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Antiphase alternating-pulse fluidized bed for improving the fluidization quality: An Eulerian–Eulerian study
IF 3.7 3区 工程技术
AIChE Journal Pub Date : 2025-02-11 DOI: 10.1002/aic.18754
Lingjie Zhang, Jiali Du, Feng Wu, Junwu Wang, Xiaoxun Ma
{"title":"Antiphase alternating-pulse fluidized bed for improving the fluidization quality: An Eulerian–Eulerian study","authors":"Lingjie Zhang, Jiali Du, Feng Wu, Junwu Wang, Xiaoxun Ma","doi":"10.1002/aic.18754","DOIUrl":"https://doi.org/10.1002/aic.18754","url":null,"abstract":"To address poor radial mixing in conventional pulsed fluidized beds (PFB), a novel antiphase alternating-pulse fluidized bed (AAPFB) is proposed to improve the fluidization quality by combining a well-designed air distributor and a non-steady-state gas intake technique. Detailed analysis of flow field differences among uniform flow fluidized bed (UFB), PFB, and AAPFB was conducted through numerical simulations, with a particular focus on examining variations in dispersion coefficients, elucidating the mechanism of the regulation of the flow fields by antiphase alternating pulsed airflow. The study also explored the modulation of inlet waveform, pulse frequency and vibration amplitude on flow characteristics. Results indicated that (i) AAPFB achieves uniform particle disturbance, significantly enhancing gas and particle dispersion; (ii) Rectangular flow improves particle distribution more than sinusoidal and triangular flows; and (iii) A 1 Hz pulse frequency and 0.3<i>u</i><sub><i>m</i></sub> amplitude optimally balances flow disturbances and bubble dynamics, resulting in superior dispersion for gas and particles.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"15 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-02-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143385842","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
Thioether-bridged surfactants for interfacial hydrophobic regulation and enhanced mineral flotation recovery
IF 3.7 3区 工程技术
AIChE Journal Pub Date : 2025-02-11 DOI: 10.1002/aic.18772
Qing Sun, Diling Yang, Jingsi Chen, Ziqian Zhao, Hao Zhang, Hong Zhong, Hongbo Zeng
{"title":"Thioether-bridged surfactants for interfacial hydrophobic regulation and enhanced mineral flotation recovery","authors":"Qing Sun, Diling Yang, Jingsi Chen, Ziqian Zhao, Hao Zhang, Hong Zhong, Hongbo Zeng","doi":"10.1002/aic.18772","DOIUrl":"https://doi.org/10.1002/aic.18772","url":null,"abstract":"Surfactant modification to improve interfacial hydrophobicity is widely employed in separation applications such as mineral recovery. However, few modifications effectively enhance both the inherent hydrophobicity of the surfactant and its surface-anchoring capacity. In this study, we propose a strategy to incorporate a thioether group into a hydroxamate surfactant, resulting in the synthesis of N-hydroxy-2-(octylthio)acetamide (OTHA). Compared to the thioether-free surfactant (OHA), the thioether group significantly improves the metal-anchoring capability of the surfactant, demonstrating a twofold increase in adsorption on hydrophilic cassiterite surfaces. Meanwhile, the inherent hydrophobicity of the thioether group enhances the hydrophobization of the target mineral surface and improves bubble-surface interactions. The robust hydrophobicity-inducing ability of OTHA successfully increases the flotation recovery of hydrophilic cassiterite particles, with a marked improvement from 72.5% to 95.0%. This work presents a paradigm for surfactant modification, enabling tailored hydrophobic interfaces for practical applications such as mineral separation, oil-gas extraction, waterproof materials, and functional coatings.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"41 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-02-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143385839","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
Hydrogen-bonded organic framework membranes through dispersion-controlled deposition method for efficient CO2 separation
