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Desulfurization performance of iron-manganese-based sorbent for hot coal gas

Xiurong REN, Weiren BAO, Fan LI, Liping CHANG, Kechang XIE

《化学科学与工程前沿（英文）》 2010年第4卷第4期页码 429-434 doi: 10.1007/s11705-010-0504-y

摘要： A series of iron-manganese-based sorbents were prepared by co-precipitation and physical mixing method, and used for H S removal from hot coal gas. The sulfidation tests were carried out in a fixed-bed reactor with space velocity of 2000 h (STP). The results show that the suitable addition of manganese oxide in iron-based sorbent can decrease H S and COS concentration in exit before breakthrough due to its simultaneous reaction capability with H S and COS. Fe O and MnO are the initial active components in iron-manganese-based sorbent, and FeO and Fe are active components formed by reduction during sulfidation. The crystal phases of iron affect obviously their desulfurization capacity. The reducibility of sorbent changes with the content of MnO in sorbent. S7F3M and S3F7M have bigger sulfur capacities (32.68 and 32.30 gS/100 g total active component), while S5F5M has smaller sulfur capacity (21.92 gS/100 g total active component). S7F3M sorbent has stable sulfidation performance in three sulfidation-regeneration cycles and no apparent structure degradation. The sulfidation performance of iron- manganese-based sorbent is also related with its specific surface area and pore volume.

关键词： iron-manganese-based sorbent sulfidation performance regeneration hot coal gas

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Redox reactions of iron and manganese oxides in complex systems

Jianzhi Huang, Huichun Zhang

《环境科学与工程前沿（英文）》 2020年第14卷第5期 doi: 10.1007/s11783-020-1255-8

摘要： • Mechanisms of redox reactions of Fe- and Mn-oxides were discussed. • Oxidative reactions of Mn- and Fe-oxides in complex systems were reviewed. • Reductive reaction of Fe(II)/iron oxides in complex systems was examined. • Future research on examining the redox reactivity in complex systems was suggested. Conspectus Redox reactions of Fe- and Mn-oxides play important roles in the fate and transformation of many contaminants in natural environments. Due to experimental and analytical challenges associated with complex environments, there has been a limited understanding of the reaction kinetics and mechanisms in actual environmental systems, and most of the studies so far have only focused on simple model systems. To bridge the gap between simple model systems and complex environmental systems, it is necessary to increase the complexity of model systems and examine both the involved interaction mechanisms and how the interactions affected contaminant transformation. In this Account, we primarily focused on (1) the oxidative reactivity of Mn- and Fe-oxides and (2) the reductive reactivity of Fe(II)/iron oxides in complex model systems toward contaminant degradation. The effects of common metal ions such as Mn2+ , Ca2+, Ni2+, Cr3+ and Cu2+, ligands such as small anionic ligands and natural organic matter (NOM), and second metal oxides such as Al, Si and Ti oxides on the redox reactivity of the systems are briefly summarized.

关键词： Iron oxides manganese oxides reduction oxidation complex systems reaction kinetics and mechanisms

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Migration of manganese and iron during the adsorption-regeneration cycles for arsenic removal

