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Heat-integrated reactive-extractive distillation with internally integrated preconcentration for energy-efficient separation of multi-azeotropic mixture 内集成预富集热集成反应萃取精馏高效分离多共沸混合物
IF 6.3 3区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-12-10 DOI: 10.1016/j.jtice.2025.106575
Tianshuo Zheng , Qiuyu Wang , Bo Zhang , Jiaxing Zhu
Background: Efficient treatment of multi-azeotropic mixtures such as tetrahydrofuran (THF)/methanol (MeOH)/methyl acetate (MeAc) remains a critical challenge. Reactive-extractive distillation (RED) has recently been developed for separating MeOH/MeAc-containing multi-azeotropes, while exhibiting high energy demands for THF-rich feeds.
Methods: Using THF/MeOH/MeAc as a case study, this study proposes a novel intensified separation strategy for MeOH/MeAc-containing multi-azeotropic systems via combining RED, preconcentration, and heat integration (HI). Two baseline processes, three-column reactive-extractive distillation (TCRED) and extractive-reactive distillation (TCERD) are initially developed. By integrating preconcentration columns (IDC) in extractive and solvent recovery sections, TCRED-IDC and TCERD-IDC configurations are respectively proposed. Subsequently, process optimizations are conducted, followed by HI implementation, yielding the final HITCRED-IDC and HITCERD-IDC as process intensification configurations. Finally, key performance evaluation is used to highlight the proposed RED processes.
Significant finding: HITCRED-IDC and HITCERD-IDC demonstrates superior performance over the corresponding baseline processes, achieving 15.9 % and 27.6 % TAC reductions, 28.4 % and 57.8 % exergy efficiency improvements, and 16.5 % and 25.6 % CO₂ emission reductions. Additionally, all proposed configurations outperform recently reported four-column extractive distillation, with 27.4 %–54.5 % TAC reductions, 22.1 %–55.7 % CO₂ emission reductions, and 295 %–753 % exergy efficiency improvement. This work successfully integrates IDC and HI within RED systems for energy-efficient processing of MeOH/MeAc-containing azeotropic mixtures.
背景:高效处理四氢呋喃(THF)/甲醇(MeOH)/乙酸甲酯(MeAc)等多共沸混合物仍然是一个严峻的挑战。反应萃取精馏(RED)最近被开发用于分离含有MeOH/ meac的多共沸物,同时对富含thf的进料具有高能量需求。方法:以THF/MeOH/MeAc为例,提出了一种结合RED、预富集和热集成(HI)的新型强化分离策略,用于含MeOH/MeAc多共沸体系。最初开发了两个基线工艺,三柱反应萃取精馏(TCRED)和萃取反应精馏(TCERD)。通过整合萃取段和溶剂回收段的预富集柱(IDC),分别提出了TCRED-IDC和TCERD-IDC配置。随后,进行流程优化,然后实施HI,产生最终的HITCRED-IDC和HITCERD-IDC作为流程强化配置。最后,使用关键绩效评估来突出提出的RED过程。重大发现:HITCRED-IDC和HITCERD-IDC在相应的基线过程中表现出卓越的性能,TAC减少15.9%和27.6%,火用效率提高28.4%和57.8%,二氧化碳排放量减少16.5%和25.6%。此外,所有建议的配置都优于最近报道的四柱萃取精馏,TAC减少27.4% - 54.5%,CO₂排放量减少22.1% - 55.7%,火用效率提高295% - 753%。这项工作成功地将IDC和HI集成到RED系统中,用于高效处理含MeOH/ meac的共沸混合物。
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引用次数: 0
Hollow MoS2 nanosphere-decorated halloysite nanotubes for enhanced water-based lubrication 空心二硫化钼纳米球装饰高岭土纳米管,增强水基润滑
IF 6.3 3区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-12-10 DOI: 10.1016/j.jtice.2025.106566
Si-yu Ren , Xiang-li Wen , Zhi-lin Cheng

Background

Despite their superior mechanical properties(wear resistance, heat dissipation, etc.) and environmental friendliness, water-based lubricants have garnered significant attention. However, their low lubricity and weak load-bearing capacity limited their use in many industrial applications. Herein, the hollow nanosphere MoS₂ was successfully fabricated on the surface of HNTs by soft-template method, and the resulting hollow nanosphere-MoS₂/HNTs manifested a cauliflower-like stacked structure and preferable improvement ability of friction and wear resistance.