IF 3.7 3区 工程技术
AIChE Journal Pub Date : 2025-02-11 DOI: 10.1002/aic.18771
Yuhan Wang, Yanxiong Ren, Yu Cao, Junyi Zhao, Jingqi Fu, Guangwei He, Ziting Zhu, Qian Sun, Fusheng Pan, Zhongyi Jiang
{"title":"Hydrogen-bonded organic framework membranes through dispersion-controlled deposition method for efficient CO2 separation","authors":"Yuhan Wang, Yanxiong Ren, Yu Cao, Junyi Zhao, Jingqi Fu, Guangwei He, Ziting Zhu, Qian Sun, Fusheng Pan, Zhongyi Jiang","doi":"10.1002/aic.18771","DOIUrl":"https://doi.org/10.1002/aic.18771","url":null,"abstract":"Hydrogen-bonded organic frameworks (HOFs) feature a highly ordered pore structure, abundant organic functional groups, and unique solution-processability, holding great promise in gas separations. In this study, we explored the fabrication of HOF membranes utilizing a dispersion-controlled deposition (DCD) method. To achieve homogeneous dispersion, the bulk HOF aggregates were initially dispersed in solvent and then switched to anti-solvent to generate the precipitated nanoparticles. Under vacuum-assisted assembly, the HOF colloidal solution containing nanoparticles was uniformly deposited, and the intracrystalline defects were spontaneously healed during the mixed-solvent evaporation. For the first time, HOF polycrystalline membranes were fabricated on flexible polymer substrates and demonstrated an ultrathin HOF selective layer of ~100 nm. The prepared HOF membranes exhibited high separation performance, with the CO<sub>2</sub> permeance exceeding 600 GPU and the CO<sub>2</sub>/N<sub>2</sub> selectivity exceeding 30. This work establishes a platform technology for HOF membrane fabrication and expands the families of carbon capture membranes.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"21 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-02-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143385888","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
Multiphysics and multizone modeling of electrically switched ion exchange with self-driven adsorption for Li+ extraction
IF 3.7 3区 工程技术
AIChE Journal Pub Date : 2025-02-11 DOI: 10.1002/aic.18778
Xuefeng Zhang, Tong Pei, Fengfeng Gao, Xiao Du, Zhonglin Zhang, Lei Xing, Zhong Liu, Jun Li, Xiaogang Hao
{"title":"Multiphysics and multizone modeling of electrically switched ion exchange with self-driven adsorption for Li+ extraction","authors":"Xuefeng Zhang, Tong Pei, Fengfeng Gao, Xiao Du, Zhonglin Zhang, Lei Xing, Zhong Liu, Jun Li, Xiaogang Hao","doi":"10.1002/aic.18778","DOIUrl":"https://doi.org/10.1002/aic.18778","url":null,"abstract":"Electrically switched ion exchange (ESIX) is a promising approach for extracting Li<sup>+</sup> from brines with high Mg/Li ratios. However, the effect of operating conditions and film electrode parameters on electrochemical performance remains unclear. Herein, a dynamic multiphysics and multizone model was developed to describe the ESIX process with self-driven adsorption, using an LMO/PPy electrode pair for ion and charge transport. The results revealed that a flow velocity of 0.0125 m/s and a PPy/LMO mass ratio of 15:1 can effectively reduce Li<sup>+</sup> concentration polarization and activate electroactive sites, respectively. Additionally, the high solid volume fraction of LMO particles increases the concentration difference of electroactive sites, thereby enhancing Li<sup>+</sup> extraction performance. Meanwhile, low currents (≤25 mA/g) narrow the gap between the interfacial exchange current and the applied current, hence improving Li<sup>+</sup> extraction efficiency. This model serves as an efficient in-silico tool for designing and optimizing electrochemical Li<sup>+</sup> extraction processes.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"29 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-02-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143385892","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
Entropy-induced frustrated Lewis pairs in CeO2 for efficiently synthesizing dimethyl carbonate from CO2 and methanol
