CHEMICAL ENGINEERING JOURNAL
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2023
·
IF 15.1
Ji Shu,Xiping Xu,Yichong Zhang,Kanming Wang,Yuanxin Zhu,Xiran Lian,Hongyu Wang
This paper describes the ferrate(VI) (Fe(VI)) activation by mineral zincite for efficient micropollutants removal such as carbamazepine (CBZ). In the Fe(VI)-zincite activation system, the zincite stimulated the Fe(V) production and impelled the Fenton reaction by preventing the transformation of Fe(II), generated from the Fe(VI), to Fe(III). Furthermore, adducts formation between Lewis sites derived from zincite and Fe(VI) induced the generation of organic radical. The mechanism was unveiled via kinetic study, reactive species identification, Fe(VI)-zincite deposit characterization and CBZ degradation products detection. Results indicated that hydroxyl radical (•OH), Fe(V) and carboxyl radical (R-COO ) contribute to the CBZ degradation in Fe(VI)-zincite system and play different roles with pH change. The optimum application condition of [Fe(VI)]:[CBZ] = 5:1, [zincite] = 5 mg/L, the zincite particle size of 500–750 mesh and pH of 7.0 was further determined. Under this condition, 91% CBZ removal and 61% mineralization were achieved by the Fe(VI)-zincite system. The feasibility of Fe(VI)-zincite system for real condition was also evaluated. The CBZ removal and mineralization were decreased 6% and 8%, respectively, suggesting that Fe(VI)-zincite system was still highly effective for CBZ degradation in real natural water. Furthermore, amphoteric property of zincite contributed to the stability of pH in deficient buffering solution, ensuring the stability of reaction activity. Importantly, this study provided new insight into the Fe(VI) activation which was not achieved by the traditional introduced reducing substance, and has potential applications for micropollutant remediation in aquatic environment.
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INORGANIC CHEMISTRY
·
2023
·
IF 4.6
Dehuo Zhou,Fuhe Le,Wei Jia,Xianhao Chen
The successful preparation of a perovskite-based heterostructure is important for broadening the applications of perovskites in the field of electrocatalysis, especially in a hydrogen evolution reaction (HER). Nevertheless, the limited active sites of perovskites severely hindered the HER properties. Herein, an in situ exsolution method was used to construct a nanocomposite based on V-doped BaCoO3−δ decorated with Ba3(VO4)2 (BVCO19) for alkaline HER. The exsolved Ba3(VO4)2 can induce more Co4+ ions on BaCoO3−δ, which serves as active sites for the release of H2. Meanwhile, by regulating the valency of V and Co species, the catalyst can reach a charge balance by generating more oxygen vacancies, which greatly facilitates the adsorption and dissociation of H2O molecules. The synergistic effect between the oxygen vacancies and high-valence Co4+ leads to an enhanced HER performance of BVCO19. The as-obtained catalyst delivers a low overpotential of 194 mV at 10 mA cm–2 as well as impressive stability for 100 h in alkaline media, which outperforms pristine BaCoO3−δ and most of the nonprecious-based perovskite oxides. This work provides new insights into the preparation of perovskite-based heterostructure for boosting HER.
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高影响因子
Analytical Methods
·
2019
·Vol. 11
·期 7
·955-964
·
IF 2.378
Lina Wang,Yong Li,Xike Tian,Chao Yang,Liqiang Lu,Zhaoxin Zhou,Yunjie Huang,Yulun Nie
Arsenic contamination in groundwater is a severe and major environmental problem that endangers public health. As such, a sensitive and selective methodology for the detection of this toxic metalloid must be urgently developed. Aldimine condensation reactions of p-phenylenediamine with salicylaldehyde derivatives yielded “turn-on” fluorescence probes (HBHP, HBBP and HMBP) for the detection of As(V) with high sensitivity. Among these, as a typical AIEgen, HBHP exhibits the highest detection sensitivity. The detection limit of HBHP for As(V) was calculated to be 0.88 ppb, which is due to its higher ability to form intermolecular hydrogen bonds to convert twisted intramolecular charge transfer (TICT) into planar intramolecular charge transfer (PICT) and its higher molecular planarity triggered by specific electronic effects. Job's plots and DFT theoretical studies indicate that HBHP binds to As(V) with a stoichiometry of 1 : 2, and the binding constant was determined using the Benesi–Hildebrand equation to be 4.26 × 104 M2. Commonly existing anions and cations in groundwater exhibited no interference with the selective detection of As(V). Spiking and recovery tests of HBHP in the presence of As(V) in actual water samples gave satisfactory experimental results. Our research would provide novel principles of molecular construction and materials for the detection of As(V) in groundwater.
