{"title":"用于微米级工艺强化的创新微通道结构珠:用于消除磺胺甲恶唑的水处理案例研究","authors":"Jiaojiao Zheng , Zhentao Wu","doi":"10.1016/j.cej.2024.158527","DOIUrl":null,"url":null,"abstract":"<div><div>This study focuses on the development of innovative microchannel-structured beads, designed to revolutionize diffusional mass transfer inside porous materials. Specifically, we created microchannel-structured alumina beads (AS0, 3 mm in diameter), using a combined phase-inversion and sintering process. This was followed by incorporating varying amounts of mesoporous γ-Al<sub>2</sub>O<sub>3</sub> phase through a sol–gel process for the first time to enhance the internal specific surface area (S<sub>BET</sub>) of the AS0 beads, along with a 2 wt% cobalt catalytic phase applied via impregnation (2Co/AS<em>x</em>). A second approach for integrating cobalt-γ-Al<sub>2</sub>O<sub>3</sub> inside the beads is a one-step co-impregnation process (2Co/AS<em>x</em> (co-imp.), <em>x</em> ranges from 0 to 4 with varying amounts of γ-Al<sub>2</sub>O<sub>3</sub> sols). These samples were then subjected to the degradation of sulfamethoxazole (SMX) in the peroxymonosulfate (PMS)-activated AOPs system under mild reaction conditions. Experimental results demonstrated that the microchannel-structured beads with higher S<sub>BET</sub> displayed enhanced catalytic activity, with 2Co/AS<em>x</em> (co-imp.) achieving better catalytic efficiency compared to 2Co/AS<em>x</em>. This improvement was attributed to larger exposed open surface pores on the beads, which facilitated diffusional mass transfer of reactants and products. However, overloading γ-Al<sub>2</sub>O<sub>3</sub> could reduce the accessibility of surface pores, increase mass transfer resistance at high pollutant concentrations (40 mg/L SMX), and consequently reduce SMX removal efficiency. More importantly, it is unexpected that the catalyst exhibited substantially higher performance after regeneration, achieving 96.32 % SMX removal in 20 min, compared to 95.75 % in 120 min for the fresh catalyst. This was attributed to the enhanced accessibility of open pores on the bead surface during regeneration, highlighting the significance of intensifying the diffusional transfer process to benefit catalytic reactions. Such benefits are highly transferable to a broader spectrum of heterogeneous catalysis applications.</div></div>","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"504 ","pages":"Article 158527"},"PeriodicalIF":13.2000,"publicationDate":"2025-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Innovative microchannel-structured beads for microscale process intensification: A case study on water treatment for sulfamethoxazole abatement\",\"authors\":\"Jiaojiao Zheng , Zhentao Wu\",\"doi\":\"10.1016/j.cej.2024.158527\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>This study focuses on the development of innovative microchannel-structured beads, designed to revolutionize diffusional mass transfer inside porous materials. Specifically, we created microchannel-structured alumina beads (AS0, 3 mm in diameter), using a combined phase-inversion and sintering process. This was followed by incorporating varying amounts of mesoporous γ-Al<sub>2</sub>O<sub>3</sub> phase through a sol–gel process for the first time to enhance the internal specific surface area (S<sub>BET</sub>) of the AS0 beads, along with a 2 wt% cobalt catalytic phase applied via impregnation (2Co/AS<em>x</em>). A second approach for integrating cobalt-γ-Al<sub>2</sub>O<sub>3</sub> inside the beads is a one-step co-impregnation process (2Co/AS<em>x</em> (co-imp.), <em>x</em> ranges from 0 to 4 with varying amounts of γ-Al<sub>2</sub>O<sub>3</sub> sols). These samples were then subjected to the degradation of sulfamethoxazole (SMX) in the peroxymonosulfate (PMS)-activated AOPs system under mild reaction conditions. Experimental results demonstrated that the microchannel-structured beads with higher S<sub>BET</sub> displayed enhanced catalytic activity, with 2Co/AS<em>x</em> (co-imp.) achieving better catalytic efficiency compared to 2Co/AS<em>x</em>. This improvement was attributed to larger exposed open surface pores on the beads, which facilitated diffusional mass transfer of reactants and products. However, overloading γ-Al<sub>2</sub>O<sub>3</sub> could reduce the accessibility of surface pores, increase mass transfer resistance at high pollutant concentrations (40 mg/L SMX), and consequently reduce SMX removal efficiency. More importantly, it is unexpected that the catalyst exhibited substantially higher performance after regeneration, achieving 96.32 % SMX removal in 20 min, compared to 95.75 % in 120 min for the fresh catalyst. This was attributed to the enhanced accessibility of open pores on the bead surface during regeneration, highlighting the significance of intensifying the diffusional transfer process to benefit catalytic reactions. Such benefits are highly transferable to a broader spectrum of heterogeneous catalysis applications.