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Dual-site Re/In2O3 enables selective hydrodeoxygenation of fatty acids via suppressed decarbonylation 双位点Re/In2O3可通过抑制脱羰作用实现脂肪酸的选择性加氢脱氧
IF 3.7 3区 工程技术 Q2 ENGINEERING, CHEMICAL Pub Date : 2026-03-07 DOI: 10.1002/aic.70304
Xuexue Dong, Benhuan Xu, Jian Tian, Bo Jiang, Yu Deng, Bin Chen, Yixin Li, Gen Li, Guowu Zhan
Selective deoxygenation of fatty acids to diesel-range alkanes without carbon-chain shortening is essential for sustainable biomass upgrading, but high selectivity remains challenging by competing decarbonylation/decarboxylation pathways. Here, a Re/In2O3 featuring Re single atoms and ReO3 clusters was synthesized for the hydrodeoxygenation of stearic acid. In contrast to In2O3, which primarily yields 1-octadecanol (93.1% selectivity) with minimal n-octadecane (1.2% selectivity), the optimized Re/In2O3 catalyst achieves 100% selectivity diesel-range alkanes (>85% n-octadecane). Isotopic labeling, in situ spectroscopy, and kinetic analyses reveal Re-induced synergy: ReO3 enhance H2 dissociation, while Re single atoms promote bidentate adsorption of fatty acids, and oxygen vacancies in In2O3 facilitate selective C–O bond cleavage. This multifunctional synergy suppresses C–C bond scission and significantly lowers the apparent activation energy for hydrodeoxygenation by 36.5 kJ·mol−1. The catalyst exhibits broad applicability across diverse carboxylic acids, including unsaturated and aromatic substrates, underscoring its potential for efficient biomass utilization.
脂肪酸在不缩短碳链的情况下选择性脱氧为柴油链烷烃是可持续生物质升级的必要条件,但由于脱羰/脱羧途径的竞争,高选择性仍然是一个挑战。本文合成了具有Re单原子和ReO3簇的Re/In2O3,用于硬脂酸的加氢脱氧。In2O3主要生成1-十八醇(选择性93.1%)和少量正十八烷(选择性1.2%),而优化后的Re/In2O3催化剂可生成100%选择性柴油烷烃(85%正十八烷)。同位素标记、原位光谱和动力学分析揭示了Re诱导的协同作用:ReO3促进H2解离,而Re单原子促进脂肪酸双齿吸附,In2O3中的氧空位促进选择性C-O键裂解。这种多功能协同作用抑制了C-C键的断裂,显著降低了氢脱氧的表观活化能36.5 kJ·mol−1。该催化剂广泛适用于多种羧酸,包括不饱和和芳香底物,强调了其高效生物质利用的潜力。
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引用次数: 0
Electricity-driven CO2-to-PHB conversion via enriched hydrogen-oxidizing bacterial consortia in a gas-lift bioreactor 在气举式生物反应器中通过富氢氧化菌群实现电力驱动的二氧化碳到phb的转化
IF 3.7 3区 工程技术 Q2 ENGINEERING, CHEMICAL Pub Date : 2026-03-07 DOI: 10.1002/aic.70300
Bingyan Wang, Menglong Zhao, Yuhan Guo, Hong Zhang, Jiahao Cao, Jie Han, Kai Cui, Wenfang Cai, Kun Guo
Coupling water electrolysis with hydrogen-oxidizing bacteria (HOB) fermentation represents a promising strategy for sustainable polyhydroxybutyrate (PHB) production and CO2 mitigation. In this study, a novel PHB-producing HOB consortium dominated by Acinetobacter was selectively enriched in a custom-designed gas-lift bioreactor supplied with electrolytic H2 and O2. The effects of nitrogen limitation, oxygen limitation, and combined nitrogen–oxygen dual limitation on PHB accumulation were systematically investigated. Results demonstrated that oxygen limitation more effectively promoted PHB accumulation compared to nitrogen limitation, while dual limitation yielded the highest PHB content (55.65% of CDW), comparable to pure cultures. Structural and compositional analyses verified successful PHB biosynthesis. Compared with reported pure and engineered strains, the enriched PHB-HOB community exhibited enhanced adaptability, lower cultivation costs, and promising scalability. These findings highlight the potential of mixed HOB consortia as an efficient and sustainable platform for PHB production from CO2, offering valuable insights into electricity-driven carbon capture and biopolymer synthesis.
