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Atomistic simulations of plasma catalytic processes

Erik C. Neyts

《化学科学与工程前沿（英文）》 2018年 第12卷 第1期   页码 145-154 doi: 10.1007/s11705-017-1674-7

摘要： There is currently a growing interest in the realisation and optimization of hybrid plasma/catalyst systems for a multitude of applications, ranging from nanotechnology to environmental chemistry. In spite of this interest, there is, however, a lack in fundamental understanding of the underlying processes in such systems. While a lot of experimental research is already being carried out to gain this understanding, only recently the first simulations have appeared in the literature. In this contribution, an overview is presented on atomic scale simulations of plasma catalytic processes as carried out in our group. In particular, this contribution focusses on plasma-assisted catalyzed carbon nanostructure growth, and plasma catalysis for greenhouse gas conversion. Attention is paid to what can routinely be done, and where challenges persist.

关键词： atomic scale simulation     plasma-catalyst    

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Effect of glow discharge plasma on rhodium-based catalyst for oxygenates synthesis

HUANG Lihong, CHU Wei, XU Junqiang, HONG Jingping, YI Min

《化学科学与工程前沿（英文）》 2007年 第1卷 第1期   页码 16-19 doi: 10.1007/s11705-007-0004-x

摘要： Rhodium-based catalysts were prepared by impregnation, treated with glow discharge plasma, characterized by X-ray diffraction, X-ray photoelectron spectroscopy, H2 temperature-programmed reduction, H2 temperature-programmed desorption and CO temperature-programmed desorption, and investigated for oxygenate synthesis from CO hydrogenation. Based on the characterization results, plasma treatment endowed the samples with smaller particle size, higher dispersion of active components, and an enrichment of active components on the surface as well. As a result, the reducibility and adsorption properties were modified. In catalytic tests, the catalytic activity for CO hydrogenation over the samples treated by plasma was improved remarkably: the conversion of CO and the yield of oxygenates increased at most by a factor of 78.62% and 51.96%, respectively, while the selectivity of ethanol and methanol in the oxygenates was enhanced as well.
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Ni/MgO catalyst prepared via dielectric-barrier discharge plasma with improved catalytic performance

Yan LI,Zhehao WEI,Yong WANG

《化学科学与工程前沿（英文）》 2014年 第8卷 第2期   页码 133-140 doi: 10.1007/s11705-014-1422-1

摘要： A Ni/MgO catalyst was prepared via novel dielectric-barrier discharge (DBD) plasma decomposition method. The combined characterization of Brunauer-Emmett-Teller measurement, X-ray diffraction, hydrogen temperature-programmed reduction and transmission electron microscopy shows that DBD plasma treatment enhances the support-metal interaction of Ni/MgO catalyst and facilitates the formation of smaller Ni particles. Sphere-like Ni particles form on plasma treated Ni/MgO catalysts. The plasma treated Ni/MgO catalyst shows a significantly improved low temperature activity and good stability for CO reforming of methane to syngas.

关键词： CO2 reforming     methane     dielectric-barrier discharge (DBD)     plasma     Ni/MgO    

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Abatement of mixed volatile organic compounds in a catalytic hybrid surface/packed-bed discharge plasma

Lianjie Guo, Nan Jiang, Jie Li, Kefeng Shang, Na Lu, Yan Wu

《环境科学与工程前沿（英文）》 2018年 第12卷 第2期 doi: 10.1007/s11783-018-1017-z

摘要： In this study, post plasma-catalysis degradation of mixed volatile organic compounds (benzene, toluene, and xylene) has been performed in a hybrid surface/packed-bed discharge plasma reactor with Ag-Ce/ g-Al O catalyst at room temperature. The effect of relative air humidity on mixed VOCs degradation has also been investigated in both plasma-only and PPC systems. In comparison to the plasma-only system, a significant improvement can be observed in the degradation performance of mixed VOCs in PPC system with Ag-Ce/ g-Al O catalyst. In PPC system, 68% benzene, 89% toluene, and 94% xylene were degraded at 800 J·L , respectively, which were 25%, 11%, and 9% higher than those in plasma-only system. This result can be attributed to the high catalytic activity of Ag-Ce/ g-Al O catalyst to effectively decompose O and lead to generating more reactive species which are capable of destructing the VOCs molecules completely. Moreover, the presence of Ag-Ce/ g-Al O catalyst in plasma significantly decreased the emission of discharge byproducts (NO and O ) and promoted the mineralization of mixed VOCs towards CO . Adding a small amount of water vapor into PPC system enhanced the degradation efficiencies of mixed VOCs, however, further increasing water vapor had a negative impact on the degradation efficiencies, which was primarily attributed to the quenching of energetic electrons by water vapor in plasma and the competitive adsorption of water vapor on the catalyst surface. Meanwhile, the catalysts before and after discharge were characterized by the Brunauer-Emment-Teller and X-ray photoelectron spectroscopy.

