CHEMICAL ENGINEERING JOURNAL
·
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
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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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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PubMed
高影响因子
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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MICROPOROUS AND MESOPOROUS MATERIALS
·
2021
·
IF 5.455
Hao Guo,Huifang Li,Chuanyong Jing,Xinbo Wang
Adsorbents have been a long-standing territory of insoluble solid materials in the field of adsorption technique for organic pollutants removal from wastewater. While the robust porous frameworks with high surface areas can give high uptakes and good sorption kinetics, their practical applications are impaired as fouling and sorbent attrition always occur and decay their performance. Here, we describe a simple approach based on the permanently microporous polymer, PIM-1, overcoming the above mentioned issues. PIM-1 demonstrates comparable adsorption capacity to the state-of-the-art phenolic pollutant adsorbents, with the benefit that PIM-1 is resistant to water but soluble in common organic solvents , making it eminently viable for fabrication into different morphologies, and permitting reuse after simple treatments if fouled or blocked. Additionally, PIM-1 presents pH controlled high selectivity for different phenols and low pollutant residue ability to achieve the safety stand of drinking water . DFT calculation revealed that H-bonding between the CN groups of PIM-1 and the phenoxy groups played a critical role for adsorption. This work opens new window of using soluble polymer with microporosity as adsorbents.
研究领域:
环境科学
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材料科学
·
化学工程
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2021
·
IF 4.539
Rongchuang Geng,Hanxiao Tang,Qiujuan Ma,Luping Liu,Weisheng Feng,Zhijuan Zhang
In this work, a series of bimetallic Ag/Zn-ZIF-8 materials were successfully developed for sensing toward traces of Fe 3+ and Cu 2+ . The bimetallic Ag/Zn-ZIF-8 was synthesized via a one-pot method. Interestingly, this obtained bimetal Ag/Zn-ZIF-8 exhibited high photoluminescence property and excellent fluorescence quenching response to target analytes with high selectivity , sensitivity and detection limits of 3.9 μM for Fe 3+ , 6.7 μM for Cu 2+ ions, respectively, both of which have been confirmed to be very comparable or better than the reported LMOFs sensors. The possible photoluminescence quenching mechanisms were studied in detail, revealing that the competitive absorption of excitation source and resonance energy transfer (RET) resulted from the host (imidazole of the framework, Lewis basic sites)-guest (metal ions of Cu 2+ and Fe 3+ , Lewis acid sites) interaction should be responsible for high efficiency fluorescence quenching. The binding energies of metal ions adsorption on the ZIF-8 obtained by DFT simulation were further performed to explain the higher quenching effect of Fe 3+ than Cu 2+ .
研究领域:
材料科学
·
分析化学
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纳米技术
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Nature Communications
·
2020
·Vol. 11
·期 1
·1-7
·
IF 12.121
Yu Fei-Yang,Lang Zhong-Ling,Yin Li-Ying,Feng Kun,Xia Yu-Jian,Tan Hua-Qiao,Zhu Hao-Tian,Zhong Jun,Kang Zhen-Hui,Li Yang-Guang
The oxidized platinum (Pt) can exhibit better electrocatalytic activity than metallic Pt 0 in the hydrogen evolution reaction (HER), which has aroused great interest in exploring the role of oxygen in Pt-based catalysts. Herein, we select two structurally well-defined polyoxometalates Na 5 [H 3 Pt (IV) W 6 O 24 ] (PtW 6 O 24 ) and Na 3 K 5 [Pt (II) 2 (W 5 O 18 ) 2 ] (Pt 2 (W 5 O 18 ) 2 ) as the platinum oxide model to investigate the HER performance. Electrocatalytic experiments show the mass activities of PtW 6 O 24 /C and Pt 2 (W 5 O 18 ) 2 /C are 20.175 A mg −1 and 10.976 A mg −1 at 77 mV, respectively, which are better than that of commercial 20% Pt/C (0.398 A mg −1 ). The in situ synchrotron radiation experiments and DFT calculations suggest that the elongated Pt-O bond acts as the active site during the HER process, which can accelerate the coupling of proton and electron and the rapid release of H 2 . This work complements the knowledge boundary of Pt-based electrocatalytic HER, and suggests another way to update the state-of-the-art electrocatalyst.
