FUEL
·
2024
·
IF 6.7
Ranlei Shao,Lu Zhang,Luyuan Wang,Jianmei Wang,Xingyu Zhang,Shiwang Han,Xingxing Cheng,Zhiqiang Wang
In this study, Ru catalysts supported on Ce-Al composite carriers were prepared using the precipitation-hydrothermal method, significantly enhancing ammonia decomposition efficiency. The test results show that the Ru/3Ce-Al catalyst, with a Ru loading of only 0.8 wt%, achieves a reaction rate of 14.17 mmol g cat −1 min −1 at 500 °C, and reaches a 95 % conversion rate at 525 °C. No decline in efficiency was observed after 48 h of durability testing, which significantly reduces the usage of Ru. The RuO 2 particle size in the samples was only 2–4 nm. Ce-Al composite increased the specific surface area and pore volume of the catalyst, facilitating the uniform distribution of Ru. Additionally, it increased the number of surface acidic sites and strengthened the metal-support interaction. The unique low redox potential and oxygen vacancies of CeO 2 allowed for faster electron transfer to the Ru surface. DFT calculations revealed that bridge site adsorption was more stable, with the rate-determining step of the ammonia decomposition reaction being the formation of N 2 . Ce-Al composite catalysts enhanced NH 3 adsorption strength and lowered the reaction energy barrier.
研究领域:
催化化学
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材料科学
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理论计算
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Qian Liu,Kangping Cui,Minshu Cui,Shijie Sun,Haiyang Li
As a green photocatalyst with simple synthesis method, excellent electronic structure, and metal-free properties, the deficiencies of pristine graphitic carbon nitride, such as high electron transfer resistance and narrow energy band gap, inhibit its photocatalytic activity to some extent. In this paper, we synthesized a sulfur and chlorine co-doped g-C 3 N 4 (SCl-CN) capable of efficient photocatalytic activation of peroxymonosulfate (PMS) by calcining a mixture of ammonium chloride and thiourea. By means of DFT calculation, the contribution of sulfur and chlorine to photogenic electron hole separation was discussed. The electrostatic potential of SCl-CN and the adsorption model between SCl-CN and PMS were deduced, and the activation mechanism of PMS was further analyzed. According to the calculated results, the incorporation of sulfur and chlorine tuned the electronic configuration of the material and intensified the interactions between SCl-CN and PMS. It is shown that free and non-free radicals act simultaneously in the SCl-CN/PMS/Vis system. This study provides a new idea for the study of photocatalytic activation of PMS by non-metallic co-doped carbon nitride.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
·
2022
·Vol. 29
·期 16
·e202203142
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IF 5.02
Jingwen Luo,Anqi Huang,Yao-Yue Yang,Xing-Yu Ma,Quan-Liang Chen,Junxian Chen,Yajuan Wu
Graphical Put to good use : A Pd-doped Co (Pd/Co) catalyst with high Pd atom utilization efficiency was designed and prepared for hydrogenation of nitroarenes. Its catalytic activity was much better than commercial Pd powder (>150 times) in nitrobenzene hydrogenation reaction. This work might provide a simple and low-cost methodology to design and synthesize highly efficient catalysts. Enhancing catalytic performance as well as reducing catalyst cost are the eternal pursuit for the catalysis community. Herein, a simple and effective palladium-doped cobalt (Pd / Co) catalyst with high Pd atom utilization efficiency was synthesized via galvanic replacement reaction for the selective hydrogenation of nitrobenzene with H 2 at room temperature, delivering >99 % yield of aniline with up to 158 times higher catalytic activity than commercial palladium powder. Detailed characterizations and DFT calculations revealed that Co−Pd interaction leads to a decrease in electron density of Pd and the distance between Pd atoms that results in the enhanced catalytic performance. Further experiments indicated that the Pd / Co catalyst serves as a highly efficient, selective, and recyclable catalyst for a range of nitroarene substrates. This work might provide a green and sustainable methodology to design and synthesize highly active catalysts with high utilization efficiency of the noble metals in fundamental and applied research.
研究领域:
催化化学
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材料科学
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理论计算化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Yan-nan Wang,Jin Li,Zhenyu Yuan,Fanli Meng
An optical fiber toluene gas sensor working at room temperature is proposed based on CQDs@SiO 2 (-OH) porous film. The CQDs@SiO 2 (-OH) porous film was elaborated on the surface of the hollow core fiber (HCF) using the templating method, where the evanescent field is excited by a misaligned structure. The precursor solution formed by mixing CQDs with SiO 2 (-OH) enhances CQDs dispersion within the film, preventing aggregation and preserving active sites. Experimental results indicate that the gas-sensitive layer doped with CQDs demonstrates a sensitivity of 5.1 pm/ppm to toluene gas at room temperature, which is approximately 3.13 times greater than that of the SiO 2 (-OH) porous film. Additionally, it demonstrates a response time of 12 s and a limit of detection (LOD) of 3.9 ppm. The gas sensing mechanism is thoroughly investigated using DFT, exploring the electronic distribution of the gas-sensitive layer before and after CQDs doping and analyzing the sensitization mechanism. This study presents a novel approach for toluene gas detection at room temperature using an optical fiber sensor.
