, 97.1 % for Co, 96.1 % for Ni, and 95.7 % for Mn. The pH of the NMC leachate was initially adjusted to 5 to precipitate Fe, Al and Cu impurities. Thereafter, active metal species (Ni, Mn and Co) were precipitated at a pH of 13 as Ni<sub>0.5</sub>Co<sub>0.2</sub>Mn<sub>0.3</sub>(OH)<sub>2</sub> composite microparticles by adding LiOH precipitant. Thereafter, the Li-rich resultant liquor was further used to recover the Li by adding 3.4 mol of CO<sub>2</sub> bubbled at 0.068 mol (CO<sub>2</sub>)/L.min and 40 °C for 45 min. The Li<sub>2</sub>CO<sub>3</sub> precipitates were separated from the suspension through filtration followed by washing using deionised water and hot air drying. The reaction time is 45 mins, and the agitation speed is 150 rpm. Through this multi-stage precipitation process, &gt;98 % of Ni, Co, Mn and &gt; 91 % of Li can be recovered in the form of Ni<sub>0.5</sub>Mn<sub>0.3</sub>Co<sub>0.2</sub>OH<sub>2</sub> and Li<sub>2</sub>CO<sub>3</sub> respectively. The process exhibits great potential for recovery of valuable materials from spent Li-ionBs. The recovered Ni<sub>0.5</sub>Co<sub>0.2</sub>Mn<sub>0.3</sub>(OH)<sub>2</sub> and Li<sub>2</sub>CO<sub>3</sub> materials will be used as precursors in the anhydrous NMC cathode production process.</p></div>","PeriodicalId":9749,"journal":{"name":"Chemical Engineering Journal Advances","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2023-12-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2666821123001394/pdfft?md5=7e9eaa8983b2171b215ee2047fbf3738&pid=1-s2.0-S2666821123001394-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139100051","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Carbon capture from low CO2 concentration stream through ternary alkali metal nitrates promotion of MgO sorbents at intermediate temperature and low space velocity 在中温和低空间速度下,通过三元碱金属硝酸盐促进氧化镁吸附剂从低二氧化碳浓度流中捕获碳
Q2 Engineering Pub Date : 2023-12-13 DOI: 10.1016/j.ceja.2023.100578
Kian Hoong Chai , Loong Kong Leong , Sumathi Sethupathi , Kok Chung Chong , Thomas Chung-Kuang Yang , Sze Pheng Ong , Yeow Hong Yap

Many MgO sorbents exhibit high CO2 uptake in the presence of high concentration CO2 and aided by high space velocity, which unfortunately leads to low CO2 capture efficiency from the gas stream. This study investigates the effect of Li/Na/K ratio on sorption performance in dilute CO2 streams (15% CO2) using alkali metal nitrates-promoted MgO sorbents at a low space velocity of 20 ml/g·min in fixed bed reactor. Study shows that the ratio of Li/Na/K in ternary alkali nitrate salt mixture significantly affects the induction periods for the second phase CO2 sorption, which is a key contributor to high CO2 uptake. High LiNO3 content in ternary mixture leads to long induction period, and therefore lower CO2 capacity during the 4 h period. Conversely, high ratios of NaNO3 and KNO3 leads to shorter induction periods. Among the samples, MgO with 9 mol% (Li0.18Na0.52K0.3) exhibits the highest CO2 sorption capacity of 5.56 mmol/g at 240°C in 4 h (20.6% CO2 capture efficiency) and 3.18 mmol/g after 5 cycles (10.8% CO2 capture efficiency). Comparative studies show that optimal temperatures for CO2 sorption are higher when using pure CO2 (280 to 320°C) than when using 15% CO2 (240°C) due to the thermodynamic equilibrium. CO2-TPD results indicate that CO2 desorption proceeds in two phases similar to CO2 sorption, and the presence of alkali salt in MgO also promotes the decomposition of bulk carbonate to CO2. It is shown that molten salt migration and agglomeration of MgO particles are likely the factors that lead to decline in CO2 uptake over the sorption-desorption cycles.

