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Sustainable biosynthesis of caproate from waste activated sludge via electro-fermentation: Perspectives of product spectrum, economic and environmental impacts 通过电发酵从废弃活性污泥中可持续地生物合成己酸酯:产品谱系、经济和环境影响展望
IF 15.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2024-11-19 DOI: 10.1016/j.cej.2024.157768
Dengfei Li, Shuanglan Cheng, Cristiano Varrone, Bing-Jie Ni, Jingyang Luo, Zhihong Liu, Zhangwei He, Wenzong Liu, Aijuan Zhou, Xiuping Yue
Electro-fermentation (EF) has emerged as a promising method to produce value-added medium chain fatty acids (MCFAs) via chain elongation (CE). The biorefinery of waste activated sludge (WAS) to MCFAs has been attracting increasing attention. However, so far anaerobic_CE process was commonly employed, while the contribution and mechanism of EF_CE still remain unclear. In the present study, a comprehensive analysis of caproate biosynthesis from prefermented WAS via EF_CE was performed. The reduction in substrates resulted in an increase in caproate production, yielding the maximum caproate (299.8 mg COD/g volatile suspended solid) in the minimum substrate concentration (25 % prefermented WAS, EF13 group). The highest utilization rate (78.76 %) of soluble proteins was also achieved in EF13. Significant positive correlation among caproate yield, electrochemically active bacteria, caproate-synthesizing consortium and homo-acetogen was revealed by molecular ecological network and Mantel test. Further analysis of the metabolic pathways revealed that EF13 demonstrated more key enzymes participated in the production of acetyl-CoA via the Wood-Ljungdahl pathway and the conversation of acetyl-CoA to caproate via the reverse β-oxidation pathway. Moreover, compared to the anaerobic_CE process, the economic benefits of the EF_CE process significantly increased, and the environmental impacts were greatly reduced. The life cycle assessment and economic benefits analysis identified the strengths of EF_CE and proposed a sustainable strategy to facilitate the commercialization of electro-fermentation assisted biorefinery technology.
电发酵(EF)已成为通过链延伸(CE)生产高附加值中链脂肪酸(MCFAs)的一种有前途的方法。将废弃活性污泥(WAS)生物炼制成中链脂肪酸(MCFAs)已引起越来越多的关注。然而,迄今为止,人们普遍采用厌氧 CE 工艺,而 EFCE 的贡献和机理仍不清楚。本研究全面分析了预处理 WAS 通过 EF_CE 进行己酸酯生物合成的过程。底物的减少导致了己酸酯产量的增加,在底物浓度最低的情况下(25% 预处理 WAS,EF13 组),己酸酯产量最高(299.8 毫克 COD/克挥发性悬浮固体)。EF13 组的可溶性蛋白质利用率也最高(78.76%)。分子生态网络和曼特尔检验显示,己酸盐产量、电化学活性菌、己酸盐合成联合体和同源乙酸根之间存在显著的正相关。对代谢途径的进一步分析表明,EF13 表现出更多的关键酶参与了通过伍德-荣格达尔途径产生乙酰-CoA 和通过反向 β 氧化途径将乙酰-CoA 转化为己酸的过程。此外,与厌氧_CE 工艺相比,EF_CE 工艺的经济效益显著提高,对环境的影响大大降低。生命周期评估和经济效益分析确定了 EF_CE 的优势,并提出了促进电发酵辅助生物精炼技术商业化的可持续战略。
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引用次数: 0
MOFs-based 0D-2D-3D nanoarchitectonics as catalytic converters for peroxymonosulfate activation 基于 MOFs 的 0D-2D-3D 纳米结构作为过一硫酸盐活化的催化转换器
IF 15.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2024-11-19 DOI: 10.1016/j.cej.2024.157809
Rongfu Peng, Taiyang Cao, Minghui Wang, Chaohai Wang, Yingyi Li, Xinfeng Zhu, Shangru Zhai
Peroxymonosulfate-based advanced oxidation processes (PMS-AOPs) are promising trend for degrading of toxic organic pollutants. In this work, the novel 0D-2D-3D nanoarchitectonics (sandwich structure) are fabricated as advanced catalysts for PMS-AOPs. The distinctive sandwich structure of ZIF-67-AG-CA allows for the complete exposure of the active sites of ZIF-67, which can effectively activate PMS to generate both radical and non-radical species for the degradation of organic pollutants. Furthermore, the nano-reactive sites are distributed uniformly in layers, which provides additional PMS adsorption sites and enhances the efficiency of the catalytic reaction. Consequently, ZIF-67-AG-CA was observed to exhibit an excellent performance in the removal of organic pollutants by activating PMS, achieving a 99% degradation of 4-NP in 60 min and demonstrating good cycling stability through cycling experiments. Furthermore, quenching experiments and EPR demonstrated that SO42− and O2radical dot radicals were involved in a synergistic manner in the catalytic reaction process with 1O2 non-radicals during the catalytic process.
