ChemistrySelect
·
2022
·Vol. 7
·期 46
·e202202684
·
IF 2.307
Dehui Kong,Wenyu Xie,Jinxiong Wu,Xiuling Yan,Andrei Ivanets,Lijuan Zhang,Shasha Chu,Bo Yang,Bekchanov Davronbek,Xintai Su
Graphical Here, we used a two-phase solvothermal method to prepare electroplating sludge into LDHs. the conditions for the formation of LDHs were achieved by sodium oleate intercalation and the addition of divalent metal ions to prepare a material with a layered nanostructure. The adsorption of Congo red was mainly realized by surface metal complexation, formation of hydrogen bond and electrostatic attraction. It is a challenge to achieve the harmless treatment and resourceful use of various metal elements in electroplating sludge, and converting them into functional materials has become an important technological direction. Based on the existence of various metal ions in electroplating sludge, sodium oleate intercalated Zn−Cr-LDHs (Zn−Cr-layered double hydroxides) were prepared by two-phase solution heating method. The adsorption process of the prepared LDHs for Congo red (CR) in aqueous solution can be described by Langmuir isotherm model and pseudo-second-order kinetic model and the maximum adsorption capacity is 2750.43 mg/g. The results of TEM and XPS show that the adsorption mechanism is dominated by electrostatic adsorption, ion exchange process, hydrogen bonding interaction and surface complexation. Therefore, this paper provides a strategy for recovering metal elements from electroplating sludge to prepare LDHs adsorption materials with ultra-high adsorption capacity.
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NANOTECHNOLOGY
·
2023
·Vol. 34
·期 13
·135601
·
IF 3.5
Yudan Chai,Xuedong Wei,Yufen Wang,Shuangyan Qiao
In this paper, a Cr(OH)3 NSs@ZIF67 (NSs = nanosheets) electrocatalyst is prepared on foam Ni via a simple and rapid electrochemical deposition method. Excellent electrocatalytic activity of Cr(OH)3 NSs@ZIF67 is demonstrated. It can use the overpotential of 281 mV and 390 mV respectively to drive 10 mA cm−2 and 50 mA cm−2. It is observed that the Cr(OH)3 NSs@ZIF67 electrode has the highest initial current density at 1.57 V compared with the other two monomer electrodes and shows excellent stability at the end of 60 000 s. It has the largest electrochemical activity specific surface and lowest charge-transfer resistance, and M–O bonds (M = Co, Cr) and shifting of binding energy peaks at the interface lead to more active sites and more efficient electron transfer for oxygen evolution reaction. This work highlights the construction of highly efficient composite electrocatalysts composted of low-dimensional non-precious transition metal compounds and metalorganic frameworks, promoting the development of low-cost non-noble metal composites in energy chemistry.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Ming Li,Xi Chen,Jinjin He,Shucheng Liu,Yi Tang,Xiaogang Wen
Hierarchical NiCo-LDH microspheres (NiCo-LDHM) were synthesized via a simple one-step hydrothermal process in the presence of 2-methylimidazole, and a freeze-drying technique was subsequently used to further adjust its microstructure. The obtained porous hierarchical microspheres are about 5 µm in average diameter, and consist of ultrathin nanosheets with an average thickness of 5 nm. The freeze-drying endows LDH microspheres with higher surface area and improved pore structure . The unique hierarchical porous structure, high specific surface area and positive surface charge together contribute NiCo-LDHM’ excellent capability for anionic dyes and heavy metal ions removal, its theoretical adsorption capacities for Congo red (CR), acid fuchsin (AF) and Cr(VI) are 2120, 1176 and 123 mg/g at room temperature respectively. The adsorption of pollutant molecules/ions onto NiCo-LDH microspheres conforms to the quasi-secondary kinetics model. Isotherm studies suggest that the CR adsorption onto adsorbent fits Langmiur model, while AF/Cr(VI) adsorption fits Freundlich model, indicating that the size and morphology of pollutant molecules influence the adsorption process . The adsorption is a spontaneous endothermic process and NiCo-LDHM demonstrates good recyclability, the removal rates of CR, AF and Cr(VI) can still reach 90.7%, 84.7% and 82% after five cycles, respectively. In addition, NiCo-LDH hierarchical microspheres also exhibit good anionic selective adsorption capacity in mixed-dye systems, displaying great potential for water restoration and dye recycling.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Yongli Shi,Jie Feng,Zhaoxin Zhang,Ningning Cao,Jiahao Li,Heping Li,Linji Li,Quanxian Hua,Qun Ma,Kai Zhang
