Polymer Chemistry
·
2017
·Vol. 8
·期 31
·4520-4527
·
IF 5.375
Lu Wang,Wencong Wang,Wei Cao,Huaping Xu
Nanomaterials with hierarchical responsiveness are of great significance not only for fundamental science but also for future biomedical applications due to sophisticated and hierarchical physiological environments. Herein, we report a selenium- and tellurium-containing block copolymer that can be stepwise oxidized by both chemical methods and electrochemical methods. Differences in sensitivity to the oxidation of selenium and tellurium were employed. By tuning the concentration of the oxidant and oxidation periods, self-assembly behaviors of the copolymer were tuned by stepwise chemical oxidation. After oxidation, some interesting morphological evolution was observed that the polymer micelles crosslinked with each other without any swelling. In the case of electrochemical oxidation, the voltage during the electrochemical oxidation and the oxidation period also affected the level of oxidation. Furthermore, we showed that the degree of electrochemical oxidation varied with a different PEG block length. Considering sophisticated physiological conditions in vivo, this hierarchically responsive system may provide new possibilities as smart delivery vehicles in biological environments.
研究领域:
材料科学
·
生物医学工程
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产品关联
DOI
高影响因子
Journal of Physical Chemistry C
·
2021
·
IF 4.126
Hui-Yuan Peng,Yuan-Hui Xiao,Huan-Huan Yu,Jia-Zheng Wang,Jian-De Lin,Rajkumar Devasenathipathy,Jia Liu,Pei-Hang Zou,Meng Zhang,Jian-Zhang Zhou,De-Yin Wu,Zhong-Qun Tian
The analysis of plasmonic photoelectrochemical reactions on nanostructured noble metal electrodes is an attractive field, but little is known about the detailed competition between the photochemical and electrochemical reaction processes, product selectivity, and synergistic kinetics. In this work, para-aminothiophenol (PATP), as a probe molecule in surface-enhanced Raman spectroscopy (SERS), was used to investigate electrochemical and photochemical oxidation on nanostructured gold electrodes. Using electrochemical SERS (EC-SERS) and density functional theory (DFT) calculations, the sophisticated oxidation process and the selectivity of PATP oxidation (electrochemical oxidation and photochemical oxidation) under different conditions were determined. Moreover, based on the provided oxidation pathways of PATP on the gold electrode, the oxidation kinetics of PATP was studied by COMSOL simulation and a spectroscopic tool. The increasing rate constant of cationic radical formation due to hot holes at a high laser power has induced the selective generation of photochemical products. This work built a system to modulate the reaction selectivity and will inspire photoelectrochemical kinetic research in other plasmonic metal electrode–adsorbate systems of nanostructures.
研究领域:
电化学
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材料科学
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纳米技术
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理论计算
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产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2024
·
IF 5.8
He Sun,Jiaming Chen,Yusheng Yang,Min Qiu,Milin Zhang
A low-grade ore containing 4 % niobium and 7 % titanium has been extracted from Bayan Obo tailing, but its potential has not been fully utilized. This study aims to recover the niobium and titanium elements from this low-grade ores in the form of their carbides. The process involves reducing niobium and titanium to (Nb,Ti)C through a carbothermal process. During this process, iron and silicon are also reduced to Fe-Si intermetallic compounds, allowing (Nb,Ti)C to diffuse into them. Subsequently, selective electrochemical oxidation is used to separate (Nb,Ti)C from the Fe-Si intermetallic compounds in an aqueous ferrous sulfate solution. The Fe-Si intermetallic compounds are first oxidized to the Fe 3 Si phase, and then to the Fe 5 Si 3 phase in the solution with pH 0.35. The (Nb,Ti)C/matrix interfaces are identified as the preferred site of electrochemical pitting corrosion. By exploiting the electrochemical oxidation reaction of iron in the matrix, (Nb,Ti)C powders are separated along these interfaces. The by-products of this process are FeSi alloys, which are evaluated for their electrocatalytic properties in oxygen evolution reactions. It is found that the Fe 5 Si 3 alloy by-product exhibits good electrocatalytic activity and kinetics in the oxygen evolution reaction, demonstrating its potential for practical applications.