Methods

The structure and composition of HNS-MoS2/HNTs were determined by a series of characterizations, such as X-ray diffraction(XRD), Fourier transform infrared(FTIR),Raman spectra,Energy dispersive X-ray spectroscopy(EDS),Scanning electron microscope(SEM) and Transmission electron microscope(TEM). The dispersibility of hollow nanosphere-MoS2/HNTs in water was implemented by placing different days and water contact angles. Friction performance of hollow nanosphere-MoS2/HNTs as nanoadditive was tested on an MMW-1 four-ball tester. Morphology and surface roughness of wear track were evaluated via 3D profilometry system and optical micrograph. Worn surface analysis was detected by X-ray Photoelectron Spectroscopy(XPS).
尽管水基润滑剂具有优异的机械性能(耐磨性、散热性等)和环境友好性,但它已经引起了人们的广泛关注。然而,它们的低润滑性和弱承载能力限制了它们在许多工业应用中的使用。采用软模板法在HNTs表面成功制备了空心纳米球MoS 2,得到的空心纳米球MoS 2 /HNTs具有花椰菜状的堆叠结构,具有较好的摩擦耐磨性能。方法采用x射线衍射(XRD)、傅里叶变换红外(FTIR)、拉曼光谱(Raman)、x射线能谱(EDS)、扫描电镜(SEM)和透射电镜(TEM)等一系列表征手段对HNS-MoS2/HNTs的结构和组成进行表征。通过放置不同的日接触角和水接触角,研究了空心纳米球mos2 /HNTs在水中的分散性。在MMW-1四球测试机上测试了空心纳米球- mos2 /HNTs作为纳米添加剂的摩擦性能。利用三维轮廓测量系统和光学显微照片对磨损轨迹的形貌和表面粗糙度进行了评价。用x射线光电子能谱(XPS)对磨损表面进行分析。
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引用次数: 0
Bifunctional acidic carbon catalyst from dragon fruit peel for selective glucose conversion into 5-hydroxymethylfurfural 火龙果皮双功能酸性碳催化剂选择性葡萄糖转化为5-羟甲基糠醛
IF 6.3 3区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-12-10 DOI: 10.1016/j.jtice.2025.106568
Thinh An Tan Le , Vinh Thanh Chau Doan , Phuong Hoang Tran

Background

This study aims to develop a low-cost, eco-friendly carbon-based catalyst for the conversion of glucose into 5-hydroxymethylfurfural (HMF), a valuable biomass-derived platform chemical. The research addresses the need for efficient catalytic systems combining both Brønsted and Lewis acid functionalities.

Methods

Three novel bifunctional carbon catalysts (Al/C-SO3HCl-Y) were synthesized from dragon fruit peel via a hydrothermal process, incorporating –SO3H groups and then AlCl₃ to provide Brønsted and Lewis acid sites, respectively. The catalysts were characterized using FTIR, SEM-EDX elemental mapping, TGA, NH3-TPD, Raman, and XRD analyses. Reaction parameters, including catalyst type, substrate type, solvent, catalyst loading, substrate concentration, temperature, and the role of Lewis acid sites, were systematically investigated. A leaching test and a scale-up experiment were also conducted to assess catalyst stability and practical applicability.

Significant findings

Optimal conditions for HMF production were achieved using 50 mg of Al/C-SO3HCl-2 catalyst in dimethyl sulfoxide (DMSO) at 140 °C for 16 h, yielding 89% HMF. The catalyst demonstrated high efficiency, stability, and potential for scale-up. A catalytic mechanism was proposed based on experimental data, and the results compared favorably with previous studies, confirming the effectiveness of Al/C-SO3HCl-2 as a sustainable catalyst.
本研究旨在开发一种低成本、环保的碳基催化剂,用于将葡萄糖转化为5-羟甲基糠醛(HMF),这是一种有价值的生物质衍生平台化学品。该研究解决了结合Brønsted和Lewis酸功能的高效催化系统的需求。方法以火龙果皮为原料,通过水热法合成了3种新型双功能碳催化剂Al/C-SO3HCl-Y,它们分别由-SO3H基团和AlCl₃构成Brønsted和Lewis酸位。采用FTIR、SEM-EDX元素图、TGA、NH3-TPD、Raman和XRD分析对催化剂进行了表征。系统地研究了反应参数,包括催化剂类型、底物类型、溶剂、催化剂负载、底物浓度、温度和Lewis酸位点的作用。并进行了浸出试验和放大试验,以评估催化剂的稳定性和实际适用性。在二甲亚砜(DMSO)中,使用50 mg Al/C- so3hcl -2催化剂,在140°C下反应16 h,获得了生产HMF的最佳条件,产量为89%。该催化剂具有较高的效率、稳定性和规模化应用潜力。根据实验数据提出了催化机理,并与前人的研究结果进行了比较,证实了Al/C-SO3HCl-2作为可持续催化剂的有效性。
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引用次数: 0
Zn4B6O33/reduced graphene oxide nano architectures for integrated water-splitting and urea-assisted hydrogen production via synergistic bifunctional electrocatalysis Zn4B6O33/还原氧化石墨烯纳米结构通过协同双功能电催化集成水分解和尿素辅助制氢
IF 6.3 3区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-12-09 DOI: 10.1016/j.jtice.2025.106544
Bodicherla Naresh , T.V.M. Sreekanth , Chandra Reddy Niragatti Suma , Kisoo Yoo , Jonghoon Kim

Background

Efficient and sustainable hydrogen production is a critical challenge in renewable energy technologies. Coupling water-splitting with urea oxidation provides a low-energy pathway for hydrogen generation, but conventional catalysts often suffer from limited activity and stability. Developing bifunctional electrocatalysts capable of driving both reactions efficiently is therefore essential for practical hydrogen production.

