SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Meiling Wu,Yang Tao,Yuwei Liu,Sanying Hou,Tiyang Xiao,Qing Fu,Guowen Peng,Lang Shi
In this study, Fe/N co-doped graphene-like honeycomb porous carbon (Fe-NC)was produced and used for the activating PMS to degrade TC. The Fe-NC catalyst has shown high activity in the TC degradation by activated PMS, with an efficiency of up to 94 % in 30 min. while the blank catalyst without N and Fe doping exhibited the lowest performance with 47.3 % TC degradation. Moreover, other operational factors of Fe-NC catalysts were also investigated to evaluate its catalytic activity. The burst experiments and electron paramagnetic resonance (EPR) experiments demonstrated that free radical paths (O 2 ·- ) and non-free radical paths ( 1 O 2 ) coexist inside the Fe-NC/PMS system. The experiment results and degradation mechanism analysis revealed that N species(Pyridine N, Graphite N,Fe-N x ) and iron species (Fe0) were possible to be the active species of catalysts. Furthermore, Fe-NC/PMS system was investigated for possible pathway of TC degradation by liquid mass spectrometry (LC-MS), and the presence of intermediates was analyzed for toxicity magnitude by ECOSAR software.
研究领域:
环境科学
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催化材料
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产品关联
DOI
高影响因子
ADVANCED MATERIALS
·
2022
·Vol. 34
·期 28
·2202874
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IF 32.086
Li An,Yang Hu,Jianyi Li,Jiamin Zhu,Mingzi Sun,Bolong Huang,Pinxian Xi,Chun-Hua Yan
The oxygen reduction reaction (ORR) has been demonstrated as a critical technology for both energy conversion technologies and hydrogen peroxide intermediate production. Herein, an in situ oxygen evolution reaction (OER) surface evolution strategy is applied for changing the surface structure of MnCo 2 O 4 oxide with tetrahedral and octahedral cations vacancies to realize reaction pathway switching from 2e − ORR and 4e − ORR. Interestingly, the as-synthesized MnCo 2 O 4 -pristine (MnCo 2 O 4 -P) with the highest surficial Mn/Co octahedron occupation favors two electrons reaction routes exhibiting high H 2 O 2 selectivity (≈80% and reaches nearly 100% at 0.75 V vs RHE); after surface atoms reconstruction, MnCo 2 O 4 -activation (MnCo 2 O 4 -A) with the largest Mn/Co tetrahedron occupation present excellent ORR performance through the four-electron pathway with an ultrahigh onset potential and half-wave potential of 0.78 and 0.92 V, ideal mass activity (MA), and turnover frequencies (TOF) values. Density functional theory (DFT) calculations reveal the concurrent modulations of both Co and Mn by the surface reconstructions, which improve the electroactivity of MnCo 2 O 4 -A toward the 4e − pathway. This work provides a new perspective to building correlation of OER activation–ORR property, bringing detailed understating for reaction route transformation, and thus guiding the development of certain electrocatalysts with specific purposes.
研究领域:
材料科学
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电化学
✓ 已验证
DOI
高影响因子
Journal of Environmental Chemical Engineering
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2025
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IF 7.2
Zehui Fan,Zhisen Li,Dan Mo,Jingyang Zhang,Shuyi Yang,Yun Li,Changlong Bi,Chong Peng,E Tao
Modulation of nano electrocatalysts for targeted excitation of different reactive oxygen species (ROS) is a key challenge to achieve environmentally catalyzed efficient pollutant degradation. In this study, multivalent copper catalysts (Cu (0)/Cu (I)/Cu (II)) load on the surface of biochar (CBX) are prepared by the hydrothermal-impregnation method, and the modulation effect of different valences of copper on the pathway of reactive oxygen species (ROS) generation is investigated. X-ray diffraction (XRD) analysis shows the coexistence of three copper valence states. Radical scavenging experiment and DFT calculations indicate that Cu (I) dominates the adsorption and activation of peroxodisulfate (PS) to efficiently generate ·SO 4 - and ·OH. Cu (II) selectively generates 1 O 2 by modulating the dissolve oxygen conversion pathway; whereas Cu (0) acts as an activation center for bound oxygen and significantly promotes ·O 2 - generation. The nano-electrocatalytic system prepared at 600°C (CB6-PS) degraded 98.3% of enrofloxacin (ENR) over a period of time (60 min). Mechanistic studies indicate that the catalytic system realizes the coupling reaction between the radical pathway (·SO 4 - /·OH /·O 2 - ) and the nonradical pathway ( 1 O 2 ) by the synergistic action of multivalent copper, which providing a new theoretical basis and technical strategy for the development of targeted ROS generation function.
