Chemical Engineering Journal最新文献

{"title":"Liquid versus gas-phase operation in heterogeneously catalyzed hydroformylation","authors":"Maria Herrero Manzano, Jeroen Poissonnier, Sébastien Siradze, Joris W. Thybaut","doi":"10.1016/j.cej.2025.159766","DOIUrl":"https://doi.org/10.1016/j.cej.2025.159766","url":null,"abstract":"Heterogeneously catalyzed hydroformylation over a commercial 5 % rhodium nanoparticle catalyst has been performed within the intrinsic kinetics regime in a high-throughput kinetics setup. Owing to the use of a paraffinic solvent, the reaction was carried out either in the gas or the liquid phase. An ethylene conversion of around 4 % mol/mol was obtained in the gas-phase, whereas liquid-phase operation allowed achieving around 9 % mol/mol conversion under comparable reaction conditions. The presence of the paraffinic solvent is supposed to better tune the reactant concentration to which the catalyst is exposed. Propanal and ethane were the main products observed, the highest propanal selectivity, 75 % mol/mol, being obtained at the lowest temperature, 120 °C. Apparent activation energies for both hydroformylation (59 kJ/mol (l) / 68 kJ/mol (g)) and hydrogenation (87 kJ/mol (l) / 94 kJ/mol (g)) were found to be lower at liquid compared to gas-phase conditions, suggesting a lower overall surface coverage at liquid-phase conditions. Ethylene and hydrogen were found to exhibit a positive impact on gas-phase hydroformylation and hydrogenation, resulting in higher ethylene conversion when increasing their molar reactant ratios. Based on the positive impact of ethylene observed in the gas-phase operation, it is likely that in the liquid phase, where ethylene solubility is higher, the altered molar ratio distribution at the catalyst surface further enhances yields toward propanal.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"32 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142990997","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}

{"title":"CDs@ZnO multi-core@shell structure: Rational designed versatile platform for multiple wavelength RTP, TADF and lasing in high security anti-counterfeiting","authors":"Shaofeng Zhang, Jiatong Wang, Wenfei Zhang, Zefeng Wu, Siufung Yu","doi":"10.1016/j.cej.2025.159674","DOIUrl":"https://doi.org/10.1016/j.cej.2025.159674","url":null,"abstract":"The rational design of a versatile platform capable of producing multi-wavelength afterglow carbon dots (CDs) with varied structures remains a significant obstacle, particularly in enabling the concurrent realization of room-temperature phosphorescence (RTP) and thermally activated delayed fluorescence (TADF). Here, a novel approach is proposed: the chemical encapsulation of CDs within a ZnO multi-core@shell structure to enable dual RTP and TADF emissions under visible light excitation. This is possible because a three-dimensional spatial constraint, coupled with chemical bonding for immobilization, introduces a pivotal role in stabilizing the triplet state within the CDs. Furthermore, CDs with diverse structures are validated to achieve multi-color afterglow emission through this versatile platform, which demonstrates broad applicability. Given the singlet excitons regeneration through the reverse intersystem crossing (RISC) process random lasing is successfully realized from CDs@ZnO. Hence the synergistic integration of RTP, TADF, and lasing construct the multi-levels anti-counterfeiting strategy, greatly enhance the security level. This work not only paves the way for the creation of afterglow materials and lasing media based on CDs but also holds potential for applications in advanced anti-counterfeiting techniques, encryption methods, and optical devices.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"26 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142991004","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}