许多氧化镁吸附剂在高浓度二氧化碳的存在下,在高空间速度的帮助下表现出较高的二氧化碳吸收率,但遗憾的是,这导致气流中的二氧化碳捕获效率较低。本研究采用碱金属硝酸盐促进的氧化镁吸附剂,在固定床反应器中以 20 毫升/克-分钟的低空间速度吸附稀二氧化碳气流(15% CO2),研究了 Li/Na/K 比率对吸附性能的影响。研究表明,三元碱式硝酸盐混合物中的 Li/Na/K 比率会显著影响第二阶段二氧化碳吸附的诱导期,而诱导期是高二氧化碳吸收率的关键因素。三元混合物中的 LiNO3 含量高,诱导期就长,因此 4 小时内的 CO2 容量就低。相反,高比例的 NaNO3 和 KNO3 会导致较短的诱导期。在各种样品中,含 9 摩尔%(Li0.18Na0.52K0.3)的氧化镁在 240°C 下 4 小时内的二氧化碳吸附容量最高,为 5.56 毫摩尔/克(二氧化碳捕获效率为 20.6%),5 个周期后的二氧化碳吸附容量为 3.18 毫摩尔/克(二氧化碳捕获效率为 10.8%)。比较研究表明,由于热力学平衡,使用纯二氧化碳(280 至 320°C)时的二氧化碳吸附最佳温度高于使用 15% 二氧化碳(240°C)时的最佳温度。CO2-TPD 结果表明,二氧化碳解吸分两阶段进行,与二氧化碳吸附类似,氧化镁中碱盐的存在也促进了块状碳酸盐分解为二氧化碳。结果表明,熔盐迁移和氧化镁颗粒团聚可能是导致二氧化碳吸收量在吸附-解吸循环中下降的因素。
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引用次数: 0
Elevating oil-in-water emulsion separation: Unleashing the power of exfoliated graphitic carbon nitride composite membranes 提升水包油型乳液分离技术:释放剥离石墨氮化碳复合膜的能量
Q2 Engineering Pub Date : 2023-12-13 DOI: 10.1016/j.ceja.2023.100580
Swathi Divakar , Prajwal Sherugar , K.K. Nagaraja , R. Geetha Balakrishna , Mahesh Padaki

The current study describes composite membranes that utilise exfoliated graphitic carbon nitride (Eg-C3N4) as a promising membrane additive for oily-water separation, owing to its hydrophilic nature and high functionality. The integrated membranes have been discovered to have outstanding properties when Eg-C3N4 is used as a composite material in polysulphone (PSf) membranes. The study provides provide insights into the usage of such nanosheets to achieve good chemical interaction with the membrane matrix, enabling both Eg-C3N4 and PSf synergistic characteristics. The well-planned exfoliated g-C3N4-PSf composite demonstrated promising oil-water separation with an oil rejection capacity of >99 %. Furthermore, these exfoliated laminar planes interacted well with the polymer, resulting in membranes that were both thermally and mechanically stable. The membrane also has a high porosity range of 46.13 % to 76.03 % and a high-water uptake range of 42.23 + 1.68 % to 71.34 + 1.24 %, which explains the membrane's enhanced hydrophilicity and appropriate oily-water treatment capacity. Furthermore, the addition of Eg-C3N4 lowers surface roughness, which explains for the great antifouling capacity exhibited by the composite membrane, demonstrating a remarkable flux recovery ratio of about 99.1 % with no compromise in oil rejection during subsequent cycles.