研究领域:
环境催化
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材料化学
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污染控制
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纳米催化
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环境功能材料
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高级氧化技术
✓ 已验证
产品关联
DOI
高影响因子
CHINESE CHEMICAL LETTERS
·
2014
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IF 1.178
Cheng-Xi Zhang,Yu-Yuan Deng,Yi-Yang Zhang,Po Yang,Yi Gu
To study the synthesis of 3,4-dihydro-2 H -3-phenyl-1,3-benzoxazine (benzoxazine), the reaction paths of phenol, aniline and formaldehyde were investigated by analyzing the synthesis crude products. With the aid of high-performance liquid chromatography (HPLC), chromatographic column and preparative HPLC, seven compounds originated from the crude products were obtained and their chemical structures were elucidated. Possible reaction paths are proposed based on these compounds. Results show that N -hydroxymethyl aniline (HMA) derived from the reaction of formaldehyde and aniline is probably the key intermediate during the reaction. HMA can react with itself or other reactants to form other intermediates, such as 1,3,5-triphenyl-1,3,5-triazinane and 2-((phenylamino)methyl)phenol, and further form benzoxazine and byproducts.
研究领域:
有机化学
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合成化学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
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IF 13.2
Cong Wan,Jianwen Zhang,Honglei Zhang,Min Liu,Yiming Li,Zijun Yan,Chengheng Pang,Tao Wu
The catalytic reduction of CO₂ into valuable chemicals and fuels is a promising strategy for mitigating global carbon emissions. This study explores the synergistic co-reduction of CO₂ and H₂O using nanoscale zero-valent iron (NZVI) as a dual-function catalyst. Under light irradiation at 300 °C, the CO₂ reduction rate increased by more than 10-fold compared to dark conditions, demonstrating significant photothermal synergy. The study reveals that NZVI undergoes a phase transformation, where Fe₃O₄ functions as a photocatalyst while Fe 0 serves as an electron donor, enabling a unique dual-functionality that facilitates efficient electron transfer. The addition of 10 vol% H₂ stabilizes the reaction, leading to a higher and more consistent CO yield. When investigating the simultaneous reduction of CO₂ and H₂O, we discovered competitive adsorption and reaction pathways that significantly influence product distribution. In-situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) and density functional theory (DFT) calculations revealed three distinct mechanistic pathways for CO₂ conversion: direct C O bond cleavage, a carboxylate-mediated pathway and bicarbonate-mediated pathway, with the carboxylate and bicarbonate pathways being uniquely promoted by H and OH from H₂O dissociation. The addition of H₂O into the CO₂ and H₂ reaction significantly enhanced CH₄ generation due to the extra H source from H₂O dissociation. These findings offer valuable insights into the competitive mechanistic pathways of CO₂-H₂O co-reduction and contribute to the design of more efficient iron-based catalysts for sustainable CO₂ conversion and water splitting in energy and environmental applications.
研究领域:
环境催化
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纳米科技
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可再生能源
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表面化学
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理论化学
✓ 已验证
产品关联
DOI
高影响因子
Catalysts
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2022
·Vol. 12
·期 11
·1328
·
IF 4.501
Liang-Qiu Huang,Zhi-Jun Diao,Bo Chen,Qing-Pan Du,Kai-Yang Duan,Si-Jia Zhao
Efficient depolymerization of C–O linkages is essential for converting lignin into fuels and higher value-added chemicals. In this work, CoRuP/SiO2, an amorphous Ru-Co phosphide composite, was fabricated for the efficient hydrogenolysis of ether linkages. The 4–O–5 andα–O–4 linkages containing lignin-related compounds, such as diphenyl ether, benzyl phenyl ether, 3-methyl diphenyl ether, and dibenzyl ether, are selected as representatives of linkages in lignin. Under mild conditions, Ru-containing metallic phosphides have high-performance for the catalytic depolymerization of C–O linkages. Compared with other catalysts, CoRuP/SiO2shows an outstanding selectivity for benzene and excellent efficiency in depolymerizing diphenyl ethers, yielding only a small amount of by-products. Furthermore, the total acidity shows a linear relationship with the hydrogenolysis reactivity in cleaving aromatic ether bonds. The mechanisms for the catalytic hydrogenolysis of 4–O–5 andα–O–4 bonds over CoRuP/SiO2are proposed. Moreover, two-dimensional heteronuclear single quantum coherence nuclear magnetic resonance spectroscopic analysis demonstrates that CoRuP/SiO2could effectively depolymerize C–O bonds of lignin. These dominant hydrogenolysis products from lignin have excellent potential in the production of high value-added drugs or pharmaceutical intermediates. The hydrogenolysis of lignin can be a highly efficient alternative to the existing method of lignin utilization.Keywords:hydrogenolysis;C–O linkages;metallic phosphides;reaction pathway