电解水与氧化细菌(HOB)发酵耦合是一种可持续生产聚羟基丁酸盐(PHB)和减少二氧化碳排放的有前途的策略。在这项研究中,以不动杆菌为主导的新型phb产菌HOB联合体在定制设计的气举生物反应器中选择性富集,并提供电解H2和O2。系统地研究了限氮、限氧和氮氧双限制对PHB积累的影响。结果表明,与氮限制相比,氧限制更有效地促进了PHB的积累,而双重限制产生的PHB含量最高(占CDW的55.65%),与纯培养相当。结构和组成分析证实PHB生物合成成功。与报道的纯菌株和工程菌株相比,富集的PHB-HOB群落表现出更强的适应性、更低的培养成本和良好的可扩展性。这些发现突出了混合HOB联盟作为从二氧化碳中生产PHB的高效和可持续平台的潜力,为电力驱动的碳捕获和生物聚合物合成提供了有价值的见解。
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引用次数: 0
Deciphering viscosity-driven mechanisms governing chaotic flow dynamics and mixing efficiency in micromixers 微混合器中控制混沌流动动力学和混合效率的粘度驱动机制
IF 3.7 3区 工程技术 Q2 ENGINEERING, CHEMICAL Pub Date : 2026-03-07 DOI: 10.1002/aic.70344
Shi-Xiao Wei, Ting-Liang Xie, Shuang-Feng Yin
Understanding how viscosity modulates chaotic dynamics in microfluidic systems has remained elusive, despite its importance for high-viscosity mixing. This study investigates viscosity-dependent chaos and mixing in an oscillating feedback micromixer (OFM) through experiments and simulations. Systematic Reynolds-number correlations reveal that feedback intensity, vorticity, deformation, vortex distortion, and helicity all follow unified inertia-dominated scaling laws, indicating a common chaotic evolution mechanism linked with viscosity. Attractor reconstruction and Lyapunov analysis demonstrate the viscosity tolerance of the chaotic state, showing only a moderate attenuation of chaotic intensity once chaos is established. Within the chaotic regime, multiscale mixing metrics (mixing efficiency and norm, micromixing time) show consistent Reynolds-number-dependent scaling-law behavior, with mixing efficiency and micromixing time sharing an exponent of about 0.25. These results establish a unified viscosity-mediated Reynolds linkage among secondary flows, chaotic advection, and multiscale mixing, clarifying that viscosity primarily shifts the transition threshold while inertially intensified chaos governs mixing performance.
了解粘度如何调节微流体系统中的混沌动力学仍然难以捉摸,尽管它对高粘度混合很重要。本文通过实验和仿真研究了振动反馈微混合器(OFM)中粘度依赖的混沌和混合。系统的雷诺数相关性表明,反馈强度、涡度、变形、涡畸变和螺旋度都遵循统一的惯性主导标度规律,表明了一种与粘度相关的共同混沌演化机制。吸引子重建和Lyapunov分析证明了混沌状态的黏度容忍性,表明一旦混沌建立,混沌强度只有适度的衰减。在混沌状态下,多尺度混合指标(混合效率和范数,微混合时间)表现出一致的雷诺数依赖标度律行为,混合效率和微混合时间共享约0.25的指数。这些结果在二次流、混沌平流和多尺度混合之间建立了统一的粘度介导的雷诺兹联系,阐明了粘度主要改变了过渡阈值,而惯性强化的混沌控制了混合性能。
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引用次数: 0
Silicon-modulated NiFeOOH enables stable oxide-pathway oxygen evolution under high-current-density operation 硅调制的NiFeOOH在高电流密度操作下实现稳定的氧化途径析氧
IF 3.7 3区 工程技术 Q2 ENGINEERING, CHEMICAL Pub Date : 2026-03-07 DOI: 10.1002/aic.70333
Jie Yu, Haolin Cheng, Yan Fu, Jinli Zhang, Jiangjiexing Wu
Stabilizing oxygen evolution catalysts under high-current-density operation remains a key challenge for alkaline water electrolysis, where reaction kinetics, mass transport, and structural degradation are strongly coupled. Herein, we report a SiO2-modified NiFeOOH electrocatalyst that enables sustained oxygen evolution via the oxide path mechanism (OPM) by concurrent regulation of surface structure and electronic states. Silicon incorporation reconstructs surface topography and stabilizes high-valence Ni/Fe active sites, while mitigating gas-bubble accumulation and metal dissolution under demanding conditions. Operando spectroscopic combined with density functional theory calculations reveal that Si modulation lowers the energetic barrier for direct OO coupling along the OPM pathway and suppresses degradation pathways. The catalyst delivers an overpotential of 300 mV at 500 mA·cm−2 with stable operation for over 120 h, achieving overall water splitting at 1.74 and 1.87 V in a membrane flow cell. This works provides engineering insights into stabilizing oxide-pathway electrocatalysis under high-rate electrolysis.
