APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Ruiqi Ge,Bingqiao Yang,Bing Deng,Hui Shao,Yimei Xiao,Rudolph Martin,Huihua Luo,Hanquan Zhang
The efficient removal of dolomite from phosphate ores is vital for the subsequent production of phosphate fertilizer. This work investigated the interaction mechanism of poly(sodium styrene sulfonate) (PSS) on apatite and dolomite surface and its implication on flotation through Micro-flotation, adsorption capacity, Zeta potential, SEM-EDS and density functional theory simulation. Flotation results proved that PSS was able to depress dolomite efficiently in broad pH range (8–12). Contact angle, Zeta potential, adsorption capacity and SEM-EDS measurement confirmed that PSS was more prone to adsorb on dolomite rather than that on apatite, which hindered sodium oleate (NaOL) to adsorb on dolomite but almost didn’t influence NaOL to interact with apatite surface. DFT calculations confirmed that the 2p orbital of oxygen atoms within sulfonate groups hybridized with 4s orbital of calcium and 3s orbital of magnesium atoms on dolomite surface to form O Ca, O Ca and O Mg covalent bond, while PSS weakly physisorbed on apatite via electrical interaction, due to the significant difference in steric hindrance and active atom density. PSS exhibited good selectivity and environmental compatibility as dolomite depressant in the beneficiation of phosphate ores for sustainable production of phosphate fertilizer.
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Nanomaterials
·
2019
·Vol. 9
·期 2
·172
·
IF 4.034
Xinyue Lao,Xiyu Li,Hans Ågren,Guanying Chen
Although all-inorganic CsPbX3(X = Cl, Br, I) perovskite quantum dots (PQDs) have evoked exciting new opportunities for optoelectronic applications due to their remarkable optical properties, their emission color tunability has not been investigated to any appreciable extent. In this work, double/triple CsPbX3perovskite quantum dots with precise ratios of Cl/Br or Br/I are synthesized and their luminescence (410–700 nm) is explored. A group of down-converted CsPbX3(X = Cl, Br, I) perovskite quantum dot light-emitting diode (LED) devices were constructed to demonstrate the potential use of such double/triple-halide CsPbX3perovskite quantum dots with full-spectrum luminescence. Based on density functional theory, we theoretically explored the properties of CsPbX3with double/triple anion atoms. The calculated band gaps provided strong support that the full-spectrum luminescence (410–700 nm) of double/triple CsPbX3can be realized with the change of the mixed-halide ratios, and hence that such PQDs are of potential use in optoelectronic devices.Keywords:perovskite quantum dots;light-emitting diode;density functional theory;band gap
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JOURNAL OF ENVIRONMENTAL MANAGEMENT
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2024
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IF 8
Tao Chen,Guangzhu Cao,Yi Qiang,Yanfeng Lu,Ronggao Qin,Wan Xu,Yiming Xie,Ruoyu Mao
The modified walnut shell biochar (WBC) was prepared through zinc-iron bimetallic oxide modification (ZF@WBC) at 600 °C under oxygen-limited conditions in this study. Through adsorption experiments, characterization analyses, and density functional theory (DFT) calculations, the adsorption properties of ZF@WBC to Pb (II) were investigated and the mechanism underlying such adsorption was elucidated. Characterization results showed that the surface area (375.9709 m 2 /g) and total pore volume (0.205319 cm 3 /g) of ZF@WBC were significantly greater than those of walnut shell biochar. The maximum adsorption capacity of ZF@WBC for Pb (II) was found to be 104.26 mg/g, which is 2.57 times higher than that of WBC according to the adsorption experiments conducted. The observed adsorption behavior followed both the pseudo-second-order (PSO) kinetic model and Langmuir isothermal adsorption model, suggesting that chemisorption plays a major role in the absorption process. Based on SEM, XRD, XPS, FTIR characterizations along with DFT calculations performed in this study, it can be concluded that surface complexation, ion exchange, electrostatic attraction, physical absorption are among the main mechanisms responsible for absorption of Pb (II) by ZF@WBC. Furthermore, even in the presence of interfering ions at different concentrations, ZF@WBC exhibited a removal rate above 70% for Pb (II). Therefore, ZF@WBC has great potential as an effective absorbent for removing Pb (II) from wastewater, while also offering opportunities for biomass waste resource utilization.
