Devising a desirable adsorbent for efficiently selective capture of Ag(Ⅰ) from wastewater has attracted much attention but faced with huge challenges. Herein, a novel linear o-phenanthroline-based polymer L-PRL was p...Devising a desirable adsorbent for efficiently selective capture of Ag(Ⅰ) from wastewater has attracted much attention but faced with huge challenges. Herein, a novel linear o-phenanthroline-based polymer L-PRL was prepared via chemical oxidative polymerization for the adsorption of Ag(Ⅰ). The maximum adsorption capacity for Ag(Ⅰ) by L-PRL is 325.8 mg/g at pH 0. In addition, L-PRL owes ascendant selectivity for Ag(Ⅰ) from aqueous solutions containing various interfering metal ions of Pb(Ⅱ), Co(Ⅱ), Ni(Ⅱ), Cd(Ⅱ)and Fe(Ⅲ). Multiple characterizations of FT-IR and XPS uncover that the N groups on L-PRL act as adsorption sites to coordinate with Ag(Ⅰ). Density functional theory(DFT) calculations further evidence the mechanism that L-PRL is provided with the admirable adsorptivity and selectivity for Ag(Ⅰ). It is mainly attributed to the most stable complexes of L-PRL with Ag(Ⅰ), which possesses shortest Ag-N bond length compared with other heavy metal ions. Furthermore, 93.5% of initial adsorption capacity is reserved after four continuous regeneration cycles, indicating that L-PRL is equipped with superior recyclability and durability, and L-PRL is capable of removing Ag(Ⅰ) in low-concentration actual Ag(Ⅰ)-containing wastewater completely. This study shed light on the rational design of polymer adsorbents and in-depth insight into selective removal of aqueous Ag(Ⅰ).展开更多
Hierarchically structured macro-mesoporous carbon catalysts were synthesized using dual templates of poly(methyl methacrylate)(PMMA)and Pluronic-123 to enhance cellulose saccharification.Characterizations conducted th...Hierarchically structured macro-mesoporous carbon catalysts were synthesized using dual templates of poly(methyl methacrylate)(PMMA)and Pluronic-123 to enhance cellulose saccharification.Characterizations conducted through scanning electron microscopy(SEM),X-ray diffraction(XRD),N2 adsorption-desorption isotherms,Fourier transform infrared(FT-IR)spectroscopy,and titration techniques confirmed high surface areas and specific pore size distributions,with macropores ranging from 78.3 to 251 nm and mesopores around 2.43-6.23 nm.An optimal PMMA-to-Tetraethyl orthosilicate(TEOS)ratio of 1:1.6 facilitated the highest cellulose conversion rate of 59.3%and a glucose yield of 22.1%.Notably,the medium-sized macropore catalyst,MMCS60-M,outperformed its purely mesoporous counterpart,with conversion rates and glucose yields of 80.8% and 45.5%,respectively.These results suggest the importance of a tailored pore architecture to enhance the accessibility of acid sites and facilitate effective mass transport,which is beneficial for optimizing saccharification processes.展开更多
The selective capture of copper from strongly acidic solutions is of vital importance from the perspective of sustainable development and environmental protection.Metal organic frameworks(MOFs)have attracted the inter...The selective capture of copper from strongly acidic solutions is of vital importance from the perspective of sustainable development and environmental protection.Metal organic frameworks(MOFs)have attracted the interest of many scholars for adsorption due to their fascinating physicochemical characteristics,including adjustable structure,strong stability and porosity.Herein,pz-UiO-66 containing a pyrazine structure is successfully synthesized for the efficient separation of copper from strongly acidic conditions.Selective copper removal at low pH values is accomplished by using this material that is not available in previously reported metal–organic frameworks.Furthermore,the material exhibits excellent adsorption capacity,with a theoretical maximum copper uptake of 247 mg/g.As proven by XPS and FT-IR analysis,the coordination of pyrazine nitrogen atoms with copper ions is the dominant adsorption mechanism of copper by pz-UiO-66.This work provides an opportunity for efficient and selective copper removal under strongly acidic conditions,and promises extensive application prospects for the removal of copper in the treatment for acid metallurgical wastewater.展开更多
The adsorbents–adsorbates interaction is critical for resourcelization in heavy metal wastewater treatment.Nevertheless,it is still indistinct to depict the impact of metal center effect on heavy metals removal perfo...The adsorbents–adsorbates interaction is critical for resourcelization in heavy metal wastewater treatment.Nevertheless,it is still indistinct to depict the impact of metal center effect on heavy metals removal performance in metal-organic frameworks(MOFs)-based adsorbents.Herein,a series of MOFs with different metal centers of Mg(II),La(III),and Zr(IV)are rationally designed,and the effect of electronic structure on the Sb(V)removal performance is systematically investigated.The obtained La-MGs achieve Sb(V)adsorption capacity of 897.6 mg/g,which is about 1.2 and 4.5 times above average than those of Zr-MGs and Mg-MGs,respectively.On account of more edge adsorption sites achieve,the sites utilization efficiency of La-MGs(92.1%)is much better than Zr-MGs(75.0%)and Mg-MGs(20.4%).Furthermore,density functional theory(DFT)calculations reveal that La-MGs are more active than Mg-MGs and Zr-MGs,owing to the lower adsorption energy,higher charge transfer,and stronger bonding interaction,which will promote the Sb(V)removal performance.The experimental results in practical water indicate that La-MGs effectively capture antimony at low concentration,reaching drinking water standard in samples from Ganjiang River.This study opens an avenue for atomic-level insight into high-efficient absorbents design for water treatment from electronic structuremodification of active centers.展开更多