基于过一硫酸盐的高级氧化工艺(PMS-AOPs)是降解有毒有机污染物的大势所趋。在这项工作中,新型 0D-2D-3D 纳米架构(三明治结构)被制作成 PMS-AOPs 的高级催化剂。ZIF-67-AG-CA 独特的三明治结构使 ZIF-67 的活性位点完全暴露出来,能有效激活 PMS,生成自由基和非自由基物种,从而降解有机污染物。此外,纳米活性位点均匀地分布在各层中,为 PMS 提供了额外的吸附位点,提高了催化反应的效率。结果表明,ZIF-67-AG-CA 在活化 PMS 去除有机污染物方面表现出色,60 分钟内对 4-NP 的降解率达到 99%,并且通过循环实验显示出良好的循环稳定性。此外,淬灭实验和 EPR 显示,在催化反应过程中,SO42- 和 O2- 自由基与 1O2 非自由基以协同方式参与了催化反应过程。
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引用次数: 0
Hexagonal liquid crystals as emerging quasi solid-state electrolytes for aqueous lithium-ion batteries 六方液晶作为水性锂离子电池的新兴准固态电解质
IF 15.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2024-11-19 DOI: 10.1016/j.cej.2024.157794
Weirong Ren, Zhaowei Hou, Long Su, Xinpei Gao, Yanping Chu, Liqiang Zheng, Fei Lu
The increasing market demand ranging from portable electronics to electric vehicles drives the advancement of lithium-ion batteries. However, traditional liquid electrolytes used in LIBs are plagued by issues such as leakage, vaporization, and the degradation of active materials, which compromise performance and pose safety risks. To address these challenges, herein, the liquid-crystalline electrolytes with hexagonal phase were designed based on the self-assembly of amphiphilic molecules, which exhibit both high ionic conductivity and a high Li+ transference number. The hexagonal liquid crystal structure reconfigures the Li+ solvation structure and provides a transport pathway for the Li+ structural diffusion, facilitating the efficient transport of Li+ and contributing to the high ionic conductivity. Furthermore, the ordered arrangement of amphiphilic anion significantly restricts anion diffusion, resulting in an exceptionally high Li+ transference number of 0.92. Additionally, when utilizing NaV3O8 (NVO) as the anode and LiMn2O4 (LMO) as the cathode, the resultant full cell delivers impressive rate performance and stable cycling performance. This work highlights the potential of lyotropic liquid crystals in the development of high-performance quasi solid-state electrolytes for aqueous lithium-ion batteries and beyond
从便携式电子产品到电动汽车,日益增长的市场需求推动了锂离子电池的发展。然而,锂离子电池中使用的传统液态电解质存在泄漏、汽化和活性材料降解等问题,从而影响了电池的性能并带来安全风险。为了应对这些挑战,本文基于两亲性分子的自组装,设计了具有六方相的液晶电解质,这种电解质同时具有高离子电导率和高锂离子转移率。六方液晶结构重新配置了 Li+ 溶解结构,为 Li+ 结构扩散提供了传输途径,促进了 Li+ 的高效传输,从而实现了高离子电导率。此外,两亲阴离子的有序排列极大地限制了阴离子的扩散,从而使 Li+ 的传输数达到了 0.92 的超高水平。此外,当使用 NaV3O8(NVO)作为阳极和 LiMn2O4(LMO)作为阴极时,所产生的全电池具有令人印象深刻的速率性能和稳定的循环性能。这项工作凸显了各向同性液晶在开发用于水性锂离子电池及其他应用的高性能准固态电解质方面的潜力。
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引用次数: 0
Fluorescence resonance energy transfer system coupled with photonic crystals labeling strategy for multiplexed detection of microRNAs from breast cancer 荧光共振能量转移系统与光子晶体标记策略相结合,用于乳腺癌微 RNA 的多重检测
IF 15.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2024-11-19 DOI: 10.1016/j.cej.2024.157798
Sanxia Wang, Shixin Cai, Yi Zhao, Xin Chen, Sha Zhu, Maolin Li, Xiaoli Wang, Yuting Zhang, Nandi Zhou
MicroRNAs (miRNAs) play a crucial role in post-transcriptional gene expression and freely circulate in the body. Dysregulation of miRNA signaling is associated with various diseases, including breast cancer (BC). The miRNA profiles from liquid biopsies offer a promising strategy for cancer diagnosis, prognosis and monitoring. Particularly, the simultaneous profiling of multiple miRNA levels greatly enhances the accuracy of cancer diagnosis. In this study, photonic crystals (PhCs) serve as both labels and carriers enabling synchronous optical detection of multiple miRNA targets overexpressed in BC. The process is achieved by triggering enzyme-free amplification reactions through target interactions, generating fluorescence resonance energy transfer (FRET). The method offers high sensitivity, sequence specificity, and