ChemNanoMat
·
2023
·Vol. 9
·期 5
·e202300051
·
IF 3.8
Qiankun Xu,Yaru Li,Wen Ji,Jun Mei,Xianbiao Wang
Graphical TiO 2 hollow sphere/UiO-66-NH 2 heterostructures were successfully synthesized by an adsorption-induced in-situ solvothermal growth strategy. The integration of TiO 2 and UiO-66-NH 2 could construct a type-II heterojunction to broaden the absorption range of light and suppress the recombination of photoproduced electrons and holes, thus boosting the photoreduction activity toward Cr(VI) of TiO 2 /UiO-66-NH 2 . Water contamination caused by highly toxic Cr(VI) should be resolved imminently with a more efficient photocatalytic approach. The interaction between photocatalyst heterostructure is critical for charge separation which largely affects the photocatalytic efficiency. Herein, TiO 2 hollow sphere/UiO-66-NH 2 (TiO 2 /UiO-66-NH 2 ) heterostructures were successfully synthesized by an adsorption-induced in-situ solvothermal growth strategy. The UiO-66-NH 2 particles were well dispersed on TiO 2 hollow spheres by solvothermal treatment of Zr 4+ adsorbed TiO 2 hollow spheres with NH 2 -BDC ligand. The photocatalytic activities of TiO 2 /UiO-66-NH 2 heterostructures were investigated by reduction of Cr(VI) with visible light irradiation. With the introduction of UiO-66-NH 2 , the reduction efficiency toward Cr(VI) by TiO 2 /UiO-66-NH 2 heterostructures reached 89% after 180 min of irradiation, which is much higher than those of TiO 2 hollow spheres (10%) and UiO-66-NH 2 crystals (29%). Moreover, the TiO 2 /UiO-66-NH 2 heterostructures display good regeneration ability and can still maintain 70% of Cr(VI) removal ability after four cycles. The integration of TiO 2 and UiO-66-NH 2 could construct a type-II heterojunction to broaden the absorption range of light and suppress the recombination of photoproduced electrons and holes. As a result, such unique composite structure significantly enhance the photocatalytic performance towards Cr(VI) reduction. This work not only inspires a new approach for in-situ solvothermal synthesis of semiconductor@MOFs composites, but provides a novel photocatalyst for highly efficient removal of Cr(VI) from wastewater.
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ACS Applied Nano Materials
·
2023
·
IF 5.9
Wenjuan Zou,Jintao Dong,Mengxia Ji,Bin Wang,Yingjie Li,Sheng Yin,Huaming Li,Jiexiang Xia
Though heterogeneous Fenton-like reactions possess various characteristics such as a wide application range and mild reaction conditions, their reactivity is currently restricted by unsatisfactory H2O2 decomposition efficiency and low pH adaptation. Hence, Bi25FeO40 nanoparticles prepared via the mechanical ball-milling method (Bi25FeO40-B) with extensive oxygen vacancies possess high reactive oxygen species production performance by enhancing the H2O2 decomposition for tetracycline hydrochloride oxidation and Cr(VI) reduction. H2O2 decomposition efficiency can reach 55.3% in the presence of the Bi25FeO40-B catalyst, which is much higher than that of Bi25FeO40 prepared by the traditional hydrothermal method (23.8%). The Bi25FeO40-B/H2O2 heterogeneous Fenton system demonstrates efficient performance for simultaneous oxidation of tetracycline hydrochloride (TCH) and reduction of Cr(VI). It is capable of removing 75.2% of 50 mg/L TCH and 93.0% of 20 mg/L Cr(VI) at pHinitial = 7, respectively. Abundant oxygen vacancies on the surface of Bi25FeO40-B nanoparticles due to the nanometer size effect can accelerate the decomposition of H2O2 to promote the formation of reactive oxygen species for removing the target organic pollutants and reduction of Cr(VI). Consequently, this work provides a strategy for the preparation of oxygen-rich Bi25FeO40 catalysts for efficient degradation of contaminants and depicts the bright future of Fe-based metal oxides with oxygen vacancies on H2O2 activation in Fenton-like reactions.