Methods

A Zn₄B₆O₁₃/reduced graphene oxide (rGO) composite was synthesized via solid-state reaction followed by hydrothermal integration. The incorporation of rGO enhanced surface roughness, crystallinity, and charge-transfer kinetics, as confirmed by SEM, TEM, Raman, XRD, and Rietveld refinement. Electrochemical performance was evaluated using linear sweep voltammetry (LSV), electrochemical impedance spectroscopy (EIS), and electrochemical surface area (ECSA) measurements.

Significant findings

The Zn₄B₆O₁₃/rGO composite exhibited superior bifunctional electrocatalytic activity with reduced overpotentials of 327 mV for the oxygen evolution reaction (OER) and 170 mV for the urea oxidation reaction (UOR), and Tafel slopes of 95.1 mV dec⁻¹ (OER) and 55.8 mV dec⁻¹ (UOR). The ECSA increased from 80 to 110 cm² (OER) and from 97.5 to 125 cm² (UOR), indicating more active sites. Long-term chronoamperometry over 25 h demonstrated excellent durability, while EIS confirmed improved charge-transfer behavior. These results highlight the strong synergistic interaction between Zn₄B₆O₁₃ and rGO, positioning the composite as a cost-effective, durable, and practical catalyst for integrated water-splitting and urea-assisted hydrogen production.
高效和可持续的氢气生产是可再生能源技术面临的关键挑战。耦合水裂解与尿素氧化为制氢提供了低能量途径,但传统催化剂的活性和稳定性往往有限。因此,开发能够有效驱动两种反应的双功能电催化剂对于实际制氢至关重要。方法采用固相反应-水热合成法制备sa Zn₄B₆O₁₃/还原氧化石墨烯(rGO)复合材料。通过SEM, TEM, Raman, XRD和Rietveld精细化证实,rGO的加入增强了表面粗糙度,结晶度和电荷转移动力学。电化学性能通过线性扫描伏安法(LSV)、电化学阻抗谱(EIS)和电化学表面积(ECSA)测量进行评估。4₄B₆O₁₃/rGO复合材料表现出良好的双功能电催化活性,出氧反应(OER)的过电位为327 mV,尿素氧化反应(UOR)的过电位为170 mV, Tafel斜率为95.1 mV dec⁻¹(OER)和55.8 mV dec⁻¹(UOR)。ECSA从80 cm²(OER)增加到110 cm²,从97.5 cm²增加到125 cm²(UOR),表明活性位点增加。超过25小时的长期计时电流测量显示出优异的耐久性,而EIS证实了改进的电荷转移行为。这些结果突出了Zn₄B₆O₁₃和rGO之间的强协同作用,使该复合材料成为一种经济、耐用、实用的综合水裂解和尿素辅助制氢催化剂。
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引用次数: 0
Unraveling the role of oxygen species in Pt/MnO2 catalysts for low-temperature HCHO abatement: A precursor-dependent study 揭示氧在Pt/MnO2催化剂中用于低温HCHO减排的作用:前体依赖研究
IF 6.3 3区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-12-08 DOI: 10.1016/j.jtice.2025.106541
Wei Tong , Jie Yang , Yaxiong Ji , Hongli Wu

Backgrounds

Formaldehyde (HCHO) is a hazardous indoor pollutant requiring efficient low-temperature abatement. Catalytic oxidation effectiveness hinges on active oxygen species generation.

Methods

Pt/δ-MnO2 catalysts were synthesized using five manganese precursors (acetate, sulfate, carbonate, chloride, nitrate) via impregnation-reduction. Catalytic performance was assessed for HCHO oxidation (200–460 ppm, 80,000 mL/(g·h)), with mechanisms probed via in situ DRIFTS, DFT, XPS, EPR, Raman, H2-TPR, SEM, TEM and N2 adsorption-desorption.