在高电流密度操作下稳定析氧催化剂仍然是碱性电解的关键挑战,因为反应动力学、质量传递和结构降解是紧密耦合的。在此,我们报道了一种二氧化硅修饰的NiFeOOH电催化剂,通过表面结构和电子态的同步调节,通过氧化路径机制(OPM)实现持续的析氧。硅的掺入重建了表面形貌,稳定了高价Ni/Fe活性位点,同时在苛刻的条件下减轻了气泡积聚和金属溶解。Operando光谱结合密度泛函理论计算表明,Si调制降低了沿OPM途径直接O - O耦合的能垒,抑制了降解途径。该催化剂在500 mA·cm−2下提供300 mV的过电位,稳定运行超过120 h,在膜流电池中实现了1.74 V和1.87 V的总体水分解。这项工作为在高速率电解下稳定氧化途径电催化提供了工程见解。
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引用次数: 0
A continuum particle–wall heat transfer model for polydisperse fluidized beds 多分散流化床连续介质颗粒-壁面传热模型
IF 3.7 3区 工程技术 Q2 ENGINEERING, CHEMICAL Pub Date : 2026-03-06 DOI: 10.1002/aic.70338
Yaxiong Yu, Feng Lu, Lin Chai, Jun Xue, Fei Wei, Chenxi Zhang
A continuum particle–wall heat transfer model is essential for continuum simulations of gas–solid fluidized beds, yet models applicable to polydisperse systems remain lacking. In this study, a modified version of the Rong and Horio discrete element method (DEM) particle–fluid–particle/wall heat transfer model was proposed by incorporating particle thermal conductivity. The modified DEM model accurately predicts the effective thermal conductivity in an experimental packed bed. Based on computational fluid dynamics–discrete element method data, a continuum particle–wall heat transfer model was developed for monodisperse systems and successfully extended to polydisperse systems by introducing a volume-averaged particle size. Additionally, a theoretical expression was established to predict the contribution of each particle component to the overall heat transfer coefficient in polydisperse beds. The model predictions agree well with simulation results, especially at relatively low fines contents (<15%). This work provides a reliable particle–wall heat transfer model for continuum simulations of polydisperse fluidized beds.
