{"title":"Zero-Dimensional perovskite-like Cs2CoCl4 crystal for highly sensitive X-ray direct detection and imaging","authors":"Xiong Zhang, Renyan Huang, Zhongyuan Zhang, Hao Lu, Hongyuan Sha, Xieming Xu, Yi Zheng, Xin Huang, Shuaihua Wang, Shaofan Wu","doi":"10.1016/j.cej.2024.158729","DOIUrl":"https://doi.org/10.1016/j.cej.2024.158729","url":null,"abstract":"Lead-free perovskites have recently attracted huge interest in direct-type radiation detectors. In this work, a zero-dimensional perovskite-like halide Cs<sub>2</sub>CoCl<sub>4</sub> is prepared by an all-water solvent method that enables large-area production for X-ray imaging. The outstanding radiation detection performance of Cs<sub>2</sub>CoCl<sub>4</sub> is demonstrated by a single crystal device. Specifically, the X-ray detector based on Cs<sub>2</sub>CoCl<sub>4</sub> single crystal has a large carrier mobility-lifetime (<em>μτ</em>) product of 1.63 × 10<sup>−4</sup> cm<sup>2</sup> V<sup>−1</sup> under X-ray irradiation, a sensitivity of up to 2421 μC Gy<sub>air</sub><sup>−1</sup>cm<sup>−2</sup> at 287.8 V mm<sup>−1</sup>, and it could detect X-ray as low as 54.3 nGy<sub>air</sub> s<sup>−1</sup>. In addition, Cs<sub>2</sub>CoCl<sub>4</sub>@fiber composite films prepared by aqueous solution evaporation are used to confirm the feasibility of X-ray imaging application. The uniformity of composite films is achieved by adjusting pressure and concentration to control homogeneous nucleation and growth. Excitingly, a switching test lasting more than 300 min at a dose rate of 1169 μGy<sub>air</sub> s<sup>−1</sup> indicates that Cs<sub>2</sub>CoCl<sub>4</sub>@fiber has excellent radiation stability. As a proof of concept, a 5 × 5 pixelated detector array is prepared to achieve a clearly observed outline of the imaged object, offering an inspiring material design strategy conducive to realizing environmentally friendly film devices.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"31 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2024-12-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142867048","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}
Reshma Nair, Kiranmai Uppuluri, Febin Paul, Keith Sirengo, Dorota Szwagierczak, Suresh C Pillai, Libu Manjakkal
{"title":"Electrochemical energy storing performances of printed LaFeO3 coated with PEDOT: PSS for hybrid supercapacitors","authors":"Reshma Nair, Kiranmai Uppuluri, Febin Paul, Keith Sirengo, Dorota Szwagierczak, Suresh C Pillai, Libu Manjakkal","doi":"10.1016/j.cej.2024.158781","DOIUrl":"https://doi.org/10.1016/j.cej.2024.158781","url":null,"abstract":"Developing advanced smart energy storage devices demanded new functional materials to store energy effectively and deliver power quickly. In this work, we studied the energy-storing performance of perovskite material, lanthanum ferrite (LaFeO<sub>3</sub>), prepared by the solid-state reaction method. The screen-printed LaFeO<sub>3</sub> and graphite electrodes are used to develop hybrid supercapacitors (HSCs) with KOH electrolyte. Varying the sintering temperature of the LaFeO<sub>3</sub> perovskite electrode (800 °C, 900 °C, and 1000 °C) leads to changes in the surface and crystalline properties, which impact the electrochemical properties and overall energy-storing performance of the HSC. The surface of the LaFeO<sub>3</sub> electrode is modified with organic conducting polymer poly(3,4-ethylenedioxythiophene) polystyrene sulfonate (PEDOT: PSS), which enhances the energy storage of the HSC. The developed HSC based on LaFeO<sub>3</sub>, sintered at 1000 °C and surface modified with PEDOT: PSS, exhibited a specific capacitance of 12.007 mF∙cm<sup>−2</sup> at a current density of 0.075 mA∙cm<sup>−2</sup>. This value is two times higher than (5.874 mF∙cm<sup>−2</sup>) without the surface modification of LaFeO<sub>3</sub> at 1000 °C. This study provides valuable insights into the electrochemical performances of the ABO<sub>3</sub> perovskite (LaFeO<sub>3</sub>) electrodes for the next generation of portable energy storage devices.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"31 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2024-12-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142867080","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}