研究领域:
化学传感器
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材料科学
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光学工程
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Lan Wang,Chen Hou,Lingfeng Luo,Biao Xiang,Zhiqiang Zhu,Chuanyi Wang
The sluggish Fe(III)/Fe(II) conversion in the Fenton reaction strongly restrains the continuous generation of reactive oxygen species towards the oxidation of refractory pollutants. Herein, an ultrathin 2D/2D FeSi/GLC hybrid architecture is constructed by confining graphite-like carbon (GLC) in the layered-nanospace of Fe-bearing beidellite (FeSi) silicate for efficient photo-Fenton-like catalytic degradation of refractory pollutants. The 2D space-confinement effect of FeSi realizes the graphitization of carbonated glucose, in turn enhancing the electrical conductivity and visible-light harvesting ability of FeSi. By integrating the experimental and DFT calculation results, two pathways of Fe(II) recovery for enhancing Fenton oxidation are proposed: 1) GLC as electron-transfer channels significantly accelerates the photogenerated electrons transfer for Fe(II) reduction from Fe(III), as well as enhances electron shuttle from Fe(II) sites to H 2 O 2 , thus strongly promoting the cleavages of H 2 O 2 into •OH; 2) GLC mediates electron transfer from H 2 O 2 to Fe(III), boosting the regeneration of Fe(II) accompanied by •O 2 − production. As a demonstration, the hybrid FeSi 1.0 /C0.3–500 exhibits high-efficiency performance in photo-Fenton reaction with impressive catalytic activity (0.82 min −1 ), over 410 and 150 times faster than its analogue carbon-free system and commercial Fe 3 O 4 using phenol as the probe, respectively, accompanied by the mineralization of 74.4 % in 60 min. Additionally, the reaction system could remove 80 % of chemical oxygen demand (COD) from real coal chemical wastewater (200 mg·L −1 ) during 300 min of continuous operation. This study offers a new perspective for developing high-performance photo-Fenton catalysts, also confirms a promising practical application potential in industrial wastewater treatment.
研究领域:
环境科学
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材料科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
HYDROMETALLURGY
·
2023
·
IF 4.7
Hongrui Xiang,Zhihui Yang,Xiaobo Min,Yanjie Liang,Cong Peng,Xiaoyun Liu,Rui Yuan,Qingwei Wang,Feiping Zhao
The recovery of germanium (Ge) from zinc residue leachate has attracted increasing attention. Herein, this study report on the development of a tartaric acid functionalized chitosan (TA-CS) material serving as an efficient adsorbent for Ge(IV). The introduction of TA resulted in abundant protonatable hydroxyl and carboxyl groups , which endows materials with excellent buffering capacity under acidic conditions. Adsorption kinetics and isotherms showed a fast and efficient adsorption capacity of 57.28 mg/g for Ge(IV). In binary systems, Ge(IV) was preferentially adsorbed over Zn(II), a major coexisting ion, with a separation factor of 3.22. The SEM–EDS FT-IR, XPS and DFT results revealed that mechanisms in combination, including electrostatic adsorption, complexation, hydrogen bonding, and ion exchange, promoted the immobilization of Ge(IV) on TA. The TA-CS material also exhibited great reusability with an adsorption efficiency of 70% after 3 recycles. For the recovery of Ge(IV) in practical zinc residue leachate, the TA-CS material showed superior affinity toward Ge(IV) and a 10-fold higher of adsorption capacity compared to that of pristine chitosan. Together, TA-CS demonstrates that it is a viable and economical material for the separation and preconcentration of Ge(IV) from zinc residue leachate.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2022
·
IF 7.139
Run Zhang,Youling Hou,Gangqiang Fan,Dejun Huang,Xiaoming Ding,Jie Dang
The utilization of titanium-bearing blast furnace slag (TBFS) has been widely concerned, which is mainly related to the recovery of titanium resources. In order to realize the efficient and clean recovery of titanium resource, the main titanium-bearing phases (CaTiO 3 , MgTiO 3 and Mg 2 TiO 4 ) in TBFS with high content of MgO were investigated in CH 4 –H 2 system in this work. Thermodynamic calculation indicated that CaTiO 3 , MgTiO 3 and MgTi 2 O 4 could be ultimately reduced to TiC x O y at 1300 °C, 1200 °C and 1200 °C respectively. The reduction experiments were carried out in flowing CH 4 –H 2 , which considered the influences of time, temperature and addition, the results of which showed that the optimal reduction temperatures of CaTiO 3 and MgTiO 3 were 1400 °C and 1200 °C respectively. DFT calculation results also confirmed that MgTiO 3 had stronger CH 4 adsorption capacity than CaTiO 3 and Mg 2 TiO 4 . However, Mg 2 TiO 4 could not be reduced completely even at 1450 °C, because excessive MgO in the reduced products prevented further reaction in kinetics. Both increasing temperature and adding iron oxides contributed to the reduction kinetics . The results suggested that the appropriate increase of the proportion of MgO in TBFS was beneficial to titanium extraction. This work provides a way to develop new process to extract titanium from TBFS, especially the slag with high MgO.