{"title":"Advanced fabrication of three-dimensional bicontinuous MXene/agarose composite monoliths for high-selective rapid separation of antibodies","authors":"Xiang-Dong Xu, Jing Li, Jun-Qi Zhang, Yuan Peng, Chen-Mei Sun, Ru-Qi Liang, Jian-Bo Qu","doi":"10.1016/j.cej.2025.159755","DOIUrl":"https://doi.org/10.1016/j.cej.2025.159755","url":null,"abstract":"Conventional polysaccharide monoliths with irregular interstitial channels are suffering from low mechanical strength, specific surface areas, permeabilities and large eddy diffusion. In this work, the 3D bicontinuous MXene/agarose composite (BMAC) monoliths were facilely fabricated for the first time by a bicontinuous medium internal phase emulsion (MIPE) templating method. Poly (1-vinylimidazole) (PVIM) brushes were further grafted onto the 3D BMAC (BMAC@PVIM) monolith for highly selective enrichment of antibodies. Molecular docking simulation revealed that the adsorption mechanism of human immunoglobulin G (hIgG) on the monolith is primarily driven by multiple hydrogen bonding and hydrophobic interactions, and the optimal number of VIM units in the PVIM brush is determined to be 9. The resulting 3D BMAC@PVIM monolith exhibited a well-ordered structure, featuring a sturdy framework with diffusive mesopores (∼9 nm) and interconnected gigapores (∼10.1 μm). This composite monolith demonstrated a significantly higher specific surface area (46.6 m²/g), enhanced column permeability (1.67 × 10⁻¹² m²), and increased operating flow rate (20 mL/min) compared to its counterpart (GMAC@PVIM monolith) prepared using the conventional MIPE template. Benefiting from its uniform and ordered skeleton and pore channels, the maximum equilibrium adsorption capacity of hIgG on the monolith could achieve 217.4 mg/g, which is superior to most reported separation materials. Meanwhile, the high adsorption rate constant in the film mass transfer stage also confirmed the satisfactory mass transfer efficiency of interconnected gigapores within the monolith. The 3D BMAC@PVIM monolith can efficiently purify antibodies with a purity of 94.1 % from human serum at a flow rate of 12 mL/min, demonstrating great potential in the field of rapid antibody purification","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"24 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142990664","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}

{"title":"An efficient, robust, and affordable photothermal membrane using polyvinyl alcohol encapsulated MXene/non-woven fibers for solar desalination/sewage purification","authors":"Ye Cao, Pingping Gong, Peng Yu, Yijing Wang, Zhenli Zuo, Changyuan Pan, Xinbing Wang, Peng Zhong, Xiaohua Ma","doi":"10.1016/j.cej.2025.159742","DOIUrl":"https://doi.org/10.1016/j.cej.2025.159742","url":null,"abstract":"Recently Ti₃C₂T_x (MXene) has become an ideal photothermal material for solar interface evaporation, due to its near unit photothermal conversion efficiency, unique layered structures, and abundant surface terminals. However, MXene photothermal membranes still face key issues including evaporation performance, stability, and cost, which restrict their commercialization. Hence, a composite photothermal membrane (MPF) of MXene/polyvinyl alcohol (PVA)/nonwoven fiber (NWF) is constructed in this study, simply by soaking NWF into a MXene solution to achieve saturated adsorption, followed by dropping PVA as an encapsulation layer. The evaporation rate and efficiency of MPF reach 1.84 kgm⁻²h⁻¹ and 99.82 %, respectively, at 1 sun in a siphon-model solar evaporator. The high evaporation performance is attributed to a synergistic effect of improved light absorption, water transport, and thermal management, as well as reduced evaporation enthalpy, by modulating the microstructures of MPF. MPF maintains stable evaporation after 15 cycles in 3.5 wt% simulated seawater, and in simulated seawater with different salinities (0–15 wt%). MPF also shows great light intensity adaptability (0.5–3 sun), and outstanding salt resistance and structural stability. The high stability of MPF is contributed by the encapsulation of PVA, which firmly welds MXene onto NWF and protect MXene from water and oxygen. In addition, MPF exhibits excellent water purification capabilities for different simulating seawater/wastewater. Finally, it is estimated that MPF has a low cost of 23.2 $m⁻² and a high cost-effectiveness of 79.3 gh⁻¹/$, showing significant cost advantages compared to other reported photothermal membranes. A large-area (e.g., 12 × 12 cm²) and flexible MPF can be easily obtained by cutting NWF into any size as needed. This work promotes the practical application of MXene photothermal membranes in solar water treatment.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"6 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142990736","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}

{"title":"Data-based optimization approach for the automatic operation of solar photo-Fenton plants","authors":"D. Rodríguez-García, E. Gualda-Alonso, J.L. García Sánchez, J.L. Guzmán, J.L. Casas López, J.A. Sánchez Pérez","doi":"10.1016/j.cej.2025.159688","DOIUrl":"https://doi.org/10.1016/j.cej.2025.159688","url":null,"abstract":"This work showcases the main design guidelines for implementing a data-based decision-making approach for the automatic operation of solar photo-Fenton plants. The case study explores the removal of microcontaminants (MCs) from an urban wastewater treatment plant secondary effluent using a 100-m² raceway pond reactor (RPR). Automatic system design was based on the computational simulation of the plant, using a kinetic model of the photo-Fenton process at acidic pH. The model was validated for the continuous flow operation of the 100-m² photoreactor. Afterwards, a simulation study was conducted to correlate MC removal yield, residual H₂O₂ concentration and operating cost with the main experimental factors using polynomial models. These models were then incorporated into an optimization routine to determine optimal plant configuration for different environmental scenarios (UVA irradiances and RPR temperatures). As a result, two data-based self-automatic procedures were obtained for 80-% and 90-% MC removal targets, operating cost minimization being the optimization target. Plant performance was evaluated in manual and automatic mode for both clear and cloudy days. The simulation results showed the robustness and reliability of the automatic solution under adverse environmental conditions, achieving stable treated water quality throughout the operation. Furthermore, improvements in cost efficiencies and water treatment capacities of up to 34.4 % and 61.6 % were attained, respectively, leading to reductions in the operating cost of up to 26.2 %. The results delivered highlight the potential of a reliable and easy-to-implement automatic operation strategy for immediate application in existing solar photo-Fenton plants. This approach paves the way for treatment automation, promoting further research on its commercial scale-up.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"18 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142991002","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}