IF 3.7 3区 工程技术
AIChE Journal Pub Date : 2025-02-11 DOI: 10.1002/aic.18777
Qiaoyu Zhang, Zhichao Liu, Qing Zu, Daoyun Zhu, Yangqiang Huang, Hao Chen, Xiao Luo, Zhiwu Liang
{"title":"Entropy-induced frustrated Lewis pairs in CeO2 for efficiently synthesizing dimethyl carbonate from CO2 and methanol","authors":"Qiaoyu Zhang, Zhichao Liu, Qing Zu, Daoyun Zhu, Yangqiang Huang, Hao Chen, Xiao Luo, Zhiwu Liang","doi":"10.1002/aic.18777","DOIUrl":"https://doi.org/10.1002/aic.18777","url":null,"abstract":"Chemical conversion of carbon dioxide (CO<sub>2</sub>) to dimethyl carbonate (DMC) through reaction with methanol is an attractive and green synthesis strategy with the advantage of 100% atom economy for CO<sub>2</sub>. However, efficient CO<sub>2</sub> activation to achieve high DMC yield remains challenging. Herein, we report defect-rich cerium dioxide (CeO<sub>2</sub>) with abundant unsaturated Ce<sup>3+</sup> and lattice oxygen induced by high-entropy doping of five metals, which act as Lewis acid and base sites. Series characterizations reveal that incorporating five equimolar metals into CeO<sub>2</sub> contributes to the formation of frustrated Lewis pairs (FLP) due to steric hindrance. Density functional theory calculations demonstrate that FLP sites transfer more charge to adsorbed CO<sub>2</sub>, bending the angle of the O‑C‑O bond to 119.4°, which is vital for CO<sub>2</sub> activation. Efficient CO<sub>2</sub> activation achieves a high DMC yield up to 14.0 mmol<sub>DMC</sub>/g<sub>cat</sub>, which is almost 4.5 times that obtained using commercial CeO<sub>2</sub> (3.1 mmol<sub>DMC</sub>/g<sub>cat</sub>).","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"22 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-02-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143385843","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
Asymmetrically coordinated nickel-based catalysts for enhanced hydrogen evolution reaction
IF 3.7 3区 工程技术
AIChE Journal Pub Date : 2025-02-11 DOI: 10.1002/aic.18775
Shiyi Li, Keyu Wang, Chen Liang, Linfeng Lei, Yixing Wang, Linzhou Zhuang, Zhi Xu
{"title":"Asymmetrically coordinated nickel-based catalysts for enhanced hydrogen evolution reaction","authors":"Shiyi Li, Keyu Wang, Chen Liang, Linfeng Lei, Yixing Wang, Linzhou Zhuang, Zhi Xu","doi":"10.1002/aic.18775","DOIUrl":"https://doi.org/10.1002/aic.18775","url":null,"abstract":"Developing non-noble metal hydrogen evolution reaction (HER) catalysts with high efficiency for water dissociation in alkaline environments is crucial for achieving cost-effective alkaline water electrolyzer. Surface engineering offers immense potential to design promising HER catalysts with enhanced performance, but it faces multiple challenges such as optimizing hydrogen adsorption energy. Herein, Ni-based hydroxide catalysts doped with heteroatoms are synthesized via electrodeposition, forming a Co-doped asymmetric S–Ni–F coordination structure, which requires the overpotential of only 20 mV to reach a current density of −10 mA cm<sup>−2</sup>, and remains stable for over 100 h at −0.5 A cm<sup>−2</sup>. DFT calculations reveal that sulfur and fluorine doping could effectively mitigate the energy associated with active hydrogen adsorption and facilitate water molecule dissociation. Furthermore, the electron coupling within the <i>d</i>-orbital of the Ni–O–Co structure further amplifies the catalytic efficacy. This asymmetric structure offering a pathway for designing high-efficiency and non-noble metal alkaline HER catalysts.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"27 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-02-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143385840","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
Highly efficient propyne semihydrogenation over tin-modified Co-based intermetallic catalyst
IF 3.7 3区 工程技术
AIChE Journal Pub Date : 2025-02-10 DOI: 10.1002/aic.18761
Ziqi Bian, Minhao Chen, Xiaohu Ge, Ningchao Zhu, Yueqiang Cao, Hao Jiang, Jing Zhang, Gang Qian, Xinggui Zhou, Xuezhi Duan
