Mass transfer

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  • 文章类型: Journal Article
    电氧化(EO)技术在废水处理中显示出巨大的潜力。然而,高能耗已成为阻碍其大规模实施的关键制约因素。在这里,我们设计了EO和4电子氧还原反应耦合系统(EO-4eORR)来取代传统的EO和氢析出反应(HER)耦合系统(EO-HER)。电解反应器的理论阴极电位从0V(vs.RHE)在她的1.23V(与RHE)在4eORR中,这大大降低了电抗器所需的工作电压。此外,我们证明了对流可以改善反应系统中氧气和有机污染物的传质,导致低阴极极化和高污染物去除率。与传统的EO-HER系统相比,EO-4eORR系统在空气曝气下去除95%总有机碳(TOC)的能耗大大降低至2.61kWh/kgTOC(仅考虑电解槽能耗),这优于以前报道的基于EO的水处理系统。本研究报告的结果为开发高效和可持续的基于EO的处理系统以去除废水中的有机污染物提供了一种新的技术模式。
    Electro-oxidation (EO) technology demonstrates significant potential in wastewater treatment. However, the high energy consumption has become a pivotal constraint hindering its large-scale implementation. Herein, we design an EO and 4-electron oxygen reduction reaction coupled system (EO-4eORR) to replace the traditional EO and hydrogen evolution reaction (HER) coupled system (EO-HER). The theoretical cathodic potential of the electrolytic reactor is tuned from 0 V (vs. RHE) in HER to 1.23 V (vs. RHE) in 4eORR, which greatly decreases the required operation voltage of the reactor. Moreover, we demonstrate that convection can improve the mass transfer of oxygen and organic pollutants in the reaction system, leading to low cathodic polarization and high pollutant removal rate. Compared with traditional EO-HER system, the energy consumption of the EO-4eORR system under air aeration for 95% total organic carbon (TOC) removal is greatly decreased to 2.61 kWh/kgTOC (only consider the electrolyzer energy consumption), which is superior to previously reported EO-based water treatment systems. The reported results in this study offer a new technical mode for development of highly efficient and sustainable EO-based treatment systems to remove organic pollutants in waste water.
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  • 文章类型: Journal Article
    人们广泛关注用于水净化的电活性细菌(EAB)的胞外电子转移(EET)过程,但其功效在复杂的环境基质中往往受到阻碍。在这项研究中,具有EET能力的工程生活材料(e-ELM)首次使用三维(3D)生物打印平台使用定制的几何结构进行污染物去除。通过结合EAB和定制的粘弹性基质,一种用于3D生物打印的生物相容性和可调的电活性生物墨水最初被开发出来,具有调谐的流变特性,能够对微生物的空间排列和密度进行细致的操纵。然后通过在3D打印过程中调整长丝直径和取向来设计和构建具有不同空间微结构的e-ELM。扩散和流体动力学的模拟共同展示了具有不同空间微结构的e-ELM的内部传质速率和EET效率,为出色的去污性能做出贡献。我们的研究推动3D生物打印技术进入环境领域,能够创建设计复杂的e-ELM,并提供有希望的路线来解决新出现的水污染问题。
    Attention is widely drawn to the extracellular electron transfer (EET) process of electroactive bacteria (EAB) for water purification, but its efficacy is often hindered in complex environmental matrices. In this study, the engineered living materials with EET capability (e-ELMs) were for the first time created with customized geometric configurations for pollutant removal using three-dimensional (3D) bioprinting platform. By combining EAB and tailored viscoelastic matrix, a biocompatible and tunable electroactive bioink for 3D bioprinting was initially developed with tuned rheological properties, enabling meticulous manipulation of microbial spatial arrangement and density. e-ELMs with different spatial microstructures were then designed and constructed by adjusting the filament diameter and orientation during the 3D printing process. Simulations of diffusion and fluid dynamics collectively showcase internal mass transfer rates and EET efficiency of e-ELMs with different spatial microstructures, contributing to the outstanding decontamination performances. Our research propels 3D bioprinting technology into the environmental realm, enabling the creation of intricately designed e-ELMs and providing promising routes to address the emerging water pollution concerns.