Yang Ming, Shuo Shi, Wei Cai, Jing Liu, Daming Chen, Xin Hu, Rujun Yu, Xia Zhou, Benjamin Tawiah, Bin Fei
{"title":"A scalable wood-based interfacial evaporator assisted with localized joule heating for round-the-clock operations","authors":"Yang Ming, Shuo Shi, Wei Cai, Jing Liu, Daming Chen, Xin Hu, Rujun Yu, Xia Zhou, Benjamin Tawiah, Bin Fei","doi":"10.1016/j.cej.2024.158690","DOIUrl":"https://doi.org/10.1016/j.cej.2024.158690","url":null,"abstract":"The evaporation efficiency of solar-driven interfacial steam is significantly affected by the diurnal variations in solar irradiance and is further compressed by the absence of light. This work proposes a wood-based interfacial evaporator with an auxiliary heat mode to achieve round-the-clock operations. The device was constructed using sustainable, cost-effective in-situ Ni-P electroless plating followed by hole drilling and surface graphite spray-coating. The self-floating evaporator achieves an evaporation rate of 2.20 kg m<sup>−2</sup>h<sup>−1</sup> under 1 Sun illumination and 2 V input in 3.5 wt% NaCl solution. The realized rate can be attributed to the localized interfacial heat induced by the electroless-plated Ni-P alloy (R<sub>sheet</sub> = 1.45 Ω/sq). Moreover, adopting the novel hierarchical advantages, including mesoporous nature, low anisotropic thermal conductivity of wood, and reduced evaporation enthalpy in Ni-P film (1893 J/g), the device further reaches a daytime evaporation yield of 8.47kg m<sup>−2</sup> on cloudy days and 14.68 kg m<sup>−2</sup> on sunny days, respectively. And a yield of 5.33 kg m<sup>−2</sup> with an electrical energy input of ∼ 0.71 kW m<sup>−2</sup> is recorded during nighttime. This performance implies a significant step towards wood-based evaporators for round-the-clock water harvesting and shows potential for upscaling devices to all-weather 3D evaporators.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"7 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2024-12-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142867013","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}
Joemer Absalon Adorna, Van Dien Dang, Thanh van Nguyen, Bishal Kumar Nahak, Keng-Ku Liu, Ruey-An Doong
{"title":"Functionalization of MXenes [Ti3C2(=O/OH/F)X] with highly mesoporous NH2-activated biochar for permselective salty ions removal by capacitive deionization","authors":"Joemer Absalon Adorna, Van Dien Dang, Thanh van Nguyen, Bishal Kumar Nahak, Keng-Ku Liu, Ruey-An Doong","doi":"10.1016/j.cej.2024.158802","DOIUrl":"https://doi.org/10.1016/j.cej.2024.158802","url":null,"abstract":"Capacitive deionization (CDI) is a cutting-edge solution for efficient saltwater desalination. In this study, the gas-hydrolyzed nanoflake MXenes (OMX) was hydrothermally synthesized and then coupled with amine-charged activated biochar (cAB) to form the asymmetric CDI for enhanced salty ion removal. The ratio of negatively charged –OH/=O/-F terminal group of Ti<sub>3</sub>C<sub>2</sub>T<sub>X</sub> MXenes was optimized for better ion intercalation. Concurrently, the positively-charged cAB was used as an anode to eliminate the need for expensive ion-exchange membranes. The cAB structure creates a multi-porous network ideally for ion accommodation, which can retain 80 % of its original surface area after amination. Moreover, the interlayer spacing of OMX can expand from 9.3 to 13.4 Å after hydrolyzation at 120 °C. Electrochemical tests of OMX exhibits a specific capacitance of 185.0 F g<sup>−1</sup> at 5 mV/s, while the strong interaction between amine functional groups and Na<sub>2</sub>SO<sub>4</sub> electrolyte enhances the capacitance of cAB up to 255 F g<sup>−1</sup> at 5 mV/s and retains 75 % of the original value at 100 mV/s. The asymmetric cAB||OMX hybrid CDI can minimize the co-ion repulsion, resulting in the enhancement of CDI efficiency. The specific electrosorption capacity of cAB||OMX can achieve 49.3 mg g<sup>−1</sup> at 5000 mg L<sup>−1</sup> NaCl and at 1.2 V. The Ragone plot of SEC and SAR in cAB||OMX highlights the minimal requirement of IEM on gas-hydrolyzed MXene hybrid CDI system, which can open the avenue to enhance the desalination performance for diverse water-energy nexus