the capability to detect multiple targets. The limits of detection (LOD) of the sensor for miRNA-21, miRNA-155 and miRNA-10b were 6.36 fM, 8.52 fM and 6.06 fM, respectively. Moreover, the sensor can be directly applied to untreated human serum with a minimal sample volume requirement of only 1 μL. The simultaneous detection of miRNAs in clinical serum samples from healthy individuals and BC patients was carried out. The results show that the average relative expression levels of miRNA-21, miRNA-155 and miRNA-10b in the BC patient group were 12.18 ± 3.20, 17.27 ± 2.17 and 12.17 ± 1.59 times that of the healthy group, respectively. Therefore, the developed multi-detection strategy can precisely identify these cancer biomarkers and offer a crucial pathway for minimally invasive cancer diagnostics, cancer prevention, early intervention and treatment.
微RNA(miRNA)在转录后基因表达中起着至关重要的作用,并在体内自由循环。miRNA 信号传导失调与多种疾病有关,包括乳腺癌(BC)。来自液体活检的 miRNA 图谱为癌症诊断、预后和监测提供了一种前景广阔的策略。尤其是同时分析多种 miRNA 水平可大大提高癌症诊断的准确性。在这项研究中,光子晶体(PhCs)既是标签又是载体,可对 BC 中过表达的多个 miRNA 靶标进行同步光学检测。这一过程是通过目标相互作用触发无酶放大反应,产生荧光共振能量转移(FRET)来实现的。该方法灵敏度高、序列特异性强,并能检测多个靶标。该传感器对 miRNA-21、miRNA-155 和 miRNA-10b 的检测限分别为 6.36 fM、8.52 fM 和 6.06 fM。此外,该传感器可直接用于未经处理的人体血清,所需样品量极少,仅为 1 μL。研究人员同时检测了健康人和 BC 患者临床血清样本中的 miRNA。结果显示,在 BC 患者组中,miRNA-21、miRNA-155 和 miRNA-10b 的平均相对表达水平分别是健康组的 12.18 ± 3.20 倍、17.27 ± 2.17 倍和 12.17 ± 1.59 倍。因此,所开发的多重检测策略可精确识别这些癌症生物标志物,为微创癌症诊断、癌症预防、早期干预和治疗提供了重要途径。
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引用次数: 0
Optimized few-layer MoS2 confined in carbon bowls via pore filling and chemical bond enabling fast kinetics for high-rate potassium storage 通过孔隙填充和化学键将优化的少层 MoS2 限制在碳碗中,从而实现高速钾存储的快速动力学效应
IF 15.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2024-11-19 DOI: 10.1016/j.cej.2024.157821
Lei Yang, Xinyu Wang, Chunliu Zhu, Haozhi Wang, Jing Shi, Jingwei Chen, Weiqian Tian, Yue Zhu, Minghua Huang, Jingyi Wu, Huanlei Wang
Molybdenum sulfide (MoS2) is a prospective anode material for potassium-ion batteries, owing to its large interlayer spacing and superior theoretical capacity. Nevertheless, its practical application is hindered by sluggish kinetics and inferior structural stability, which limit its potassium storage performance. Herein, we employ hollow hard-soft carbon bowls (HSCB), consisting of soft carbon uniformly coated on hard carbon bowls, as nanoreactors to confine few-layered MoS2 nanosheets. The mesoporous carbon shells of HSCB enhance electrolyte penetration and enable rapid charge transfer and robust structural protection, while the mechanical coupling induced by pore filling, alongside the exist of Csingle bondSsingle bondMo chemical bonds, further reinforces the structural integrity of MoS2. Additionally, the creation of few-layered MoS2 structures and MoS2/carbon heterostructures promotes efficient K-ion adsorption and diffusion. Notably, there is a strong linear relationship between MoS2 content and electrochemical performance, including initial Coulomb efficiency, rate performance, and reaction kinetics. Consequently, the optimized MoS2/HSCB anode demonstrating a superior reversible capacity of 630 mAh g−1 at 0.1 A g−1, an exceptional rate capacity of 251 mAh g−1 at 10 A g−1, and excellent cycling stability, retaining 369 mAh g−1 at 0.5 A g−1 after 700 cycles. Remarkably, a potassium-ion hybrid capacitor assembled with MoS2/HSCB anode achieves superior energy/power densities of 122 Wh kg−1/11266 W kg−1, along with splendid capacity retention of 89.5 % after 5000 cycles. This work not only offers an innovative approach for the structural engineering of high-performance sulfide-based composite materials but also elucidates the impact of sulfide content on electrochemical performance.