本研究介绍了利用剥离石墨氮化碳(Eg-C3N4)作为油水分离膜添加剂的复合膜,因为它具有亲水性和高功能性。研究发现,当 Eg-C3N4 用作聚砜(PSf)膜的复合材料时,集成膜具有出色的性能。这项研究深入探讨了如何利用这种纳米片实现与膜基质的良好化学作用,从而实现 Eg-C3N4 和 PSf 的协同特性。经过精心设计的 g-C3N4-PSf 剥离复合材料显示出良好的油水分离效果,其排油能力高达 99%。此外,这些剥落的层状平面与聚合物相互作用良好,从而产生了热稳定性和机械稳定性都很高的膜。膜的孔隙率范围为 46.13 % 至 76.03 %,吸水率范围为 42.23 + 1.68 % 至 71.34 + 1.24 %,这说明膜具有更强的亲水性和适当的油水处理能力。此外,Eg-C3N4 的加入降低了表面粗糙度,因此复合膜具有很强的防污能力,通量恢复率高达 99.1%,而且在后续循环中的排油效果也没有受到影响。
{"title":"Elevating oil-in-water emulsion separation: Unleashing the power of exfoliated graphitic carbon nitride composite membranes","authors":"Swathi Divakar ,&nbsp;Prajwal Sherugar ,&nbsp;K.K. Nagaraja ,&nbsp;R. Geetha Balakrishna ,&nbsp;Mahesh Padaki","doi":"10.1016/j.ceja.2023.100580","DOIUrl":"https://doi.org/10.1016/j.ceja.2023.100580","url":null,"abstract":"<div><p>The current study describes composite membranes that utilise exfoliated graphitic carbon nitride (Eg-C<sub>3</sub>N<sub>4</sub>) as a promising membrane additive for oily-water separation, owing to its hydrophilic nature and high functionality. The integrated membranes have been discovered to have outstanding properties when Eg-C<sub>3</sub>N<sub>4</sub> is used as a composite material in polysulphone (PSf) membranes. The study provides provide insights into the usage of such nanosheets to achieve good chemical interaction with the membrane matrix, enabling both Eg-C<sub>3</sub>N<sub>4</sub> and PSf synergistic characteristics. The well-planned exfoliated g-C<sub>3</sub>N<sub>4</sub>-PSf composite demonstrated promising oil-water separation with an oil rejection capacity of &gt;99 %. Furthermore, these exfoliated laminar planes interacted well with the polymer, resulting in membranes that were both thermally and mechanically stable. The membrane also has a high porosity range of 46.13 % to 76.03 % and a high-water uptake range of 42.23 + 1.68 % to 71.34 + 1.24 %, which explains the membrane's enhanced hydrophilicity and appropriate oily-water treatment capacity. Furthermore, the addition of Eg-C<sub>3</sub>N<sub>4</sub> lowers surface roughness, which explains for the great antifouling capacity exhibited by the composite membrane, demonstrating a remarkable flux recovery ratio of about 99.1 % with no compromise in oil rejection during subsequent cycles.</p></div>","PeriodicalId":9749,"journal":{"name":"Chemical Engineering Journal Advances","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2023-12-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2666821123001370/pdfft?md5=0b93403c119cd0f2a6915b87bca71df2&pid=1-s2.0-S2666821123001370-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138838932","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Selective electrodeposition of Co-Ni composites from synthetic quasi LiB NMC 532 cathode sulphate solutions using rotating plate potentiostatic electrowinning 利用旋转板恒电位电沉积技术从合成的准 NMC 532 硫酸盐溶液中选择性电沉积 Co-Ni 复合材料
Q2 Engineering Pub Date : 2023-12-01 DOI: 10.1016/j.ceja.2023.100579
Tendai Tawonezvi , Dorcas Zide , Myalelo Nomnqa , Leslie Petrik , Bernard Jan Bladergroen