关键词： Mixed VOCs     HSPBD plasma reactor     Degradation     Catalyst     Relative humidity    

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Liquid discharge plasma for fast biomass liquefaction at mild conditions: The effects of homogeneous

Sen Wang, Shiyun Liu, Danhua Mei, Rusen Zhou, Congcong Jiang, Xianhui Zhang, Zhi Fang, Kostya (Ken) Ostrikov

《化学科学与工程前沿（英文）》 2020年 第14卷 第5期   页码 763-771 doi: 10.1007/s11705-019-1896-y

摘要： Non-thermal plasma exhibits unique advantages in biomass conversion for the sustainable production of higher-value energy carriers. Different homogeneous catalysts are usually required for plasma-enabled biomass liquefaction to achieve time-and energy-efficient conversions. However, the effects of such catalysts on the plasma-assisted liquefaction process and of the plasma on those catalysts have not been thoroughly studied. In this study, an electrical discharge plasma is employed to promote the direct liquefaction of sawdust in a mixture of polyethylene glycol 200 and glycerol. Three commonly used chemicals, sulfuric acid, nitric acid and sodium -toluene sulfate, were selected as catalysts. The effects of the type of catalyst and concentration on the liquefaction yield were examined; further, the roles of the catalysts in the plasma liquefaction process have been discussed. The results showed that the liquefaction yield attains a value of 90% within 5 min when 1% sulfuric acid was employed as the catalyst. Compared with the other catalysts, sulfuric acid presents the highest efficiency for the liquefaction of sawdust. It was observed that hydrogen ions from the catalyst were primarily responsible for the significant thermal effects on the liquefaction system and the generation of large quantities of active species; these effects directly contributed to a higher efficacy of the plasma-enabled liquefaction process.

关键词： discharge plasma     biomass liquefaction     catalyst     homogeneous catalysts    

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Diagnostic evaluation of plasma aldosterone concentration to plasma renin activity ratio in primary aldosteronism

ZHANG Huilan, WANG Daowen

《医学前沿（英文）》 2008年 第2卷 第1期   页码 11-14 doi: 10.1007/s11684-008-0003-4

摘要： Using the plasma aldosterone concentration to plasma renin activity ratio (PAC/PRA ratio) as the screening test of choice for primary aldosteronism in hypertensive patients, we studied the clinical characteristics and the diagnostic value of PAC/PRA ratio in primary aldosteronism. The plasma aldosterone concentration (PAC) and plasma renin activity (PRA) levels were measured by radioimmunoassay in 902 hypertensive patients from out-patient clinics or hospitals. One hundred and twenty-six suspected primary aldosteronism patients whose PAC/PRA ratio was > 25 ng/dL/ng/mL/hr had a lamellar computed tomography (CT) scan in the adrenal gland and follow-up visits. The proportion of primary aldosteronism in hypertensive patients was 14% (126/902). There were 54 patients with unilateral or bilateral hyperplasia and 25 patients with adenoma according to the CT scan. 39% (49/126) of the patients with primary aldosteronism had hypokalemia. Twenty-five patients received surgical treatment. The efficacy and cure rates were 100% (25/25) and 48% (12/25), respectively. The effective rate of aldactone and the single-drug cure rate were 89% (48/54) and 24% (13/54), respectively. Primary aldosteronism affects over 10% of hypertensive patients in China. The PAC/PRA ratio can be considered as a routine screening test in hypertensives, especially resistant hypertensive patients and a high PAC/PRA ratio is an invaluable index in primary aldosteronism diagnosis.
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Important parameters in plasma jets for the production of RONS in liquids for plasma medicine: A brief