applications","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"15 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2024-12-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142867047","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":"Diverse siloxane-terminated side chain ameliorated simple polymer donors towards efficient and stable air-processed organic solar cells","authors":"Xing Chen, Lianjie Zhang, Mingqing Chen, Dongge Ma, Jun Wang, Junwu Chen","doi":"10.1016/j.cej.2024.158404","DOIUrl":"https://doi.org/10.1016/j.cej.2024.158404","url":null,"abstract":"Side chain engineering plays an important role on performance of an organic semiconducting material. Herein, three linear siloxane-terminated side chains of different siloxane lengths and a novel <em>T</em>-shaped siloxane-terminated side chain were attached on a simple quinoxaline-thiophene backbone to construct four polymer donors PMQ-L3Si, PMQ-L5Si, PMQ-L7Si, and PMQ-T4Si for organic solar cells (OSCs). The different siloxane terminals showed great impacts on photophysical and aggregation properties of polymers. When pairing with acceptor BTP-H2, the resulting binary OSCs showed power conversion efficiencies (PCEs) between 16.76% and 18.15%. The highest PCE and OSC stability were achieved with PMQ-L5Si. Fibrous blend morphology, high glass transition temperature, efficient exciton dissociation, high face-on ratio, and balanced charge transport were found for the PMQ-L5Si based binary active layers. All the polymer based active layers, being processed in high humidity air, could exhibit comparable efficiencies to nitrogen condition, confirming advantage of the siloxane-terminated side chains. Polymer PMQ-L5Si was selected to construct ternary active layer, giving higher PCE of 18.82%. This work initiates the linear and <em>T</em>-shaped siloxane-terminated side chains to decorate polymer donors for OSC application, and also provides a guidance for side chain engineering aiming on tunable morphology and optimal matching to non-fullerene acceptor.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"267 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2024-12-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142867056","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}
Yuxuan Zhang, Jian Sun, Yuyao Tan, Yi Shi, Zijian Zhou, Chuanwen Zhao, Wenqiang Liu
{"title":"Hydrophobic layer assisting-casted dark Ca-based CO2 sorbent pellets for solar-driven calcium looping: Insights into pellet configuration and properties","authors":"Yuxuan Zhang, Jian Sun, Yuyao Tan, Yi Shi, Zijian Zhou, Chuanwen Zhao, Wenqiang Liu","doi":"10.1016/j.cej.2024.158808","DOIUrl":"https://doi.org/10.1016/j.cej.2024.158808","url":null,"abstract":"Solar radiation heat replaces pulverized coal as the heat source in the calcination reactor of the direct solar-driven Calcium Looping (CaL) system, eliminating the adverse impact of in-situ coal combustion on Ca-based sorbents. To ensure the system’s efficiency, the Ca-based sorbents must exhibit strong light absorption capabilities, with manganese incorporation being an effective strategy to enhance this characteristic. The integration of impregnated layer solution combustion with hydrophobic layer-assisted casting is a promising approach for fabricating highly efficient Mn-incorporated Ca-based sorbent pellets. Constructing Mn-incorporated Ca-based sorbent pellets with a graphite hydrophobic layer results in better performance compared to using a Nano-TiO<sub>2</sub> hydrophobic layer. The latter is prone to forming a white shell on the sorbent pellets’ surface, which seriously affects the light absorption features. High levels of Mn loading work to increase the optical absorbance of hydrophobic graphite layer assisting-casted Ca-based sorbent pellets, but this inevitably leads to a sacrifice in their CO<sub>2</sub> sorption capacity. Therefore, the core–shell structured Ca-based sorbent pellets, comprising a highly active Al-stabilized CaO pristine core and a dark Mn-based outer shell, fabricated with a graphite/MnO<sub>2</sub> mixture as the hydrophobic layer, exhibit exceptional optical absorbance (88.4 %) alongside excellent CO<sub>2</sub> sorption capabilities (maintaining average CO<sub>2</sub> uptake of 0.39 g/g during 20 cycles), making them optimal candidates for direct solar-driven CaL.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"24 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2024-12-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142867088","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}