连续介质颗粒壁传热模型是气固流化床连续介质模拟的必要条件,但目前还缺乏适用于多分散系统的模型。本研究提出了一种改进的Rong and Horio离散元法(DEM)颗粒-流体-颗粒/壁面传热模型,加入了颗粒导热系数。改进的DEM模型能准确地预测实验充填床的有效导热系数。基于计算流体力学-离散元法数据,建立了单分散系统的连续颗粒-壁面传热模型,并通过引入体积平均粒径成功推广到多分散系统。此外,建立了一个理论表达式来预测各颗粒组分对多分散床层总传热系数的贡献。模型预测结果与模拟结果吻合较好,特别是在相对较低的细粒含量(<15%)下。为多分散流化床的连续模拟提供了可靠的颗粒壁传热模型。
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引用次数: 0
Unlocking structure–property relationships in organic dyes with machine learning and statistics 用机器学习和统计学解开有机染料的结构-性质关系
IF 3.7 3区 工程技术 Q2 ENGINEERING, CHEMICAL Pub Date : 2026-03-06 DOI: 10.1002/aic.70318
Hao Wu, Zhiwei Yang, Haoyu Jiang, Qirui Yuan, Liangyin Zhao, Ran Tan, Lichun Dong, Chenyang Lu, Luxi Tan, Guanxin Zhang, Shayu Li
Designing organic dyes with precise spectral properties remains challenging despite their importance in downstream industries. This work introduces a machine learning framework (MMoE-CV, with MAEs <8 nm for absorption and <13 nm for emission) integrated with statistical analysis to uncover interpre- structure–property relationships. Experimental validation with newly synthesized thiadiazole derivatives confirms the model's high accuracy even for de novo compounds. Analysis of a library of 729 dye derivatives demonstrates that substituent effects are strongly modulated by both the parent chromophore scaffold and substitution position. This nuance is often overlooked in traditional design approaches. Statistical analysis reveals quantitative insights into these complex interactions, providing a novel rule framework for dye optimization. This approach bridges predictive power with chemical understanding, accelerating the discovery of functional organic dyes for applications in various areas and offering a new perspective on the integration of artificial intelligence in materials design and industrial implementation.
尽管有机染料在下游工业中具有重要意义,但设计具有精确光谱特性的有机染料仍然具有挑战性。这项工作引入了一个机器学习框架(MMoE-CV,吸收MAEs <;8 nm,发射MAEs <;13 nm)与统计分析相结合,以揭示解释结构-性质关系。新合成的噻二唑衍生物的实验验证证实了该模型即使对新化合物也具有很高的准确性。对729个染料衍生物文库的分析表明,取代基效应受到母体发色团支架和取代位置的强烈调节。这种细微差别在传统的设计方法中经常被忽视。统计分析揭示了对这些复杂相互作用的定量见解,为染料优化提供了新的规则框架。这种方法将预测能力与化学理解联系起来,加速了功能性有机染料在各个领域应用的发现,并为人工智能在材料设计和工业实施中的整合提供了新的视角。
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引用次数: 0
Erosion of granular sediments by submerged impinging jets: Particle size effects and cohesion onset 浸没式冲击射流对颗粒状沉积物的侵蚀:粒径效应和黏聚力的开始
IF 3.7 3区 工程技术 Q2 ENGINEERING, CHEMICAL Pub Date : 2026-03-05 DOI: 10.1002/aic.70336
Ahmad Mohamadiyeh, Jeffrey Peakall, Michael Fairweather, Martyn Barnes, Timothy N. Hunter
This study investigates the erosion behavior and modeling of glass particle beds under impinging jet conditions, with a focus on particle size effects and the onset of cohesion. Ultrasonic profiling is implemented to scan and measure static crater profiles. Results indicate that particle size significantly affects crater dimensions, ring peak formation, and overall crater shape. The smallest glass particles (d50 = 35 μm) studied deviate from the trends in crater size, yield stress, and analytical modeling established using larger particles, indicating the onset of cohesion effects at this small particle size. The standard erosion parameter worked well for modeling cohesionless particles down to a certain size limit, beyond which cohesive forces become significant. A new parameter, Eτ based on particle critical shear stress, is introduced for erosion modeling in this study. The transition to cohesive behavior observed in the smallest glass particles is successfully accounted for using Eτ.