Polypyrrole-based adsorbents have emerged in removing Cr(VI) from wastewater based on their reduction, chelation, electrostatic attraction and ion exchange. However, it is still a formidable challenge to remove metal cations simultaneously due to electrostatic repulsion. In fact, metal ions originating from industrial activities such as chemical manufacturing and metal electroplating are always complex and multifarious. Here, we report a EDTA-crosslinking-chitosan/polypyrrole composite (EDTA-CS/PPy) with multiple types of adsorption sites (carboxyl, hydroxyl, amino), successfully realizing simultaneous removal of Cr(VI) anions and other metal cations. The maximum adsorption capacities of Cr(VI), Cu(II), Pb(II) and Cd(II) reach up to 401.25, 59.03, 77.81 and 68.31 mg/g, respectively. The adsorption mechanism is attributed to coupling interactions of the reduction, chelation, electrostatic attraction and ion exchange between targeted metal ions and EDTA-CS/PPy, investigated by experiments and DFT theories. Notably, the adsorption capacity of EDTA-CS/PPy keeps stability after three adsorption–desorption cycles. These findings may promote potential applications of EDTA-CS/PPy adsorbents in highly efficient treatment of coexisting toxic metal ions from wastewater.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2023
·
IF 7.2
Dazhi Li,Rongfei Wang,Lingya Yi,Yunpeng Wei,Junying Li,Dantong Zhao,Wei Sun,Weihua Hu
It remains challenging to design alkaline hydrogen evolution reaction (HER) electrocatalyst able to stably operate at ampere-level current density . In this work, we successfully synthesized heterostructured Ni 3 S 2 /Cr 2 S 3 nanosheets on nickel foam (Ni 3 S 2 /Cr 2 S 3 /NF) for high current HER electrocatalysis in alkaline media . As-prepared Ni 3 S 2 /Cr 2 S 3 /NF reaches 0.5 and 1.0 A cm −2 currents at 230 and 333 mV overpotential, respectively. After 50 h test at 0.5 A cm −2 , the potential of Ni 3 S 2 /Cr 2 S 3 /NF remained almost unchanged. This impressive HER performance stems from its unique hybridization nature enabled hydrogen spillover, in which Cr 2 S 3 efficiently catalyzes the Volmer step, i.e., water dissociation to generate hydrogen, and the latter further transports to neighboring Ni 3 S 2 via spillover to facilitate the molecular hydrogen formation. This work provides a feasible strategy to synthesize efficient and durable HER catalysts for ampere-level water splitting.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Tianyu Yang,Yue Zhou,Jiamin Qi,Bin Li,Zewei Liu
Discharging pollutants containing toxic metal ions has become a global problem, and improper disposal of coffee grounds can also cause environmental pollution. In this work, 1T-MoS 2 @STC (Solvothermal Carbonization, STC) was prepared from coffee grounds and molybdenum disulfide by a one-step solvothermal method that is simple in operation, low in energy consumption and low in cost, which possesses efficient adsorption of Cr (VI) in wastewater. The 1T-MoS 2 @STC was characterized by SEM, TEM, XRD, XPS, Zeta potential, FTIR, and BET analyses. The results showed that MoS 2 was successfully loaded on coffee grounds. According to the pseudo-second order (R 2 = 0.99) kinetics model, chemisorption was the main cause of adsorption. The adsorption process followed the Langmuir (R 2 = 0.99) isothermal model, and the maximum adsorption capacity was 795.17 mg/g. The adsorption mechanism can be attributed to electrostatic interaction, redox reaction between Cr (VI) and active sites, and chelation between Cr (III) and hydroxyl. When 1T-MoS 2 @STC was applied to the treatment of actual water samples, the removal rate was also maintained at a high level (90%). In addition, 1T-MoS 2 @STC can maintain long-term stability (90 days) and low leaching of molybdenum (<3 mg/L) in wastewater. Therefore, in the treatment of chromium-containing wastewater, the 1T-MoS 2 @STC composite material simultaneously exhibited significant adsorption capacity, high interference resistance, stability and low leaching rate. This study provides a new efficient and stable Cr (VI) adsorbent and promotes the practical application of MoS 2 biomass derivatives composites in water purification.
