MXenes have attracted increasing research enthusiasm owing to their unique physical and chemical properties.Although MXenes exhibit exciting potential in cations adsorption due to their unique surface groups,the adsor...MXenes have attracted increasing research enthusiasm owing to their unique physical and chemical properties.Although MXenes exhibit exciting potential in cations adsorption due to their unique surface groups,the adsorption capacity is limited by the low specific surface area and undeveloped porosity.Our work aims at enhancing the adsorption performance of a well-known MXene,Ti3C2Tx,for methylene blue(MB)by decorating tiny ZIF-8 nanoparticles in the interlayer.After the incorporation of ZIF-8,suitable interspace in the layers resulting from the distribution of tiny ZIF-8 appears.When employing in MB,the adsorption capacity of composites can reach up to 107 mg·g^(-1) while both ZIF-8(3 mg·g^(-1))and Ti_(3)C_(2)Tx(9mg·g^(-1))show nearly no adsorption capacity.The adsorption mechanism was explored,and the good adsorption capacity is caused by the synergistic effect of ZIF-8 and Ti_(3)C_(2)Tx,for neither of them is of suitable interspace or surface groups for MB adsorption.Our work might pave the way for constructing functional materials based on the introduction of nanoparticles into layered materials for various adsorption applications.展开更多
Magnetically responsive porous materials possess unique properties in adsorption processes such as magneticinduced separation and heat generation in alternating magnetic fields, which greatly facilitates recycling pro...Magnetically responsive porous materials possess unique properties in adsorption processes such as magneticinduced separation and heat generation in alternating magnetic fields, which greatly facilitates recycling procedures, favors long-term operation, and improves desorption rate, making conventional adsorption processes highly efficient. With increasing interest in magnetic adsorbents, great progress has been made in designing and understanding of magnetically responsive porous materials varying from monoliths to nanoscale particles used for adsorption including oil uptake, removal of hazardous substances from water, deep desulfurization of fuels, and CO2 capture in the past few years. Therefore, a review summarizing the advanced strategies of synthesizing these magnetically responsive adsorbents and the utilization of their magnetism in practical applications is highly desired. In this review, we give a comprehensive overview of this emerging field, highlighting the strategies of exquisitely incorporating magnetism to porous materials and subtly exploiting their magnetic responsiveness. Further innovations for fabricating or utilizing magnetic adsorbents are expected to be fueled. The potential opportunities and challenges are also discussed.展开更多
In atmospheric conditions, CuⅠis easily oxidized to CuⅡdue to the coexistence of moisture and oxygen.The poor oxidation inhibition of CuⅠrestricts the practical application of CuⅠ-containing materials.Herein we in...In atmospheric conditions, CuⅠis easily oxidized to CuⅡdue to the coexistence of moisture and oxygen.The poor oxidation inhibition of CuⅠrestricts the practical application of CuⅠ-containing materials.Herein we introduce an approach to construct a superhydrophobic microenvironment in CuⅠfunctionalized metal–organic frameworks by coordinatedly grafting organic amine compounds onto open metal sites(OMSs), which can hinder the accessibility of moisture to pores thereby enhancing the stability of CuⅠ. As a proof of concept, MIL-101(Cr) with abundant OMSs and octadecylamine(OA)with long hydrophobic alkyl groups are used as carrier and surface coating. As superhydrophobic porous materials, the resultant CuⅠM-OA exhibits improved CuⅠstability in addition to retaining high crystallinity and intact porosity while almost all CuⅠis oxidized in hydrophilic CuⅠM upon exposure in a humid atmosphere for 30 h. CuⅠM-OA owns excellent adsorption desulfurization performance(ADS) with regard to thiophene, benzothiophene, and 4,6-dimethyl dibenzothiophene. Even from hydrated fuel, the adsorption performance of CuⅠM-OA maintains well while the adsorption capacity of CuⅠM decreases to 7% after4 cycles. The remarkable moisture resistance, CuⅠstability, and high porosity make the current adsorbent CuⅠM-OA highly promising for the practical ADS process.展开更多
Amines in porous materials have been employed as active species for the selective CO_(2) adsorption from natural gas because of their target-specific interactions.Nevertheless,it is difficult to modulate such strong i...Amines in porous materials have been employed as active species for the selective CO_(2) adsorption from natural gas because of their target-specific interactions.Nevertheless,it is difficult to modulate such strong interactions to reach a high efficiency in the adsorption processes.Herein,we fabricated lightresponsive adsorbents with tunable adsorbent–adsorbate interactions for CO_(2) capture.The adsorbents were synthesized by introducing primary and secondary amines into a mesoporous silica that had been grafted with azobenzene groups on the surfaces.The target-specific amine sites render the adsorbents significantly selective in the uptake of CO_(2) over CH_(4),and the azobenzene groups were used as lightresponsive switches to influence the adsorbent–adsorbate interactions.The adsorbents can freely adsorb CO_(2) when the azobenzene groups are in the trans state.Ultraviolet-light irradiation makes the azobenzene groups transform to the cis configuration,which greatly hinders amines in the uptake of CO_(2).The caused difference of adsorption capacity can reach 34.9%.The alternative irradiation by ultravioletand visible-light can lead to a recyclable regulation on adsorption performance.The changes of the electrostatic potentials of amines are responsible for the light-induced regulation on adsorption.展开更多
基金the financial support of this work by the National Natural Science Foundation of China (21878149, 22078155, and 21808110)the project funded by China Postdoctoral Science Foundation (2020M681567)+1 种基金Postgraduate Research & Practice Innovation Program of Jiangsu Province (SJCX20_0358)the Natural Science Foundation of Jiangsu Province (BK20180709)
文摘MXenes have attracted increasing research enthusiasm owing to their unique physical and chemical properties.Although MXenes exhibit exciting potential in cations adsorption due to their unique surface groups,the adsorption capacity is limited by the low specific surface area and undeveloped porosity.Our work aims at enhancing the adsorption performance of a well-known MXene,Ti3C2Tx,for methylene blue(MB)by decorating tiny ZIF-8 nanoparticles in the interlayer.After the incorporation of ZIF-8,suitable interspace in the layers resulting from the distribution of tiny ZIF-8 appears.When employing in MB,the adsorption capacity of composites can reach up to 107 mg·g^(-1) while both ZIF-8(3 mg·g^(-1))and Ti_(3)C_(2)Tx(9mg·g^(-1))show nearly no adsorption capacity.The adsorption mechanism was explored,and the good adsorption capacity is caused by the synergistic effect of ZIF-8 and Ti_(3)C_(2)Tx,for neither of them is of suitable interspace or surface groups for MB adsorption.Our work might pave the way for constructing functional materials based on the introduction of nanoparticles into layered materials for various adsorption applications.