Fangfang CHANG, Jiuhui QU, Xu ZHAO, Wenjun LIU, Kun WU

《环境科学与工程前沿（英文）》 2011年第5卷第4期页码 512-518 doi: 10.1007/s11783-011-0372-9

摘要： Fe-Mn binary oxide incorporated into porous diatomite (FMBO-diatomite) was prepared in situ and regenerated in a fixed-bed column for arsenite [As(III)] and arsenate [As(V)] removal. Four consecutive adsorption cycles were operated under the following conditions: Initial arsenic concentration of 0.1 mg·L , empty bed contact time of 5 min, and pH 7.0. About 3000, 3300, 3800, and 4500 bed volumes of eligible effluent (arsenic concentration≤0.01 mg·L ) were obtained in four As(III) adsorption cycles; while about 2000, 2300, 2500, and 3100 bed volumes of eligible effluent were obtained in four As(V) adsorption cycles. The dissection results of FMBO-diatomite fixed-bed exhibited that small amounts of manganese and iron were transferred from the top of the fixed-bed to the bottom of the fixed-bed during As(III) removal process. Compared to the extremely low concentration of iron (<0.01 mg·L ), the fluctuation concentration of Mn in effluent of the As(III) removal column was in a range of 0.01–0.08 mg·L . The release of manganese suggested that manganese oxides played an important role in As(III) oxidation. Determined with the US EPA toxicity characteristic leaching procedure (TCLP), the leaching risk of As(III) on exhausted FMBO-diatomite was lower than that of As(V).

关键词： arsenic adsorption filtration regeneration fixed-bed

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Reaction mechanism of arsenic capture by a calcium-based sorbent during the combustion of arsenic-contaminated

Mei Lei, Ziping Dong, Ying Jiang, Philip Longhurst, Xiaoming Wan, Guangdong Zhou

《环境科学与工程前沿（英文）》 2019年第13卷第2期 doi: 10.1007/s11783-019-1110-y

摘要：

Pilot-scale combustion is required to treat arsenic-enriched biomass in China.

CaO addition to arsenic-enriched biomass reduces arsenic emission.

CaO captures arsenic via chemical adsorption to form Ca₃(AsO₄)₂.

关键词： Arsenic contamination Phytoremediation Emission control Calcium-based sorbent Biomass disposal Pilot-scale combustion

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Chemical composition and formation mechanisms in the cathode-electrolyte interface layer of lithium manganeseoxide batteries from reactive force field (ReaxFF) based molecular dynamics

Sahithya REDDIVARI, Christian LASTOSKIE, Ruofei WU, Junliang ZHANG

《能源前沿（英文）》 2017年第11卷第3期页码 365-373 doi: 10.1007/s11708-017-0500-8

摘要： Lithium manganese oxide (LiMn O ) is a principal cathode material for high power and high energy density electrochemical storage on account of its low cost, non-toxicity, and ease of preparation relative to other cathode materials. However, there are well-documented problems with capacity fade of lithium ion batteries containing LiMn O . Experimental observations indicate that the manganese content of the electrolyte increases as an electrochemical cell containing LiMn O ages, suggesting that active material loss by dissolution of divalent manganese from the LiMn O surface is the primary reason for reduced cell life in LiMn O batteries. To improve the retention of manganese in the active material, it is key to understand the reactions that occur at the cathode surface. Although a thin layer of electrolyte decomposition products is known to form at the cathode surface, the speciation and reaction mechanisms of Mn in this interface layer are not yet well understood. To bridge this knowledge gap, reactive force field (ReaxFF) based molecular dynamics was applied to investigate the reactions occurring at the LiMn O cathode surface and the mechanisms that lead to manganese dissolution. The ReaxFFMD simulations reveal that the cathode-electrolyte interface layer is composed of oxidation products of electrolyte solvent molecules including aldehydes, esters, alcohols, polycarbonates, and organic radicals. The oxidation reaction pathways for the electrolyte solvent molecules involve the formation of surface hydroxyl species that react with exposed manganese atoms on the cathode surface. The presence of hydrogen fluoride (HF) induces formation of inorganic metal fluorides and surface hydroxyl species. Reaction products predicted by ReaxFF-based MD are in agreement with experimentally identified cathode-electrolyte interface compounds. An overall cathode-electrolyte interface reaction scheme is proposed based on the molecular simulation results.