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CHEMOSPHERE
·
2019
·
IF 5.108
Kunlun Yang,Yuanli Liu,Yizhou Li,Zhen Cao,Chuchen Zhou,Zheni Wang,Xurui Zhou,Shams Ali Baig,Xinhua Xu
In this study, the selective adsorption performance of different Fe-Mn binary oxides (FMBOs) towards Sb(V) in the textile wastewater under different concentrations of coexisting anions, surfactants and dyes were investigated. Results showed that the influences of different anions on the Sb(V) removal followed an order of phosphate > carbonate > sulfate > nitrate > chloride. The frequently-used organic acid of acetate was found to have insignificant effect. The coexisting surfactant with sulfonic groups could have adverse effect on the removal due to sulfonic groups could compete the adsorptive sites on Fe oxides with Sb(V). While the quaternary ammonium surfactant might have minor effect. The influences of the three widely used dyes on the Sb(V) adsorption decreased in the following order: reactive black-5 >acid orange-7> disperse blue-60, which confirmed that the dyes with sulfonic groups would have relatively higher effect. The selective adsorption capacities of Sb(V) by FMBOs followed an order of FMBO 3 > FMBO 5 >FMBO 10 > FMBO 20 >PFO. Fixed-bed column adsorption supplied useful parameters and evidently indicated that the cyclic utilization of FMBO 3 was cost-efficient for practical dynamic Sb(V) removal. The Sb(V) removal by FMBO 3 from real textile wastewater can simultaneously improve the removal efficiency, stabilize pH and prevent the increase of iron concentration as compared to the traditional coagulation, further demonstrating the high practical applicability of FMBO 3 .
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JOURNAL OF HAZARDOUS MATERIALS
·
2018
·
IF 6.434
Xiaohui Dai,Shuxin Zhang,Geoffrey I.N. Waterhouse,Hai Fan,Shiyun Ai
Layered double hydroxides (LDHs) are very promising adsorbents for the removal of anionic pollutants from water. However, the low adsorption efficiency and recycling difficulty of conventional LDH powders are obstacles to practical applications. Herein, a novel Zn/Fe-LDH composite sponge was successfully fabricated using a simple in-situ hydrothermal method. Characterization studies revealed that the composite sponge contained flower-like Zn/Fe LDH microspheres uniformly dispersed throughout a poly vinyl alcohol (PVA) sponge matrix. The specific surface area of the Zn/Fe-LDH composite sponge was 42.5 m 2 g −1 , approximately 5 times higher than the pristine PVA sponge (8.9 m 2 g −1 ). Adsorption experiments revealed that Zn/Fe-LDH composite sponge exhibited a much higher adsorption ability for As(V) anions and methyl orange (MO) compared with a Zn/Fe-LDH powder or the pristine PVA sponge. The maximum adsorption capacity for As(V) was found to be 85.7 mg g -1 . Furthermore, the Zn/Fe-LDH composite sponge showed high thermal stability, good mechanical stability and easy recoverability, thereby allowing reuse. Results guide the development of improved, low cost water treatment materials.
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Advanced Energy Materials
·
2019
·Vol. 9
·期 40
·1902279
·
IF 24.884
Huan Zhao,Yu Han,Zhuo Xu,Chenyang Duan,Shaomin Yang,Shihao Yuan,Zhou Yang,Zhike Liu,Shengzhong (Frank) Liu
The Cs-based inorganic perovskite solar cells (PSCs), such as CsPbI 2 Br, have made a striking breakthrough with power conversion efficiency (PCE) over 16% and potential to be used as top cells for tandem devices. Herein, I − is partially replaced with the acetate anion (Ac − ) in the CsPbI 2 Br framework, producing multiple benefits. The Ac − doping can change the morphology, electronic properties, and band structure of the host CsPbI 2 Br film. The obtained CsPbI 2− x Br(Ac) x perovskite films present lower trap densities, longer carrier lifetimes, and fast charge transportation compared to the host CsPbI 2 Br films. Interestingly, the CsPbI 2− x Br(Ac) x PSCs exhibit a maximum PCE of 15.56% and an ultrahigh open circuit voltage ( V oc ) of 1.30 V without sacrificing photocurrent. Notably, such a remarkable V oc is among the highest values of the previously reported CsPbI 2 Br PSCs, while the PCE far exceeds all of them. In addition, the obtained CsPbI 2− x Br(Ac) x PSCs exhibit high reproducibility and good stability. The stable CsPbI 2− x Br(Ac) x PSCs with high V oc and PCE are desirable for tandem solar cell applications.