硫化钼(MoS2)层间距大,理论容量高,是钾离子电池的理想阳极材料。然而,其缓慢的动力学和较差的结构稳定性限制了它的储钾性能,从而阻碍了它的实际应用。在此,我们采用由均匀涂覆在硬碳碗上的软碳组成的空心硬-软碳碗(HSCB)作为纳米反应器来限制少层 MoS2 纳米片。HSCB 的介孔碳壳可增强电解质的渗透性,实现快速电荷转移和稳健的结构保护,而孔隙填充引起的机械耦合以及 CSMo 化学键的存在,则进一步加强了 MoS2 的结构完整性。此外,少层 MoS2 结构和 MoS2/carbon 异质结构的形成促进了 K 离子的有效吸附和扩散。值得注意的是,MoS2 含量与电化学性能(包括初始库仑效率、速率性能和反应动力学)之间存在很强的线性关系。因此,优化后的 MoS2/HSCB 阳极在 0.1 A g-1 电流条件下的可逆容量高达 630 mAh g-1,在 10 A g-1 电流条件下的速率容量高达 251 mAh g-1,而且循环稳定性极佳,在 0.5 A g-1 电流条件下循环 700 次后仍能保持 369 mAh g-1。值得注意的是,与 MoS2/HSCB 阳极组装的钾离子混合电容器实现了 122 Wh kg-1/11266 W kg-1 的卓越能量/功率密度,以及 5000 次循环后 89.5 % 的出色容量保持率。这项工作不仅为高性能硫化物基复合材料的结构工程提供了一种创新方法,还阐明了硫化物含量对电化学性能的影响。
{"title":"Optimized few-layer MoS2 confined in carbon bowls via pore filling and chemical bond enabling fast kinetics for high-rate potassium storage","authors":"Lei Yang, Xinyu Wang, Chunliu Zhu, Haozhi Wang, Jing Shi, Jingwei Chen, Weiqian Tian, Yue Zhu, Minghua Huang, Jingyi Wu, Huanlei Wang","doi":"10.1016/j.cej.2024.157821","DOIUrl":"https://doi.org/10.1016/j.cej.2024.157821","url":null,"abstract":"Molybdenum sulfide (MoS<sub>2</sub>) is a prospective anode material for potassium-ion batteries, owing to its large interlayer spacing and superior theoretical capacity. Nevertheless, its practical application is hindered by sluggish kinetics and inferior structural stability, which limit its potassium storage performance. Herein, we employ hollow hard-soft carbon bowls (HSCB), consisting of soft carbon uniformly coated on hard carbon bowls, as nanoreactors to confine few-layered MoS<sub>2</sub> nanosheets. The mesoporous carbon shells of HSCB enhance electrolyte penetration and enable rapid charge transfer and robust structural protection, while the mechanical coupling induced by pore filling, alongside the exist of C<img alt=\"single bond\" src=\"https://sdfestaticassets-us-east-1.sciencedirectassets.com/shared-assets/55/entities/sbnd.gif\" style=\"vertical-align:middle\"/>S<img alt=\"single bond\" src=\"https://sdfestaticassets-us-east-1.sciencedirectassets.com/shared-assets/55/entities/sbnd.gif\" style=\"vertical-align:middle\"/>Mo chemical bonds, further reinforces the structural integrity of MoS<sub>2</sub>. Additionally, the creation of few-layered MoS<sub>2</sub> structures and MoS<sub>2</sub>/carbon heterostructures promotes efficient K-ion adsorption and diffusion. Notably, there is a strong linear relationship between MoS<sub>2</sub> content and electrochemical performance, including initial Coulomb efficiency, rate performance, and reaction kinetics. Consequently, the optimized MoS<sub>2</sub>/HSCB anode demonstrating a superior reversible capacity of 630 mAh g<sup>−1</sup> at 0.1 A g<sup>−1</sup>, an exceptional rate capacity of 251 mAh g<sup>−1</sup> at 10 A g<sup>−1</sup>, and excellent cycling stability, retaining 369 mAh g<sup>−1</sup> at 0.5 A g<sup>−1</sup> after 700 cycles. Remarkably, a potassium-ion hybrid capacitor assembled with MoS<sub>2</sub>/HSCB anode achieves superior energy/power densities of 122 Wh kg<sup>−1</sup>/11266 W kg<sup>−1</sup>, along with splendid capacity retention of 89.5 % after 5000 cycles. This work not only offers an innovative approach for the structural engineering of high-performance sulfide-based composite materials but also elucidates the impact of sulfide content on electrochemical performance.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"7 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142673747","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Enhancement of organic pollutant degradation in soil with dielectric barrier discharge plasma and MnFe2O4 catalyst: Performance and mechanism 利用介质阻挡放电等离子体和 MnFe2O4 催化剂增强土壤中有机污染物的降解:性能和机理