研究领域:
化学工程
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可再生能源
✓ 已验证
产品关联
DOI
高影响因子
Journal of Water Process Engineering
·
2025
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IF 6.7
Mingjun Xie,Yuying Han,Na Wang,Zixuan Huang,Congting Sun
The efficient elimination of recalcitrant synthetic dyes from complex waters remains a pressing challenge for advanced oxidation processes (AOPs). Herein, an Fe-MOFs-derives@BC composite was fabricated by anchoring MIL-101(Fe) crystals onto rice-straw biochar followed by high-temperature carbonization. XRD, SEM and XPS confirm the formation of a crystal–amorphous hybrid in which residual MIL-101(Fe) nanocrystallites are embedded within a conductive carbon matrix rich in oxygen vacancies. The composite rapidly activates PMS via a synergistic Fe(II)/Fe(III) redox cycle and carbon-facilitated electron transfer, generating SO₄• − , •OH, and 1 O₂ to driving Rhodamine B (RhB) and Malachite Green (MG) degradation. Under optimal conditions (0.1 g L −1 catalyst, 0.1 g L −1 PMS), >90% RhB and MG were removed within 15 min across deionised, groundwater, lake and river matrices; even in the most complex river water, 90% removal is achieved in 10 min. When Fe-MOFs-derives@BC is immobilised in a poly (vinylidene fluoride) membrane, a continuous-flow micro-reactor maintains >90% removal over 600 min with negligible flux decline and undetectable Fe leaching. This hybrid radical/non-radical pathway, broad matrix tolerance and long-term membrane stability position Fe MOFs-derives@BC/PMS as a robust, scalable platform for advanced wastewater treatment.
研究领域:
环境工程
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材料科学
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化学工程
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水处理技术
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纳米技术
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Yulu Zhang,Hangyang Feng,Weifeng Kong,Meijuan Bian,Yingying He,Qianwei Liang,Yanlong Sun,Chengzhi Zhou,Liguo Shen
A functionally graded high-entropy alloy catalyst FeCoNiCuRu 0.5 @nitrogen-doped carbon (FeCoNiCuRu 0.5 @NC) was designed to address catalytic function regulation and active-site stability challenges in peroxymonosulfate-based advanced oxidation processes. Featuring a spatially separated architecture with a Ru C composite shell and a polymetallic alloy core, the catalyst suppresses transition metal dissolution, reducing ion leaching by 65.5 % versus conventional counterparts. The catalyst achieved complete carbamazepine (CBZ) removal within 30 min with a rate constant (k) of 0.460 min −1 at pH 3, and singlet oxygen ( 1 O 2 ) and sulfate radicals (SO 4 •− ) were identified as the dominant active species. At pH 7, this rate constant (0.158 min −1 ) showed a twofold increase over that of FeCoNiCu@nitrogen-doped carbon (FeCoNiCu@NC) and a fivefold enhancement over that of Ru@ nitrogen-doped carbon (Ru@NC). The concentrations of SO 4 •− and 1 O 2 over FeCoNiCuRu 0.5 @NC are 1.97 and 3.38-fold higher, respectively, than those over FeCoNiCu@NC. This enhancement correlates with the superior charge transfer capability of the Ru-modified catalyst system. Remarkably, the FeCoNiCuRu 0.5 @NC demonstrates unprecedented pH tolerance (pH 3–11) and stability. Its dual-active-species configuration enables simultaneous degradation of electron-rich and electron-deficient pollutants, establishing a new paradigm for designing robust high-entropy alloy catalysts.
研究领域:
环境催化
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材料化学
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高级氧化过程
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污染控制化学
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纳米催化材料
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Wei Guo,Yao Qin,Cheng Liu,Binbin Guo,Junhua Zou,Zenghong Xie,Ling Wu
This work reports the rapid and effective photocatalytic dechlorination of 3,3′,4,4′-trtrachlorobiphenyl (PCB77) with highly dispersed Pd nanoclusters loaded two-dimensional (2D) TiO 2 (B) nanosheets (Pd/TiO 2 (B)) under visible light irradiation, achieving a dechlorination efficiency of 100 % with H 2 O used as an H-donor source. The ultra-thin TiO 2 (B) nanosheets provide a good platform for studying the dechlorination intermediates/pathways of PCB77 at the molecular level. It is proved that the dechlorination of PCB77 is a stepwise process, in which chlorines at the para positions are much more susceptible than those at the meta positions due to the activation of the C Cl bond in the presence of Pd nanoclusters. Furthermore, in-situ FTIR results of D 2 O absorption suggest that the TiO 2 (B) nanosheets with abundant surface defects greatly promote the activation of water molecules via the formation of surficial complexes by hydrogen bonds. Finally, a synergistic mechanism is proposed for photocatalytic dechlorination of PCB77 over Pd/TiO 2 (B). The study provides an efficient method for complete dechlorination of PCB77 and an in-depth understanding photocatalyzed dechlorination reaction mechanism at the molecular level, which may extend to other photocatalytic dehalogenation reactions of halogenated pollutants.