Significant findings

Pt/MnO2-S (sulfate-derived) achieved 100 % HCHO conversion at 50 °C (200 ppm, 80,000 mL/(g·h)), outperforming other precursors due to its abundant oxygen vacancies (EPR/XPS) and high metallic Pt° content (55 %, XPS). In situ DRIFTS and DFT calculations revealed that Pt nanoparticles and oxygen vacancies synergistically generate active oxygen species, enabling a dual-path "butterfly mechanism": Under O2-rich conditions, surface radicals (O, OH) dominate oxidation to CO2/H2O; in O2-deficient environments, lattice oxygen participates, accumulating formate intermediates. Pt/MnO2-S exhibited exceptional stability (100 % conversion at 460 ppm for >4 h) and recyclability. The work establishes oxygen vacancy engineering as critical for enhancing Pt-MnO2 interfacial reactivity.
甲醛(HCHO)是一种有害的室内污染物,需要有效的低温减排。催化氧化的效果取决于活性氧的生成。方法以五种锰前驱体(乙酸、硫酸盐、碳酸盐、氯化物、硝酸盐)为原料,通过浸渍还原法制备spt /δ-MnO2催化剂。考察了HCHO氧化(200-460 ppm, 80000 mL/(g·h))的催化性能,并通过原位漂移、DFT、XPS、EPR、拉曼、H2-TPR、SEM、TEM和N2吸附-解吸探讨了机理。spt /MnO2-S(硫酸盐衍生)在50°C (200 ppm, 80,000 mL/(g·h))下实现了100%的HCHO转化,由于其丰富的氧空位(EPR/XPS)和高金属Pt°含量(55%,XPS),优于其他前驱体。原位漂移和DFT计算表明,Pt纳米颗粒和氧空位协同产生活性氧,实现了双程“蝴蝶机制”:在富氧条件下,表面自由基(O, OH)主导氧化生成CO2/H2O;在缺乏o2的环境中,晶格氧参与,积累甲酸酯中间体。Pt/MnO2-S表现出优异的稳定性(在460ppm下4小时转化率100%)和可回收性。这项工作建立了氧空位工程是提高Pt-MnO2界面反应性的关键。
{"title":"Unraveling the role of oxygen species in Pt/MnO2 catalysts for low-temperature HCHO abatement: A precursor-dependent study","authors":"Wei Tong ,&nbsp;Jie Yang ,&nbsp;Yaxiong Ji ,&nbsp;Hongli Wu","doi":"10.1016/j.jtice.2025.106541","DOIUrl":"10.1016/j.jtice.2025.106541","url":null,"abstract":"<div><h3>Backgrounds</h3><div>Formaldehyde (HCHO) is a hazardous indoor pollutant requiring efficient low-temperature abatement. Catalytic oxidation effectiveness hinges on active oxygen species generation.</div></div><div><h3>Methods</h3><div>Pt/δ-MnO<sub>2</sub> catalysts were synthesized using five manganese precursors (acetate, sulfate, carbonate, chloride, nitrate) via impregnation-reduction. Catalytic performance was assessed for HCHO oxidation (200–460 ppm, 80,000 mL/(g·h)), with mechanisms probed via in situ DRIFTS, DFT, XPS, EPR, Raman, H<sub>2</sub>-TPR, SEM, TEM and N<sub>2</sub> adsorption-desorption.</div></div><div><h3>Significant findings</h3><div>Pt/MnO<sub>2</sub>-S (sulfate-derived) achieved 100 % HCHO conversion at 50 °C (200 ppm, 80,000 mL/(g·h)), outperforming other precursors due to its abundant oxygen vacancies (EPR/XPS) and high metallic Pt° content (55 %, XPS). In situ DRIFTS and DFT calculations revealed that Pt nanoparticles and oxygen vacancies synergistically generate active oxygen species, enabling a dual-path \"butterfly mechanism\": Under O<sub>2</sub>-rich conditions, surface radicals (O, OH) dominate oxidation to CO<sub>2</sub>/H<sub>2</sub>O; in O<sub>2</sub>-deficient environments, lattice oxygen participates, accumulating formate intermediates. Pt/MnO<sub>2</sub>-S exhibited exceptional stability (100 % conversion at 460 ppm for &gt;4 h) and recyclability. The work establishes oxygen vacancy engineering as critical for enhancing Pt-MnO<sub>2</sub> interfacial reactivity.</div></div>","PeriodicalId":381,"journal":{"name":"Journal of the Taiwan Institute of Chemical Engineers","volume":"181 ","pages":"Article 106541"},"PeriodicalIF":6.3,"publicationDate":"2025-12-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145733206","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
Effect of transition metals (Co, Ni, Fe) on methanol selective catalytic oxidation performance of CeMOy mixed oxide catalysts 过渡金属(Co, Ni, Fe)对CeMOy混合氧化物催化剂甲醇选择性催化氧化性能的影响
IF 6.3 3区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-12-08 DOI: 10.1016/j.jtice.2025.106565
Junhao Jing , Zhitao Han , Liangzheng Lin , Sihan Yin , Tingjun Liu , Chuanqiu Gao , You Tian , Dong Ma

Background

Methanol selective catalytic oxidation (CH3OH-SCO) is an effective technology for CH3OH removal. However, the development of catalysts with excellent stability, cost-effectiveness, and high activity at low temperatures remains a major challenge in reducing unburned methanol emissions from methanol-fueled engines.