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JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Yifei Feng,Nan Xu,Lei Peng,Jiayu Shen,Xiangrong Yang
Remediating hexavalent chromium (Cr(VI))-contaminated soils using green synthesized nano-iron (g-nZVI), which merits high reactivity, low cost, and environmental friendliness, has attracted significant attention. However, the broad existence of nano plastics (NPs) could adsorb Cr(VI) and subsequently influence in situ remediation of Cr(VI)-contaminated soil by g-nZVI. To clarify this issue and improve the remediation efficiency, we investigated the co-transport between Cr(VI) and g-nZVI coexisting with sulfonyl-amino-modified nano plastics (SANPs) in water-saturated sand media in the presence of oxyanions (i.e., phosphate and sulfate) at environmentally relevant conditions. This study found that SANPs inhibited the Cr(VI) reduction to Cr(III) (i.e., Cr 2 O 3 ) by g-nZVI, attributed to nZVI-SANPs hetero-aggregates and Cr(VI) adsorption on SANPs. Notably, “nZVI-[SANPs•••Cr(III)]” agglomerate happened via complexation of [–NH 3 •••Cr(III)] between Cr(III) from Cr(VI) reduced by g-nZVI and amino group on SANPs. Further, the co-presence of phosphate (stronger adsorption on SANPs than g-nZVI) remarkably suppressed Cr(VI) reduction. Then, it promoted the co-transport of Cr(VI) with nZVI-SANPs hetero-aggregates, which could potentially threaten underground water. Fundamentally, sulfate would instead concentrate on SANPs, hardly impacting the reactions between Cr(VI) and g-nZVI. Overall, our findings provide crucial insights into understanding the Cr(VI) species transformation during co-transport with g-nZVI in ubiquitous complexed soil environments (i.e., containing oxyanions) contaminated by SANPs.
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Journal of Materials Chemistry B
·
2023
·Vol. 11
·期 18
·4020-4027
·
IF 7
Min Feng,Xiaofang Chen,Yuhang Liu,Yan Zhao,Pran Gopal Karmaker,Jia Liu,Ya Wang,Xiupei Yang
Single-atom catalysts with atomically dispersed sites have been widely used as nanozymes for colorimetric sensing because their tunable M–Nx active centers are similar to those of natural enzymes. However, their low metal atom loading leads to insufficient catalytic activity and affects the sensitivity of colorimetric sensing, which limits their further applications. Herein, multi-walled carbon nanotubes (MWCNs) are selected as carriers to reduce the aggregation of ZIF-8 and improve the electron transfer efficiency of nanomaterials. Meanwhile, MWCN/FeZn-NC single-atom nanozymes with excellent peroxidase-like activity were prepared by pyrolysis on ZIF-8 doped with a second metal Fe. Based on the excellent peroxidase activity of MWCN/FeZn-NCs, a dual-functional colorimetric sensing platform for Cr(VI) and 8-hydroxyquinoline was established. The detection limits of the dual-function platform are 40 nM for Cr(VI) and 55 nM for 8-hydroxyquinoline. This work provides a highly sensitive and selective strategy for the detection of Cr(VI) and 8-hydroxyquinoline in hair care products, which has great application prospects in the field of pollutant detection and control.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2022
·
IF 5.876
Chao Miao,Shumei Chen,Lixing Liang,Kaixuan Shang,Jing Ouyang
In this paper, we used kaolinite tailings as raw materials to design and prepare ZSM-5 zeolite with “flower ball” morphology. Through the functional design of the material, Cr–Ce/ZSM-5 catalysts were prepared for CO 2 -assisted ethane oxidative dehydrogenation reaction (CO 2 -ODH). The folds and grooves on the surface of the “flower ball” ZSM-5 carrier act as a good anchor site for the loading of the active components, thus better anchoring Cr and Ce metal oxides , and leading to a strong interaction between the active component and the carrier. The 5%Cr–10%Ce/ZSM-5 catalyst exhibited the best catalytic performance, the conversion rate of C 2 H 6 and the selectivity of C 2 H 4 can always maintain the initial 64% and 80% within 30 h stability test at 800 °C. The existence of abundant Cr 6+ species in catalyst strengthens the binding ability of the catalyst and active oxygen species and promotes the formation-gasification process of carbon deposits on surface of the catalyst.
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CHEMOSPHERE
·
2022
·
IF 8.943
Xiao Wang,Yanshi Zhang,Yue Zhang,Chunhua Xu
Leaching and chemical reduction are two commonly used methods for Cr(VI)-contaminated soil remediation. Leaching focuses more on leaching Cr(VI) out of the soil. Chemical reduction has the disadvantages of poor fluidity of reductant. Combining these two remediation methods, this study investigated the performance of Cr(VI)-contaminated soil when H 2 O and citric acid were used as eluant separately and sulfidated zero-valent iron (SZVI) as reductant. And based on the properties of Cr(VI) chelated with –COOH to form a complex and the characteristics of –OH anchored to FeS x , citric acid modified SZVI (Cit-SZVI) was prepared. The prepared Cit-SZVI was characterized by SEM-EDS, XPS, XRD to study its surface properties. The transformation of Cr species in soil was explored by BCR sequential extraction. The results indicated Cr(VI) removal by SZVI was significantly promoted when citric acid as eluant compared with H 2 O. With SZVI dosage of 2.0 wt%, 23.1 mg/L Cr(VI) was basically removed within 60 min when citric acid as eluant, while only 60% Cr(VI) was removed when H 2 O as eluant even after 3 h. The k obs of Cit-SZVI was 1.4 times that of SZVI when H 2 O as eluant. The characterization of Cit-SZVI showed that more FeS x was formed on the surface of the Cit-SZVI, and more –OH of citric acid was anchored to FeS x , leaving –COOH available to chelate Cr(VI). Compared with H 2 O as eluant and SZVI/Cit-SZVI as reducing agent, the removal effect of Cr(VI) was the best when citric acid as eluant and SZVI as reducing agent. BCR sequential extraction showed that Cr(VI) was effectually fixed, weak acid extractable Cr proportion decreased significantly and residual Cr proportion increased in the treated soil. The combination of leaching and chemical reduction proposed in this study can greatly enhance the Cr(VI) removal effect in soil, which is important for the remediation of Cr(VI)-contaminated soil.