Da Neub Kim, Eungsu Kang, Hwa Heon Je, Dong Hwan Kim, Keumrai Whang, Sanghak Cha, Dae-yeol Ye, Wonheum Baek, Taewook Kang, Dong Soo Hwang, Yoo Seong Choi, Gyoo Yeol Jung
{"title":"Molecular regime shift from kinetic limitation condition to mass-transfer limitation condition for stabilizing CO metabolism by microorganisms","authors":"Da Neub Kim, Eungsu Kang, Hwa Heon Je, Dong Hwan Kim, Keumrai Whang, Sanghak Cha, Dae-yeol Ye, Wonheum Baek, Taewook Kang, Dong Soo Hwang, Yoo Seong Choi, Gyoo Yeol Jung","doi":"10.1016/j.cej.2024.158801","DOIUrl":"https://doi.org/10.1016/j.cej.2024.158801","url":null,"abstract":"Carbon monoxide (CO) serves as a promising carbon source, but it adversely affects CO-metabolizing microorganisms. To address this issue, fermentation should occur under mass-transfer limitation conditions, where the rate of gaseous CO transfer is lower than its consumption rate. However, maintaining these conditions becomes challenging as microorganism physiology deteriorates during fermentation, requiring a novel strategy to sustain mass-transfer limitation conditions. In this study, cellulose-based nanocrystals coated with a tannic acid-Fe<sup>3+</sup> complex (TA-Fe<sup>3+</sup>CNC) were developed. These nanocrystals exhibited reversible CO adsorption/desorption characteristics, enabling the transformation from kinetic to mass-transfer limitation conditions. This approach effectively mitigated substrate inhibition from CO with negligibly impacting cell physiology. Kinetic studies demonstrated the effectiveness of TA-Fe<sup>3+</sup>CNCs in mitigating CO inhibition under high CO partial pressures. Furthermore, computational modeling validated the successful shifting from kinetic to mass-transfer limitation conditions at the molecular level. Overall, this study introduces a novel platform for stabilizing CO metabolism by microorganisms","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"13 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2024-12-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142867052","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}
Lixing Xue, Hongyan Pan, Yuejun Wang, Zhengyi Wang, Xuhui Wang, Qian Lin, Kuo Zhang, Xiangnan Bu, Maohui Bai, Bo Hong
{"title":"A flame-retardant and weakly solvated gel electrolyte for high-performance and high-safety Ah class sodium-ion batteries","authors":"Lixing Xue, Hongyan Pan, Yuejun Wang, Zhengyi Wang, Xuhui Wang, Qian Lin, Kuo Zhang, Xiangnan Bu, Maohui Bai, Bo Hong","doi":"10.1016/j.cej.2024.158828","DOIUrl":"https://doi.org/10.1016/j.cej.2024.158828","url":null,"abstract":"Phosphate-based electrolytes can effectively improve flame retardancy of sodium-ion batteries (SIBs), but there is a problem of incompatibility with carbon based electrodes. Here, a flame-retardant gel electrolyte (FRGE) strategy can solve the above problems simultaneously by adopting perfluorinated electrolyte and high content of phosphate ester, and cross-linked gel polymer matrix. The electrolyte solvation structure is optimized by the electrostatic adsorption action of the gel, which prompts the entry of anions into the first solvation layer, forming more ion aggregates (AGGs) and contact ion pairs (CIPs). The FRGE enhances the interaction between Na-ion and the PF<sub>6</sub><sup>−</sup> anion, promoting the decomposition of the anion at the interface to form a stable dense fluorinated SEI film, while reducing the possibility of phosphate ester co-embedding in the carbon-based anode. Remarkably, the designed 2.4 Ah Na<sub>0.9</sub>[Cu<sub>0.22</sub>Fe<sub>0.3</sub>Mn<sub>0.48</sub>]O<sub>2</sub>/HC pouch cell incorporating FRGE demonstrates an impressive low-capacity degradation rate of 0.0035 % per cycle over 1000 cycles, attesting to a high energy density of 124.6 Wh kg<sup>−1</sup>. The composite gel electrolyte not only enhances flame retardancy but also boosts electrochemical properties, furthering the practical application of SIBs.