{"title":"Energy-free and ultrafast nano pump of water","authors":"Chun Li, Dongdong Zhou, Fei Zheng, Yujuan Wang, Kedong Bi","doi":"10.1016/j.cej.2025.159765","DOIUrl":"https://doi.org/10.1016/j.cej.2025.159765","url":null,"abstract":"Addressing global freshwater scarcity and energy crises remains a critical challenge to sustainable development. Carbon nanotube (CNT)-based systems for seawater desalination offer a promising solution to these threats. In this study, we demonstrate an active water pump driven by potential energy gradients. Even in the absence of external energy, water molecules traverse the nanotubes, overcoming potential barriers at the tube ends, in stark contrast to energy-driven methods reported in previous literature. The water flux achieved by our system is almost two orders of magnitude higher than in prior studies. Furthermore, we enhance water transport efficiency by wrapping CNTs with polythiophene chains of varying lengths, establishing a continuous potential energy gradient along the nanochannels. This design presents a compelling pathway for developing low-energy, high-efficiency desalination devices, such as artificial purification systems.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"10 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142990662","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}

{"title":"Local delivery of celecoxib/indocyanine green-loaded nanomodulators for combinational photothermal/photodynamic/anti-cyclooxygenase-2 therapy of oral leukoplakia","authors":"Tingting Zhu, Zhiqin Sang, Zhou Ye, Xiaoli Guo, Xiaoru Qu, Yuanping Hao, Wanchun Wang","doi":"10.1016/j.cej.2025.159734","DOIUrl":"https://doi.org/10.1016/j.cej.2025.159734","url":null,"abstract":"Oral leukoplakia (OLK) is a typical precancerous lesion in oral clinics. Current treatments, including topical drugs and photodynamic therapy (PDT), have limitations such as complex procedures, suboptimal efficacy, high recurrence rates, and low permeability. The microneedle patches solve the problem of low permeability as a painless local delivery method. In this study, we developed double-layered dissolving microneedle patches loaded with novel multifunctional nanoparticles (ICM NPs) for treating OLK. The ICM NPs involve mesoporous polydopamine for photothermal therapy (PTT), indocyanine green for PDT, and celecoxib to regulate OLK progression. Furthermore, ICM NPs exhibited excellent photothermal properties under 808 nm laser irradiation, efficient reactive oxygen species-generating, and strong anti-cyclooxygenase (COX)-2 abilities. The patch effectively inhibited OLK cancerization in oral precancer animal models through the synergistic action of photothermal, photodynamic, and anti-COX-2 and had no apparent toxicity in vivo. Our study combines the minimally invasive and deep penetration capabilities of microneedles with PDT/PTT and COX-2 inhibitors, which is expected to be a new choice for the treatment of OPMDs.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"58 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142990671","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}