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  • 文章类型: English Abstract
    Understanding the mass transfer behaviors in hollow fiber membrane module of artificial liver is important for improving toxin removal efficiency. A three-dimensional numerical model was established to study the mass transfer of small molecule bilirubin and macromolecule bovine serum albumin (BSA) in the hollow fiber membrane module. Effects of tube-side flow rate, shell-side flow rate, and hollow fiber length on the mass transfer of bilirubin and BSA were discussed. The simulation results showed that the clearance of bilirubin was significantly affected by both convective and diffusive solute transport, while the clearance of macromolecule BSA was dominated by convective solute transport. The clearance rates of bilirubin and BSA increasd with the increase of tube-side flow rate and hollow fiber length. With the increase of shell-side flow rate, the clearance rate of bilirubin first rose rapidly, then slowly rose to an asymptotic value, while the clearance rate of BSA gradually decreased. The results can provide help for designing structures of hollow fiber membrane module and operation parameters of clinical treatment.
    了解人工肝中空纤维膜组件传质行为对其高效解毒具有重要指导意义。建立了中空纤维膜组件内流动传质的三维数值模拟模型,研究了小分子胆红素与大分子牛血清白蛋白(BSA)在组件内的传质行为,讨论了管程流量、壳程流量、中空纤维管长度对胆红素与BSA传质的影响。研究结果表明小分子胆红素的传质方式是对流传质和扩散传质二者兼具,而大分子BSA的传质方式以对流传质为主;胆红素和BSA的清除速率随着管程流量增大而提升,也随着中空纤维管长度增加而提升;随着壳程流量增大,胆红素的清除速率先快速提升再缓慢上升达到渐近值,而BSA的清除速率随壳程流量增大而逐渐减小。研究成果可以为人工肝中空纤维膜组件的结构优化设计和临床操作参数提供依据。.
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  • 文章类型: Journal Article
    合理的多孔传输层(PTL)对于减少质子交换膜水电解槽(PEMWE)中的传质损失至关重要。在这项研究中,实验证明,梯度孔隙率PTL有利于提高电解槽的性能。该研究全面研究了梯度孔隙率PTL结构对PEMWE性能的影响,考虑传质和界面接触。它使用基于实际PTL几何形状的2D数值模型提供了对PTL内的两相(氧气-水)流传输机制的见解。在微观层面,它分析了界面接触如何影响质子和电子传输机制,不仅影响接触电阻,而且影响析氧反应的有效催化位点的数量。实验结果表明,顺式梯度孔隙率PTL在2.2A/cm2下导致9.3%的性能增强。数值模拟表明,氧气传输的驱动因素包括纤维的表面张力和受局部PTL孔隙率影响的压降。进一步的分析表明,在具有顺式梯度孔隙率的PTL的底部区域中较低的氧饱和度有利于催化剂层(CL)中较低的氧覆盖面积,因为较窄的孔隙空间和较高的毛细管压力增加了进入CL的水流路径的数量。总的来说,这项研究为设计用于电解槽的高性能PTL提供了有价值的见解。
    A reasonable porous transport layer (PTL) is crucial to decreasing the mass-transfer loss in proton-exchange membrane water electrolyzers (PEMWEs). In this study, it was experimentally demonstrated that the gradient porosity PTL is beneficial in improving the performance of electrolyzers. The research comprehensively investigates the impact of gradient porosity PTL structures on the performance of the PEMWE, considering mass transfer and interfacial contact. It offers insights into the two-phase (oxygen-water) flow transport mechanisms within the PTLs using a 2D numerical model based on the actual PTL geometry. At the microscopic level, it analyzes how the interfacial contact impacts proton and electron transport mechanisms, affecting not only the contact resistance but also the number of effective catalytic sites for the oxygen evolution reaction. Experimental results demonstrate that the cis-gradient porosity PTL leads to a performance enhancement of 9.3% at 2.2 A/cm2. Numerical simulations reveal that the drivers of oxygen transport include the surface tension of the fibers and the pressure drop influenced by the local PTL porosity. Further analysis indicates that the lower oxygen saturation in the bottom region of the PTL with cis-gradient porosity favors a lower oxygen coverage area in the catalyst layers (CL) since the narrower pore space and higher capillary pressure increase the number of water flow paths into the CL. Overall, this study provides valuable insights for designing high-performance PTLs for use in electrolyzers.