研究领域:
冶金学
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材料科学
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电化学
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产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Ze Zhang,Shuying Shen,Qiaoling Xu,Lihua Cui,Rongliang Qiu,Zhujian Huang
The electrochemical conversion of ammonia into harmless nitrogen gas (N 2 ) remains a significant challenge in wastewater treatment. This study explores the utilization of granular activated carbon (GAC) as three-dimensional particle electrodes within a peroxymonosulfate (PMS)/Cl − -PbO 2 /Ti electrochemical system to enhance ammonia oxidation and N 2 transfer efficiency. In the observed experimental parameters designated as optimal, the system demonstrated a complete amelioration of ammonia within 45 min. The porous surface of GAC electrodes facilitates increased contact area, promoting better interaction with target compounds. This interaction leads to improved mass transfer efficiency, reduced chlorine overpotential, and enhanced current response. Quenching experiments reveal the substantial involvement of hydroxyl radicals (•OH), sulfate radicals (SO 4 •− ), and chloride radicals (Cl•) in the oxidation process of NH 4 + -N, with Cl• generation through the oxidative process involving Cl − and SO 4 •− under electrical stimulation. After 90 min, a significant portion of NH 4 + -N is transformed into N 2 , achieving a conversion efficiency of 71.5 %. Additionally, the system demonstrates efficient removal of ammonia from practical aqueous environments. Three-dimensional fluorescence spectroscopic analysis confirms the system's effectiveness not only in removing ammonia but also in reducing organic substances resembling fulvic acid. These findings underscore the three-dimensional electrochemical GAC/PMS/Cl − system as a promising and efficient approach for ammonia removal in wastewater treatment applications.
研究领域:
环境科学
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废水处理
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产品关联
DOI
高影响因子
JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY
·
2015
·Vol. 308
·期 3
·1095-1102
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IF 1.034
Wang Zhengshang,Wang Yun,Liao Jiali,Yang Yuanyou,Liu Ning,Tang Jun
Three types of graphene sheets (GS) were decorated by chemical oxidation, electrolysis and ball-milling, respectively. These oxidized samples were characterized using SEM, XRD, Raman, FT-IR and XPS, and then were employed to enrich U(VI) from aqueous solutions as a function of pH, contact time and initial concentration of U(VI). These results displayed that the quantities and types of oxygen-functional groups were extremely different through these methods, which highly determined the adsorption capacity of graphene oxide to uranium. This work may provide some helpful information to optimize these fabrication processes and improve the adsorption ability of GS to uranium.
研究领域:
材料科学
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环境科学
✓ 已验证
DOI
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2024
·
IF 0
Li Danni,Guo Xin,Shao Xiang,Zhou Anhui,Zhu Lin,Zhang Yuting,Li Binbin,Du Yan,Cao Limei,Yang Ji
The electrochemical advanced oxidation process (EAOP) has shown significant promise in the field of refractory organic wastewater treatment due to its high efficiency and environmentally friendly nature. In this study, Ti/Sb-SnO 2 electrodes with varying proportions of Hf were prepared using the sol–gel method. The addition of Hf transformed the original collapsing and broken surface into a flat and regular surface. The results demonstrated that Ti/Sb-SnO 2 -Hf electrode doped with 6% Hf exhibited a higher oxygen evolution potential (OEP) and excellent stability. The OEP increased from 2.315 V without Hf-doping to 2.482 V, and the corresponding actual life was 321.05% higher than that without Hf. The current density (5–40 mA·cm −2 ), electrolyte concentration (0.02–0.2 mol·L −1 ), pH (3–11), and initial pollutant concentration (5–80 mg·L −1 ) were evaluated to confirm the tetracycline (TC) degradation characterization of Ti/Sb-SnO 2 -6%Hf electrodes. It was concluded that under the optimal degradation conditions, the removal rate of TC could reach 99.66% within 2 h. The degradation of TC follows first-order reaction kinetics. The oxidative degradation of TC was achieved through indirect oxidation, with ·OH playing a dominant role. TC’s electrochemical oxidation degradation pathway has been proposed: Based on LC–MS results, three main pathways are speculated. During the electrocatalytic oxidation process, decarboxylation, deamidation, and ring-opening reactions occur under ·OH attack, producing intermediate compounds with m/z values of 427, 433, 350, 246, 461, 424, 330, 352, 309, 263, and 233. These intermediates are further oxidized to intermediate compounds with an m/z value of 218. This work introduces a new efficient anode electrochemical catalyst for the degradation of TC, providing a strategy for industrial applications.