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
FUEL
·
2022
·
IF 8.035
Yangfan Chen,Hongyan Yan,Wenxin Teng,Jiangling Li,Weizao Liu,Shan Ren,Jian Yang,Qingcai Liu
NH 3 -SCR technology with commercialized V 2 O 5 -WO 3 (MoO 3 )/TiO 2 catalysts has become the most efficient technology for the removal of NO x from coal-fired power plants. However, the weaknesses of V 2 O 5 -WO 3 (MoO 3 )/TiO 2 catalysts such as the biotoxicity of vanadium species and high cost restrict their increased applicability. Fe 2 O 3 -based NH 3 -SCR catalysts show potential in placing traditional catalysts due to their good N 2 selectivity, excellent environmentally friendly performance, high thermal stability, and low cost. In this work, low cost Fe 2 O 3 -containing solid waste was exploited as the base material for NH 3 -SCR catalyst preparing. Moreover, bulk MoO 3 and MoO 3-x nanosheets decorated Fe 2 O 3 composite NH 3 -SCR catalysts were synthesized and both revealed conspicuously improved NO x removal efficiency compared with bare-Fe 2 O 3 catalyst. However, the N 2 selectivity of these two catalysts showed significant differences. Therefore, comprehensive characterizations, NH 3 oxidation experiments, and in-situ diffusion Fourier transform infrared spectroscopy (DRIFTS) experiments were performed to determine the N 2 O formation pathways of the above two catalysts. The redox properties were highly related to the N 2 O generated from NH 3 oxidation. Moreover, the huge difference in NH 3 and NO adsorption ability led to disparate reaction mechanisms over the two catalysts. This new understanding of the N 2 O formation mechanism has the potential to guide the rational design of improved NH 3 -SCR catalysts suffering from low N 2 selectivity.
研究领域:
环境科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
Water
·
2024
·Vol. 16
·期 13
·1818
·
IF 3
Tongke Hu,Yazhen Chen,Xiaolan Guo,Yongjun Peng,Jianhua Cheng
The exploration of efficient, low-leaching, and recyclable transition-metal-based catalysts is of great importance for the removal of pollutants from peroxymonosulfate (PMS) in water purification processes. In this study, a bimetallic CoFe@CSC-700 composite was prepared by an alkaline gel pyrolysis reduction method using chitosan as a forming agent and applied to activate PMS to degrade levofloxacin (LEV). The leaching concentration of both cobalt and iron ions in the CoFe@CSC-700 catalyst was reduced by about 8-fold compared to the monometallic composite pellet catalyst. In addition, the removal efficiency of the CoFe@CSC-700 catalyst can still reach 90% after five cycles, showing good recyclability, recoverability and stability. Both free radical pathways (SO4·−, ·OH, and ·O2−) and non-free radical pathways (1O2) were detected in the oxidation reaction, with free radical pathways as the main contributor. The possible degradation pathways of LEV were proposed by LC-MS tests. Overall, this study provides new insights into the construction of efficient and stable PMS catalysts for wastewater treatment.
研究领域:
环境科学
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催化
·
水净化
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
·
2024
·
IF 8.2
Rui Yu,Yunkun Qian,Yanan Chen,Yijun Shi,Jun Guo,Dong An
Dichloroacetonitrile (DCAN) is an emerging disinfection by-product (DBP) that is widespread in drinking water. However, the pathway for DCAN formation from aromatic amino acids remains unclear, leading to a lack of an understanding of its explicit fate during chloramination. In this study, we investigated the specific formation mechanism of DCAN during the chloramination of phenylalanine based on reaction kinetics and chemical thermodynamics. The reason for differences between aldehyde and decarboxylation pathways was explained, and kinetic parameters of the pathways were obtained through quantum chemistry calculations. The results showed that the reaction rate constant of the rate-limiting step of the aldehyde pathway with 1.9 × 10 −11 s −1 was significantly higher than that of decarboxylation (3.6 × 10 −16 s −1 M −1 ), suggesting that the aldehyde pathway is the main reaction pathway for DCAN formation during the chloramination of phenylalanine to produce DCAN. Subsequently, theoretical calculations were performed to elucidate the effect of pH on the formation mechanism, which aligned well with the experimental results. Dehydrohalogenation was found to be the rate-limiting step under acidic conditions with reaction rate constants higher than those of the rate-limiting step (expulsion of amines) under neutral conditions, increasing the rate of DCAN formation. This study highlights the differences in DCAN formation between the decarboxylation and aldehyde pathways during the chloramination of precursors at both molecular and kinetic levels, contributing to a comprehensive understanding of the reaction mechanisms by which aromatic free amino acids generate DCAN.
研究领域:
环境科学
·
化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）