研究领域:
冶金工程
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Kun Xu,Zhijia Zhu,Chunyan Hu,Jian Zheng,Huitao Peng,Baojiang Liu
There is currently plenty of emphasis on measures to handle the water pollution spurred on by the misuse of antibiotics. Given its exceptional degradation accomplishment, periodate (PI), a steady solid oxidant, has promising future applications in the breakdown of antibiotics. In this research, PI was activated with UV/CoFe 2 O 4 (CFO) for the first time in an attempt to eliminate oxytetracycline (OTC). The UV/CFO/PI system eliminated 30 mg∙L -1 OTC with a removal effectiveness of almost 100 % in 12 min (OTC 30 mg∙L -1 , CFO 0.2 g∙L -1 , PI 2 mM, pH 5.5). In addition, the ferromagnetism of the CFO assisted to the system's remarkable cycling achievement, with 85.9 % of the OTC still removed after ten cycles. Various organic contaminants, which include reactive blue KN-R (KN-R), ciprofloxacin (CIP), chlortetracycline (CTC), and levofloxacin (LVX), further demonstrated the UV/CFO/PI system to be useful for degrading. The primary active substances for OTC elimination were revealed and recognized through scavenging experiments and EPR analysis as h + , •IO 4 , •IO 3 , 1 O 2 , •OH, and •O 2 – . Simultaneously, redox cycles of Fe(III)/Fe(II) and Co(III)/Co(II) were also observed by XPS test to hasten OTC deterioration. It appeared that this system may be a green approach for antibiotic elimination by investigating the degradation route of OTC and the influence it has on the surroundings employing FuKui functions, LC-MS, and toxicological analysis software (T.E.S.T.), respectively. Additionally, we observed that the CFO (2 2 2) crystal surface has the best adsorption impact on PI by computing Eads from DFT.
研究领域:
环境科学
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化学工程
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材料科学
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毒理学
✓ 已验证
产品关联
DOI
高影响因子
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2018
·Vol. 20
·期 22
·15192-15202
·
IF 3.906
Jinggao Wu,Maowen Xu,Chun Tang,Guannan Li,Hong He,Chang Ming Li
F-Doping effects on polyaniline-derived carbon coated Li3V2(PO4)3 (Li3V2(PO4)3−xFx@C) as a cathode for high performance Li rechargeable batteries are systematically investigated with a combined experimental and DFT theoretical calculation approach. The results clearly indicate that the doping amount has a significant impact on the rate capability and long cycle life. The optimal material (Li3V2(PO4)2.88F0.12@C) delivers 123.16 mA h g−1@2C, which is close to the theoretical value (133 mA h g−1), while showing a greatly improved cycle stability. Rietveld refinements show that the F− doping does not obey Vegard's Law, which may be attributed to the generated lower valence of V ions. AC impedance spectroscopy shows that the F-doping can achieve faster interfacial charge transfer for higher reaction reversibility. DFT calculations confirm that the lower V2+ (t2g↑)3 does exist in Li3V2(PO4)2.88F0.12, and the mean nearest neighbor Li–O bond length also increases for faster electrochemical kinetics, and further reveal that there is a tendency for a transition from the insulator to the n-type semiconductor due to the F dopant. The combined experimental and calculated results suggest that F-doping indeed greatly facilitates the charge transfer rate of the Li+ insertion/de-insertion process for better reversibility and enhances the Li+ diffusion rate to access the reaction sites, thus resulting in high rate capacity and cycling stability. This work not only offers a facile and effective approach to synthesize high performance Li-ion battery material for very promising practical applications, but also discloses scientific insights on element coating and doping to guide the electrode material design for fast electrode kinetics in energy storage devices.