基金financially supported by the National Science Fund for Distinguished Young Scholars(No.52125002)the National Science Foundation of China(No.52100043)+1 种基金the National Key Research and Development Program of China(No.2019YFC1907900)the National Science Foundation of Jiangxi Province(No.20202BABL213037)。
文摘Devising a desirable adsorbent for efficiently selective capture of Ag(Ⅰ) from wastewater has attracted much attention but faced with huge challenges. Herein, a novel linear o-phenanthroline-based polymer L-PRL was prepared via chemical oxidative polymerization for the adsorption of Ag(Ⅰ). The maximum adsorption capacity for Ag(Ⅰ) by L-PRL is 325.8 mg/g at pH 0. In addition, L-PRL owes ascendant selectivity for Ag(Ⅰ) from aqueous solutions containing various interfering metal ions of Pb(Ⅱ), Co(Ⅱ), Ni(Ⅱ), Cd(Ⅱ)and Fe(Ⅲ). Multiple characterizations of FT-IR and XPS uncover that the N groups on L-PRL act as adsorption sites to coordinate with Ag(Ⅰ). Density functional theory(DFT) calculations further evidence the mechanism that L-PRL is provided with the admirable adsorptivity and selectivity for Ag(Ⅰ). It is mainly attributed to the most stable complexes of L-PRL with Ag(Ⅰ), which possesses shortest Ag-N bond length compared with other heavy metal ions. Furthermore, 93.5% of initial adsorption capacity is reserved after four continuous regeneration cycles, indicating that L-PRL is equipped with superior recyclability and durability, and L-PRL is capable of removing Ag(Ⅰ) in low-concentration actual Ag(Ⅰ)-containing wastewater completely. This study shed light on the rational design of polymer adsorbents and in-depth insight into selective removal of aqueous Ag(Ⅰ).
文摘Hierarchically structured macro-mesoporous carbon catalysts were synthesized using dual templates of poly(methyl methacrylate)(PMMA)and Pluronic-123 to enhance cellulose saccharification.Characterizations conducted through scanning electron microscopy(SEM),X-ray diffraction(XRD),N2 adsorption-desorption isotherms,Fourier transform infrared(FT-IR)spectroscopy,and titration techniques confirmed high surface areas and specific pore size distributions,with macropores ranging from 78.3 to 251 nm and mesopores around 2.43-6.23 nm.An optimal PMMA-to-Tetraethyl orthosilicate(TEOS)ratio of 1:1.6 facilitated the highest cellulose conversion rate of 59.3%and a glucose yield of 22.1%.Notably,the medium-sized macropore catalyst,MMCS60-M,outperformed its purely mesoporous counterpart,with conversion rates and glucose yields of 80.8% and 45.5%,respectively.These results suggest the importance of a tailored pore architecture to enhance the accessibility of acid sites and facilitate effective mass transport,which is beneficial for optimizing saccharification processes.
基金the National Natural Science Foundation of China(Nos.52125002 and 51908270)the Natural Science Foundation of Jiangxi Province(No.20212ACB213006),and the National Key Research and Development Program of China(No.2019YFC1907900).
文摘The selective capture of copper from strongly acidic solutions is of vital importance from the perspective of sustainable development and environmental protection.Metal organic frameworks(MOFs)have attracted the interest of many scholars for adsorption due to their fascinating physicochemical characteristics,including adjustable structure,strong stability and porosity.Herein,pz-UiO-66 containing a pyrazine structure is successfully synthesized for the efficient separation of copper from strongly acidic conditions.Selective copper removal at low pH values is accomplished by using this material that is not available in previously reported metal–organic frameworks.Furthermore,the material exhibits excellent adsorption capacity,with a theoretical maximum copper uptake of 247 mg/g.As proven by XPS and FT-IR analysis,the coordination of pyrazine nitrogen atoms with copper ions is the dominant adsorption mechanism of copper by pz-UiO-66.This work provides an opportunity for efficient and selective copper removal under strongly acidic conditions,and promises extensive application prospects for the removal of copper in the treatment for acid metallurgical wastewater.
基金the National Natural Science Foundation of China(Nos.51938007,51720105001,52100039,52125002,and 52100043)the Youth Natural Science Foundation of Hunan Province(No.2020JJ5076).
文摘The adsorbents–adsorbates interaction is critical for resourcelization in heavy metal wastewater treatment.Nevertheless,it is still indistinct to depict the impact of metal center effect on heavy metals removal performance in metal-organic frameworks(MOFs)-based adsorbents.Herein,a series of MOFs with different metal centers of Mg(II),La(III),and Zr(IV)are rationally designed,and the effect of electronic structure on the Sb(V)removal performance is systematically investigated.The obtained La-MGs achieve Sb(V)adsorption capacity of 897.6 mg/g,which is about 1.2 and 4.5 times above average than those of Zr-MGs and Mg-MGs,respectively.On account of more edge adsorption sites achieve,the sites utilization efficiency of La-MGs(92.1%)is much better than Zr-MGs(75.0%)and Mg-MGs(20.4%).Furthermore,density functional theory(DFT)calculations reveal that La-MGs are more active than Mg-MGs and Zr-MGs,owing to the lower adsorption energy,higher charge transfer,and stronger bonding interaction,which will promote the Sb(V)removal performance.The experimental results in practical water indicate that La-MGs effectively capture antimony at low concentration,reaching drinking water standard in samples from Ganjiang River.This study opens an avenue for atomic-level insight into high-efficient absorbents design for water treatment from electronic structuremodification of active centers.