Methods

In this study, CeMOy (M = Co, Ni, Fe) mixed oxide catalysts were synthesized via the sol-gel method and characterized by XRD, XPS, EPR, H2-TPR, O2-TPD, CO2-TPD, and in-situ DRIFTS to investigate the influence of transition metals on CH3OH-SCO performance.

Significant findings

Catalytic activity tests demonstrated that the CeCoOy catalyst exhibited the best performance, achieving 90 % methanol conversion at 173 °C and maintaining complete conversion without detectable byproducts over a broad temperature range (200–450 °C). Furthermore, the CeCoOy catalyst showed excellent stability and sulfur resistance. Characterization analyses revealed that its superior catalytic performance was attributed to the enhanced interfacial effect between CeO2 and Co3O4. In-situ DRIFTS analysis confirmed that methanol oxidation followed the Mars-van Krevelen (MvK) mechanism. This study clarified the role of different transition metals in modulating oxygen vacancies, oxygen species, and basic sites in CeMOy catalysts, providing guidance for the design of efficient and low-cost mixed oxide catalysts.
甲醇选择性催化氧化(CH3OH- sco)是一种有效的脱除CH3OH的技术。然而,开发具有优异稳定性、成本效益和低温高活性的催化剂仍然是减少甲醇燃料发动机未燃烧甲醇排放的主要挑战。方法采用溶胶-凝胶法制备了CeMOy (M = Co, Ni, Fe)混合氧化物催化剂,并采用XRD、XPS、EPR、H2-TPR、O2-TPD、CO2-TPD和原位漂移等手段对催化剂进行了表征,研究过渡金属对CH3OH-SCO性能的影响。催化活性测试表明,CeCoOy催化剂表现出最好的性能,在173°C时达到90%的甲醇转化率,并且在200-450°C的宽温度范围内保持完全转化而无可检测的副产物。此外,该催化剂还具有良好的稳定性和抗硫性能。表征分析表明,其优异的催化性能归因于CeO2与Co3O4之间的界面效应增强。原位漂移分析证实甲醇氧化遵循火星-范-克雷文(MvK)机制。本研究阐明了不同过渡金属对CeMOy催化剂中氧空位、氧种类和碱基的调节作用,为设计高效、低成本的混合氧化物催化剂提供指导。
{"title":"Effect of transition metals (Co, Ni, Fe) on methanol selective catalytic oxidation performance of CeMOy mixed oxide catalysts","authors":"Junhao Jing ,&nbsp;Zhitao Han ,&nbsp;Liangzheng Lin ,&nbsp;Sihan Yin ,&nbsp;Tingjun Liu ,&nbsp;Chuanqiu Gao ,&nbsp;You Tian ,&nbsp;Dong Ma","doi":"10.1016/j.jtice.2025.106565","DOIUrl":"10.1016/j.jtice.2025.106565","url":null,"abstract":"<div><h3>Background</h3><div>Methanol selective catalytic oxidation (CH<sub>3</sub>OH-SCO) is an effective technology for CH<sub>3</sub>OH removal. However, the development of catalysts with excellent stability, cost-effectiveness, and high activity at low temperatures remains a major challenge in reducing unburned methanol emissions from methanol-fueled engines.</div></div><div><h3>Methods</h3><div>In this study, CeMO<em><sub>y</sub></em> (<em>M</em> = Co, Ni, Fe) mixed oxide catalysts were synthesized via the sol-gel method and characterized by XRD, XPS, EPR, H<sub>2</sub>-TPR, O<sub>2</sub>-TPD, CO<sub>2</sub>-TPD, and in-situ DRIFTS to investigate the influence of transition metals on CH<sub>3</sub>OH-SCO performance.</div></div><div><h3>Significant findings</h3><div>Catalytic activity tests demonstrated that the CeCoO<em><sub>y</sub></em> catalyst exhibited the best performance, achieving 90 % methanol conversion at 173 °C and maintaining complete conversion without detectable byproducts over a broad temperature range (200–450 °C). Furthermore, the CeCoO<em><sub>y</sub></em> catalyst showed excellent stability and sulfur resistance. Characterization analyses revealed that its superior catalytic performance was attributed to the enhanced interfacial effect between CeO<sub>2</sub> and Co<sub>3</sub>O<sub>4</sub>. In-situ DRIFTS analysis confirmed that methanol oxidation followed the Mars-van Krevelen (MvK) mechanism. This study clarified the role of different transition metals in modulating oxygen vacancies, oxygen species, and basic sites in CeMO<em><sub>y</sub></em> catalysts, providing guidance for the design of efficient and low-cost mixed oxide catalysts.