{"title":"Highly efficient propyne semihydrogenation over tin-modified Co-based intermetallic catalyst","authors":"Ziqi Bian, Minhao Chen, Xiaohu Ge, Ningchao Zhu, Yueqiang Cao, Hao Jiang, Jing Zhang, Gang Qian, Xinggui Zhou, Xuezhi Duan","doi":"10.1002/aic.18761","DOIUrl":"https://doi.org/10.1002/aic.18761","url":null,"abstract":"Designing and fabricating uniformly dispersed non-precious metal active sites with tuned geometric configurations and local coordination environments for the selective conversion of functional groups to desired products is of great importance but remains challenging in industrial catalytic processes. In this work, we propose a straightforward method for synthesizing the Co<sub>3</sub>Sn<sub>2</sub> intermetallic catalyst through the structural conversion of layered double hydroxide precursors, thereby constructing suitable Sn-modified Co active sites and an optimized catalytic environment for propyne semihydrogenation. Characterizations using x-ray diffraction, high-resolution transmission electron microscopy, and x-ray absorption spectroscopy characterizations are combined to identify the formation of <i>P6</i><sub><i>3</i></sub><i>/mmc</i> Co<sub>3</sub>Sn<sub>2</sub> intermetallic phase. Catalytic performance tests show that the Co<sub>3</sub>Sn<sub>2</sub> catalyst achieves 95.0% propylene selectivity with nearly complete propyne conversion. Temperature-programmed surface reaction and desorption measurements combined with theoretical calculations demonstrate that the good selectivity is driven by the facile desorption of propylene from Sn-modified Co sites rather than its further hydrogenation.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"62 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143375682","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
Reversible adsorption and sieving of trace NH3 from NH3-H2 fuel cells systems using sulfonated porous polydivinylbenzene
IF 3.7 3区 工程技术
AIChE Journal Pub Date : 2025-02-10 DOI: 10.1002/aic.18783
Yongfang Qu, Wentao Zhang, Shouchao Zhong, Linyu Zhuo, Xi Wang, Huihuang Fang, Changkai Lin, Yong Zheng, Fujian Liu, Lilong Jiang
{"title":"Reversible adsorption and sieving of trace NH3 from NH3-H2 fuel cells systems using sulfonated porous polydivinylbenzene","authors":"Yongfang Qu, Wentao Zhang, Shouchao Zhong, Linyu Zhuo, Xi Wang, Huihuang Fang, Changkai Lin, Yong Zheng, Fujian Liu, Lilong Jiang","doi":"10.1002/aic.18783","DOIUrl":"https://doi.org/10.1002/aic.18783","url":null,"abstract":"Trace ammonia reversible adsorption and sieving using solid adsorbents present a critical challenge in the practical deployment of ammonia-hydrogen fuel cells. Herein, we design porous polydivinylbenzene (P-PDVB) through one-pot solvothermal polymerization without additional templates. Subsequently, solvent-induced network swelling was performed to achieve deep sulfonation of the P-PDVB using chlorosulfonic acid, resulting in P-PDVB-SO<sub>3</sub>H-x, which possess large specific surface areas, abundant micro-mesoporosity, and high acid site densities. Notably, P-PDVB-SO<sub>3</sub>H-x demonstrate superior performance for the selective capture and sieving of NH<sub>3</sub> from an N<sub>2</sub>/H<sub>2</sub>/NH<sub>3</sub> mixture, outperforming most previously reported NH<sub>3</sub> adsorbents. Thus, P-PDVB-SO<sub>3</sub>H-x can serve as an efficient adsorbent for the selective removal of trace ammonia from ammonia-hydrogen fuel cell systems, significantly improving both the efficiency and longevity of the fuel cells. This work highlights the potential of P-PDVB-SO<sub>3</sub>H-x as a promising candidate for enhancing ammonia-hydrogen fuel cell performance, paving the way for further exploration of advanced adsorbent materials in energy applications.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"79 3 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143375710","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
