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基于阵列式陶瓷膜(ACMs)与粉末活性炭(PAC)偶联的高效催化臭氧氧化的混合流化床反应器(HFBR):中试规模的综合研究。

A hybrid fluidized-bed reactor (HFBR) based on arrayed ceramic membranes (ACMs) coupled with powdered activated carbon (PAC) for efficient catalytic ozonation: A comprehensive study on a pilot scale.

机构信息

State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University, Beijing, 100084, China.

State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University, Beijing, 100084, China.

出版信息

Water Res. 2020 Apr 15;173:115536. doi: 10.1016/j.watres.2020.115536. Epub 2020 Jan 24.

Abstract

Taking advantage of the high mass transfer in the bulk solution of fluidized-bed reactor (FBR), and the benefits of simultaneous particle separation and ozone catalysis on ceramic membranes, we proposed a hybrid fluidized-bed reactor (HFBR) based on arrayed ceramic membranes (ACMs) coupled with powdered activated carbon (PAC) for efficient catalytic ozonation. The optimum HFBR performance on a pilot scale was found at PAC addition of 3 g/L, ozone dosage of 25 mg/L, hydraulic retention time of 60 min and auxiliary aeration strength of 5 m/h. During the 30-day treatment of coal-gasification secondary effluent (200 L/h), the HFBR system revealed not only a 117% increase in ozone utilization efficiency (ΔCOD/ΔO) upon pure ozonation but also a highly purified effluent with better sterilization and low residual bromate (∼11 μg/L). Low-molecular-weight organic fragments and acids, as well as phthalate esters were identified as the main products in this process. By density functional theory (DFT) calculations, it was found the main functional groups (carbonyls, -C=O) on the PAC could be protected from direct ozonation in the presence of ozone-degradable organics (e.g. phenolic and aliphatic compounds) in the wastewater through an ozone-competing reaction, which prevented the rapid inactivation of the PAC in catalytic ozonation. A longer service life and cheaper materials for ceramic membranes would benefit low operation costs for the HFBR. Moreover, the addition of PAC could greatly reduce ozone demand by ∼60% in the HFBR, and therefore decrease energy consumption by ∼30%. Hence, the HFBR was proved to be a highly competitive technology for wide application in the near future.

摘要

利用流化床反应器(FBR)中主体溶液的高传质效率,以及陶瓷膜中颗粒分离和臭氧催化的协同作用,我们提出了一种基于阵列陶瓷膜(ACMs)与粉末活性炭(PAC)耦合的混合流化床反应器(HFBR),用于高效催化臭氧氧化。在中试规模下,当 PAC 添加量为 3 g/L、臭氧剂量为 25 mg/L、水力停留时间为 60 min 和辅助曝气强度为 5 m/h 时,HFBR 表现出最佳性能。在处理煤气化二级出水(200 L/h)的 30 天运行中,HFBR 系统不仅使臭氧利用率(ΔCOD/ΔO)提高了 117%,而且使出水得到了高度净化,具有更好的杀菌效果和较低的溴酸盐残留(约 11 μg/L)。在此过程中,鉴定出低分子量有机碎片和酸以及邻苯二甲酸酯是主要产物。通过密度泛函理论(DFT)计算发现,在废水存在可臭氧降解有机物(如酚类和脂肪族化合物)的情况下,PAC 上的主要官能团(羰基、-C=O)可通过臭氧竞争反应得到保护,从而防止 PAC 在催化臭氧氧化中快速失活。陶瓷膜使用寿命更长、材料更便宜,这将有利于降低 HFBR 的运行成本。此外,PAC 的添加可使 HFBR 中的臭氧需求量减少约 60%,从而使能耗降低约 30%。因此,HFBR 被证明是一种极具竞争力的技术,有望在不久的将来得到广泛应用。

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