</div></div>","PeriodicalId":381,"journal":{"name":"Journal of the Taiwan Institute of Chemical Engineers","volume":"181 ","pages":"Article 106565"},"PeriodicalIF":6.3,"publicationDate":"2025-12-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145733207","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
Alkali modification and nitrogen doping synergistically regulate sludge-derived biochar for persulfate activation and organic pollutant degradation 碱改性和氮掺杂协同调节污泥源生物炭的过硫酸盐活化和有机污染物降解
IF 6.3 3区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-12-08 DOI: 10.1016/j.jtice.2025.106569
Yujie Zhang, Shoulong Peng, Siyu Zhang, Jiani Li
Given the increasing organic pollution in industrial wastewater and the disposal risks of municipal sludge, developing advanced oxidation technology based on sludge-derived biochar-activated peroxymonosulfate (PMS) is highly promising. In this study, a series of sludge-derived biochars (SSB) were prepared via alkali modification and nitrogen doping, and their performance and mechanism in activating PMS for the degradation of organic pollutants were systematically investigated. After alkali modification, the surface of biochar becomes much rougher, and meanwhile the functional group C=O appears. After urea doping, the biochar exhibits a more porous characteristic, and the increased nitrogen species can enhance the electron transfer ability. Experimental results demonstrated that the 0.5-SSB-3/PMS reaction system could rapidly oxidize and degrade multiple organic pollutants. Characterization via SEM and BET revealed that the modified biochar has a rough surface and a relatively distinct pore structure, while both its pore size and pore volume are increased. Mechanistic investigations revealed that non-radical singlet oxygen (1O2) served as the dominant reactive species. On the one hand, it is generated by the self-decomposition of PMS; on the other hand, it is generated by the activation of PMS by special structures such as C=O, pyridinic N, and graphitic N. The catalyst maintained high efficiency across a wide pH range (3–9), and the 0.5-SSB-3/PMS system still achieved 90.7% pollutant degradation after five reuse cycles. This study provides valuable insights into the resource utilization of sludge and the degradation of organic pollutants.
鉴于工业废水中有机污染的日益增加和城市污泥的处置风险,开发基于污泥源生物炭活化过氧单硫酸根(PMS)的高级氧化技术是非常有前景的。本研究通过碱改性和氮掺杂制备了一系列污泥源生物炭(SSB),并对其激活PMS降解有机污染物的性能和机理进行了系统研究。碱改性后的生物炭表面变得更加粗糙,同时出现了官能团C=O。尿素掺杂后的生物炭表现出更多孔的特性,增加的氮种可以增强电子传递能力。实验结果表明,0.5-SSB-3/PMS反应体系能够快速氧化降解多种有机污染物。SEM和BET表征表明,改性后的生物炭表面粗糙,孔隙结构相对清晰,孔径和孔体积均有所增大。机理研究表明,非自由基单线态氧(1O2)是主要的反应物质。它一方面是由PMS自分解产生的;另一方面,它是由C=O、吡啶N和石墨N等特殊结构对PMS的活化产生的。催化剂在较宽的pH范围(3-9)内保持了较高的效率,0.5-SSB-3/PMS体系在重复使用5次后仍能达到90.7%的污染物降解率。本研究为污泥资源化利用和有机污染物的降解提供了有价值的见解。
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引用次数: 0
Predictive tuning strategies for different classes of delay dominant chemical processes 不同类型延迟优势化学过程的预测调谐策略
IF 6.3 3区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-12-05 DOI: 10.1016/j.jtice.2025.106570
Prabir Singha , Dipjyoti Das , Sudipta Chakraborty