Mechanically mediated bulk atom transfer radical polymerization enabled by high‐performance piezoelectric Bi0.5Na0.5TiO3
IF 3.7 3区 工程技术
AIChE Journal Pub Date : 2025-02-09 DOI: 10.1002/aic.18762
Juan Xiong, Ke Yu, Bing‐Hao Wang, Xin‐Yi Huang, Shu Tang, Qing Hu, Jun‐Kang Guo, Long Tang, Shuang‐Feng Yin
{"title":"Mechanically mediated bulk atom transfer radical polymerization enabled by high‐performance piezoelectric Bi0.5Na0.5TiO3","authors":"Juan Xiong, Ke Yu, Bing‐Hao Wang, Xin‐Yi Huang, Shu Tang, Qing Hu, Jun‐Kang Guo, Long Tang, Shuang‐Feng Yin","doi":"10.1002/aic.18762","DOIUrl":"https://doi.org/10.1002/aic.18762","url":null,"abstract":"This study presents the successful mechanically mediated bulk atom transfer radical polymerization (mechano‐ATRP) of methyl acrylate (MA) using the high‐performance piezoelectric material Bi<jats:sub>0.5</jats:sub>Na<jats:sub>0.5</jats:sub>TiO<jats:sub>3</jats:sub> (BNT) under ultrasonic conditions. Compared to the widely used BaTiO<jats:sub>3</jats:sub> in mechano‐ATRP, BNT demonstrates superior piezoelectric performance, enhancing carrier generation, separation, and interfacial transfer. The strong interaction between BNT and Cu catalysts facilitates the rapid capture of mechano‐induced electrons, leading to the formation of Cu<jats:sup>I</jats:sup>/L and efficient polymerization initiation. Factors such as piezoelectric material loading, Cu catalyst loading, targeted degrees of polymerization, and sonication power were systematically evaluated. The living nature of ATRP was confirmed by polymers with predetermined molecular weights and low dispersitis (&lt;1.2). This work broadens the application of ATRP and offers valuable insights into the design of piezoelectric catalytic materials for mechano‐ATRP.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"41 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143371521","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
Sequential hydrogenation enhanced by bidirectional hydrogen spillover over cascade catalyst
IF 3.7 3区 工程技术
AIChE Journal Pub Date : 2025-02-07 DOI: 10.1002/aic.18764
Shuai Wang, Daowei Gao, Rongyao Wang, Yong Wang, Yipin Lv, Lianghao Song, Huaiqing Zhao, Xuchuan Jiang, Riming Hu, Guozhu Chen
{"title":"Sequential hydrogenation enhanced by bidirectional hydrogen spillover over cascade catalyst","authors":"Shuai Wang, Daowei Gao, Rongyao Wang, Yong Wang, Yipin Lv, Lianghao Song, Huaiqing Zhao, Xuchuan Jiang, Riming Hu, Guozhu Chen","doi":"10.1002/aic.18764","DOIUrl":"https://doi.org/10.1002/aic.18764","url":null,"abstract":"Formulating a synergetic strategy to govern the catalytic function of dual metal sites is paramount to achieving precise control of cascade reactions. Herein, we construct a dual-site cascade catalyst with Pt and Ru species localized in the micropores and mesopores of zeolite, respectively. This architecture enables the spatial separation of Pt and Ru sites in nanoscale proximity. Compared to mono/bi-metallic catalysts, this cascade catalyst enables a 4.4–9.5 times enhancement in activity during the sequential hydrogenation of nitroaromatics to cyclohexylamine. Particularly, bidirectional hydrogen spillover assists hydrogenation between Pt and Ru sites is confirmed, where active hydrogen migrates from the less catalytic activity metal to the adjacent metal sites during the first/second step in the cascade reaction. Characterization studies and density functional theory calculations suggest that bidirectional hydrogen spillover enhances the coverage of active hydrogen at the active sites for each hydrogenation step, thereby reducing the energy barrier of the rate-controlling step. This intriguing phenomenon reveals the mechanism of accelerated hydrogenation and presents an opportunity for devising immensely efficient cascade catalysts.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"40 1","pages":""},"PeriodicalIF":3.7,"publicationDate":"2025-02-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143258119","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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