</div></div>\",\"PeriodicalId\":270,\"journal\":{\"name\":\"Chemical Engineering Journal\",\"volume\":\"504 \",\"pages\":\"Article 158527\"},\"PeriodicalIF\":13.2000,\"publicationDate\":\"2025-01-15\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Chemical Engineering Journal\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S1385894724100186\",\"RegionNum\":1,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"ENGINEERING, CHEMICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Chemical Engineering Journal","FirstCategoryId":"5","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S1385894724100186","RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, CHEMICAL","Score":null,"Total":0}
Innovative microchannel-structured beads for microscale process intensification: A case study on water treatment for sulfamethoxazole abatement
This study focuses on the development of innovative microchannel-structured beads, designed to revolutionize diffusional mass transfer inside porous materials. Specifically, we created microchannel-structured alumina beads (AS0, 3 mm in diameter), using a combined phase-inversion and sintering process. This was followed by incorporating varying amounts of mesoporous γ-Al2O3 phase through a sol–gel process for the first time to enhance the internal specific surface area (SBET) of the AS0 beads, along with a 2 wt% cobalt catalytic phase applied via impregnation (2Co/ASx). A second approach for integrating cobalt-γ-Al2O3 inside the beads is a one-step co-impregnation process (2Co/ASx (co-imp.), x ranges from 0 to 4 with varying amounts of γ-Al2O3 sols). These samples were then subjected to the degradation of sulfamethoxazole (SMX) in the peroxymonosulfate (PMS)-activated AOPs system under mild reaction conditions. Experimental results demonstrated that the microchannel-structured beads with higher SBET displayed enhanced catalytic activity, with 2Co/ASx (co-imp.) achieving better catalytic efficiency compared to 2Co/ASx. This improvement was attributed to larger exposed open surface pores on the beads, which facilitated diffusional mass transfer of reactants and products. However, overloading γ-Al2O3 could reduce the accessibility of surface pores, increase mass transfer resistance at high pollutant concentrations (40 mg/L SMX), and consequently reduce SMX removal efficiency. More importantly, it is unexpected that the catalyst exhibited substantially higher performance after regeneration, achieving 96.32 % SMX removal in 20 min, compared to 95.75 % in 120 min for the fresh catalyst. This was attributed to the enhanced accessibility of open pores on the bead surface during regeneration, highlighting the significance of intensifying the diffusional transfer process to benefit catalytic reactions. Such benefits are highly transferable to a broader spectrum of heterogeneous catalysis applications.
期刊介绍:
The Chemical Engineering Journal is an international research journal that invites contributions of original and novel fundamental research. It aims to provide an international platform for presenting original fundamental research, interpretative reviews, and discussions on new developments in chemical engineering. The journal welcomes papers that describe novel theory and its practical application, as well as those that demonstrate the transfer of techniques from other disciplines. It also welcomes reports on carefully conducted experimental work that is soundly interpreted. The main focus of the journal is on original and rigorous research results that have broad significance. The Catalysis section within the Chemical Engineering Journal focuses specifically on Experimental and Theoretical studies in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. These studies have industrial impact on various sectors such as chemicals, energy, materials, foods, healthcare, and environmental protection.