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Catalysts
·
2023
·Vol. 13
·期 7
·1073
·
IF 3.9
Kaiwen Yuan,Bo Gong,Chundong Peng,Yanmei Feng,Yingmo Hu,Kai Chen,Daimei Chen,Derek Hao
Cr(VI) is a common heavy metal pollutants present in the aquatic environment, which possess toxic and carcinogenic properties. In this study, a solvothermal reaction was used to prepare porphyrin (TCPP)-modified UiO-66-NH2(UNT). The UNT integrated adsorption and photocatalytics in the application for dealing with Cr(VI). The photocatalytic reduction activities of UNT for Cr(VI) were investigated under visible light illumination. We found that the TCPP doping amount of 15 mg UNT (15-UNT) had a 10 times higher reduction rate of Cr(VI) than pristine UiO-66-NH2. The optimal 15-UNT photocatalyst demonstrated the highest photocatalytic activity, and Cr(VI) was completely removed within 80 min. In addition, the introduction of porphyrin not only enhanced the absorption of light but also enabled the transport of photogenerated electrons from porphyrin to UiO-66-NH2, which promoted the separation of charge carriers. Furthermore, the effects of factors such as porphyrin content, pH and light source on the photocatalytic reduction performances of UNT were also explored. Overall, this work presented a possible relationship between the crystal structures and the performance of UNT.Keywords:photocatalytic reduction;porphyrin;UiO-66-NH2;hexavalent chromium
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Membranes
·
2023
·Vol. 13
·期 7
·651
·
IF 4.2
Lu Liu,Hongyang Ma,Madani Khan,Benjamin S. Hsiao
To achieve high throughput, low-pressure drops, and high adsorption capacity of Cr(VI) and Pb(II) in industrial wastewater treatment, cellulose membranes containing cationic and anionic groups were fabricated, respectively. In this process, cost-effective cotton fabrics were oxidized using sodium periodate, followed by quaternary ammonium or sulfonation modifications. The chemical composition, surface morphology, and thermal and mechanical properties of the cellulose membranes were investigated by ATR-FTIR, solid-state NMR, SEM, TGA, and tensile experiments. Quaternary ammonium, aldehyde, and sulfonate groups were distributed on the cationic/anionic cellulose fibers as adsorption sites, which issue remarkable adsorption capability to the cellulose membranes. The highly toxic Cr(VI) and Pb(II) ions were used to challenge the adsorption capacity of the cationic and anionic cellulose membranes, respectively. The maximum adsorption capacities of Cr(VI) and Pb(II) ions were 61.7 and 63.7 mg/g, respectively, suggested by Langmuir isotherms, kinetics, and thermodynamics in the static experiments. The dynamic adsorption capability of cationic cellulose membranes against Cr(VI) ions was determined and compared with that of commercially available anionic-exchange membranes. Spiral wound filtration cartridges were fabricated by cationic and anionic cellulose membranes, respectively, and were used to adsorb Cr(VI) and Pb(II) from lab-made wastewater, respectively. The cationic cellulose cartridge can purify 4.4 L of wastewater containing 1.0 mg/L of Cr(VI) ions with a 100% removal ratio, while the pressure drop was retained at 246 Pa. Similarly, the anionic cellulose cartridge exhibited even more impressive adsorption capability; the removal ratio against Pb(II) was 99% when 8.6 L of 1.0 mg/L of Pb(II) ions containing wastewater was treated, and the pressure drop was retained at 234 Pa. A composite cartridge fabricated by the integration of cationic and anionic cellulose membranes was successfully employed to purify the wastewater containing Cr(VI) and Pb(II) simultaneously. The possible adsorption mechanism was proposed, and the recycling ability of the cellulose membranes was also discussed.Keywords:cationic/anionic cellulose membrane;oxidation;adsorption;heavy metal ions;wastewater treatment
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高影响因子
Polymers
·
2022
·Vol. 14
·期 18
·3826
·
IF 4.967
Wei Mao,Renting Huang,Hao Xu,Hao Wang,Yi Huang,Shurong Huang,Jinghong Zhou
Metal-organic frameworks (MOFs) have attracted remarkable attention for their distinguished structural designability. Precisely controlling the particle size and improving the structural stability of MOF nanoparticles influence their catalytic activity significantly. In this study, six acids (nitric, hydrochloric, formic, acetic, succinic, and citric acids) were used as modulators to prepare bimetallic MIL-101 (Cr, Sn) (MIL stands for Materials of Institut Lavoisier) via a microwave-assisted hydrothermal method. Changes in volumetric, structural, stability, and catalytic properties, size, and shape of MIL-101 (Cr, Sn) were examined using scanning electron microscopy, X-ray diffraction, thermogravimetric analysis, and N2adsorption–desorption measurements. All modulators altered the MOF properties. Compared with other samples, acetic acid as a modulator mildly altered the MOF morphology by narrowing their particle size distribution, enhancing the specific surface area, and significantly improving their water and thermal stabilities. The addition of acetic acid was suitable for the catalytic conversion of glucose to 5-hydroxymethylfurfural (5-HMF), achieving a 43.1% 5-HMF yield with 91.4% glucose conversion in a mixed solution of γ-valerolactone and saturated salt water at 150 °C after 30 min.Keywords:modulators;microwave synthesis;bimetallic MIL-101 (Cr, Sn)