The interest in recycling spent lithium-ion batteries (Li-ionB) has surged due to the rising demand for valuable metals (e.g., Co, Ni, Li and Mn) and concerns about environmental repercussions emanating from conventional battery waste disposal. This research is centered on the recovery of Ni and Co from synthetic Ni, Co, Mn and Li sulphate solutions mimicking the NMC 532 ratio of elements using a hydro-electrometallurgy process route that integrates hydrometallurgy and potentiostatic electrometallurgy techniques. This quasi-model is done to elucidate the effect of multiple influencing parameters, through isolation and varying, on the selective electrodeposition of Co-Ni from multi-ion (Li, Ni, Mn and Co) complex solutions before applying it using real cathode leachates. The selective electrowinning metal recovery process route is a cost-effective alternative to the energy, cost and material-intensive hydrometallurgy intermediate purification processes such as solvent extraction, selective precipitation, and ion-exchange. The study delves into the effects of various electrowinning parameters, including applied potential, temperature, pH, Co, Ni, Na2SO4, NaH2PO4 buffer concentration, and cathode rotational speed. These parameters were thoroughly investigated and effectively optimised to achieve the recovery of 97.2% pure Ni0.65Co0.35 at a rate of 0.060 g/cm2.h with an impressive 89.25 % current efficiency. The composition of the electrowon deposit was meticulously quantified using Inductively Coupled Plasma Optical Emission Spectroscopy (ICP-OES) and subjected to analysis through a Scanning Electron Microscope (SEM-EDS). Additionally, the phase composition was evaluated using X-Ray Diffraction analysis (XRD). The results successfully demonstrate the technical feasibility of recovering Ni-Co composites, yielding high quantities of industrial-grade pure Ni-Co composites. This comprehensive electro-hydrometallurgical process, designed for both closed and loop recycling purposes, promotes a more environmentally preservative approach to recycling spent lithium-ion battery cathode material. The approach contributes significantly to the development of sustainable resource management infrastructure.

由于对有价金属(如钴、镍、锂和锰)的需求不断增加,以及对传统电池废物处理方式造成的环境影响的担忧,人们对回收利用废旧锂离子电池(Li-ionB)的兴趣大增。本研究的核心是利用水冶和静电电冶技术相结合的水电冶工艺路线,从模拟 NMC 532 元素比例的合成镍、钴、锰和锂硫酸盐溶液中回收镍和钴。该准模型旨在通过分离和改变多个影响参数,阐明其对从多离子(锂、镍、锰和钴)复杂溶液中选择性电沉积 Co-Ni 的影响,然后再将其应用于实际阴极浸出液。选择性电沉积金属回收工艺路线是一种具有成本效益的方法,可替代能源、成本和材料密集型湿法冶金中间净化工艺,如溶剂萃取、选择性沉淀和离子交换。研究深入探讨了各种电解参数的影响,包括应用电位、温度、pH 值、Co、Ni、Na2SO4、NaH2PO4 缓冲浓度和阴极转速。通过对这些参数的深入研究和有效优化,以 0.060 g/cm2.h 的速率回收了 97.2% 的纯 Ni0.65Co0.35,电流效率高达 89.25%。使用电感耦合等离子体光学发射光谱 (ICP-OES) 对电解质沉积物的成分进行了细致的量化,并通过扫描电子显微镜 (SEM-EDS) 进行了分析。此外,还利用 X 射线衍射分析 (XRD) 对相组成进行了评估。结果成功证明了回收镍钴复合材料的技术可行性,并获得了大量工业级纯镍钴复合材料。这种全面的电液冶金工艺设计用于封闭和循环回收目的,促进了一种更环保的回收废旧锂离子电池正极材料的方法。这种方法极大地促进了可持续资源管理基础设施的发展。
{"title":"Selective electrodeposition of Co-Ni composites from synthetic quasi LiB NMC 532 cathode sulphate solutions using rotating plate potentiostatic electrowinning","authors":"Tendai Tawonezvi ,&nbsp;Dorcas Zide ,&nbsp;Myalelo Nomnqa ,&nbsp;Leslie Petrik ,&nbsp;Bernard Jan Bladergroen","doi":"10.1016/j.ceja.2023.100579","DOIUrl":"10.1016/j.ceja.2023.100579","url":null,"abstract":"<div><p>The interest in recycling spent lithium-ion batteries (Li-ionB) has surged due to the rising demand for valuable metals (e.g., Co, Ni, Li and Mn) and concerns about environmental repercussions emanating from conventional battery waste disposal. This research is centered on the recovery of Ni and Co from synthetic Ni, Co, Mn and Li sulphate solutions mimicking the NMC 532 ratio of elements using a hydro-electrometallurgy process route that integrates hydrometallurgy and potentiostatic electrometallurgy techniques. This quasi-model is done to elucidate the effect of multiple influencing parameters, through isolation and varying, on the selective electrodeposition of Co-Ni from multi-ion (Li, Ni, Mn and Co) complex solutions