关键词： lithium manganese oxide batteries reactive force field (ReaxFF) cathode-electrolyte interface layer molecular dynamics

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首座大型生物除铁除锰水厂的实践

李冬,杨宏,张杰

《中国工程科学》 2003年第5卷第7期页码 53-57

摘要：

以生物固锰除锰理论为指导，设计了弱曝气一级过滤生物除铁除锰简缩流程。采集了土著除锰菌扩增后接种于除铁除锰滤层，再经2～3个月的滤层培养，取得了强劲的除锰能力。当原水Mn²⁺为1～3 mg/L，Fe²⁺为0.1～0.5 mg/L，在正常滤速下，滤后水Mn²⁺减至0.05 mg/L，总铁为痕量，优于国家标准。该厂出水常年良好稳定，满足了高新产业优良用水之需。生物固锰除锰理论的工程实践解决了半个世纪以来水质净化工程上除锰的难题，创建了我国乃至世界上首座大型生物除铁除锰水厂。

关键词：生物固锰除锰弱曝气简缩流程同时去除

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New nanostructured sorbents for desulfurization of natural gas

Lifeng WANG, Ralph T. YANG

《化学科学与工程前沿（英文）》 2014年第8卷第1期页码 8-19 doi: 10.1007/s11705-014-1411-4

摘要： Desulfurization of natural gas is achieved commercially by absorption with liquid amine solutions. Adsorption technology could potentially replace the solvent extraction process, particularly for the emerging shale gas wells with production rates that are generally lower than that from the large conventional reservoirs, if a superior adsorbent (sorbent) is developed. In this review, we focus our discussion on three types of sorbents: metal-oxide based sorbents, Cu/Ag-based and other commercial sorbents, and amine-grafted silicas. The advantages and disadvantages of each type are analyzed. Possible approaches for future developments to further improve these sorbents are suggested, particularly for the most promising amine-grafted silicas.

关键词： desulfurization natural gas desulfurization hydrogen sulfide sorbent amine-silica sorbent

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Performance and kinetics of iron-based oxygen carriers reduced by carbon monoxide for chemical looping

Xiuning HUA,Wei WANG,Feng WANG

《环境科学与工程前沿（英文）》 2015年第9卷第6期页码 1130-1138 doi: 10.1007/s11783-015-0821-y

摘要： Chemical looping combustion is a promising technology for energy conversion due to its low-carbon, high-efficiency, and environmental-friendly feature. A vital issue for CLC process is the development of oxygen carrier, since it must have sufficient reactivity. The mechanism and kinetics of CO reduction on iron-based oxygen carriers namely pure Fe O and Fe O supported by alumina (Fe O /Al O ) were investigated using thermo-gravimetric analysis. Fe O /Al O showed better reactivity over bare Fe O toward CO reduction. This was well supported by the observed higher rate constant for Fe O /Al O over pure Fe O with respective activation energy of 41.1±2.0 and 33.3±0.8 kJ·mol . The proposed models were compared via statistical approach comprising Akaike information criterion with correction coupled with F-test. The phase-boundary reaction and diffusion control models approximated to 95% confidence level along with scanning electron microscopy results; revealed the promising reduction reactions of pure Fe O and Fe O /Al O . The boosting recital of iron-based oxygen carrier support toward efficient chemical looping combustion could be explained accurately through the present study.

关键词： chemical looping combustion iron-based oxygen carriers reduction kinetics carbon monoxide statistics

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Preparation and selection of Fe-Cu sorbent for COS removal in syngas

Bowu CHENG, Zhaofei CAO, Yong BAI, Dexiang ZHANG

《化学科学与工程前沿（英文）》 2010年第4卷第4期页码 441-444 doi: 10.1007/s11705-010-0507-8

摘要： A series of iron-based sorbents prepared with iron trioxide hydrate, cupric oxide by a novel method was studied in a fixed-bed reactor for COS removal from syngas at moderate temperature. In addition, the sorbents mixed with various additives in different ratios were tested. The effects of additive type and ratio on the breakthrough capacity and desulfurization performance, as well as the influence of operating conditions on sulfidation behavior of the sorbent, were investigated. The simulate gas contained 1% COS, 5% CO , 20%–30% CO and 60%–70% H . The outlet gases from the fixed-bed reactor were automatically analyzed by on-line mass spectrometry, and the COS concentration before breakthrough can be kept steady at 1 ppmv. The result shows that the breakthrough sulfur capacity of the sorbent is as high as 25 g-S/100 g. At 700 K and space velocity of 1000 h , the efficiency of sulfur removal and breakthrough sulfur capacity of the sorbent increase with the increase of copper oxide with an optimum value. The result shows that the species and content of additives also affect desulfurization performance of the sorbent.