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2022
·
IF 7.139
Nan Xue,Yue Zhang,Chunyan Wang,Xueyan Xue,Dandan Ouyang,Hui Zhu,Jiao Yin
Currently, it is a great challenge to improve the stability of Fe-based oxygen reduction reaction (ORR) catalysts in acidic medium, because the Fenton reaction between Fe-based catalyst and H 2 O 2 will reduce the stability of the catalyst. In this study, Fe, Cr and nitrogen-doped carbon (FeCr-N-C) was synthesized via co-impregnation of biomass walnut shells with metal precursor solutions. The FeCr-N-C catalyst has an onset potential of 0.88 V vs. RHE and outperforms the Fe-N-C catalyst in acidic media. Moreover, FeCr-N-C shows negligible activity decay (ΔE 1/2 = 14 mV) in 0.1 M HClO 4 after 20 000 cycles. The experimental results proved that the bimetal synergism can produce low yield of H 2 O 2 (<2%), which might attribute to variations of local electronic structure. The reactive oxygen species of the catalyst were analyzed by Ultraviolet-visible (UV-Vis) absorption spectra . It was proved that the presence of bimetal inhibited the Fenton reaction between Fe 2+ /Fe 3+ and H 2 O 2 , and further improved the stability of the catalysts. Hence, this study proposes an efficient strategy to facilitate the practical application of Fe-based catalysts in acidic media.
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
·
2022
·
IF 6.76
Shaojie Wu,Mingyang Li,Lili Xin,Hongming Long,Xiangpeng Gao
Conventional photocatalysts for environmental applications are mainly transitional metal compounds or precious metal nanoparticles, which suffer from weak pollutant adsorption performance, thus limited their applications for high concentrated wastewaters. In this study, asynchronous cross-linked triethylenetetramine modified sodium alginate (CFTS) was used as photocatalyst for the simultaneously catalytic degradation of Cr(VI) and metronidazole (MNZ). Experimental results suggested that asynchronous cross-linking and triethylenetetramine modification have dramatically enhanced the chemical stability as well as the adsorption and photocatalytic behavior of the material. The grafted amino functional groups and cross-linked Fe 3+ ions can promote the rapid separation and transfer of electrons, thus reducing the recombination rate of photo-generated electron-hole pairs. The optimum removal rate of Cr(VI) has reached 99.5 % and MNZ can be completely removed within 20 and 30 min at pH 1.0 under UV light irradiation, respectively. The removal mechanism of Cr(VI) by CFTS is the synergistic effect of electrostatic adsorption and photocatalytic reduction, while photocatalytic oxidation dominated the degradation process of MNZ. Moreover, the removal efficiency can be enhanced in the binary solution of these two pollutants due to the utilization of photo generated electron-hole pairs, which provides new pathways in the treatment of complicated pharmaceutical and domestic sewage wastewaters.
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JOURNAL OF SOLID STATE CHEMISTRY
·
2022
·
IF 3.656
Zirui Song,Kai Guo,Wenjuan Bai,Chengchun Tang
Heavy metals in water environment do great harm to the life and health of the public and the stability of the ecological environment. Therefore, it is necessary to find an efficient solution to deal with the increasingly serious problem of heavy metal pollution. In this paper, N, N'-methylene bisacrylamide was loaded on porous boron nitride (pBN) surface with a simple synthesis method using 3-aminopropyltriethoxysilane as a coupling agent for the adsorption of Cr(VI). The prepared adsorbents were characterized with XRD , SEM, TEM , FTIR, XPS , BET, and other analytical methods. We discovered that the capacity of pBN-AS@MBA reached 83.78 mg/g, which was significantly higher than that of pBN, with an initial concentration of 20 mg/L of Cr(VI). Besides, the chemosorption of exothermic spontaneity predominated the entire process, determined from pseudo-second-order kinetics, intra-particle diffusion model, thermodynamics, and Langmuir isotherm. Not only Cr(VI) chemically react with amine groups on the sorbent , but also elicited electrostatic attractions. The reusability of sorbent was proved with a reduction rate of lower than 20%, after a few cycles of running.
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