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  • 文章类型: Journal Article
    废水中含有各种有机污染物,对人体健康和环境造成极大危害。一种蛋白质/多糖衍生的气凝胶,即,ICMA,被开发为一种高性能吸附剂,用于同时有效地去除废水中的多种污染物,包括黑素苷(MLE),刚果红(CR),和双氯芬酸(DIC)。金属有机骨架(UiO-66-NH2),作为一个调节因素,显著提高了ICMA的孔隙率和孔体积,提高了对污染物的捕集性能。由于掺入了大量的多胺官能团及其发达的孔结构,ICMA表现出出色的吸附效率。大孔隙度和孔隙体积,和显着的耐热性。对于MLE,ICMA的平衡捕获能力分别为1364、2031和539mg/g,CR,还有DIC,分别,相应的去除效率均超过90%。此外,ICMA可以通过MLE/CR/DIC-桥接相互作用捕获阳离子染料。五个周期后,使用的ICMA仍然可以保持较高的污染物去除率/量,展示了良好的可重用性。经典吸附模型表明,ICMA对污染物的捕获是双层和非均相吸附取向。一个全新的LWAMTM模型表明,吸附传质过程是由外部传质共同决定的,孔隙扩散,和吸附在活性位点上。多重表征表明,污染物在ICMA上的吸附主要是由电荷相互作用促进的,H-键发挥次要作用。量子化学理论模拟进一步提供了有关捕获污染物的原子级机制的见解。Hirshfeld表面分析表明,ICMA在污染物吸附过程中既充当H键受体又充当供体。进行放大和升级吸附以处理实际/模拟废水,为ICMA的工业实施奠定基础。
    Wastewater contains various organic contaminants that pose great hazards to human health and the environment. A protein/polysaccharide-derived aerogel, namely, ICMA, was developed as a high-performance adsorbent for the simultaneous and efficient removal of diverse contaminants from wastewater, including melanoidin (MLE), Congo red (CR), and diclofenac (DIC). Metal organic framework (UiO-66-NH2), as a regulatory factor, significantly improved the porosity and pore volume of the ICMA to enhance the capture performance of contaminants. The ICMA exhibited outstanding adsorption efficiency owing to the incorporation of ample polyamine functional groups and its well-developed pore structure, large porosity and pore volume, and remarkable heat resistance. The equilibrium capture capacities of the ICMA were 1364, 2031, and 539 mg/g for MLE, CR, and DIC, respectively, with corresponding removal efficiencies all exceeding 90%. Furthermore, the ICMA can capture cationic dyes through MLE/CR/DIC-bridging interactions. After five cycles, the used ICMA can still maintain a high contaminant removal rate/amount, demonstrating good reusability. The classic adsorption model showed that the capture of contaminants by the ICMA is a double-layered and heterogeneous adsorption orientation. A brand new LWAMTM model demonstrated that the adsorption mass-transfer process is jointly determined by the external mass conveyance, pore diffusion, and adsorption on the active site. Multiple characterizations indicated that the contaminant adsorption onto the ICMA was mainly facilitated by charge interactions, with H-bonds playing a secondary role. Quantum chemical theory simulations further provide insights into the atomic-level mechanisms involved in the capture of contaminants. Hirshfeld surface analysis revealed that the ICMA functions as both an H-bond acceptor and a donor during contaminant adsorption. Scale-up and upgrade adsorption were performed to treat actual/simulated wastewater, establishing the groundwork for the industrial implementation of the ICMA.