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WATER AIR AND SOIL POLLUTION
·
2023
·Vol. 234
·期 2
·1-16
·
IF 2.9
Kang Yongfeng,Yu Yingyuan,Zhang Bingqian,Fu Jianning,Jiang Xixi,Jia Baiyun,Men Xiaoling,Li Li
Metal–organic frameworks (MOFs) are ideal adsorbents for wastewater treatment and excellent antibacterial agents. In this study, Cu-NH 2 -MOF chitosan composite microspheres were prepared by the in situ method, and the synthesized microspheres solved the disadvantages of poor recoverability of powder adsorbent and complex operation process. Cr(VI) was removed by adsorption, and the microspheres had a good bacteriostatic effect. The synthesized MOF chitosan composite microspheres were systematically characterized. The adsorption kinetics, isotherms, and thermodynamic properties were appraised, and influences of adsorption conditions toward Cr(VI) adsorption were studied. The kinetic study demonstrated that the adsorption of Cr(VI) by CS@Cu-MOF-M conformed to the pseudo-second-order model. The adsorption isotherms fit the Sips model, and the maximum adsorption capacity of CS@Cu-MOF-M for Cr(VI) was 159.25 mg/g under optimal conditions. The thermodynamic result showed that the removal of Cr(VI) was a spontaneous endothermic process. The adsorption rate of CS@Cu-MOF-M was still more than 80% of that of the first one after four cycles of regeneration experiments. The antibacterial activity results showed that MOF chitosan composite microspheres had good antibacterial properties with MIC value of 0.2 mg/mL and MBC value of 1 mg/mL. These results demonstrated that the synthesized CS@Cu-MOF-M had a great potential to treat wastewater containing Cr(VI) and bacterial contamination. Graphical Abstract
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INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
·
2023
·Vol. 24
·期 14
·11480
·
IF 5.6
Wei Mao,Jiawen Hao,Lingyu Zeng,Hao Wang,Hao Xu,Jinghong Zhou
Herein, we report the synthesis of bimetal–organic frameworks (BMOFs) with both Brønsted and Lewis acidities, in which phosphotungstic acid (PTA) was encapsulated in BMOFs. It is efficient in converting starch to 5-hydroxymethyl-furfural (HMF) in deep eutectic solvents (DESs) such as choline chloride and formic acid. The highest yield of HMF (37.94%) was obtained using P0.5/BMOFs1.0to catalyze starch in a mixed solvent system comprising DESs and ethyl acetate (EAC) (v/v; 2:3) at 180 °C and a reaction time of 10 min. Employing a DES as a cocatalyst and solvent reduced the use of organic solvents. The catalyst showed adequate reusability, and the HMF yield only decreased by 2.88% after six cycles of reuse compared with that of the initial catalyst. This study demonstrates the application potential of BMOFs in the conversion of biomass to useful molecules with commercial and/or research value.Keywords:bimetal–organic frameworks;phosphotungstic acid;loading;cassava starch;catalysis
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Jie Xiong,Hong-Yan Zeng,Chen-Fei Liu,Jin-Feng Peng,Zhuo-Lin Yang,Wan-Ying Ji
A new approach for constructing amorphous/crystalline heterophase W-Zn(Ti)O photocatalyst was develpoed via calcination topological transformation of the self-sacrificial WO 4 2− -pillared ZnTi-LDH (WO 4 -LDH) precursor together with in-situ W-doping. The amorphous/crystalline heterophase formation could expose enriched active sites, which promoted the transfer and separation of photogenerated e − - h + pairs. Density functional theory (DFT) calculations further verified that in-situ W-doping regulated the electronic structure and reduced bandgap energy, which made the transport of photogenerated carriers more rapid. Benefiting from the construction of the amorphous/crystalline heterophase, the W-Zn(Ti)O had suitable photo-oxidation/reduction activities, achieving 99.7% removal rate for Cr(VI) reduction, 78.1% for TC oxidation, and simultaneous Cr(VI) reduction (78.0% removal) and TC oxidation (63.2% removal) for 120 min under visible-light. This work provides a new idea for the design of amorphous/crystalline heterophase nanomaterials.