IF 15.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2024-11-19 DOI: 10.1016/j.cej.2024.157737
Mengye Jin, Tao Zhu, Yusheng Liu, Weifang Li
The Dielectric Barrier Discharge plasma (DBD)-catalyst system holds promise for soil decontamination, but catalyst recycling is still challenging. In this study, a MnFe2O4 catalyst with recyclability and redox properties was prepared and applied in a DBD system to remove phenanthrene (Phe) from soil. The redox reaction in the MnFe2O4 improved the synthesis of reactive oxygen species (ROS), boosting Phe degradation from 80.21 % to 90.21 % within 5 min, with the corresponding kinetic constants was 1.4 and 2.1 times higher than DBD alone. After four recycling cycles, the Phe removal efficiency remained at 88.7 %. Based on the experiment results, the synergistic effect between DBD and MnFe2O4 induced oxygen vacancy formation and accelerated redox reactions, favoring the decomposition of O3 and the degradation of Phe. Furthermore, the Phe degradation pathways were elucidated through the analysis of intermediates in the DBD-MnFe2O4 system. This work provides new insight for developing soil remediation systems with environmentally friendly and high efficiency.
介质阻挡放电等离子体(DBD)-催化剂系统有望用于土壤净化,但催化剂的回收利用仍具有挑战性。本研究制备了一种具有可回收性和氧化还原特性的 MnFe2O4 催化剂,并将其应用于 DBD 系统,以去除土壤中的菲。MnFe2O4 中的氧化还原反应改善了活性氧(ROS)的合成,在 5 分钟内将菲的降解率从 80.21% 提高到 90.21%,相应的动力学常数分别是单独 DBD 的 1.4 倍和 2.1 倍。经过四个循环后,Phe 的去除率仍为 88.7%。实验结果表明,DBD 和 MnFe2O4 的协同作用诱导了氧空位的形成,加速了氧化还原反应,有利于 O3 的分解和 Phe 的降解。此外,通过分析 DBD-MnFe2O4 系统中的中间产物,还阐明了 Phe 的降解途径。这项研究为开发环保、高效的土壤修复系统提供了新的思路。
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引用次数: 0
Nepenthes-inspired saliva-amassing low-dosed risk-factor alerted detecting (SALAD) mouthguard for forewarning of the intraoral cancer 由尼泊金斯启发的唾液低剂量风险因素警报检测(SALAD)护齿器,用于口腔内癌症预警
IF 15.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2024-11-19 DOI: 10.1016/j.cej.2024.157802
Yuan Liu, Xiuli Chen, Guanyue Li, Jiarong Xu, Qi Zeng, Rengui Xu, Yusheng Gong, Wei Chen
Oral cancers pose a significant challenge to global public health with devastating incidence and poor prognosis, highlighting the urgent need for early detection and intervention. Herein, inspired by the unique water-collecting structure (peristome) of the Nepenthes pitcher plant, an innovative saliva-amassing low-dosed risk-factor alerted detecting (SALAD) system was integrated into the wearable mouthguard for in situ, specific, and sensitive detection of tumor necrosis factor-alpha (TNF-α) in saliva, serving as a potential early indicator for oral cancers. This system employed an efficient liquid amassing (LA) module to collect and immobilize intraoral biomarkers in dynamic and complex saliva environments. Moreover, the Aggregation-Induced Emission (AIE)-related fluorescent signal was activated directly in the center of the mouthguard in conjunction with a household UV lamp, simplifying the detection process and amplifying the visibility of the diagnostic readings. Encouragingly, the SALAD mouthguard demonstrated exceptional capability in detecting target biomarkers in simulated intraoral environments. Promisingly, it received highly positive support from the volunteers who underwent preliminary testing with the SALAD mouthguard. Overall, validated by numerous simulated and realistic in vitro and in vivo tests, the SALAD mouthguard was demonstrated to act as a promising candidate for forewarning of oral cancer, highlighting potential for clinical translation and improving patient care experiences.