本文研究了冲击射流条件下玻璃颗粒床的侵蚀行为和模型,重点研究了颗粒尺寸效应和黏聚的发生。采用超声剖面法对静态弹坑剖面进行扫描和测量。结果表明,颗粒大小显著影响陨石坑尺寸、环峰形成和整体陨石坑形状。最小的玻璃颗粒(d50 = 35 μm)偏离了弹坑尺寸、屈服应力和使用大颗粒建立的分析模型的趋势,表明在这个小颗粒尺寸上开始发生粘聚效应。标准侵蚀参数可以很好地模拟小于一定尺寸极限的无黏性颗粒,超过该尺寸极限黏结力就变得显著。本文引入了一个基于颗粒临界剪应力的新参数Eτ用于侵蚀模型。用Eτ成功地解释了在最小玻璃颗粒中观察到的向内聚行为的转变。
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引用次数: 0
Monitoring and control of a continuous, integrated filtration-drying system with in-line mass spectrometry via PharmaPy 通过PharmaPy在线质谱监测和控制连续集成过滤干燥系统
IF 3.7 3区 工程技术 Q2 ENGINEERING, CHEMICAL Pub Date : 2026-03-05 DOI: 10.1002/aic.70291
Inyoung Hur, Daniel Casas-Orozco, Gintaras Reklaitis, Zoltan K. Nagy
This article demonstrates the integration of in-line mass spectrometry as a process analytical technology (PAT) tool with model-based soft sensors in a continuous filtration-drying carousel system for solid–liquid separation (SLS) of crystal slurries. A hybrid monitoring framework, combining real-time PAT data and model-based soft sensors via moving horizon estimation, is used to optimize process parameters and mitigate disturbances. Two disturbance scenarios—variations in critical material attributes and control variable changes—are investigated. The framework successfully monitors process disturbances and adjusts control variables to achieve desired moisture content. Additionally, it provides insights into mass and heat transfer kinetics and, when coupled with a proportional-integral controller, enables online feedback control for improved process performance. This study highlights the potential of the hybrid framework for enhancing control and optimization in continuous SLS processes.
本文展示了在线质谱作为一种过程分析技术(PAT)工具与基于模型的软传感器在连续过滤-干燥旋转系统中的集成,用于晶体浆料的固液分离(SLS)。混合监测框架,结合实时PAT数据和基于模型的软传感器通过移动水平估计,用于优化工艺参数和减轻干扰。研究了两种干扰情景——关键材料属性的变化和控制变量的变化。该框架成功地监测过程干扰和调整控制变量,以达到所需的水分含量。此外,它提供了对质量和传热动力学的见解,当与比例积分控制器相结合时,可以实现在线反馈控制,以提高过程性能。该研究强调了混合框架在增强连续SLS过程控制和优化方面的潜力。
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引用次数: 0
Continuous and rapid manufacturing of ultrathin zeolite membranes with exceptional gas separation performance 连续快速制造具有优异气体分离性能的超薄沸石膜
IF 3.7 3区 工程技术 Q2 ENGINEERING, CHEMICAL Pub Date : 2026-03-05 DOI: 10.1002/aic.70321
Haolin Wu, Hongbin Liu, Bin Wang, Fan Wang, Amr F. M. Ibrahim, Miao Yu, Shenglai Zhong, Weihong Xing, Rongfei Zhou
The industrial application of microporous crystalline membranes for gas separation has been persistently hindered by the inefficiency of conventional batch synthesis. To address this limitation, we reported a continuous and ultrafast synthesis (CUS) strategy that enables the efficient production of ultrathin b-oriented MFI and SSZ-13 zeolite membranes in just 10–15 min. The resulting MFI and SSZ-13 membranes exhibited superior separation performance in n-butane/i-butane and CO2/N2 mixtures, respectively, far exceeding those of previously reported membranes. Remarkably, the CUS process achieved a two-order-of-magnitude reduction in synthesis time, a 95% decrease in energy consumption and a 98% reduction in gel consumption compared to the batch process. Process simulation using Aspen Plus confirmed that energy consumption was reduced by over 87.6% with membrane separation compared to conventional distillation for butane isomer separation. This work establishes an efficient, scalable, and economically viable pathway for industrial-scale fabrication of zeolite membranes for gas separation.