研究领域:
环境科学
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材料科学
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产品关联
DOI
PubMed
MACROMOLECULAR CHEMISTRY AND PHYSICS
·
2011
·Vol. 212
·期 17
·1900-1909
·
IF 2.437
Wenguang Leng,Shuxue Zhou,Limin Wu
Nail/spindle-shaped polyaniline is synthesized by chemically oxidizing aniline with ammonium persulfate in a near-neutral aqueous medium using PVP as the stabilizing agent. The type of dispersing agent, APS content and aniline concentration have obvious impacts on the morphology of the resulting polyaniline. Typically, in the concentration ranges of 1.5–6 × 10 −4 M PVP and 0.02–0.05 M aniline and for molar ratios [APS]:[aniline] of 0.4:1 to 0.8:1, nail/spindle-shaped polyaniline can be obtained. A possible mechanism is proposed to elucidate the formation process.
研究领域:
材料科学
·
化学
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产品关联
DOI
高影响因子
PETROLEUM SCIENCE AND TECHNOLOGY
·
2016
·
IF 0.418
Jing-Jing Li,Fei Zhou,Xiao-Dong Tang,Fang Wang,Na Hu
An electrochemical oxidation−distillation method with constant current 500 mA was proposed to reduce the sulfur content in gasoline in this work. After electrochemical oxidation−distillation, the sulfur content of gasoline decreased from 514.65 to 10.20 μg/g. On the basis of these experimental results, an oxidation mechanism of electrochemical oxidative desulfurization for gasoline was proposed.
研究领域:
环境科学
·
化学工程
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DOI
高影响因子
Journal of Water Process Engineering
·
2025
·
IF 6.7
Lixian Zhong,Peidi Luo,Yaoyao Wu,Kai Yang,Can Zhang,Ruihao Peng,Chuanhao Li,Xianping Luo
Thallium (Tl), an unconventional and highly toxic metal, is increasingly recognized as a significant contaminant in wastewater. One promising strategy to enhance Tl removal is the electrocatalytic oxidation of Tl(I), yet the contribution of chloride ions—prevalent in wastewater from metallurgical and smelting industries—has often been overlooked in such processes. Herein, this study introduces a novel chlorine-mediated electrochemical oxidation system, coupled with a coagulation process, designed to efficiently treat thallium-contaminated saline wastewater. The dimensionally stable anode (Ti/TiO 2 -RuO 2 -IrO 2 , DSA) demonstrates exceptional electrocatalytic chlorine evolution and efficient oxidation of Tl(I), with a kinetic rate constant of 0.131 min −1 , which is 21.8 times faster than that of a carbon cloth anode (0.006 min −1 ) in the presence of Cl − ions. Under optimized conditions of 5 mM Cl − ions at pH 3.0, over 98.3 % of Tl(I) was removed within 30 min. After coagulation treatment, the total Tl removal efficiency reached 98.5 %, in stark contrast to the mere 18.0 % achieved without the pre-electro-oxidation step. Mechanistic analysis revealed that the reactive chlorine species (Cl•) plays a more significant role in the oxidation of thallium (Tl) compared to the hydroxyl radicals. Notably, the system exhibits excellent recyclability (up to 35 cycles) and stable performance in the presence of various competing ions and actual wastewater, even under unsteady-state continuous-flow conditions. These findings offer valuable insights into chlorine-mediated electrocatalytic oxidation coupling with coagulation processes for thallium removal, providing guidance for practical applications in purifying thallium-contaminated industrial wastewater.