Anna Khlyustova, Cédric Labay, Zdenko Machala, Maria-Pau Ginebra, Cristina Canal

《化学科学与工程前沿（英文）》 2019年 第13卷 第2期   页码 238-252 doi: 10.1007/s11705-019-1801-8

摘要： Reactive oxygen and nitrogen species (RONS) are among the key factors in plasma medicine. They are generated by atmospheric plasmas in biological fluids, living tissues and in a variety of liquids. This ability of plasmas to create a delicate mix of RONS in liquids has been used to design remote or indirect treatments for oncological therapy by treating biological fluids by plasmas and putting them in contact with the tumour. Documented effects include selective cancer cell toxicity, even though the exact mechanisms involved are still under investigation. However, the “right” dose for suitable therapeutical activity is crucial and still under debate. The wide variety of plasma sources hampers comparisons. This review focuses on atmospheric pressure plasma jets as the most studied plasma devices in plasma medicine and compiles the conditions employed to generate RONS in relevant liquids and the concentration ranges obtained. The concentrations of H O , NO , NO and short-lived oxygen species are compared critically to provide a useful overview for the reader.

关键词： atmospheric plasma jets     liquids     ROS     RNS     plasma-dose    

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Kinetic Monte Carlo simulations of plasma-surface reactions on heterogeneous surfaces

Daniil Marinov

《化学科学与工程前沿（英文）》 2019年 第13卷 第4期   页码 815-822 doi: 10.1007/s11705-019-1837-9

摘要： Reactions of atoms and molecules on chamber walls in contact with low temperature plasmas are important in various technological applications. Plasma-surface interactions are complex and relatively poorly understood. Experiments performed over the last decade by several groups prove that interactions of reactive species with relevant plasma-facing materials are characterized by distributions of adsorption energy and reactivity. In this paper, we develop a kinetic Monte Carlo (KMC) model that can effectively handle chemical kinetics on such heterogenous surfaces. Using this model, we analyse published adsorption-desorption kinetics of chlorine molecules and recombination of oxygen atoms on rotating substrates as a test case for the KMC model.

关键词： plasma-surface interaction     kinetic Monte Carlo     plasma nano technology    

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From plasma to plasmonics: toward sustainable and clean water production through membranes

《化学科学与工程前沿（英文）》 2023年 第17卷 第12期   页码 1809-1836 doi: 10.1007/s11705-023-2339-3

摘要： The increasing demand for potable water is never-ending. Freshwater resources are scarce and stress is accumulating on other alternatives. Therefore, new technologies and novel optimization methods are developed for the existing processes. Membrane-based processes are among the most efficient methods for water treatment. Yet, membranes suffer from severe operational problems, namely fouling and temperature polarization. These effects can harm the membrane’s permeability, permeate recovery, and lifetime. To mitigate such effects, membranes can be treated through two techniques: plasma treatment (a surface modification technique), and treatment through the use of plasmonic materials (surface and bulk modification). This article showcases plasma- and plasmonic-based treatments in the context of water desalination/purification. It aims to offer a comprehensive review of the current developments in membrane-based water treatment technologies along with suggested directions to enhance its overall efficiency through careful selection of material and system design. Moreover, basic guidelines and strategies are outlined on the different membrane modification techniques to evaluate its prerequisites. Besides, we discuss the challenges and future developments about these membrane modification methods.

关键词： water treatment     membrane-based process     plasma treatment     plasma polymerization     plasmonic     light-to-heat conversion    

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Plasma-catalysis: Is it just a question of scale?

J. Christopher Whitehead

《化学科学与工程前沿（英文）》 2019年 第13卷 第2期   页码 264-273 doi: 10.1007/s11705-019-1794-3

摘要： The issues of describing and understanding the changes in performance that result when a catalyst is placed into plasma are discussed. The different chemical and physical interactions that result and how their combination might produce beneficial results for the plasma-catalytic processing of different gas streams are outlined with particular emphasis being placed on the different range of spatial and temporal scales that must be considered both in experiment and modelling. The focus is on non-thermal plasma where the lack of thermal equilibrium creates a range of temperature scales that must be considered. This contributes in part to a wide range of inhomogeneity in different properties such as species concentrations and electric fields that must be determined experimentally by methods and be incorporated into modelling. It is concluded that plasma-catalysis is best regarded as conventional catalysis perturbed by the presence of a discharge, which modifies its operating conditions, properties and outcomes often in a very localised way. The sometimes used description “plasma-activated catalysis” is an apt one.