传统间歇式合成的低效率一直阻碍着微孔晶体膜用于气体分离的工业应用。为了解决这一限制,我们报道了一种连续和超快合成(CUS)策略,可以在10-15分钟内高效地生产超薄b取向MFI和SSZ-13沸石膜。所制备的MFI膜和SSZ-13膜分别在正丁烷/正丁烷和CO2/N2混合物中表现出优异的分离性能,远远超过之前报道的膜。值得注意的是,与间歇式工艺相比,CUS工艺的合成时间缩短了两个数量级,能耗降低了95%,凝胶消耗降低了98%。使用Aspen Plus进行的过程模拟证实,与传统蒸馏分离丁烷异构体相比,膜分离的能耗降低了87.6%以上。这项工作为工业规模的气体分离沸石膜制造建立了一个高效、可扩展和经济可行的途径。
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引用次数: 0
Green synthesis of aminated lignin via biocatalytic pathway for removal of Cu(II) from wastewater 生物催化途径绿色合成胺化木质素去除废水中Cu(II)
IF 3.7 3区 工程技术 Q2 ENGINEERING, CHEMICAL Pub Date : 2026-03-05 DOI: 10.1002/aic.70320
Zhiyi Huang, Pingxian Feng, Xiao Wu, Yaru Luo, Hui Luo, Wei Liu, Wei Wang, Huan Wang
The amination of lignin is crucial for its high-value utilization, but conventional chemical methods suffer from low selectivity and environmental drawbacks. Here, the amination of industrial alkali lignin was achieved for the first time via a biocatalytic pathway. A cascade catalytic system was constructed based on the mechanistic analysis of lignin model compounds. Aryl alcohol oxidase (AAO) selectively oxidizes hydroxyl groups, while ω-transaminase (ω-TA) mediates the transamination of aldehyde groups. The –NH2 group ratio in nitrogen reached 93.63% in bio-aminated lignin (EAL1), reflecting a ~9% increase over chemically aminated lignin (AAL1). The enzymatic pathway enabled efficient and selective amination, avoiding byproducts and structural damage from traditional Mannich reactions. Notably, EAL1 exhibited 100% removal efficiency under the experimental conditions for low-concentration Cu(II) solution via amino-coordination chemisorption, as verified by density functional theory (DFT) calculations. This study presents a novel approach for green functionalization of lignin, demonstrating potential applications in wastewater treatment.
木质素的胺化是木质素高价值利用的关键,但传统的化学方法存在选择性低和环境缺陷。本研究首次通过生物催化途径实现了工业碱木质素的胺化。在分析木质素模型化合物机理的基础上,构建了木质素级联催化体系。芳香醇氧化酶(AAO)选择性氧化羟基,而ω-转氨酶(ω-TA)介导醛基的转氨化。生物胺化木质素(EAL1)的氮中-NH2基团比达到93.63%,比化学胺化木质素(AAL1)提高了约9%。酶途径实现了高效和选择性胺化,避免了传统曼尼希反应的副产物和结构破坏。值得注意的是,在实验条件下,EAL1通过氨基配位化学吸附对低浓度Cu(II)溶液的去除效率为100%,这得到了密度泛函理论(DFT)计算的验证。本研究提出了一种新的木质素绿色功能化方法,展示了木质素在废水处理中的潜在应用。
{"title":"Green synthesis of aminated lignin via biocatalytic pathway for removal of Cu(II) from wastewater","authors":"Zhiyi Huang, Pingxian Feng, Xiao Wu, Yaru Luo, Hui Luo, Wei Liu, Wei Wang, Huan Wang","doi":"10.1002/aic.70320","DOIUrl":"https://doi.org/10.1002/aic.70320","url":null,"abstract":"The amination of lignin is crucial for its high-value utilization, but conventional chemical methods suffer from low selectivity and environmental drawbacks. Here, the amination of industrial alkali lignin was achieved for the first time via a biocatalytic pathway. A cascade catalytic system was constructed based on the mechanistic analysis of lignin model compounds. Aryl alcohol oxidase (AAO) selectively oxidizes hydroxyl groups, while ω-transaminase (ω-TA) mediates the transamination of aldehyde groups. The –NH<sub>2</sub> group ratio in nitrogen reached 93.63% in bio-aminated lignin (EAL1), reflecting a ~9% increase over chemically aminated lignin (AAL1). The enzymatic pathway enabled efficient and selective amination, avoiding byproducts and structural damage from traditional Mannich reactions. Notably, EAL1 exhibited 100% removal efficiency under the experimental conditions for low-concentration Cu(II) solution via amino-coordination chemisorption, as verified by density functional theory (DFT) calculations. This study presents a novel approach for green functionalization of lignin, demonstrating potential applications in wastewater treatment.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"6 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2026-03-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147360056","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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
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