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Polymer Chemistry
·
2018
·Vol. 9
·期 20
·2830-2842
·
IF 4.927
Mo Zhu,Nairong Hao,Jinxian Yang,Lianwei Li
V-type (B∼∼A∼∼B) and Y-type (A∼∼∼∼B2) macromonomer approaches are two of the most widely adopted synthetic methodologies for the preparation of long-subchain hyperbranched polymers (LHPs) with a controlled subchain length. However, little attention has been paid to the difference of the structural regularity of hyperbranched polymers prepared via the two approaches in previous related studies. This work aims to elucidate how these two synthetic approaches quantitatively influence the polymerization, branching pattern and solution properties of the prepared hyperbranched polymers. First, two sets of model hyperbranched polystyrenes (HPSV and HPSY) were prepared from V-type and Y-type macromonomers by a combination of atom transfer radical polymerization (ATRP) and azide–alkyne cycloaddition coupling reaction, respectively. The intrachain cyclization study indicated that the macromonomer self-cyclization during the interchain coupling process was strongly affected by the chain length and the structure of the used macromonomer as well as the reaction concentration. The V-type macromonomer was found to be less inclined to undergo interchain coupling due to the stronger steric hindrance effect. Furthermore, via triple-detection size exclusion chromatography (TD-SEC) characterization, the intrinsic viscosity ([η]) and the radius of gyration (Rg) were found to be scaled to the molar mass of the macromonomer (Mm) and the molar mass of the entire chain (Mt) as [η] = KηMtνMmμ (μ ≃ 0.25 and ν ≃ 0.40) and Rg = HRMtαMmβ (α ≃ 0.47 and β ≃ 0.083) for both HPSV and HPSY samples. These scaling relationships evidenced that both HPSV and HPSY hyperbranched structures hold a similar statistically fractal feature. More importantly, the determined values of ratios Kη,Y/Kη,V (∼1.5) and HR,Y/HR,V (∼1.2) demonstrated, for the first time, that the average equivalent length of the branching subchain (Ls) for HPSY is much longer than the initial macromonomer chain length (Lm), i.e. Ls = 2.5Lm while Ls is exactly equal to 1/2Lm for HPSV. This finding clearly clarified the difference between Ls and Lm, and thus the terms of Ls and Lm should not be misused in the future structure–property study. Finally, the value of the Rg/Rη ratio is determined to be ∼1.05 and ∼1.15 for HPSV and HPSY samples (Rη: viscometric radius), respectively, which are much smaller than the typical values for linear chains in good solvents (1.20–1.40), revealing the less draining nature of these hyperbranched structures.
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Desalination and Water Treatment
·
2024
·
IF 1
Shifeng Li,Tiankuo Zang,Xiaoyun Yang,Min Xiao,Haibo Wang,Shuhua Yao,Zhongliang Shi
The utilization of waste melamine-formaldehyde foam to produce value-added carbon foam has been identified as a promising approach to polymer recycling. Nickel-Iron layered double hydroxides (NiFe-LDHs) and its complex oxides (NiFe 2 O 4 ) were synthesized in this study through a hydrothermal method, growing in situ on the above-mentioned carbon foam substrate. Comparative analysis revealed that CF@NiFe 2 O 4 exhibited superior removal efficiency compared to CF@NiFe-LDHs. Furthermore, arsenate adsorption on CF@NiFe-LDHs and CF@NiFe 2 O 4 conformed more to the pseudo-second-order model; meanwhile, the isothermal adsorption characteristic fitted the Langmuir isothermal model better. The negative ΔG (free energy changes, <−37.68 kJ/mol) and positive ΔH (enthalpy change, 7.64 kJ/mol) indicate that it is spontaneous and endothermic for As(V) to adsorb on CF@NiFe 2 O 4 . Potential mechanisms such as surface complexation, electrostatic interaction, and hydrogen bonding were suggested. This innovative approach offers a novel method for utilizing LDHs-based adsorption materials and recycling waste polymers.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Xin Ke,HuiPing Shao,HaiHong Liu,Wengang Liu
In this study, an Fe-La-CS adsorbent with a reticulated structure was prepared by an in situ method, which was able to adsorb arsenate efficiently over a wide pH range of 3–11. The incorporation of iron and lanthanum ions broadened the tolerant pH range of the adsorbent compared with chitosan beads (CS). Arsenic was mainly present in the pH range of 3–9 as two forms, H 2 AsO 4 − and HAsO 4 2− . Calculations using the density-functional theory (DFT) showed that in the Ligand interactions and electrostatic interactions dominate in the pH range, with surface precipitation, and hydrogen bonding interactions playing a facilitating role. The background ions mainly compete with arsenic adsorption for electrostatic interaction sites. However, due to the different valence states of the background ions, the competition intensity is different. Such as low valence state representative ions Na + , K + competitiveness is weak, and arsenic competition adsorption first occupy different adsorption sites, therefore, from the quantum chemistry and molecular dynamics point of view of Na + , K + on arsenic adsorption almost no effect. Cl − , SO4 2− will have some influence on arsenic adsorption because of the same charge with arsenic, but the charged amount is smaller than arsenic and the molecular structure is different from that of arsenic, so the influence is not very big. In summary, the material design of Fe-La-CS adsorbent has great potential and theoretical significance for selective purification of heavy metal wastewater at wide pH.