Background:

Delay-dominant processes are characterized by significant time lags between input actions and output responses. Accounting for these delays is crucial in control design to avoid oscillations and achieve accurate set-point tracking. This study proposes a novel target-loop-based Smith Predictor PID (Proportional-Integral-Derivative) tuning methodology tailored for various delay-dominant systems, including stable, unstable, integrating, double integrating, and inverse response processes.

Methods:

A Stabilizing/ disturbance rejection controller is first designed based on the Maximum Sensitivity (Ms) criterion. Using both stability margin and Ms, a set-point tracking controller is then developed. To further improve performance under plant dynamics variation, a derivative action is introduced in the outer loop.

Significant findings

: Step-by-step design calculations are provided, and the controller’s effectiveness is quantitatively evaluated using error indices such as Integral Square Error (ISE), Integral Time Absolute Error (ITAE), and Integral Absolute Error (IAE). Lastly, the suggested design is experimentally validated with a Two-Tank system setup.
背景:延迟主导过程的特点是输入动作和输出响应之间存在显著的时间滞后。考虑这些延迟在控制设计中是至关重要的,以避免振荡和实现精确的设定点跟踪。本研究提出了一种新的基于目标环的Smith预测器PID(比例-积分-导数)整定方法,适用于各种延迟主导系统,包括稳定、不稳定、积分、双积分和逆响应过程。方法:首先基于最大灵敏度(Ms)准则设计一种稳定/抗扰控制器。利用稳定裕度和Ms,设计了一种设定值跟踪控制器。为了进一步提高在植物动态变化下的性能,外环引入了一个导数作用。重要发现:提供了一步一步的设计计算,并使用误差指标如积分平方误差(ISE)、积分时间绝对误差(ITAE)和积分绝对误差(IAE)对控制器的有效性进行了定量评估。最后,通过双罐系统的实验验证了所建议的设计。
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引用次数: 0
Suppression mechanism of chloride salts-based composite dry water against purified terephthalic acid dust explosion 氯盐基复合干水对净化对苯二甲酸粉尘爆炸的抑制机理
IF 6.3 3区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-12-05 DOI: 10.1016/j.jtice.2025.106561
Qingjun Xia , Yunqiang Wu , Xundong Zhang , Zhengwei Li , Qingwu Zhang , Yajie Bu , Yuan Yu , Juncheng Jiang

Background

The widespread production and utilization of purified terephthalic acid (PTA) dust in the chemical industry pose significant explosion hazards, driving the need for efficient suppression technologies. Composite dry water (DW) suppressants functionalized with abundant and recyclable chloride salts (NaCl, KCl, CaCl2) were developed to address this risk.

Methods

The explosibility of PTA, the suppression effectiveness and mechanism of composite DW were systematically investigated using a 20-L explosion chamber and physicochemical analyses. The pyrolysis characteristics and gaseous species were investigated through thermogravimetry coupled with Fourier transform infrared spectroscopy (TG-FTIR) analysis.

Significant findings

The results confirmed the severe explosibility of PTA, with a maximum explosion pressure (Pmax) of 6.3 bar and deflagration index (KSt) of 116 bar·m·s-1. Its decomposition generated gaseous aromatics and olefins, with subsequent combustion mainly controlled by homogeneous reactions. All composite DW agents significantly reduced the explosion parameters of PTA, outperforming both pure DW and powdered chloride salts, with efficiency enhanced alongside increased additive loading. Notably, KCl-based DW exhibited better performance, achieving complete explosion scavenging at a 40% addition ratio across all its formulations. The suppression mechanism was attributed to a synergistic effect: physical actions involving water evaporation cooling and silica coating that delays pyrolysis, combined with chemical radical scavenging to disrupt combustion chain reactions. These findings affirm that chloride salts-based composite DW, particularly the KCl-modified DW, presents a highly effective and promising strategy for mitigating PTA dust explosion risks in industrial scenarios.
化学工业中广泛生产和使用的纯化对苯二甲酸(PTA)粉尘具有重大的爆炸危险,因此需要高效的抑制技术。为了解决这一问题,研究人员开发了含有大量可回收氯盐(NaCl, KCl, CaCl2)的复合干水(DW)抑制剂。方法采用20 l爆炸室对PTA的爆炸性能、复合DW的抑制效果及机理进行了系统研究和理化分析。采用热重法结合傅里叶变换红外光谱(TG-FTIR)对热解特征和气态组分进行了研究。结果证实了PTA的严重爆炸,最大爆炸压力(Pmax)为6.3 bar,爆燃指数(KSt)为116 bar·m·s-1。其分解生成气态芳烃和烯烃,随后的燃烧主要由均相反应控制。所有复合DW剂都显著降低了PTA的爆炸参数,优于纯DW和粉末状氯化物盐,效率随着添加剂负荷的增加而提高。值得注意的是,kcl基DW表现出更好的性能,在所有配方中添加比例为40%时都能实现完全的爆炸清除。抑制机理归因于协同效应:物理作用包括水蒸发冷却和二氧化硅涂层延迟热解,结合化学自由基清除破坏燃烧链反应。这些研究结果证实,氯盐基复合DW,特别是氯化钾改性DW,在工业场景中是一种非常有效和有前途的降低PTA粉尘爆炸风险的策略。
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引用次数: 0
Engineered miniature CRISPR activation system promotes dodecanedioic acid production in Candida viswanathii 工程微型CRISPR激活系统促进viswanathii念珠菌十二烷二酸的产生
IF 6.3 3区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-12-04 DOI: 10.1016/j.jtice.2025.106548
Nam Ngoc Pham , Chih-Hsuan Chien , Chin-Wei Chang, Yu-Chen Hu

Background

Dodecanedioic acid (DDA) is a valuable monomer with broad industrial applications. The yeast Candida viswanathii can convert dodecane into 12-carbon DDA, making it an attractive host for metabolic engineering toward sustainable production. A recently developed miniature dCasMINI protein, when fused with the VPR activator, enables efficient CRISPR activation (CRISPRa) in mammalian cells, thereby simplifying gene cloning and advancing gene therapy applications. However, its potential for metabolic engineering in yeast has yet to be explored.