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  • 文章类型: Journal Article
    基于过氧单硫酸盐(PMS)的高级氧化工艺(AOPs),作为一种有前途的水净化技术,由于有限的反应选择性和传质而受到低反应动力学的限制。在这里,我们设计了一种用于PMS活化的流通模式下的纳米约束的FeCo2O4嵌入式陶瓷膜(FeCo2O4-CM)。在纳米通道(3.0-4.7nm)内限制PMS和FeCo2O4增强了吸附相互作用(-7.84eVvs-2.20eV),从而促进传质。纳米限制效应通过调节纳米限制的FeCo2O4-CM中的活性位点转化为εCo(III)来调节从PMS到FeCo2O4-CM的电子转移途径,使选择性地产生1O2。通过动力学溶剂同位素实验和指示性蒽内过氧化物(DPAO2)证实了1O2在纳米约束系统中的主要作用。该系统能够在2.124ms的水力停留时间内100%去除阿特拉津(ATZ),表明速率常数比非约束系统高5个数量级(3.50×103s-1vs0.42min-1)。它还表现出对pH变化(3.3-9.0)和共存物质的强烈复原力,通过一致的100%ATZ去除14天显示出优异的稳定性。这项研究揭示了通过纳米限制效应调节电子转移途径以选择性产生1O2,促进基于PMS的AOPs在环境修复中的实际应用,并有可能将其应用于各种其他AOPs。
    Peroxymonosulfate (PMS)-based advanced oxidation processes (AOPs), as a promising technology for water decontamination, are constrained by low reaction kinetics due to limited reaction selectivity and mass transfer. Herein, we designed a nanoconfined FeCo2O4-embedded ceramic membrane (FeCo2O4-CM) under flow-through pattern for PMS activation. Confining PMS and FeCo2O4 within nanochannels (3.0-4.7 nm) enhanced adsorption interactions (-7.84 eV vs -2.20 eV), thus boosting mass transfer. Nanoconfinement effect regulated electron transfer pathways from PMS to FeCo2O4-CM by modulating the active site transformation to ≡Co(III) in nanoconfined FeCo2O4-CM, enabling selectively generating 1O2. The primary role of 1O2 in the nanoconfined system was confirmed by kinetic solvent isotope experiments and indicative anthracene endoperoxide (DPAO2). The system enabled 100% removal of atrazine (ATZ) within a hydraulic retention time of 2.124 ms, demonstrating a rate constant over 5 orders of magnitude higher than the nonconfined system (3.50 × 103 s-1 vs 0.42 min-1). It also exhibited strong resilience to pH variations (3.3-9.0) and coexisting substances, demonstrating excellent stability indicated by consistent 100% ATZ removal for 14 days. This study sheds light on regulating electron transfer pathways to selectively generate 1O2 through the nanoconfinement effect, boosting the practical application of PMS-based AOPs in environmental remediation and potentially applying them to various other AOPs.
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  • 文章类型: Journal Article
    高氨氮消化已成为限制有机固体废物厌氧消化的关键瓶颈。真空氨气提可同时去除和回收氨氮,近年来引起了很多关注。为了研究参数对效率和传质的影响,五种组合条件(53°C15kPa,60°C20kPa,65°C25kPa,72°C35kPa,和81°C50kPa)进行污泥消化物的氨汽提。结果表明,所有实验组在45分钟内脱去80%的氨氮,但氨传递系数在不同条件下变化,随着沸点温度的升高而增加,在81℃50kPa时达到最大值(39.0mm/hr)。将初始pH值调节至9.5以上后,真空汽提30min的氨氮去除效率在80%以上,并且初始碱度的调节也会影响液体消化液的pH值。发现pH和碱度是影响氨氮解离和去除效率的关键因素,而温度和真空度主要影响氨氮的传质和脱除速度。在真空氨汽提的机理方面,它经历了碱度破坏,pH值增强,氨氮解离,和游离氨去除。在这项研究中,还进行了碱度破坏和氨去除的两阶段实验,这表明两级配置有利于氨的去除。为有机固体废物液体消化产物中的真空氨汽提提供了理论依据和实用技术。