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CHEMICAL ENGINEERING JOURNAL
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2024
·
IF 13.3
Zhengwen Wei,Liuqing Li,Wei Wang,Wankui Ni,Xiang-fei Lü,Giuseppe Mele,Zhen-Yi Jiang
The widespread presence of harmful and stubborn amine organic contaminants in aquatic environments motivated the exploration of efficient technologies for alleviating their serious environmental crisis. Herein, the recyclable magnetic Schiff base polymer (Fe 3 O 4 -TENE) with satisfactory and promising capacity in treating aniline and 3,4-diaminotoluene as representative amine organic contaminants was fabricated via a simple in-situ polymerization method, which combined the magnetic separability advantage of magnetic oxides with the abundant aromatic carbon content properties of Schiff base polymer. Multiple characterization methods verified the effectiveness of the in-situ polycondensation coating reaction and analyzed the physicochemical properties of Fe 3 O 4 -TENE. The Fe 3 O 4 -TENE possessed abundant homogeneous reaction sites and excellent regeneration performance, multiple diffusion driving forces and micro-mechanisms co-participated in the removal reaction. The adsorption pathway, underlying reaction mechanism and the most probable bonding system were identified based on the statistical modelling and DFT quantitative calculations. Especially, the visible electrostatic potential molecular and molecular orbitals verified the π-π interaction and electrostatic forces greatly contributed to the removal reaction. The Driving forces – Challenges – Breakthrough – Application framework was proposed for comprehensively assessing the possible environmental application of Fe 3 O 4 -TENE. Overall, this work not only provides important insights into the utilization of magnetic polymer composite to alleviate ecological and environmental risks caused by amine organic pollutants, but also contributes to an in-depth excavation of the bonding types and removal mechanisms from both micro and macro perspectives.
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CHEMICAL ENGINEERING JOURNAL
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2024
·
IF 13.3
Tongqing Wu,Zhihui Hu,Jiaqi Yang,Yan Jia,Zekun Dong,Yu Tang,Yan Zhang
Textile wastewater was typically characterized by high concentrations of chloride ions, with Acid Red 14 (AR14) representing a significant pollutant. Nevertheless, research into the degradation of AR14 by electrochemical advanced oxidation processes (EAOPs) had largely overlooked the influence of chloride ions. In this regard, the EC-Chlorine-MMO/Ti system was designed, and the degradation mechanism of AR14 was subjected to meticulous investigation. The adopted anode was composed of Ti/IrO 2 -Ta 2 O 5 (mixed metal oxide, MMO). It demonstrated superior efficiency in degrading AR14 within a sodium chloride (NaCl) electrolyte, registering an apparent kinetic constant rate approximately 16.76 times greater than that observed within a sodium perchlorate (NaClO 4 ) electrolyte. The optimal chloride ion concentration was identified as 0.04 mol/L. Besides, alkaline conditions were not conducive to the degradation of AR14. It was noteworthy that the electrochemical byproducts chlorite (ClO 2 − ), chlorate (ClO 3 − ), perchlorate (ClO 4 − ), and trihalomethane (THMs) were not produced in the solution treated by the EC-Chlorine-MMO/Ti system. Electron paramagnetic resonance (EPR) spectroscopy, probe, and quenching experiments identified that hydroxyl radicals ( • OH), superoxide radicals (O 2 •− ), and dichloride radicals/chlorine monoxide radicals (Cl 2 •− / ClO • ) were the major reactive species. Of these, • OH played a pivotal role in AR14 degradation. Additionally, the three principal degradation pathways of AR14 were deduced by LC-MS analysis, UV–vis spectra, density-functional theory (DFT) calculations, and excitation-emission matrix (EEM) fluorescence spectroscopy. Furthermore, the generation mechanism of reactive species and the proposed mechanism of AR14 degradation by the EC-Chlorine-MMO/Ti system were presented. The study made a significant contribution to the understanding of the electrochemical reactions occurring in textile wastewater and provided valuable insights into the rational control of electrolytic conditions for the treatment of saline wastewater.