关键词： plasma catalysis     plasma-activated catalysis     non-thermal plasma     CO2 conversion    

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Submerged arc plasma system combined with ozone oxidation for the treatment of wastewater containing

《环境科学与工程前沿（英文）》 2021年 第15卷 第5期 doi: 10.1007/s11783-020-1384-0

摘要：

• Submerged arc plasma was introduced in terms of wastewater treatment.

关键词： Thermal plasma     Submerged arc plasma     Wastewater     Ozone     Phenol     Highly energetic electron    

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Modelling and diagnostics of multiple cathodes plasma torch system for plasma spraying

Kirsten BOBZIN, Nazlim BAGCIVAN, Lidong ZHAO, Ivica PETKOVIC, Jochen SCHEIN, Karsten HARTZ-BEHREND, Stefan KIRNER, José-Luis MARQUéS, Günter FORSTER

《机械工程前沿（英文）》 2011年 第6卷 第3期   页码 324-331 doi: 10.1007/s11465-011-0125-2

摘要：

Usage of a multiple-arcs system has significantly improved process stability and coating properties in air plasma spraying. However, there are still demands on understanding and controlling the physical process to determine process conditions for reproducible coating quality and homogeneity of coating microstructure. The main goal of this work is the application of numerical simulation for the prediction of the temperature profiles at the torch outlet for real process conditions. Behaviour of the gas flow and electric arcs were described in a three-dimensional numerical model. The calculated results showed the characteristic triangular temperature distribution at the torch nozzle outlet caused by three electric arcs. These results were compared with experimentally determined temperature distributions, which were obtained with specially developed computed tomography equipment for reconstructing the emissivity and temperature distribution of the plasma jet close to the torch exit. The calculated results related to temperature values and contours were verified for the most process parameters with experimental ones.

关键词： plasma spraying     electric arc     three-cathode plasma torch     numerical simulation     computed tomography    

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Gender differences in the relationship between plasma lipids and fasting plasma glucose in non-diabetic

null

《医学前沿（英文）》 2014年 第8卷 第4期   页码 477-483 doi: 10.1007/s11684-014-0346-y

摘要：

The association between dyslipidemia and elevated fasting glucose in type 2 diabetes is well known. In non-diabetes, whether this association still exists, and whether dyslipidemia is an independent risk factor for high fasting plasma glucose (FPG) levels are not clear. This cross-sectional study recruited 3460 non-diabetic Chinese subjects (1027 men, and 2433 women, aged 35–75 years old) who participated in a health survey. Men and women were classified into tertiles by levels of plasma lipids respectively. In women, the prevalence of impaired fasting glucose (IFG) was decreased with increased HDL-C. A stepwise increase in HDL-C was associated with decreasing FPG levels (lowest tertiles, FPG: 5.376±0.018; middle tertiles, 5.324±0.018; highest tertiles, 5.276±0.018 mmol/L; P=0.001). Reversely, FPG levels increased from lowest tertiles to highest tertiles of LDL-C, TC, and TG. we found that women in the first tertile with lower HDL-C level had a 1.75-fold increase in risk of IFG compared with non-diabetic women in the third tertile with higher HDL-C level (OR: 1.75; 95% CI: 1.20--2.56). In men, no significant association was found. We took age, BMI, waist/hip ratio, education, smoking, alcohol drinking, and physical exercise as adjusted variables. In Chinese non-diabetic women, dyslipidemia is independently associated with high levels of FPG; TG, HDL-C, and LDL-C are predictors of IFG independent of BMI and waist/hip ratio.

关键词： dyslipidemia     plasma lipids     plasma fasting glucose     impaired fasting glucose     non-diabetes    

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Cross-sectional network analysis of plasma proteins/metabolites correlated with pathogenesis and therapeutic

《医学前沿（英文）》 doi: 10.1007/s11684-023-1022-x

摘要： The treatment of PML/RARA+ acute promyelocytic leukemia (APL) with all-trans-retinoic acid and arsenic trioxide (ATRA/ATO) has been recognized as a model for translational medicine research. Though an altered microenvironment is a general cancer hallmark, how APL blasts shape their plasma composition is poorly understood. Here, we reported a cross-sectional correlation network to interpret multilayered datasets on clinical parameters, proteomes, and metabolomes of paired plasma samples from patients with APL before or after ATRA/ATO induction therapy. Our study revealed the two prominent features of the APL plasma, suggesting a possible involvement of APL blasts in modulating plasma composition. One was characterized by altered secretory protein and metabolite profiles correlating with heightened proliferation and energy consumption in APL blasts, and the other featured APL plasma-enriched proteins or enzymes catalyzing plasma-altered metabolites that were potential trans-regulatory targets of PML/RARA. Furthermore, results indicated heightened interferon-gamma signaling characterizing a tumor-suppressing function of the immune system at the first hematological complete remission stage, which likely resulted from therapy-induced cell death or senescence and ensuing supraphysiological levels of intracellular proteins. Overall, our work sheds new light on the pathophysiology and treatment of APL and provides an information-rich reference data cohort for the exploratory and translational study of leukemia microenvironment.