    High ammonia-nitrogen digestate has become a key bottleneck limiting the anaerobic digestion of organic solid waste. Vacuum ammonia stripping can simultaneously remove and recover ammonia nitrogen, which has attracted a lot of attention in recent years. To investigate the parameter effects on the efficiency and mass transfer, five combination conditions (53 °C 15 kPa, 60 °C 20 kPa, 65 °C 25 kPa, 72 °C 35 kPa, and 81 °C 50 kPa) were conducted for ammonia stripping of sludge digestate. The results showed that 80% of ammonia nitrogen was stripped in 45 min for all experimental groups, but the ammonia transfer coefficient varied under different conditions, which increased with the rising of boiling point temperature, and reached the maximum value (39.0 mm/hr) at 81 °C 50 kPa. The ammonia nitrogen removal efficiency was more than 80% for 30 min vacuum stripping after adjusting the initial pH to above 9.5, and adjustment of the initial alkalinity also affects the pH value of liquid digestate. It was found that pH and alkalinity are the key factors influencing the ammonia nitrogen dissociation and removal efficiency, while temperature and vacuum mainly affect the ammonia nitrogen mass transfer and removal velocity. In terms of the mechanism of vacuum ammonia stripping, it underwent alkalinity destruction, pH enhancement, ammonia nitrogen dissociation, and free ammonia removal. In this study, two-stage experiments of alkalinity destruction and ammonia removal were also carried out, which showed that the two-stage configuration was beneficial for ammonia removal. It provides a theoretical basis and practical technology for the vacuum ammonia stripping from liquid digestate of organic solid waste.
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  • 文章类型: Journal Article
    淀粉基食品在肠道中的消化对人体健康很重要。对细节进行建模增强了基本理解和血糖预测准确性。是的,然而,考虑粒度属性的挑战。已提出多尺度消化模型来表征肠尺度和颗粒尺度的传质和水解反应,无缝集成规模间的质量交换。为粒子计算域的收缩和传输制定了特定的网格方案。通过加入额外的血糖相关过程,例如,肠道吸收,已经开发了基于饮食特性的血糖预测系统.基于人类对米饭颗粒的耐受性实验验证了其有效性。基于模型的调查全面揭示了初始大小对消化行为的影响,特别是在酶分布和粒子进化方面。这项工作还证明了模拟颗粒尺度扩散和肠道尺度运输的重要性,一个以前没有探索过的组合。结果表明,忽略前一种机制会导致血糖峰值高估至少50.8%,而忽略后者会导致16.3%的低估。
    The digestion of starch-based foods in the intestinal tract is important for human health. Modeling the details enhances fundamental understanding and glycemic prediction accuracy. It is, however, a challenge to take granular properties into account. A multiscale digestion model has been proposed to characterize mass transfer and hydrolysis reaction at both the intestine and particle scales, seamlessly integrating inter-scale mass exchange. A specific grid scheme was formulated for the shrinkage and transport of the particle computational domain. By incorporating additional glycemic-related processes, e.g., intestinal absorption, a dietary property-based glycemic prediction system has been developed. Its effectiveness was validated based on a human tolerance experiment of cooked rice particles. The model-based investigation comprehensively reveals the impact of initial size on digestion behavior, specifically in terms of enzyme distribution and particle evolution. This work also demonstrates the significance of modeling both particle-scale diffusion and intestine-scale transport, a combination not previously explored. The results indicate that ignoring the former mechanism leads to an overestimation of the glycemic peak by at least 50.8%, while ignoring the latter results in an underestimation of 16.3%.