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Sustainable Materials and Technologies
·
2024
·
IF 8.6
Lei Guo,Yan-He Chen,Li-Mei Xu,Xiao-Lu Chen,Jin-Qiu Shen,Jian-Yong Zhang,Zhen-Jiang Liu
Herein, a fern-like p-n heterojunction by anchoring Ni 3 Fe-LDH nanoplates onto Co 3 O 4 nanoneedles have been optionally constructed. Essentially, p-n heterojunction ensured to induce strong built-in electric field, and inherit interfacial electron redistribution. Based on their compatible and well-matched electronic band structures, a staggered type-II photo-generated electron/holes transfer pathway have been elaborated by density functional theory calculation (DFT), in situ irradiation X-ray photoelectron spectroscopy (XPS), and fluorescent decay. This band bending and charge migrating module conferred the architecture with strong redox ability, sufficient exciton dissociation, and admirable optoelectronic characteristics. Moreover, the heterostructure acquired broad absorption spectrum to exhibit outperforming photocatalytic effect. Totally, this electron redistribution at the hierarchical interface, a type-II scheme charge-transfer pathway and the oxygen defects would lead to high efficiency in solar light assisted N 2 reduction. Typically, Co@Ni 3 Fe-2 catalyst exhibited the highest NH 3 production rate of 16.15 μg h −1 mg cat. −1 and Faraday efficiency (FE) of 31.57% at −0.6 V vs. RHE in 0.1 M Na 2 SO 4 solution. Fortunately, with light exposure, the NH 3 production rate and FE could increase by 27.9% and 18.1% than that under dark. This work would provide a plausible attitude towards the design of high efficient photocatalyst for artificial photosynthesis with multi-functionalized coupling effect.
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APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Guangdong Wu,Juanqin Xue,Dashi Lei,Yanyan Zhou,Zhaoyuan Cao,Kang Ren,Qiang Bi,Zhihua Leng
Currently, upconversion nanoparticles (UCNPs) based photocatalysts have been extensively developed to improve solar energy utilization. However, the mechanisms underlying interfacial energy migration of upconversion photocatalyst remain unclear. Herein, a promising composite photocatalyst with complementary properties is designed by integrating β -NaGdF 4 :Yb 3+ /Er 3+ (NGFYE), CdS and multi-walled carbon nanotubes (MWCNTs). The morphology, structure and chemical properties of NGFYE@CdS/MWCNTs ternary photocatalyst are characterized. In addition, the existence of Förster resonance energy transfer process in NGFYE@CdS/MWCNTs photocatalysts, i.e., the migration of excitation energy from Er 3+ − 4 S 3/2 excitation level and higher excitation level (e.g., Er 3+ − 2 H 11/2 ) to CdS nanoparticles, was further confirmed by density functional theory (DFT) calculations. The optimized NGFYE@CdS/MWCNTs photocatalyst presents 71.65 % and 35.29 % degradation of tetracycline hydrochloride (TCH) and ciprofloxacin (CIP) under λ ≥ 800 nm irradiation for 3 h, respectively. This work not only illustrates the interfacial energy migration mechanism between NGFYE and CdS, but also provides insights for the rapid construction of heterojunction materials with efficient energy transfer interfaces.
