Thallium is a highly toxic metal,and trace amount of thallium(I)(Tl+)in potable water could cause a severe water crisis,which arouses the exploitation of highly-effective technology for purification of Tl+contaminated...Thallium is a highly toxic metal,and trace amount of thallium(I)(Tl+)in potable water could cause a severe water crisis,which arouses the exploitation of highly-effective technology for purification of Tl+contaminated water.This report proposes the multi-layered Prussian blue(PB)-decorated composite membranes(PBx@PDA/PEI-FP)based on the aminated filter papers for Tl+uptake.Extensively characterization by Fourier transform infrared spectrometer-attenuated total reflectance,scanning electron microscope,thermogravimetric analysis,X-ray photoelectron spectroscopy and X-ray diffraction were performed to confirm the in situ growth of cubic PB crystals on filter paper membrane surfaces via the aminated layers,and the successful fabrication of multi-layered PB overcoats via the increasing of aminated layers.The effect of PB layers on Tl+removal by PBx@PDA/PEI-FP from simulated drinking water was evaluated as well as the influence of different experimental conditions.A trade-off between PB decoration layer number and PB distribution sizes is existed in Tl+uptake by PBx@PDA/PEI-FP.The double-layered PB2@PDA/PEI-FP membrane showed the maximum sorption capacity,but its Tl+uptake performance was weakened by the acid,coexisting ions(K+and Na+)and powerful operation pressure,during filtrating a large volume of low-concentrated Tl+-containing water.However,the negative effect of coexisting ions on the Tl+uptake could be effectively eliminated in weak alkaline water,and the Tl+removal was increased up to 100%without any pressure driving for PB2@PDA/PEI-FP membrane.Most importantly,PB2@PDA/PEI-FP displayed the high-efficiency and high-selectivity in purifying the Tl+-spiked Pearl River water,in which the residual Tl+in filtrate was less than 2μg·L^(–1) to meet the drinking water standard of United States Environmental Protection Agency.This work provides a feasible avenue to safeguard the drinking water in remote and underdeveloped area via the energy-free operation.展开更多
具有良好析氧反应(OER)活性的层状双氢氧化物(LDHs)在储能/转化领域得到了广泛的研究.然而,导电性差、易团聚、本征活性低等特点限制了其实际应用.通过改善NiFeLDHs的本征活性和稳定性(如引入杂原子或与其他导电基质结合)以提高全解水性...具有良好析氧反应(OER)活性的层状双氢氧化物(LDHs)在储能/转化领域得到了广泛的研究.然而,导电性差、易团聚、本征活性低等特点限制了其实际应用.通过改善NiFeLDHs的本征活性和稳定性(如引入杂原子或与其他导电基质结合)以提高全解水性能,受到越来越多的关注.本文通过水热和煅烧磷化两步反应,成功合成了在碳化钛二维薄片上的垂直交错的三元相磷化镍/铁杂化物(NiFeP/MXene).优化后的NiFe P/MXene在电流密度为10 mA cm^(-2)时仅有286 mV的低过电位和较低的塔菲尔斜率35 mV dec^(-1),超过了许多现有的NiFe基催化剂的性能.进一步将NiFeP/MXene应用于碱性电解质中全解水的阳极,仅需要1.61 V的电池电压就能达到10 mA cm^(-2)的电流密度.密度函数理论(DFT)计算结果表明,无论是MXene还是磷化,都能有效调整电催化剂表面的电子结构和密度,提升d带中心的能级,从而实现对OER性能的提升.该研究为设计高性能的OER催化剂提供了新的思路.展开更多
基金supported by the National Natural Science Foundation of China(Grant Nos.22006026,52270001)Guangdong Basic and Applied Basic Research Foundation(Grant Nos.2023A1515012506,2019A1515110546)+4 种基金Science and Technology Program of Guangzhou(Grant No.202102080160)Project of Young Innovative Talents in Colleges and Universities of Guangdong Province(Grant No.2019KQNCX111)Outstanding Youth Project of Guangdong Natural Science Foundation(Grant No.2022B1515020030)Guangzhou Science and Technology Project(Grant Nos.202201020530,202201020200)Research Project of Guangzhou University(Grant No.YJ2023026).
文摘Thallium is a highly toxic metal,and trace amount of thallium(I)(Tl+)in potable water could cause a severe water crisis,which arouses the exploitation of highly-effective technology for purification of Tl+contaminated water.This report proposes the multi-layered Prussian blue(PB)-decorated composite membranes(PBx@PDA/PEI-FP)based on the aminated filter papers for Tl+uptake.Extensively characterization by Fourier transform infrared spectrometer-attenuated total reflectance,scanning electron microscope,thermogravimetric analysis,X-ray photoelectron spectroscopy and X-ray diffraction were performed to confirm the in situ growth of cubic PB crystals on filter paper membrane surfaces via the aminated layers,and the successful fabrication of multi-layered PB overcoats via the increasing of aminated layers.The effect of PB layers on Tl+removal by PBx@PDA/PEI-FP from simulated drinking water was evaluated as well as the influence of different experimental conditions.A trade-off between PB decoration layer number and PB distribution sizes is existed in Tl+uptake by PBx@PDA/PEI-FP.The double-layered PB2@PDA/PEI-FP membrane showed the maximum sorption capacity,but its Tl+uptake performance was weakened by the acid,coexisting ions(K+and Na+)and powerful operation pressure,during filtrating a large volume of low-concentrated Tl+-containing water.However,the negative effect of coexisting ions on the Tl+uptake could be effectively eliminated in weak alkaline water,and the Tl+removal was increased up to 100%without any pressure driving for PB2@PDA/PEI-FP membrane.Most importantly,PB2@PDA/PEI-FP displayed the high-efficiency and high-selectivity in purifying the Tl+-spiked Pearl River water,in which the residual Tl+in filtrate was less than 2μg·L^(–1) to meet the drinking water standard of United States Environmental Protection Agency.This work provides a feasible avenue to safeguard the drinking water in remote and underdeveloped area via the energy-free operation.
基金supported by the National Natural Science Foundation of China(21875048)the Outstanding Youth Project of Guangdong Natural Science Foundation(2020B1515020028)+1 种基金the Yangcheng Scholars Research Project of Guangzhou(201831820)the Science and Technology Research Project of Guangzhou(202002010007)。
文摘具有良好析氧反应(OER)活性的层状双氢氧化物(LDHs)在储能/转化领域得到了广泛的研究.然而,导电性差、易团聚、本征活性低等特点限制了其实际应用.通过改善NiFeLDHs的本征活性和稳定性(如引入杂原子或与其他导电基质结合)以提高全解水性能,受到越来越多的关注.本文通过水热和煅烧磷化两步反应,成功合成了在碳化钛二维薄片上的垂直交错的三元相磷化镍/铁杂化物(NiFeP/MXene).优化后的NiFe P/MXene在电流密度为10 mA cm^(-2)时仅有286 mV的低过电位和较低的塔菲尔斜率35 mV dec^(-1),超过了许多现有的NiFe基催化剂的性能.进一步将NiFeP/MXene应用于碱性电解质中全解水的阳极,仅需要1.61 V的电池电压就能达到10 mA cm^(-2)的电流密度.密度函数理论(DFT)计算结果表明,无论是MXene还是磷化,都能有效调整电催化剂表面的电子结构和密度,提升d带中心的能级,从而实现对OER性能的提升.该研究为设计高性能的OER催化剂提供了新的思路.