before applying it using real cathode leachates. The selective electrowinning metal recovery process route is a cost-effective alternative to the energy, cost and material-intensive hydrometallurgy intermediate purification processes such as solvent extraction, selective precipitation, and ion-exchange. The study delves into the effects of various electrowinning parameters, including applied potential, temperature, pH, Co, Ni, Na<sub>2</sub>SO<sub>4</sub>, NaH<sub>2</sub>PO<sub>4</sub> buffer concentration, and cathode rotational speed. These parameters were thoroughly investigated and effectively optimised to achieve the recovery of 97.2% pure Ni<sub>0.65</sub>Co<sub>0.35</sub> at a rate of 0.060 g/cm<sup>2</sup>.h with an impressive 89.25 % current efficiency. The composition of the electrowon deposit was meticulously quantified using Inductively Coupled Plasma Optical Emission Spectroscopy (ICP-OES) and subjected to analysis through a Scanning Electron Microscope (SEM-EDS). Additionally, the phase composition was evaluated using X-Ray Diffraction analysis (XRD). The results successfully demonstrate the technical feasibility of recovering Ni-Co composites, yielding high quantities of industrial-grade pure Ni-Co composites. This comprehensive electro-hydrometallurgical process, designed for both closed and loop recycling purposes, promotes a more environmentally preservative approach to recycling spent lithium-ion battery cathode material. The approach contributes significantly to the development of sustainable resource management infrastructure.</p></div>","PeriodicalId":9749,"journal":{"name":"Chemical Engineering Journal Advances","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2023-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2666821123001369/pdfft?md5=d404ef01cd93c95b9ef943fd1b25018d&pid=1-s2.0-S2666821123001369-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138617847","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Zeolitic imidazolate framework-8 nanosheet assemblies for high-efficiency small molecule adsorption 沸石咪唑酸框架-8纳米片组件用于高效小分子吸附
Q2 Engineering Pub Date : 2023-11-15 DOI: 10.1016/j.ceja.2023.100573
Fraz Saeed Butt , Nurul A. Mazlan , Allana Lewis , Norbert Radacsi , Xianfeng Fan , Shuiqing Yang , Yi Huang

Metal-organic frameworks (MOFs) have gained tremendous attention based on the prospect of application-oriented structural tuning. In this study, the surfactant (SDS)-directed hydrothermal synthesis route was adopted for a one-pot, bottom-up synthesis of ZIF-8 spherical assemblies, stacked with externally oriented and intergrown two-dimensional (2D) nanosheets. The as-obtained nanosheet assemblies exhibited good crystallinity, a large surface area, and excellent thermal stability, as shown by XRD, BET, and TGA, respectively. More importantly, the ZIF-8 nanosheet assemblies displayed excellent small molecule adsorption characteristics, especially for the negatively charged dyes, including rose bengal (RB), uni-blue A (UA), and methyl orange (MO). Furthermore, samples showed a pseudo-second-order adsorption mechanism for dye molecules and presented a good fit for Langmuir's and Temkin's adsorption isotherms with an R2 value of 0.98 and 0.94, respectively. Adsorbent–adsorbate electrostatic interaction, nanosheet structures, molecular size and structural aromaticity of the dye, and the presence of SDS functionalities were found as the essential components for the high-capacity dye adsorption as compared with previous studies.