研究领域:
材料科学
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电化学
·
理论计算
✓ 已验证
DOI
PubMed
高影响因子
Chemical Science
·
2023
·Vol. 14
·期 25
·7016-7025
·
IF 8.4
Xiuping Yin,Xinxing Li,Xuyi Li,Malgorzata Biczysko,Shourong Zhu,Jiaqiang Xu,Yue-Ling Bai
The dark-colored viologen radical cations are unstable in air and easily fade, thus greatly limiting their applications. If a suitable substituent is introduced into the structure, it will have the dual function of chromism and luminescence, which will broaden its application field. Here, Vio1·2Cl and Vio2·2Br were synthesized by introducing aromatic acetophenone and naphthophenone substituents into the viologen structure. The keto group (–CH2CO–) on the substituents is prone to isomerize into the enol structure (–CHCOH–) in organic solvents, especially in DMSO, resulting in a larger conjugated system to stabilize the molecular structure and enhance fluorescence. The time-dependent fluorescence spectrum shows obvious keto-to-enol isomerization-induced fluorescence enhancement. The quantum yield also increased significantly (T = 1 day, ΦVio1 = 25.81%, ΦVio2 = 41.44%; T = 7 days, ΦVio1 = 31.48%, and ΦVio2 = 54.40%) in DMSO. The NMR and ESI-MS data at different times further confirmed that the fluorescence enhancement was caused by isomerization, and no other fluorescent impurities were produced in solution. DFT calculations show that the enol form is almost coplanar throughout the molecular structure, which is conducive to stabilizing the structure and enhancing fluorescence. The fluorescence emission peaks of the keto and enol structures of Vio12+ and Vio22+ were at 416–417 nm and 563–582 nm, respectively. The fluorescence relative oscillator strength of Vio12+ and Vio22+ enol structures is significantly higher than that of keto structures (f value changes from 1.53 to 2.63 for Vio12+ and from 1.62 to 2.81 for Vio22+), indicating stronger fluorescence emission of the enol structure. The calculated results are in good agreement with the experimental results. Vio1·2Cl and Vio2·2Br are the first examples of isomerization-induced fluorescence enhancement of viologen derivatives, which shows strong solvatofluorochromism under UV light, making up for the disadvantage that it is easy for a viologen radical to fade in air, and providing a new strategy for designing and synthesizing viologen materials with strong fluorescence.
研究领域:
化学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Materials Today Communications
·
2024
·
IF 3.7
Xianze Meng,Qianru Zhang,Xuantong Lv,Jiabo Chen,Yingzi Peng,Pengxuan Dong,Qingqing Sun
The corrosion inhibition performance of three amino acids, namely L-Phenylalanine (Phe), L-Methionine (Met) and L-Histidine (His) on 7150 Al alloy in 0.1 M HCl + 1 M NaCl solution was investigated by using electrochemical impedance spectroscopy (EIS), cyclic polarization, DFT and MD simulations. Electrochemical results indicate that all the studied amino acid inhibitors are cathodic type, and the inhibition efficiency follows the following order under all studied temperatures (25, 35 and 45 ℃): His > Met > Phe. A strong correlation between corrosion inhibition efficiency and DFT parameters is not evident, but the adsorption sites (N and O of NH 2 -COOH-, S atom of Met and two N atoms in the imidazolyl ring of His) can be determined by Fukui indices and Mulliken charges of the local atoms. In addition, MD simulations indicate that corrosion inhibition efficiency increases with the decreasing of adsorption energy.
研究领域:
材料科学
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电化学
·
理论计算
✓ 已验证
产品关联
DOI
高影响因子
Surfaces and Interfaces
·
2023
·
IF 6.2
Guoqing Feng,Shihan Wang,Siqing Wang,Pengcheng Wang,Chuntao Wang,Andargie Abebe Setiye,Massamba-Courtois Joanes Benedicte,Jingkun Xiao,Chengwen Song
Assembling a heterojunction-based composite nanomaterial to simultaneously achieve higher response and superior selectivity towards NO 2 under room-temperature conditions remains a great challenge. In this work, the MXene@Polypyrrole heterojunction was synthesized via a facile in-suit chemical polymerization approach. The distribution of sphere-like PPy nanoparticles was confirmed via various characterization techniques. The response value of the 0.5MXP sensor toward 50 ppm NO 2 is significantly higher than that of the pristine MXene based sensor, entailing greater response (6.5-fold). Nearly 98.11% recovery to the base resistance was observed in each sensing cycle. Noteworthy, the Schottky barriers formed between MXene and PPy contact surface, leading to the ideal selectivity and a lower limit of detection. Additionally, the sensor was tested for a 31-days-period with minimal deviation, predicting outstanding reproducibility and durability. The detailed polypyrrole sensitization mechanism containing selectivity mechanism, underlying heterojunction mechanism as well as the Density Function Theory (DFT) calculation were also revealed, offering new ideas for the development of room-temperature nitrogen dioxide sensors. Simultaneously, DFT calculation (21 models, 42 images) revealed the adsorption energy, electron transfer , and charge density differences between the NO 2 molecules and the substrate (MXene, PPy and MXene@PPy). In summary, the outstanding MXene surface functionalization has been exploited by decorating with polypyrrole (PPy) nanoparticles.
研究领域:
材料科学
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化学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）