研究领域:
环境科学
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化学工程
·
水处理技术
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产品关联
DOI
高影响因子
JOURNAL OF POWER SOURCES
·
2024
·
IF 8.1
Jia Cheng,Zhiwei Zeng,Xun Huang,Zidong Wei
The electrocatalytic oxidation of furfural (FA) for the production of valuable chemicals, such as 2-furancarboxylic acid (FAC), presents an attractive alternative to the sluggish oxygen evolution reaction during water electrolysis for hydrogen production. However, the activity and stability of the current electrocatalysts still require further enhancement. In this study, NiMoP is fabricated on Ni foam through pulsed electrodeposition to facilitate the electrooxidation of FA for FAC production in an alkaline environment. A low voltage of 1.43 V vs. reversible hydrogen electrode (RHE) is adequate to achieve a current density of 500 mA cm −2 , with FAC selectivity and Faraday efficiency reaching 97.5 % and 95.2 %, respectively. The extended electrolysis of FA using a continuous-flow electrolytic cell under high current density (500 mA cm −2 ) demonstrates consistent stability at a cell voltage around 1.8 V over a 35-h duration.
研究领域:
化学工程
·
电催化
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产品关联
DOI
高影响因子
ENVIRONMENTAL TECHNOLOGY
·
2025
·
IF 2
Chunyun Gu,Jiayi An,Shuyu Liu,Feng Xiong,Wei Zhou,Liting Tian,Yuruo Wan,Qian Wu,Jie Ma
Oxidants used in the ISCO technology usually require activation by activators to degrade contaminants. However, this study investigated degradation of 15 typical halogenated hydrocarbons by five common ISCO oxidants (PS, PMS, H2O2, KMnO4, SPC) without activation in both pure water and real groundwater. Unactivated PS could degrade 14 halogenated hydrocarbons, excluding tetrachloromethane. Unactivated KMnO4 could degrade chlorinated alkenes. Unactivated SPC could degrade 1,1,2,2-tetrachloroethane by a base-promoted second-order elimination reaction. PMS, H2O2, and SPC could be activated by the natural matrix constituents in groundwater, enabling them to degrade some halogenated hydrocarbons. Among the 15 halogenated hydrocarbons studied, only tetrachloromethane cannot be degraded by any oxidant due to its carbon being in its highest oxidation state. The experimental data in the pure water indicate that the overall degradation rate of unactivated PS for chlorinated alkanes increased with increases in the number of chlorine substituents. The degradation rate of unactivated PS for halogenated hydrocarbons decreased with increases in the carbon chain length. Chlorinated alkenes are more easily degraded than chlorinated alkanes while chlorinated alkanes are more readily degraded than brominated alkanes. The degradation rate of unactivated KMnO4 for chlorinated alkenes decreased with increases in the number of chlorine substituents and decreased with increases in the carbon chain length. Overal, results of this study show that unactivated ISCO is a promising and environmentally friendly in-situ remediation technology that may be a good candidate for the remediation of contaminated sites by halogenated hydrocarbons.
研究领域:
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2021
·Vol. 168
·期 12
·124516
·
IF 4.316
Yongfang Zhou,Yi Shen,Hongying Li
The presence of metallic impurities in the electrolyte greatly affects electrocatalytic performance. A systematic study on this topic can not only provide guidance for rigorous practices on electrochemical measurements, but also in-depth fundamental understanding on the mechanisms of the electrochemical reactions. Herein, nine types of metallic ions including Cu2+, Ni2+, Fe3+, Fe2+, Co2+, Mn2+, Zn2+, Ce3+ and Al3+ are intentionally introduced into the electrolytes with a controlled manner and their effects on electro-oxidation of water, 5-hydroxymethylfurfural (HMF) and glycerol are investigated in details. Among these metal ions, Co2+ has the most pronounced effects on H2O electro-oxidation while Cu2+ species displays superior activity toward HMF and glycerol electro-oxidation, but negligible effects on H2O electro-oxidation. Such a unique feature of Cu2+ can also be noted from electro-oxidation of other small molecules, such as ethylene glycol, ethanol and furfural. More importantly, the effects of metallic impurities are independent of the composition of the electrodes, only rely on the pH of the electrolytes. In-situ electrochemical Raman spectroscopy, control electrochemical experiments and X-ray photoelectron spectroscopy analyses reveal that the origin of impurity effects is attributed to the formation of hydroxides during the electrochemical measurements.
研究领域:
电化学
·
材料科学
✓ 已验证
DOI
高影响因子
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