基于面向应用的结构调谐前景,金属有机框架(MOFs)得到了广泛的关注。在本研究中,采用表面活性剂(SDS)导向的水热合成路线,采用一锅法,自下而上合成了ZIF-8球形组件,并与外向和互生的二维(2D)纳米片堆叠。XRD、BET和TGA测试结果表明,所制备的纳米片具有良好的结晶度、较大的表面积和优异的热稳定性。更重要的是,ZIF-8纳米片组件表现出优异的小分子吸附特性,特别是对带负电荷的染料,包括玫瑰红(RB)、单蓝A (UA)和甲基橙(MO)。此外,样品对染料分子具有准二级吸附机理,符合Langmuir和Temkin吸附等温线,R2分别为0.98和0.94。与以往的研究相比,发现吸附剂-吸附质静电相互作用、纳米片结构、染料的分子大小和结构芳香性以及SDS功能的存在是高容量染料吸附的重要组成部分。
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引用次数: 0
Synthesis and design of NaNi1/3Fe1/3Mn1/3O2 cathode materials for long-life sodium-ion batteries 长寿命钠离子电池负极材料NaNi1/3Fe1/3Mn1/3O2的合成与设计
Q2 Engineering Pub Date : 2023-11-15 DOI: 10.1016/j.ceja.2023.100572
Tengfei Song , Qiyao Zhang , Yongxiu Chen , Pengcheng Zhu , Emma Kendrick

To enable the widespread adoption of residential energy storage, sustainable, low-cost, long-life, and energy-dense battery technologies are required. Sodium-ion offers many of these characteristics, however often the system is tailored for energy rather than cycle life. In this work, the effect of synthesis conditions upon the primary and agglomerated secondary particle size and shape of the sodium-ion cathode material NaNi1/3Fe1/3Mn1/3O2 was investigated for optimization of energy and cycle life. A two-level full factorial experimental design was utilized to examine how the synthesis parameters (pH, molar ratio of ammonia/metal precursor salt, and stirring speed) affect the physical and electrochemical properties. This approach enabled a comprehensive investigation of the main effects and interactions of these parameters. The data from multiple synthesis runs were analyzed using statistical methods and regression analysis. This experimental design provided valuable insights into the relationship between synthesis parameters and material properties. Statistical analysis indicates that both physical and electrochemical properties are mainly controlled through pH and NH4OH, while the effects of stirring speed are less pronounced. The optimal synthetic conditions producing the highest cycling performance were extrapolated from the statistical analysis. A validation experiment showed that particles synthesized with optimum parameters displayed a threefold increase in cycling performance together with uniformly distributed particle size and a high tap density.