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ENERGY & FUELS
·
2024
·
IF 5.2
Lan Li,Tingxue Fang,Fuming Lai,Xinyue Li,Tingting Qu,Lin Wang,Xiaoshi Lang,Kedi Cai
Vanadium pentoxide (V2O5) is regarded as a promising sulfur-wrapped matrix for high-performance lithium–sulfur batteries, owing to its desirable structural and functional characteristics. In this paper, a large number of defective sites arise in the vanadium pentoxide structure via a codecoration strategy of the V, O sites, which is more beneficial to improving the electroconductivity and allows for the uniform loading of sulfur on the surface, thereby reducing the polarization resistance and elevating the kinetic rates during the electrochemical reaction. Electrochemical test results indicate that Mg2+/S-codecorated V2O5/S composite cathodes have 1131.15, 942.39, and 804.71 mAh·g–1 of discharge-specific capacities at 0.1, 0.2, and 0.5 C rates, respectively, with the lowest charge/discharge plateau voltage difference, and the capacity retention rate after 140 cycles can be 57.95%. Besides that, the multidefect V2O5 can effectively promote the adsorption strength of lithium polysulfide and catalytically accelerate the rate of liquid-phase conversion between lithium polysulfide so as to achieve the stable electrochemical properties for sulfur composite cathodes.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Xuli Hu,Zhen Zhang,Zhenyao Li,Yushan Wu,Wei Wei,Yao Wang,Junchen Xu,Mingyue Ding
Regulating oxidation state of Cu-based chalcogenides catalysts during electrolysis is of great significance for efficient CO 2 electrochemical reduction reaction (CO 2 RR) to methanol, which still remains a dramatic challenge. Herein, we construct a heterogeneous Cu 3 VS 4 /CuS electrocatalyst (denoted as CuV x S), in which the in-situ growing Cu-S-V bonds avoid the accumulated electrons on oxidized Cu sites and inhibit the deep reduction of CuS to metallic Cu during electrolysis, maintaining stable and abundant reactive Cu + /Cu 2+ species to promote CO 2 RR performance to methanol. By this design, the CuV 0.1 S catalyst achieves an ultrahigh methanol selectivity of 79.8 %. In-situ FTIR measurement reveals that the synergistic effect of Cu + /Cu 2+ species and Cu-S-V bonding facilitates the *CO adsorption and the subsequent *CO hydrogenation process, which improve the generation of *CHO and *OCH 3 intermediates for enhanced methanol selectivity. This work provides a new insight into stabilizing high oxidation state of Cu-based electrocatalyst to maintain sufficient active sites for CO 2 RR.
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Advanced Energy Materials
·
2018
·Vol. 8
·期 31
·1802346
·
IF 21.875
Jialong Duan,Yuanyuan Zhao,Xiya Yang,Yudi Wang,Benlin He,Qunwei Tang
All-inorganic cesium lead bromide (CsPbBr 3 ) perovskite solar cells have attracted enormous attention owing to their outstanding stability in comparison with organic–inorganic hybrid devices. The greatest weakness for inorganic CsPbBr 3 solar cells is their lower power conversion efficiencies, mainly arising from inferior light-absorbance range and serious charge recombination at interfaces or within perovskite films. To address this issue, the lattice doping of lanthanide ions (Ln 3+ = La 3+ , Ce 3+ , Nd 3+ , Sm 3+ , Eu 3+ , Gd 3+ , Tb 3+ , Ho 3+ , Er 3+ , Yb 3+ , and Lu 3+ ) into CsPbBr 3 films for all-inorganic solar cells free of hole-transporting materials and precious metal electrodes is presented. Arising from the enlarged grain size and prolonged carrier lifetimes upon incorporating Ln 3+ ions into perovskite lattice, the performances of these inorganic CsPbBr 3 solar cell devices are significantly enhanced, achieving a champion efficiency as high as 10.14% and an ultrahigh open-circuit voltage of 1.594 V under one sun illumination. Meanwhile, the nearly unchanged efficiency upon persistent attack by 80% RH in air atmosphere over 110 d and enhanced thermal stability at 80 °C over 60 d provide new opportunities of promoting commercialization of all-inorganic CsPbBr 3 perovskite solar cells.
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