As promising catalysts for the degradation of organic pollutants,metal–organic frameworks(MOFs)often face limitations due to the particle agglomeration and challenging recovery in liquid-catalysis application,stemmin...As promising catalysts for the degradation of organic pollutants,metal–organic frameworks(MOFs)often face limitations due to the particle agglomeration and challenging recovery in liquid-catalysis application,stemming from their powdery nature.Engineering macroscopic structures from pulverous MOF is thus of great importance for broadening their practical applications.In this study,three-dimensional porous MOF aerogel catalysts were successfully fabricated for degrading organic dyes by activating peroxymonosulfate(PMS).MOF/gelatin aerogel(MOF/GA)catalysts were prepared by directly integrating bimetallic FeCo-BDC with gelatin solutions,followed by freeze-drying and low-temperature calcination.The FeCo-BDC-0.15/GA/PMS system exhibited remarkable performance in degrading various organic dyes,eliminating 99.2%of rhodamine B within a mere 5 min.Compared to the GA/PMS system,there was over a 300-fold increase in the reaction rate constant.Remarkably,high removal efficiency was maintained across varying conditions,including different solution pH,co-existing inorganic anions,and natural water matrices.Radical trapping experiments and electron paramagnetic resonance analysis revealed that the degradation involved radical(SO_(4)^(-)·)and non-radical routes(^(1)O_(2)),of which ^(1)O_(2) was dominant.Furthermore,even after a continuous 400-min reaction in a fixed-bed reactor at a liquid hourly space velocity of 27 h^(-1),the FeCo-BDC/GA composite sustained a degradation efficiency exceeding 98.7%.This work presents highly active MOF-gelatin aerogels for dye degradation and expands the potential for their large-scale,continuous treatment application in organic dye wastewater management.展开更多
The novel Fe-N co-doped ordered mesoporous carbon with high catalytic activity in m-cresol removal was prepared by urea-assisted impregnation and simple pyrolysis method.During the preparation of the Fe-NC catalyst,th...The novel Fe-N co-doped ordered mesoporous carbon with high catalytic activity in m-cresol removal was prepared by urea-assisted impregnation and simple pyrolysis method.During the preparation of the Fe-NC catalyst,the complexation of N elements in urea could anchor Fe,and the formation of C3N4during urea pyrolysis could also prevent migration and aggregation of Fe species,which jointly improve the dispersion and stability of Fe.The FeN4sites and highly dispersed Fe nanoparticles synergistically trigger the dual-site peroxymonosulfate (PMS) activation for highly efficient m-cresol degradation,while the ordered mesoporous structure of the catalyst could improve the mass transfer rate of the catalytic process,which together promote catalytic degradation of m-cresol by PMS activation.Reactive oxygen species (ROS) analytic experiments demonstrate that the system degrades m-cresol by free radical pathway mainly based on SO_(4)^(-)·and·OH,and partially based on·OH as the active components,and a possible PMS activation mechanism by 5Fe-50 for m-cresol degradation was proposed.This study can provide theoretical guidance for the preparation of efficient and stable catalysts for the degradation of organic pollutants by activated PMS.展开更多
目的:多元线性回归模型在保持输入自变量光谱信息和空间特征的同时,通过线性变换获取自变量和因变量的光谱拟合关系,对原输入自变量的光谱信息进行优化,从而获得高空间分辨率和丰富光谱信息的重构数据。方法:利用同期获取的OLI(Operatio...目的:多元线性回归模型在保持输入自变量光谱信息和空间特征的同时,通过线性变换获取自变量和因变量的光谱拟合关系,对原输入自变量的光谱信息进行优化,从而获得高空间分辨率和丰富光谱信息的重构数据。方法:利用同期获取的OLI(Operational Land Imager)和PMS(Panchromatic and Multispectral Scanner)多光谱遥感影像,根据最小二乘法构建多元线性回归模型,重构生成具有丰富光谱特征和空间特征的遥感影像,从主客观两个方面评价重构影像的质量。结果:在目视解译(主观)方面,重构影像在一定程度上保留了原OLI影像的光谱特性,提升了原PMS影像的清晰度和分辨性;在量化角度(客观)方面,重构影像的信息量和平均梯度比原OLI对应波段影像的信息量(在部分波段上)和平均梯度要低,但比原PMS影像的信息量和平均梯度要高,可见重构影像的质量介于原PMS影像和OLI影像的质量之间。结论:以青海省门源回族自治县的耕地内不同作物为实例对象,利用最大似然法获取门源县青稞和油菜的空间分布,研究区实测数据验证表明,重构影像对耕地内部青稞与油菜的提取精度高于原PMS和OLI多光谱影像的提取精度。展开更多
基金funded by the Natural Science Foundation of Fujian Province(2023J05180)the President's Foundation of Minnan Normal University(KJ2021011).