口腔癌的发病率高、预后差,是全球公共卫生面临的重大挑战,因此迫切需要早期检测和干预。在本文中,受莲雾草(Nepenthes pitcher plant)独特的集水结构(peristome)的启发,一种创新的唾液聚集低剂量风险因素警报检测(SALAD)系统被集成到可穿戴护齿中,用于原位、特异、灵敏地检测唾液中的肿瘤坏死因子-α(TNF-α),作为口腔癌的潜在早期指标。该系统采用了高效的液体聚集(LA)模块,可在动态和复杂的唾液环境中收集和固定口腔内生物标记物。此外,与聚合诱导发射(AIE)相关的荧光信号直接在护齿中心与家用紫外线灯结合激活,简化了检测过程并提高了诊断读数的可见度。令人鼓舞的是,SALAD 护齿在模拟口腔内环境中检测目标生物标记物方面表现出了卓越的能力。令人欣慰的是,使用 SALAD 护齿进行初步测试的志愿者对它给予了高度肯定。总之,经过大量模拟和真实的体外和体内测试验证,SALAD 护齿被证明是一种很有前途的口腔癌预警候选产品,具有临床转化和改善患者护理体验的潜力。
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引用次数: 0
Does the active surface area determine the activity of silica supported nickel catalysts in CO2 methanation reaction? 活性表面积是否决定了二氧化硅支撑镍催化剂在二氧化碳甲烷化反应中的活性?
IF 15.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2024-11-19 DOI: 10.1016/j.cej.2024.157827
Karolina Karpińska-Wlizło, Witold Zawadzki, Grzegorz Słowik, Wojciech Gac
Two series of silica supported catalysts with comparable nickel contents varying from 2.5 to 20 wt% were prepared by wet impregnation method in the absence and presence of citric acid in the impregnation solution. Temperature-programmed reduction, X-ray diffraction and electron microscopy studies indicated changes of reducibility of nickel oxide species in the corresponding catalysts and formation of nickel nanoparticles of different size and morphology. A gradual increase in the performance of catalysts in the CO2 methanation reaction was observed with increasing Ni loading. The application of a modified impregnation method led to a reduction in the size of the nickel crystallites, which increased the active surface area of the catalysts, improving their activity and selectivity towards methane at low temperatures, as well as their stability at high temperatures. It was shown that the high active surface area of silica-supported nickel catalysts, due to the presence of small crystallites, is a key factor in increasing their activity, pointing out that other catalyst properties may also play an important role. Hydrogen temperature-programmed desorption and in-situ DRIFTS adsorption/desorption of CO, CO2 and CO2 hydrogenation reaction studies indicated that modification of the method of catalyst synthesis led to changes in the surface properties of the catalysts, affecting the way CO2 and H2 activation and the transformation of resulted intermediate species to the final reaction products
在浸渍溶液中柠檬酸不存在和存在的情况下,通过湿浸渍法制备了两个系列的二氧化硅支撑催化剂,其镍含量从 2.5 wt% 到 20 wt% 不等。温度编程还原、X 射线衍射和电子显微镜研究表明,相应催化剂中氧化镍物种的还原性发生了变化,并形成了不同大小和形态的镍纳米颗粒。随着镍负载量的增加,催化剂在 CO2 甲烷化反应中的性能逐渐提高。改良浸渍法的应用减小了镍晶体的尺寸,从而增加了催化剂的活性表面积,提高了催化剂在低温下的活性和对甲烷的选择性,以及在高温下的稳定性。研究表明,由于存在小晶体,二氧化硅支撑镍催化剂的高活性表面积是提高其活性的关键因素,同时指出催化剂的其他特性也可能起到重要作用。氢气温度编程解吸和原位 DRIFTS 吸附/解吸 CO、CO2 和 CO2 加氢反应研究表明,催化剂合成方法的改变会导致催化剂表面性质的变化,影响 CO2 和 H2 的活化方式以及由此产生的中间产物向最终反应产物的转化。
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引用次数: 0
Tailoring Na2FePO4F nanoparticles as the high-rate capability and Long-life cathode towards fast chargeable sodium-ion full batteries 定制 Na2FePO4F 纳米粒子,作为可快速充电的钠离子全电池的高倍率和长寿命正极
IF 15.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2024-11-19 DOI: 10.1016/j.cej.2024.157784
Weihuang Wang, Shuhui Li, Yixin Jia, Dongqiang Cao, Rui Liu, Zheng Wang, Zicheng Xie, Lantian Zhang, Liangbing Wang