基金Supported by the National Natural Science Foundation of China(21722606,21676138,and 21576137)China Postdoctoral Science Foundation(2018M632295)the Project of Priority Academic Program Development of Jiangsu Higher Education Institutions
文摘Magnetically responsive porous materials possess unique properties in adsorption processes such as magneticinduced separation and heat generation in alternating magnetic fields, which greatly facilitates recycling procedures, favors long-term operation, and improves desorption rate, making conventional adsorption processes highly efficient. With increasing interest in magnetic adsorbents, great progress has been made in designing and understanding of magnetically responsive porous materials varying from monoliths to nanoscale particles used for adsorption including oil uptake, removal of hazardous substances from water, deep desulfurization of fuels, and CO2 capture in the past few years. Therefore, a review summarizing the advanced strategies of synthesizing these magnetically responsive adsorbents and the utilization of their magnetism in practical applications is highly desired. In this review, we give a comprehensive overview of this emerging field, highlighting the strategies of exquisitely incorporating magnetism to porous materials and subtly exploiting their magnetic responsiveness. Further innovations for fabricating or utilizing magnetic adsorbents are expected to be fueled. The potential opportunities and challenges are also discussed.
基金supported by the National Science Fund for Distinguished Young Scholars (22125804)the National Natural Science Foundation of China (22008112, 22078155, and 21878149)+1 种基金the China Postdoctoral Science Foundation (2019M661813)the Project of Priority Academic Program Development of Jiangsu Higher Education Institutions。
文摘In atmospheric conditions, CuⅠis easily oxidized to CuⅡdue to the coexistence of moisture and oxygen.The poor oxidation inhibition of CuⅠrestricts the practical application of CuⅠ-containing materials.Herein we introduce an approach to construct a superhydrophobic microenvironment in CuⅠfunctionalized metal–organic frameworks by coordinatedly grafting organic amine compounds onto open metal sites(OMSs), which can hinder the accessibility of moisture to pores thereby enhancing the stability of CuⅠ. As a proof of concept, MIL-101(Cr) with abundant OMSs and octadecylamine(OA)with long hydrophobic alkyl groups are used as carrier and surface coating. As superhydrophobic porous materials, the resultant CuⅠM-OA exhibits improved CuⅠstability in addition to retaining high crystallinity and intact porosity while almost all CuⅠis oxidized in hydrophilic CuⅠM upon exposure in a humid atmosphere for 30 h. CuⅠM-OA owns excellent adsorption desulfurization performance(ADS) with regard to thiophene, benzothiophene, and 4,6-dimethyl dibenzothiophene. Even from hydrated fuel, the adsorption performance of CuⅠM-OA maintains well while the adsorption capacity of CuⅠM decreases to 7% after4 cycles. The remarkable moisture resistance, CuⅠstability, and high porosity make the current adsorbent CuⅠM-OA highly promising for the practical ADS process.
基金supported by the National Natural Science Foun-dation of China(22078155,21808110,21878149,and 21676138)China Postdoctoral Science Foundation(2020M681567)。
文摘Amines in porous materials have been employed as active species for the selective CO_(2) adsorption from natural gas because of their target-specific interactions.Nevertheless,it is difficult to modulate such strong interactions to reach a high efficiency in the adsorption processes.Herein,we fabricated lightresponsive adsorbents with tunable adsorbent–adsorbate interactions for CO_(2) capture.The adsorbents were synthesized by introducing primary and secondary amines into a mesoporous silica that had been grafted with azobenzene groups on the surfaces.The target-specific amine sites render the adsorbents significantly selective in the uptake of CO_(2) over CH_(4),and the azobenzene groups were used as lightresponsive switches to influence the adsorbent–adsorbate interactions.The adsorbents can freely adsorb CO_(2) when the azobenzene groups are in the trans state.Ultraviolet-light irradiation makes the azobenzene groups transform to the cis configuration,which greatly hinders amines in the uptake of CO_(2).The caused difference of adsorption capacity can reach 34.9%.The alternative irradiation by ultravioletand visible-light can lead to a recyclable regulation on adsorption performance.The changes of the electrostatic potentials of amines are responsible for the light-induced regulation on adsorption.