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MOLECULES
·
2024
·Vol. 29
·期 5
·1052
·
IF 4.2
Weiwei Wang,Zhengyao Li,Weiyao Zhu,Shaochun Hou,Chunlei Guo
The atomic-level structure and electronic properties of monazite were investigated using a first-principles method based on density functional theory (DFT). First, the geometric structure of monazite was optimized, followed by calculations of its Mulliken population, electron density, and density of states, which were subsequently analyzed. The findings of this analysis suggest that monazite is highly susceptible to cleavage along the {100} plane during crushing and grinding. When SPA was utilized as the collector, the recovery rate of monazite was higher than that when LF-P8 was used. The zeta potential and adsorption energy results indicated that the zeta potential after SPA adsorption tended towards negativity, and the adsorption energy was smaller, indicating that SPA exhibited stronger adsorption performance. LF-P8 was stably adsorbed on the monazite (100) surface via mononuclear double coordination. SPA was stably adsorbed on the surface of monazite (100) via binuclear double coordination. The results of this study provide valuable insights into the adsorption of monazite by commonly used flotation collectors. These findings are of substantial importance for future endeavors in designing flotation collectors capable of achieving selective monazite flotation.
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APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Tianyun Zhao,Qiuwan Shen,Martin Andersson,Shian Li,Jinliang Yuan
High-entropy perovskite catalyst was synthesized and utilized for the first time in the MSR catalytic reaction. Among the HEPs, La(CoCuFeAlCe) 0.2 O 3 exhibited excellent MSR activity and high selectivity. The mechanism of the MSR reaction on the catalyst (100) surface was studied by employing DFT. The results indicate that the surface of La(CoCuFeAlCe) 0.2 O 3 catalyst has the lowest energy barrier, where the aldehyde hydrogenation reaction is the rate-determining step, explaining its high activity and selectivity. This research contributes additional evidence for the creation of high-entropy perovskite catalysts for MSR.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Juntian Li,Zhiling Xu,Junhui Zhou,Xinjie Wang,Jiachun Cao,Qianyu Li,Teng Wang,Juan Li,Didi Li,Zhimin Ao
Designing multifunctional catalysts for low-temperature co-oxidation of volatile organic compounds (VOCs) and CO is challenging, as conventional catalysts cannot simultaneously achieve VOCs activation and CO poisoning resistance below 200 °C—where CO preferentially adsorbs and severely inhibits VOCs oxidation. Herein, we proposed a density functional theory (DFT)-guided atomic engineering strategy integrating d-band center modulation and adsorption energy screening to construct metal-organic frameworks (MOFs)-hosted Au-Pt single-atom alloys (SAAs). By leveraging the coordination confinement of UiO-66 to stabilize Au-Pt SAAs sites, the optimized Au-Pt SAAs/UiO-66 catalyst achieved exceptional performance in co-oxidation of toluene and CO, attaining 90 % toluene conversion at 160 °C with robust stability under CO-poisoning conditions. Mechanistic studies and DFT calculations revealed that atomically dispersed Au sites induced Pt δ− -Au δ+ charge polarization on Pt nanoparticles charge polarization via interfacial electron transfer, weakening CO adsorption while enhancing toluene activation through dual-pathway mechanisms (Eley-Rideal and Langmuir-Hinshelwood) mechanisms. This synergy decouples the traditional trade-offs between activity and stability, offering a 4.7-fold higher turnover frequency than conventional Pt catalysts. Our work established a paradigm for electronic cooperativity in MOF-hosted SAAs, providing atomic-level insights into the design of multifunctional catalysts for environmental remediation.