Na2FePO4F (NFPF) with two-dimensional channels for transferring Na ions is considered as the promising cathode material for high-performance sodium-ion batteries (SIBs), while the electrochemical performance in full-cell devices remains unsatisfactory. Here, we developed a method combining high-boiling organic solvents assisted colloidal synthesis (HOS-CS) and subsequent calcination for preparing 20–30 nm of NFPF nanoparticles (NPs) wrapped by conductive carbon as the efficient cathode. HOS-CS demonstrated merits in terms of high utilization of precursors, high synthetic efficiency, and uniform distribution of both sizes and composition of NPs. Impressively, the as-obtained NFPF/C/MWCNTs delivered a reversible capacity up to 118.4 mAh/g at 0.1C. As a bonus, the full-cell configuration fabricated via NFPF/C/MWCNTs cathode and hard carbon (HC) anode demonstrated extraordinary rate capability and cyclic stability. Even at an ultrahigh rate of 10C, 54.7 mAh/g of initial reversible capacity and nearly 80.7 % of capacity retention after 200 cycles were achieved, highlighting the great potentials of NFPF/C/MWCNTs||HC full cell for practical applications in the fields of fast chargeable SIBs. This work offers a novel synthetic method for the preparation of efficient NFPF-based cathode.
具有二维钠离子传输通道的 Na2FePO4F(NFPF)被认为是高性能钠离子电池(SIB)的理想正极材料,但其在全电池装置中的电化学性能仍不令人满意。在此,我们开发了一种结合高沸点有机溶剂辅助胶体合成(HOS-CS)和后续煅烧的方法,用于制备导电碳包裹的 20-30 纳米 NFPF 粒子(NPs),作为高效阴极。HOS-CS 具有前驱体利用率高、合成效率高、NPs 大小和成分分布均匀等优点。令人印象深刻的是,获得的 NFPF/C/MWCNT 在 0.1C 时的可逆容量高达 118.4 mAh/g。此外,通过 NFPF/C/MWCNTs 阴极和硬碳(HC)阳极制造的全电池配置还表现出了非凡的速率能力和循环稳定性。即使在 10C 的超高速率下,也能实现 54.7 mAh/g 的初始可逆容量和 200 次循环后近 80.7 % 的容量保持率,这凸显了 NFPF/C/MWCNTs||HC 全电池在快速充电 SIB 领域实际应用的巨大潜力。这项工作为制备基于 NFPF 的高效阴极提供了一种新的合成方法。
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引用次数: 0
Electrospun nanofiber Surface-Modified polyethylene separator for enhanced cycling stability and Low-Temperature performance of Sodium-Ion batteries 用于增强钠离子电池循环稳定性和低温性能的电纺纳米纤维表面改性聚乙烯隔膜
IF 15.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2024-11-19 DOI: 10.1016/j.cej.2024.157803
Bin Li, Yan Liu, Xiaohui Han, Yihao Zhou, Feng Xiao, Wenqi Xian, Yuehuan Chu, Guocong Liu, Zhouguang Lu
Sodium-ion batteries (SIBs) are emerging as promising low-cost and long-cycle energy storage systems. However, the poor wettability of the conventional polyolefin separators with polar electrolytes leads to low ionic conductivity and high battery resistance, causing rapid capacity decay. Herein, we propose using a polyethylene (PE) separator coated with a nanofiber composited of poly(vinylidene fluoride) (PVDF) and Al2O3 filler via electrospinning. Compared to the standard PE separators, this composite separator offers much improved electrolyte wettability, mechanical strength, and electrochemical stability. Electrochemical tests demonstrate that the Na[Ni1/3Fe1/3Mn1/3]O2||hard carbon pouch cells based on the PVDF-Al2O3/PE composite separator exhibit a capacity retention of 95.1% after 800 cycles at 1C. Additionally, the separator significantly enhances low-temperature discharge performance and cycling stability. Characterizations based on Fourier transform infrared spectroscopy, scanning electron microscopy, and X-ray diffraction confirm the successful integration of Al2O3 nanoparticles into the PVDF matrix, resulting in a homogeneously dispersed and well-connected structure, which improves ion transport efficiency and stability, thereby effectively boosting battery performance. This research highlights the potential of PVDF-Al2O3 nanofiber composite separators for advanced SIBs with high reversibility, a wide operating temperature range, and long cycling life.