研究领域:
电化学
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催化
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材料科学
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Inorganic Chemistry Frontiers
·
2021
·Vol. 9
·期 2
·249-258
·
IF 6.569
Fangfang Chang,Yongpeng Liu,Qing Zhang,Zhichao Jia,Xiaolei Wang,Lin Yang,Zhengyu Bai
The electrocatalytic activity of nanoalloy catalysts could be effectively manipulated by tuning their intrinsic physical and chemical properties (e.g., compositions, facets, lattice strain, morphologies, etc.). However, it still remains a challenge how to integrate these beneficial physical and chemical properties to promote the electrocatalytic performances for anode and cathode reactions in fuel cells. Herein, highly catalytic PtnCu100−n catalysts with many active sites were synthesized through optimizing the compositions of precursors and reaction conditions and a surfactant-free thermal solvent method, which showed a subtle lattice strain. Transmission electron microscopy and X-ray diffraction results revealed that the lattice strain of PtnCu100−n alloy nanostellates could be modulated by the alloy compositions. Electrochemical results showed that the high catalytic activity of PtnCu100−n alloy nanostellate catalysts for both the oxygen reduction and alcohol oxidation reactions was related to lattice shrinkage, facets and bimetallic compositions. Interestingly, Pt69Cu31/C nanostellate catalysts with lattice shrinking revealed the maximum activity and stability compared with other compositions and commercial Pt/C, which was also supported by DFT results. This study will provide a new path for the design of robust and active nanoalloy catalysts with lattice mismatch and dominant active facets for both the cathode and anode reactions in fuel cells.
研究领域:
材料科学
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电化学
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催化
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能源材料
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ChemPlusChem
·
2024
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IF 3
Yong Wang,Xueying Lin,Xianyu Ying,Shan Hu,Hongjun Zhu
A facile C–H amination of quinazoline employing N-fluorobenzenesulfonimide (NFSI) as the amination source has been disclosed in the absence of any metal, oxidant or additive. The methodology shows a board range of quinazolines with different functional groups in moderate to good yields up to 87%. Furthermore, gram-scale reaction, desulfonylation to amine and synthesis of pharmaceutical intermediate were also investigated, which demonstrates potential applications in medicinal chemistry. A plausible amination mechanism is proposed via F+ transfer accompanied by the removal of one molecule of PhSO2F. DFT studies with experimental work suggest that the mechanism via F+ transfer is more favorable than the free radical one.
研究领域:
有机化学
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药物化学
·
合成化学
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Wen He,Qianxiang Xiao,Zhenglemei Qiu,Feng He,Qixu Chen,Lijun Hu,Hongqing Wang
Photocatalysis has been applied to the reduction of U(VI), but how to improve the separation of photogenerated carriers, realize photocatalysis without sacrificial agents, and still have a certain catalytic activity in the absence of light are still problems that need to be solved. In this paper, a series of Zn x Cd 1-x S (0 ≤ x ≤ 1) solid solutions with different Zn/Cd molar ratios are synthesized for piezo-photocatalytic reduction of U(VI) under air atmosphere and without the addition of sacrificial agent. Under combined visible light and ultrasound irradiation, the homojunction with bicrystalline structure, i.e., wurtzite (WZ) and zinc-blende (ZB) formed from Zn 0.7 Cd 0.3 S solid solution , provides effective space charge separation and exhibits a prominently synergetic piezo-photocatalytic U(VI) removal rate of 99.3 % for 15 min, which is 34.2 times higher than that of ultrasound alone (2.9 % in 15 min) and 1.2 times greater than that of light alone (80.7 % in 15 min). Meanwhile, the charge transfer in Zn 0.7 Cd 0.3 S homojunction was revealed in this study through DFT calculations and a mechanism for the piezo-photocatalytic synergistic reduction of U(VI) was proposed. This work promises to provide a new coupled catalytic reaction design strategy for the efficient reduction of U(VI).
研究领域:
环境科学
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材料科学
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催化
·
核废料管理
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Journal of Physical Chemistry C
·
2025
·
IF 3.2
Qiuchen Yang,Yamei Xu,Ziluo Ding,Ruijun Hou
PdCu bimetallic catalysts can enhance both selectivity and activity simultaneously in the selective hydrogenation of 1,3-butadiene, although the mechanism behind the enhanced performance of the PdCu catalysts remains insufficiently understood. The presence of mixed and disordered alloy phases on the bimetallic catalyst surface hinders the identification of the intrinsic reaction mechanism. In the current work, catalysts with well-defined Pd, Pd1Cu1, Pd1Cu3 alloy phases were controllably synthesized to investigate the selective hydrogenation performance of 1,3-butadiene. It is found that Pd1Cu1/SiO2 and Pd1Cu3/SiO2 exhibit not only higher intrinsic activity but also higher selectivity toward total butenes and 1-butene than Pd/SiO2 due to the electronic effect, which becomes more significant with increasing Cu/Pd. Furthermore, ideal Pd(111), Pd1Cu1(111), and Pd1Cu3(111) surfaces were modeled by DFT calculations to conduct theoretical studies. It is found that the electronic effect is more significant and the adsorption energy to butenes decreases with increasing Cu/Pd ratio. By analyzing the transition states of the elementary reactions in the reaction pathways, the reaction mechanisms are revealed on different surface sites. It is indicated that the bimetallic PdCu surfaces exhibit higher intrinsic hydrogenation activity and higher selectivity to total butene and 1-butene, in agreement with the experimental results.
研究领域:
催化化学
·
材料化学
·
表面科学
·
理论化学
·
纳米催化
·
能源化学
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