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  • 文章类型: Journal Article
    在这里,枸杞用碳酸钠(Na2CO3)预处理,然后通过超声辅助空气干燥或微波干燥进行干燥。在干燥条件下研究了枸杞的水分迁移和酚类化学。三维椭球体输水模型,考虑孔隙度和温度波动,是为了探索干燥机理的复杂性而建立的。一般来说,与超声干燥相比,微波干燥促进了内部水的运输。在所有的干燥方法中,240W(MW-240W)的微波干燥表现出最高的De(从7.34×10-9到9.61×10-9m2/s)和kc(6.78×10-4m/s)值。在所有干燥处理的前2s内,枸杞的表面和中心之间的含水量梯度相当高。微波干燥比空气干燥和超声辅助空气干燥处理更早地降低了水含量梯度。此外,在酚类物质之间观察到的大多数相关性,氧化酶活性,细胞壁果胶与既定的理论不一致,强调了枸杞干燥过程中酚类化学的高度非线性性质。本研究为研究枸杞的传质机理提供了三维模型,并分析了干燥过程中多酚的演变规律。
    Herein, goji berries were pretreated with sodium carbonate (Na2CO3) and then dried via ultrasound-assisted air drying or microwave drying. Water migration and phenolic chemistry of goji berries were studied under drying. A three-dimensional ellipsoid water transport model, accounting for porosity and temperature fluctuations, was established to explore the intricacies of the drying mechanism. Generally, microwave drying promoted interior water transport compared to ultrasound drying. Among all the drying methods, microwave drying at 240 W (MW-240 W) exhibited the highest De (from 7.34 × 10-9 to 9.61 × 10-9 m2/s) and kc (6.78 × 10-4 m/s) values. The goji berries received a considerably high water content gradient between its surface and center within the first 2 s of all the drying treatments. Microwave drying diminished the water content gradient earlier than air drying and ultrasound-assisted air drying treatments. Furthermore, most correlations observed among phenolics, oxidase activity, and cell wall pectin did not align with the established theories, highlighting the highly nonlinear nature of phenolic chemistry during goji berry drying. This study provides a three-dimensional model to study the mass transfer mechanism of goji berries and analyzes the evolution of polyphenols during the drying process.
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  • 文章类型: Journal Article
    整体水分解是可持续制氢的有前途的技术,但主要的挑战是从电极表面迅速去除气泡,以增加氢气产量。受天然生物表面的定向流体传输特性的启发,如猪笼草和Morpho蝴蝶的翅膀,在这里证明了一种策略,通过气泡引导电极实现高效的整体水分解,也就是说,各向异性凹槽微/纳米结构多孔电极(GMPE)。GMPE上的梯度凹槽微/纳米结构用作高速气泡传输通道,并具有出色的气泡引导能力。微尺度多孔结构和凹槽图案之间产生的不对称拉普拉斯压力和沿着凹槽图案的浮力的协同效应推动产生的气泡定向扩散,运输,并及时从电极表面脱离。此外,低粘性纳米片阵列有利于减小气泡尺寸和增加气泡释放频率,与微尺度结构协同改善传质。值得注意的是,GMPE在氢/氧析出反应中优于平面微/纳米结构多孔电极(PMPE),GMPE||GMPE显示出比市售RuO2||20wt.%Pt/C。这项工作改善了电极在固-液-气界面的电化学反应中更好的传质和动力学,为设计和制备涉及气体的光电化学电极提供见解。
    Overall water splitting is a promising technology for sustainable hydrogen production, but the primary challenge is removing bubbles from the electrode surface quickly to increase hydrogen production. Inspired by the directional fluid transport properties of natural biological surfaces like Nepenthes peristome and Morpho butterfly\'s wings, here a strategy is demonstrated to achieve highly efficient overall water splitting by a bubble-guidance electrode, that is, an anisotropic groove-micro/nanostructured porous electrode (GMPE). Gradient groove micro/nanostructures on the GMPE serve as high-speed bubble transmission channels and exhibit superior bubble-guidance capabilities. The synergistic effect of the asymmetric Laplace pressure generated between microscale porous structure and groove patterns and the buoyancy along the groove patterns pushes the produced bubbles directionally to spread, transport, and detach from the electrode surface in time. Moreover, the low adhesive nanosheet arrays are beneficial to reduce bubble size and increase bubble release frequency, which cooperatively improve mass transfer with the microscale structure. Notably, GMPE outperforms planar-micro/nanostructured porous electrode (PMPE) in hydrogen/oxygen evolution reactions, with GMPE||GMPE showing better water splitting performance than commercially available RuO2||20 wt.% Pt/C. This work improves electrodes for better mass transfer and kinetics in electrochemical reactions at solid-liquid-gas interfaces, offering insight for designing and preparing gas-involved photoelectrochemical electrodes.
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