钠离子电池(SIB)是一种前景广阔的低成本长周期储能系统。然而,传统的聚烯烃隔膜与极性电解质的润湿性较差,导致离子传导性低、电池电阻高,从而造成容量快速衰减。在此,我们建议使用聚乙烯(PE)隔膜,通过电纺丝技术在其表面涂覆由聚偏二氟乙烯(PVDF)和 Al2O3 填料组成的纳米纤维。与标准聚乙烯隔膜相比,这种复合隔膜在电解质润湿性、机械强度和电化学稳定性方面都有很大改进。电化学测试表明,基于 PVDF-Al2O3/PE 复合隔膜的 Na[Ni1/3Fe1/3Mn1/3]O2||| 硬碳袋电池在 1C 下循环 800 次后,容量保持率达到 95.1%。此外,该隔膜还显著提高了低温放电性能和循环稳定性。基于傅立叶变换红外光谱、扫描电子显微镜和 X 射线衍射的表征证实,Al2O3 纳米颗粒成功地融入了 PVDF 基体,形成了均匀分散、连接良好的结构,提高了离子传输效率和稳定性,从而有效提升了电池性能。这项研究凸显了 PVDF-Al2O3 纳米纤维复合隔膜在先进 SIB 方面的潜力,它具有高可逆性、宽工作温度范围和长循环寿命。
{"title":"Electrospun nanofiber Surface-Modified polyethylene separator for enhanced cycling stability and Low-Temperature performance of Sodium-Ion batteries","authors":"Bin Li, Yan Liu, Xiaohui Han, Yihao Zhou, Feng Xiao, Wenqi Xian, Yuehuan Chu, Guocong Liu, Zhouguang Lu","doi":"10.1016/j.cej.2024.157803","DOIUrl":"https://doi.org/10.1016/j.cej.2024.157803","url":null,"abstract":"Sodium-ion batteries (SIBs) are emerging as promising low-cost and long-cycle energy storage systems. However, the poor wettability of the conventional polyolefin separators with polar electrolytes leads to low ionic conductivity and high battery resistance, causing rapid capacity decay. Herein, we propose using a polyethylene (PE) separator coated with a nanofiber composited of poly(vinylidene fluoride) (PVDF) and Al<sub>2</sub>O<sub>3</sub> filler via electrospinning. Compared to the standard PE separators, this composite separator offers much improved electrolyte wettability, mechanical strength, and electrochemical stability. Electrochemical tests demonstrate that the Na[Ni<sub>1/3</sub>Fe<sub>1/3</sub>Mn<sub>1/3</sub>]O<sub>2</sub>||hard carbon pouch cells based on the PVDF-Al<sub>2</sub>O<sub>3</sub>/PE composite separator exhibit a capacity retention of 95.1% after 800 cycles at 1C. Additionally, the separator significantly enhances low-temperature discharge performance and cycling stability. Characterizations based on Fourier transform infrared spectroscopy, scanning electron microscopy, and X-ray diffraction confirm the successful integration of Al<sub>2</sub>O<sub>3</sub> nanoparticles into the PVDF matrix, resulting in a homogeneously dispersed and well-connected structure, which improves ion transport efficiency and stability, thereby effectively boosting battery performance. This research highlights the potential of PVDF-Al<sub>2</sub>O<sub>3</sub> nanofiber composite separators for advanced SIBs with high reversibility, a wide operating temperature range, and long cycling life.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"80 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142670981","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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