关键词： acute promyelocytic leukemia     plasma proteomics     plasma metabolomics     cross-sectional correlation network     pathogenesis     treatment    

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The role of ions in plasma catalytic carbon nanotube growth: A review

Erik C. Neyts

《化学科学与工程前沿（英文）》 2015年 第9卷 第2期   页码 154-162 doi: 10.1007/s11705-015-1515-5

摘要： While it is well-known that the plasma-enhanced catalytic chemical vapor deposition (PECVD) of carbon nanotubes (CNTs) offers a number of advantages over thermal CVD, the influence of the various individual contributing factors is not well understood. Especially the role of ions is unclear, since ions in plasmas are generally associated with sputtering rather than with growing a material. Even so, various studies have demonstrated the beneficial effects of ion bombardment during the growth of CNTs. This review looks at the role of the ions in plasma-enhanced CNT growth as deduced from both experimental and simulation studies. Specific attention is paid to the beneficial effects of ion bombardment. Based on the available literature, it can be concluded that ions can be either beneficial or detrimental for carbon nanotube growth, depending on the exact conditions and the control over the growth process.

关键词： plasma-enhanced chemical vapor deposition (PECVD)     carbon nanotube (CNT)     ion bombardment     defect healing    

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标题 作者 时间 类型 操作

Atomistic simulations of plasma catalytic processes

Erik C. Neyts

期刊论文

Effect of glow discharge plasma on rhodium-based catalyst for oxygenates synthesis

HUANG Lihong, CHU Wei, XU Junqiang, HONG Jingping, YI Min

期刊论文

Ni/MgO catalyst prepared via dielectric-barrier discharge plasma with improved catalytic performance

Yan LI,Zhehao WEI,Yong WANG

期刊论文

Abatement of mixed volatile organic compounds in a catalytic hybrid surface/packed-bed discharge plasma

Lianjie Guo, Nan Jiang, Jie Li, Kefeng Shang, Na Lu, Yan Wu

期刊论文

Liquid discharge plasma for fast biomass liquefaction at mild conditions: The effects of homogeneous

Sen Wang, Shiyun Liu, Danhua Mei, Rusen Zhou, Congcong Jiang, Xianhui Zhang, Zhi Fang, Kostya (Ken) Ostrikov

期刊论文

Diagnostic evaluation of plasma aldosterone concentration to plasma renin activity ratio in primary aldosteronism

ZHANG Huilan, WANG Daowen

期刊论文

Important parameters in plasma jets for the production of RONS in liquids for plasma medicine: A brief

Anna Khlyustova, Cédric Labay, Zdenko Machala, Maria-Pau Ginebra, Cristina Canal

期刊论文

Kinetic Monte Carlo simulations of plasma-surface reactions on heterogeneous surfaces

Daniil Marinov

期刊论文

From plasma to plasmonics: toward sustainable and clean water production through membranes

期刊论文

Plasma-catalysis: Is it just a question of scale?

J. Christopher Whitehead

期刊论文

Submerged arc plasma system combined with ozone oxidation for the treatment of wastewater containing

期刊论文

Modelling and diagnostics of multiple cathodes plasma torch system for plasma spraying

Kirsten BOBZIN, Nazlim BAGCIVAN, Lidong ZHAO, Ivica PETKOVIC, Jochen SCHEIN, Karsten HARTZ-BEHREND, Stefan KIRNER, José-Luis MARQUéS, Günter FORSTER

期刊论文

Gender differences in the relationship between plasma lipids and fasting plasma glucose in non-diabetic

null

期刊论文

Cross-sectional network analysis of plasma proteins/metabolites correlated with pathogenesis and therapeutic

期刊论文

The role of ions in plasma catalytic carbon nanotube growth: A review

Erik C. Neyts

期刊论文