文摘As promising catalysts for the degradation of organic pollutants,metal–organic frameworks(MOFs)often face limitations due to the particle agglomeration and challenging recovery in liquid-catalysis application,stemming from their powdery nature.Engineering macroscopic structures from pulverous MOF is thus of great importance for broadening their practical applications.In this study,three-dimensional porous MOF aerogel catalysts were successfully fabricated for degrading organic dyes by activating peroxymonosulfate(PMS).MOF/gelatin aerogel(MOF/GA)catalysts were prepared by directly integrating bimetallic FeCo-BDC with gelatin solutions,followed by freeze-drying and low-temperature calcination.The FeCo-BDC-0.15/GA/PMS system exhibited remarkable performance in degrading various organic dyes,eliminating 99.2%of rhodamine B within a mere 5 min.Compared to the GA/PMS system,there was over a 300-fold increase in the reaction rate constant.Remarkably,high removal efficiency was maintained across varying conditions,including different solution pH,co-existing inorganic anions,and natural water matrices.Radical trapping experiments and electron paramagnetic resonance analysis revealed that the degradation involved radical(SO_(4)^(-)·)and non-radical routes(^(1)O_(2)),of which ^(1)O_(2) was dominant.Furthermore,even after a continuous 400-min reaction in a fixed-bed reactor at a liquid hourly space velocity of 27 h^(-1),the FeCo-BDC/GA composite sustained a degradation efficiency exceeding 98.7%.This work presents highly active MOF-gelatin aerogels for dye degradation and expands the potential for their large-scale,continuous treatment application in organic dye wastewater management.
基金gratefully acknowledge the financial support of the National Natural Science Foundation of China(22108145 and 21978143)the Shandong Province Natural Science Foundation(ZR2020QB189)+1 种基金State Key Laboratory of Heavy Oil Processing(SKLHOP202203008)the Talent Foundation funded by Province and Ministry Co-construction Collaborative Innovation Center of Eco-chemical Engineering(STHGYX2201).
文摘The novel Fe-N co-doped ordered mesoporous carbon with high catalytic activity in m-cresol removal was prepared by urea-assisted impregnation and simple pyrolysis method.During the preparation of the Fe-NC catalyst,the complexation of N elements in urea could anchor Fe,and the formation of C3N4during urea pyrolysis could also prevent migration and aggregation of Fe species,which jointly improve the dispersion and stability of Fe.The FeN4sites and highly dispersed Fe nanoparticles synergistically trigger the dual-site peroxymonosulfate (PMS) activation for highly efficient m-cresol degradation,while the ordered mesoporous structure of the catalyst could improve the mass transfer rate of the catalytic process,which together promote catalytic degradation of m-cresol by PMS activation.Reactive oxygen species (ROS) analytic experiments demonstrate that the system degrades m-cresol by free radical pathway mainly based on SO_(4)^(-)·and·OH,and partially based on·OH as the active components,and a possible PMS activation mechanism by 5Fe-50 for m-cresol degradation was proposed.This study can provide theoretical guidance for the preparation of efficient and stable catalysts for the degradation of organic pollutants by activated PMS.
文摘目的:多元线性回归模型在保持输入自变量光谱信息和空间特征的同时,通过线性变换获取自变量和因变量的光谱拟合关系,对原输入自变量的光谱信息进行优化,从而获得高空间分辨率和丰富光谱信息的重构数据。方法:利用同期获取的OLI(Operational Land Imager)和PMS(Panchromatic and Multispectral Scanner)多光谱遥感影像,根据最小二乘法构建多元线性回归模型,重构生成具有丰富光谱特征和空间特征的遥感影像,从主客观两个方面评价重构影像的质量。结果:在目视解译(主观)方面,重构影像在一定程度上保留了原OLI影像的光谱特性,提升了原PMS影像的清晰度和分辨性;在量化角度(客观)方面,重构影像的信息量和平均梯度比原OLI对应波段影像的信息量(在部分波段上)和平均梯度要低,但比原PMS影像的信息量和平均梯度要高,可见重构影像的质量介于原PMS影像和OLI影像的质量之间。结论:以青海省门源回族自治县的耕地内不同作物为实例对象,利用最大似然法获取门源县青稞和油菜的空间分布,研究区实测数据验证表明,重构影像对耕地内部青稞与油菜的提取精度高于原PMS和OLI多光谱影像的提取精度。