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Journal of Materials Chemistry A
·
2025
·
IF 9.5
Heng Lin,Zhouheng Xia,Kunpeng Xue,Xiaojing Zhou,Yifan Yao,Na Ma,Wei Dai
To address the challenge of balancing adsorption kinetics and capacity for the capture and separation of PFOA, there is an urgent need for the development of MOF materials with defect-free crystal structures and a well-defined hierarchical “micro-mesoporous” pore structure. This will enhance the performance of fast adsorption rates, high adsorp-tion capacity, and high selectivity. In this study, we report a core-shell structure UiO-66-NH2-on-MIL-101(Cr) composite material, which achieves efficient PFOA ad-sorption and exceptional environmental stability through the synergistic effects of Zr4+/Cr3+ unsaturated metal sites, the amino-functionalization of UiO-66-NH2, and the optimization of high surface area (SBET = 1927 m2/g) with a hierarchical pore structure (micro- mesoporous cooperation). Density functional theory (DFT) calculations, com-bined with XPS and FT-IR analysis, reveal that the primary adsorption mechanism in-volves strong coordination interactions between the PFOA carboxylate groups and met-al clusters (Cr/Zr-O) (Eb = -178.02/-121.72 kcal/mol), supplemented by hydrogen bonding (O-···H-N/H-O), π-CF hydrophobic interactions, and electrostatic attraction (verified by changes in Zeta potential (Δζ = 36.1 mV) and electrostatic potential (ESP)). Batch experiments show that at pH = 3, an adsorbent dose of 14 mg, and room temper-ature (298 K), the composite material exhibits remarkable adsorption capacity (qmax = 860 mg/g), following pseudo-second-order kinetics and Langmuir adsorption isotherms. Thermodynamic analysis confirms that the adsorption process is exothermic (ΔH = -16.33 kJ/mol) and spontaneous (ΔG < 0), with the entropy-driven hydrophobic effect offsetting some of the exothermic contributions. In extreme environmental tests (pH = 2/12, 100°C boiling water), the composite maintains its crystal structure and adsorption performance (XRD/SEM), exhibiting a capacity retention rate exceeding 85% after five regeneration cycles. This study presents a new strategy for designing PFOA adsorbents with dual metal node electronic synergistic and coordination microenvironment optimi-zation, multi-scale topological stability construction, and molecular recognition mecha-nisms, offering significant environmental application value.
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JOURNAL OF HAZARDOUS MATERIALS
·
2024
·
IF 12.2
Ming-Xing Li,Yan-Shu Xiong,Qi-Qi Huang,Yi-Wen Luo,Wei Wei,Hai-Qin Lu,Fang-Xue Hang,Wen Li,Fujie Liu,Kai Li
Wastewater contains various organic contaminants that pose great hazards to human health and the environment. A protein/polysaccharide-derived aerogel, namely, ICMA, was developed as a high-performance adsorbent for the simultaneous and efficient removal of diverse contaminants from wastewater, including melanoidin (MLE), Congo red (CR), and diclofenac (DIC). Metal organic framework (UiO-66-NH 2 ), as a regulatory factor, significantly improved the porosity and pore volume of the ICMA to enhance the capture performance of contaminants. The ICMA exhibited outstanding adsorption efficiency owing to the incorporation of ample polyamine functional groups and its well-developed pore structure, large porosity and pore volume, and remarkable heat resistance. The equilibrium capture capacities of the ICMA were 1364, 2031, and 539 mg/g for MLE, CR, and DIC, respectively, with corresponding removal efficiencies all exceeding 90%. Furthermore, the ICMA can capture cationic dyes through MLE/CR/DIC-bridging interactions. After five cycles, the used ICMA can still maintain a high contaminant removal rate/amount, demonstrating good reusability. The classic adsorption model showed that the capture of contaminants by the ICMA is a double-layered and heterogeneous adsorption orientation. A brand new LWAMTM model demonstrated that the adsorption mass–transfer process is jointly determined by the external mass conveyance, pore diffusion, and adsorption on the active site. Multiple characterizations indicated that the contaminant adsorption onto the ICMA was mainly facilitated by charge interactions, with H-bonds playing a secondary role. Quantum chemical theory simulations further provide insights into the atomic-level mechanisms involved in the capture of contaminants. Hirshfeld surface analysis revealed that the ICMA functions as both an H-bond acceptor and a donor during contaminant adsorption. Scale-up and upgrade adsorption were performed to treat actual/simulated wastewater, establishing the groundwork for the industrial implementation of the ICMA.
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