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MICROCHIMICA ACTA
·
2023
·Vol. 190
·期 8
·1-11
·
IF 5.7
Zhu Liqin,Yang Fei,Lou Congcong,Zhang Xiaomei,Yang Yanzhao
Abstract A hollow porphyrin-based porous organic polymer (H-Fe-POP) was prepared for rapid and sensitive colorimetric determination of Cr(VI), which exhibited excellent dual enzyme-like activities, including oxidase-like and peroxidase-like activities. Due to the specific binding of 8-hydroxyquinoline (8-HQ) to Cr(VI), 3,3′,5,5′-tetramethylbenzidine (TMB) was liberated, and TMB was oxidized to blue ox-TMB catalyzed by H-Fe-POP. Based on the excellent oxidase-like activity of H-Fe-POP, an ultra-fast colorimetric platform for the detection of Cr(VI) was constructed, allowing the quantification of Cr(VI) in the range 2–130 μM within 30 s with a detection limit of 0.23 μM. Importantly, the sensor can accurately determine Cr(VI) in industrial wastewater, indicating its high potential for environmental monitoring. Graphical Abstract
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2022
·
IF 10.753
Yuxin Liu,Tianye Wang,Ningning Song,Quanying Wang,Yuqing Wu,Ying Zhang,Hongwen Yu
An efficient, simple, and inexpensive N, S-co-doped hydrochar (SNHC) was synthesized from waste straw by a one-pot hydrothermal process without calcination for the removal of Cr(VI). SNHC demonstrated excellent adsorption performance for Cr(VI) and high stability, achieving a high capacity of 171.33 mg/g (293 K, pH 2) and a capacity retention of 82.73 % after five cycles. The adsorption behavior was determined as a multilayer adsorption process based on chemisorption according to the simulation the results of Freundlich adsorption isotherms and pseudo-second-order models. The characterization of SNHC revealed that graphite N and thiophene S formed by the material were the effective active sites, functioning as electron donors to contribute a significant amount of electrons to reduce Cr(VI) to Cr(III). Therefore, next to electrostatic adsorption and complexation, the synergistic reduction of Cr(VI) by graphite N and thiophene S was the main mechanism for Cr(VI) removal. Additionally, density functional theory calculations indicated a low adsorption energy of thiophene S, which increased the attractive interaction between SNHC and Cr(VI) and played the most important role in reducing Cr(VI). The mechanism of the effect of graphite N and thiophene S on Cr(VI) removal not only offered a comprehensive perspective on the role of N, S co-doped mediation in hydrochar but also provided the basic theory for its practical application.
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Journal of Environmental Chemical Engineering
·
2022
·
IF 7.968
Taotao Qiang,Shaoting Wang,Longfang Ren,Xiaodong Gao
ZIF-8 exhibits poor visible light response and rapid electron-hole recombination. To address these problems, we constructed an N-CQD/ZIF-8 framework by in-situ synthesis method, then prepared a novel Z-scheme heterostructure photocatalyst (Cu 2 O/N-CQD/ZIF-8) by reduction precipitation method for the efficient photocatalytic reduction of Cr(Ⅵ). Cu 2 O/N-CQD/ZIF-8 (with a 10% Cu 2 O loading) had a unique heterostructure and exhibited significantly improved performance for Cr(Ⅵ) photoreduction . This photocatalyst successfully reduced 98.99% of the Cr(Ⅵ) in a pH = 3 solution system, which was 6 times higher than that of ZIF-8. Meantime, due to its stable interfacial adhesion, the reduction efficiency of Cr(Ⅵ) by Cu 2 O/N-CQD/ZIF-8 still reached 97.13% after five cycles. Therefore, Cu 2 O/N-CQD/ZIF-8 exhibited superior photocatalytic activity and recyclability compared with unmodified ZIF-8. The charge transfer path of this Z-scheme heterojunction was verified by free radical trapping experiments and X-ray photoelectron spectroscopy. Moreover, a possible charge transfer mechanism was proposed. N-CQD provided a potential driving force for the construction of the internal Z-scheme charge transfer system. Moreover, the synergistic effect between Cu 2 O and ZIF-8 inhibited the rapid recombination of photogenerated electron-hole pairs. This work provides potential insights for the innovative design of high-performance photocatalysts based on metal-organic frameworks for the restoration of Cr(Ⅵ)-containing wastewater.
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