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"56 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2024-12-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142867053","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":"Regulating the photoelectric effect and built-in electric field based on the electronic and spatial effects of substituents on PDIs amide sites to enhance the photocatalytic performance of PDIs","authors":"Zhengkai Wu, Yunning Chen, Xueying Cheng, Renquan Guan, Shuyu Chen, Yingna Guo, Qingkun Shang","doi":"10.1016/j.cej.2024.158805","DOIUrl":"https://doi.org/10.1016/j.cej.2024.158805","url":null,"abstract":"How to design and optimize the single-molecule structure of perylene diimide derivatives (PDIs) to obtain high-performance photocatalysts is one of the challenges facing the current research field of PDIs photocatalysis. In this article, we regulate the π-π self-assembly stacking and optoelectronic properties of PDIs by changing the type and position of substituents on the amide site. The PDI-PBA photocatalyst with excellent performance was obtained from seven types of PDIs supramolecular materials. Theoretical calculations and optoelectronic performance tests have shown that PDI-PBA has good crystallinity and maximum dipole moment, resulting in its maximum built-in electric field, effectively promoting the separation and transport of photo-generated carriers. The transient absorption spectra further indicate that photogenerated electrons and holes of PDI-PBA have outstanding separation efficiency and ultra-long lifetime. In the batch reactor, PDI-PBA can degrade almost 100 % acetaminophen within 60 min. In the dynamic cycling system with a surface hydraulic load of 14.56 L/(m<sup>2</sup>·h), the efficiency of PDI-PBA photocatalytic degradation of acetaminophen can reach 84 %. PDI-PBA can also effectively degrade phenol, levofloxacin, and ciprofloxacin. This work provides a successful example for the design of novel and efficient PDIs supramolecular materials, and lays the foundation for the application of PDIs photocatalysts in practical wastewater treatment.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"31 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2024-12-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142867083","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 stackable membrane microreactor for gas–liquid-solid reactions: Design, operation, and scale-up","authors":"Yanjiao Xu, Mengbo Zhang, Hengyu Zhong, Shuying Xie, Xuxin Zhu, Haomiao Zhang, Jingdai Wang, Yongrong Yang","doi":"10.1016/j.cej.2024.158798","DOIUrl":"https://doi.org/10.1016/j.cej.2024.158798","url":null,"abstract":"We present a 3D-printed stackable miniature membrane reactor to handle gas–liquid-solid reactions effectively and showcase its application in the synthesis of alkylaluminoxanes. The combination of membrane dispersion and microreaction techniques allows for better process control of the ultrafast and highly exothermic reactions of alkylaluminums hydrolysis with pyrophoric reactants. Droplet generation experiments guide the optimization of the reactor structure and operating parameters, highlighting its ability to produce clustered microdroplets with a narrow size distribution and minimal energy consumption. Our visualized reactor design provides insights into the transient characteristics of alkylaluminoxanes formation, improving understanding of the complex chemistries and achieving room-temperature synthesis of highly active methylaluminoxane (MAO) and isobutylaluminoxane (IBAO) for ethylene polymerization. When scaled up, our compact and integrated five-layer stacked reactor demonstrates uniform flow distribution and consistent reaction performance among all layers, achieving an impressive production rate exceeding ten tons/year. Our work demonstrates a versatile membrane microreaction platform for the scalable and inherently safe production of highly reactive materials, offering a promising approach for other challenging chemical synthesis applications.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"56 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2024-12-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142867267","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}