为了使住宅储能的广泛采用,需要可持续、低成本、长寿命和高能量密度的电池技术。钠离子提供了许多这些特性,然而通常系统是针对能量而不是循环寿命量身定制的。本文研究了合成条件对钠离子正极材料NaNi1/3Fe1/3Mn1/3O2的初级和凝聚次级粒径及形状的影响,以优化其能量和循环寿命。采用两水平全因子实验设计,考察了合成参数(pH、氨/金属前体盐摩尔比、搅拌速度)对其物理和电化学性能的影响。这种方法能够对这些参数的主要影响和相互作用进行全面的研究。采用统计方法和回归分析对多次综合运行的数据进行分析。该实验设计为合成参数与材料性能之间的关系提供了有价值的见解。统计分析表明,pH和NH4OH对材料的物理性能和电化学性能的影响主要是由pH和NH4OH控制的,搅拌速度对材料的影响较小。通过统计分析,推断出产生最高循环性能的最佳合成条件。验证实验表明,优化后合成的颗粒循环性能提高了3倍,粒径分布均匀,丝锥密度高。
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引用次数: 0
Pathways to magnesium supplementation of drinking water: An overview of the saline water conversion corporation experience 饮用水镁补充途径:咸水转换公司经验综述
Q2 Engineering Pub Date : 2023-11-15 DOI: 10.1016/j.ceja.2023.100574
Christopher M. Fellows , Ali A. Al Hamzah , Seungwon Ihm

Magnesium (Mg) in drinking water is essential for human health, with low concentrations in drinking water being reported to be correlated with poor cardiovascular health outcomes. Based on the literature and suggestions that the World Health Organization would soon announce guidelines for Mg content of drinking water, the Saline Water Conversion Corporation (SWCC) announced specifications in October 2020 targeting 15–25 ppm of Mg in product water. SWCC produces approximately 6 million m3 of potable water daily for domestic and industrial use in the Kingdom of Saudi Arabia, so meeting this Mg target will require the allocation of significant resources. In this report the different approaches to adding Mg in post-treatment of the product water from the SWCC's network of desalination plants are reviewed in order to optimise the additional capital investment and ongoing operational expenses. The most cost-effective option is to mix produced water with groundwater containing Mg, but where this is not feasible the next most cost-effective method for achieving a 15 ppm target was assessed to be treating desalination brine with nanofiltration (NF) to generate a magnesium-rich brine fraction that can be mixed with produced water. A one-stage NF process can meet the 15 ppm Mg target only with levels of chloride and total dissolved solids exceeding regulatory maximums in the produced water, so a multi-stage NF process with intermediate dilution was designed. While this has a significantly higher capital expenditure and energy requirement than one-stage NF, at the cost of energy in the Kingdom of Saudi Arabia it is still significantly less expensive than alternative approaches (0.009 USD/m3). This solution was implemented at an SWCC desalination plant on the Red Sea and has been delivering Mg-enriched water (∼15 ppm) to approximately 1.3 million people since May 2022 at an estimated additional operational cost of 0.007 USD per m3. For lower target levels of Mg supplementation (∼5 ppm), replacement of limestone with dolomite in post-treatment limestone contactors has been found to be a cost-effective process in plant-scale trials at another SWCC plant on the Red Sea.

饮用水中的镁(Mg)对人类健康至关重要,据报道,饮用水中的低浓度与心血管健康状况不佳有关。根据文献和建议,世界卫生组织将很快宣布饮用水中Mg含量的指导方针,盐水转换公司(SWCC)于2020年10月宣布了产品水中Mg含量为15 - 25ppm的规格。在沙特阿拉伯王国,SWCC每天生产约600万立方米供家庭和工业使用的饮用水,因此要实现这一Mg目标将需要分配大量资源。在本报告中,为了优化额外的资本投资和持续的运营费用,审查了在SWCC海水淡化厂网络的产品水后处理中添加Mg的不同方法。最具成本效益的选择是将采出水与含镁的地下水混合,但如果这一方法不可行,那么实现15 ppm目标的下一个最具成本效益的方法是用纳滤(NF)处理海水淡化盐水,生成富镁盐水部分,可以与采出水混合。一段纳滤工艺只有在采出水中氯化物和总溶解固体含量超过规定最大值时才能达到15 ppm Mg的目标,因此设计了一种中间稀释的多级纳滤工艺。虽然这种方法的资本支出和能源需求明显高于一级NF,但在沙特阿拉伯王国,它的能源成本仍然明显低于其他方法(0.009美元/立方米)。该解决方案已在红海的SWCC海水淡化厂实施,自2022年5月以来,已向约130万人提供富镁水(约15 ppm),估计每立方米额外运营成本为0.007美元。在红海的另一家SWCC工厂进行的工厂规模试验发现,对于较低的Mg补充目标水平(~ 5ppm),在处理后的石灰石接触器中用白云石代替石灰石是一种具有成本效益的工艺。
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引用次数: 0
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