{"title":"Influence of electronic and structural properties on Au/In2O3/ZrO2 catalysts for CO2 hydrogenation to methanol","authors":"Thiago de M. Augusto, Rubén Blay- Roger, Davi D. Petrolini, Breno F. Ferreira, João Batista O. Santos, Carlos O. Ramirez, Guillaume Clet, Svetlana Ivanova, José A. Odriozola, Luiz F. Bobadilla, Jordi Llorca, José Maria C. Bueno","doi":"10.1016/j.cej.2025.159750","DOIUrl":"https://doi.org/10.1016/j.cej.2025.159750","url":null,"abstract":"Hydrogenation of CO₂ <!-- -->to methanol using H₂ <!-- -->is a promising route for renewable energy production and CO₂ utilization. Meanwhile, the development of catalysts that are both active and highly selective towards methanol production remains a significant challenge. This work investigates the methanol production performance of In₂O₃, In₂O₃/ZrO₂, ZrO₂, and the corresponding Au-promoted oxides. Techniques including XPS,<!-- --> <em>ex situ</em> <!-- -->and<!-- --> <em>operando</em> <!-- -->Raman spectroscopy,<!-- --> <em>in situ</em> and <em>operando</em> <!-- -->DRIFTS, and UV–Vis spectroscopy, together with HR-TEM, revealed that the interactions among Au, InO_x, and zirconia species led to the creation of an interface for CO₂ <!-- -->activation and hydrogenation to methanol, facilitated by oxygen vacancies generated in a reducing atmosphere. The high dispersion of Au and indium oxide species, as shown by HR-TEM, indicated that Au clusters and/or nanoparticles (NPs), together with In₂O₃, favored H₂ <!-- -->dissociation and the prevention of sintering during the reaction. The <em>0.22</em>Au/6.6In₂O₃/ZrO_{2<!-- -->}sample achieved the maximum methanol yield,<!-- --> <!-- -->with superior activity and selectivity, compared to the unpromoted catalyst.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"46 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142990675","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}

{"title":"Construction of diffusion and binding synergy in carbon-supported catalysts with varied Pd0/PdO Ratios for direct synthesis of hydrogen peroxide","authors":"Zhiheng Wang, Jiali Huang, Guancong Jiang, Tuo Ji, Han Lin, Liwen Mu, Xiaohua Lu, Jiahua Zhu","doi":"10.1016/j.cej.2025.159764","DOIUrl":"https://doi.org/10.1016/j.cej.2025.159764","url":null,"abstract":"In heterogeneous reactions, catalyst support plays an important role in tuning catalytic activity of metallic structures and regulating fluid transport during reaction, while it needs to be engineered to balance reaction and diffusion for optimized outcome. In this work, a combined delignification and activation strategy was used to prepare a series of carbon supports with varied porous structures and surface properties. Pd was then loaded on the carbon supports for direct synthesis of H₂O₂ (DSHP) reaction. Results indicated that highly developed <em>meso</em>-macropore structures significantly promoted the dispersion of Pd and exposed more active sites for H₂ dissociation. However, the enrichment of pore structure brought excessive surface oxygen groups, leading to the transition of Pd from Pd⁰ to PdO and thus inhibiting the hydrogenation activity. The optimized catalyst, with desirable porous structure and appropriate Pd⁰/PdO ratio, exhibited an extraordinarily high H₂O₂ productivity of 37346.42 mmol g_Pd^-1h⁻¹ under atmospheric conditions. This work provided a case study on the regulation of reactivity and diffusion through catalyst support engineering, demonstrating the essential role of matched reaction–diffusion in heterogeneous DSHP reactions.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"3 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142990738","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}

{"title":"A spatiotemporal probiotic spore-loaded oxygen generator Resumes gut microbiome balance and Improves hypoxia for treating viral pneumonia","authors":"Qikun Cheng, Mingzhi Xie, Hangjie Ying, Cuiyuan Jin, Lijun Yang, Dong Ma, Shumao Cui, Liyun Shi","doi":"10.1016/j.cej.2025.159706","DOIUrl":"https://doi.org/10.1016/j.cej.2025.159706","url":null,"abstract":"Although evidence indicates that the incidence of viral pneumonia is causally associated with disturbances in the microbiome and hypoxic status in the gut, there is currently no effective strategy for the co-delivery of probiotics and oxygen through oral administration. We therefore created a spatiotemporal biosystem by preparing <em>Bacillus coagulans</em> (BC) probiotic spores, coating them with a polydopamine/chitosan (PCS) nanocoating, and conjugating them with CaO₂ nanoparticles. CaO₂@PCS@BC spore rapidly diffused across the mucus layer spatially while released oxygen followed by bacterial proliferation temporally, thereby significantly enhancing the oxygen levels within intestinal epithelial cells by effectively overcoming the barriers posed by mucus layer and oxygen gradient. In a mouse model of H1N1 infection, we demonstrated that oral CaO₂@PCS@BC spore treatment reversed gut dysbiosis, alleviated intestinal hypoxia, improved metabolism, restored immune balance, and mitigated symptoms of viral pneumonia. Finally, CaO₂@PCS@BC spore facilitated spatial recovery and preserved the anaerobic environment of the gut lumen, suggesting significant biosafety. In conlusion, we have developed a spatiotemporal biosystem that effectively co-delivers probiotics and oxygen to mitigate intestinal dysbiosis in the treatment of viral pneumonia through the gut-lung axis.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"6 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2025-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142991005","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}