Methods

We reconstituted the dCasMINI system in C. viswanathii and optimized it by modifying nuclear localization signals, sgRNA design, promoters and transcriptional activators. The redesigned system was applied to activate various endogenous genes. The impact of activating different transporter genes on DDA production was evaluated.

Significant findings

The native dCasMINI-VPR system impaired C. viswanathii growth and failed to induce gene expression. By tuning design elements and replacing VPR with another yeast activator (Med2), we established a new dCasMINI-Med2 system that enabled robust activation of both constitutive and inducible genes while minimizing growth defects. Using this system, activation of transporter genes STL1_4 and HST6 enhanced DDA titers by 13–16 %. This study repurposes dCasMINI-based CRISPRa in C. viswanathii for metabolic engineering. The optimized dCasMINI-Med2 platform expands the CRISPRa toolbox for yeasts and demonstrates that transporter regulation can alleviate metabolic bottlenecks and improve DDA biosynthesis.
十二烷二酸(DDA)是一种具有广泛工业应用价值的单体。viswanathii念珠菌可以将十二烷转化为12碳DDA,使其成为可持续生产的代谢工程的一个有吸引力的宿主。最近开发的一种微型dCasMINI蛋白,当与VPR激活因子融合时,可以在哺乳动物细胞中有效激活CRISPR (CRISPRa),从而简化基因克隆和推进基因治疗应用。然而,它在酵母代谢工程方面的潜力还有待探索。方法通过核定位信号、sgRNA设计、启动子和转录激活子的修饰,重构了C. viswanathii dCasMINI系统,并对其进行了优化。重新设计的系统被用于激活各种内源基因。评估了激活不同转运基因对DDA产生的影响。重要发现:天然dCasMINI-VPR系统抑制了C. viswanathii的生长,并不能诱导基因表达。通过调整设计元素并用另一种酵母激活剂(Med2)替代VPR,我们建立了一个新的dCasMINI-Med2系统,该系统能够在最大限度地减少生长缺陷的同时激活构成基因和诱导基因。利用该系统,激活转运基因STL1_4和HST6可使DDA滴度提高13 - 16%。本研究将基于dcasmini的CRISPRa用于C. viswanathii的代谢工程。优化后的dCasMINI-Med2平台扩展了酵母的CRISPRa工具箱,并证明了转运体调控可以缓解代谢瓶颈,提高DDA的生物合成。
{"title":"Engineered miniature CRISPR activation system promotes dodecanedioic acid production in Candida viswanathii","authors":"Nam Ngoc Pham ,&nbsp;Chih-Hsuan Chien ,&nbsp;Chin-Wei Chang,&nbsp;Yu-Chen Hu","doi":"10.1016/j.jtice.2025.106548","DOIUrl":"10.1016/j.jtice.2025.106548","url":null,"abstract":"<div><h3>Background</h3><div>Dodecanedioic acid (DDA) is a valuable monomer with broad industrial applications. The yeast <em>Candida viswanathii</em> can convert dodecane into 12-carbon DDA, making it an attractive host for metabolic engineering toward sustainable production. A recently developed miniature dCasMINI protein, when fused with the VPR activator, enables efficient CRISPR activation (CRISPRa) in mammalian cells, thereby simplifying gene cloning and advancing gene therapy applications. However, its potential for metabolic engineering in yeast has yet to be explored.</div></div><div><h3>Methods</h3><div>We reconstituted the dCasMINI system in <em>C. viswanathii</em> and optimized it by modifying nuclear localization signals, sgRNA design, promoters and transcriptional activators. The redesigned system was applied to activate various endogenous genes. The impact of activating different transporter genes on DDA production was evaluated.</div></div><div><h3>Significant findings</h3><div>The native dCasMINI-VPR system impaired <em>C. viswanathii</em> growth and failed to induce gene expression. By tuning design elements and replacing VPR with another yeast activator (Med2), we established a new dCasMINI-Med2 system that enabled robust activation of both constitutive and inducible genes while minimizing growth defects. Using this system, activation of transporter genes STL1_4 and HST6 enhanced DDA titers by 13–16 %. This study repurposes dCasMINI-based CRISPRa in <em>C. viswanathii</em> for metabolic engineering. The optimized dCasMINI-Med2 platform expands the CRISPRa toolbox for yeasts and demonstrates that transporter regulation can alleviate metabolic bottlenecks and improve DDA biosynthesis.</div></div>","PeriodicalId":381,"journal":{"name":"Journal of the Taiwan Institute of Chemical Engineers","volume":"181 ","pages":"Article 106548"},"PeriodicalIF":6.3,"publicationDate":"2025-12-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145681061","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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Journal of the Taiwan Institute of Chemical Engineers
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