关键词： sorbent desulfurization COS removal syngas

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A review on research and development of iron-based sorbents for removal of hydrogen sulfide from hot

Jianglong YU, Liping CHANG, Fan LI, Kechang XIE

《化学科学与工程前沿（英文）》 2010年第4卷第4期页码 529-535 doi: 10.1007/s11705-010-0519-4

摘要： In poly-generation and integrated gasification-combined cycle (IGCC) systems for clean energy conversion, it is essential to remove impurities such as sulfur species from hot coal gases prior to entering the subsequent units. This paper provides a comprehensive review on previous studies on high temperature removal of hydrogen sulfide from high temperature coal gases using iron-based sorbents. A two-step desulphurization process for hot coal gas cleanup is highlighted, which is integrated with direct production of elemental sulfur during regeneration of iron-based sorbents in the primary desulphurization step. Different kinetic modeling approaches for sulfidation and regeneration were compared. Limited research on activated carbon supported sorbents was also briefly summarized.

关键词： hot coal gas cleanup iron-based sorbents sulfidation regeneration sulphur recovery

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钾/锰助剂对氮掺杂碳纳米管负载铁基催化剂在CO₂加氢过程中的影响研究 Article

Praewpilin Kangvansura, Ly May Chew, Chanapa Kongmark, Phatchada Santawaja, Holger Ruland, Wei Xia, Hans Schulz, Attera Worayingyong, Martin Muhler

《工程（英文）》 2017年第3卷第3期页码 385-392 doi: 10.1016/J.ENG.2017.03.013

摘要：

氮掺杂碳纳米管(NCNTs) 作为载体负载铁(Fe) 纳米颗粒，可应用于CO₂多相催化加氢反应(633 K和25 bar)。当将钾(K) 和锰(Mn) 作为助催化剂时，Fe/NCNT 展现出优异的CO₂ 加氢性能，在体积空速(GHSV) 为3.1 L·(g·h)^–1 时转化率可达34.9%。当使用K 作为助催化剂时，反应对烯烃和短链烷烃具有高的选择性。当K 和Mn 同时作为助催化剂时，其催化活性能够稳定地维持60 h。助催化剂Mn 的结构效应通过X 射线衍射、氢气程序升温还原以及近边X 射线吸收精细结构进行表征。助催化剂Mn 不仅能够稳定中间态FeO，且能降低程序升温还原的起始温度。通过探针反应NH₃ 的催化分解来表征助催化剂效应。当K 和Mn 作为助催化剂时，Fe/NCNT 具有最好的催化活性。在还原条件下，当K 作为助催化剂时，Fe/NCNT 具有最优异的热稳定性。

关键词： CO₂ 加氢铁基催化剂 n 型碳纳米管 Mn 助剂 K 助剂

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Cadmium removal mechanistic comparison of three Fe-based nanomaterials: Water-chemistry and roles of

《环境科学与工程前沿（英文）》 2022年第16卷第12期 doi: 10.1007/s11783-022-1586-8

摘要：

● nZVI, S-nZVI, and nFeS were systematically compared for Cd(II) removal.

关键词： Nano zero valent iron Sulfided zero valent iron FeS Cd(II) immobilization Fe dissolution

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Efficient MgO-doped CaO sorbent pellets for high temperature CO

Zhihong Xu, Tao Jiang, Hao Zhang, Yujun Zhao, Xinbin Ma, Shengping Wang

《化学科学与工程前沿（英文）》 2021年第15卷第3期页码 698-708 doi: 10.1007/s11705-020-1981-2

摘要： Novel MgO-doped CaO sorbent pellets were prepared by gel-casting and wet impregnation. The effect of Na and MgO on the structure and CO adsorption performance of CaO sorbent pellets was elucidated. MgO-doped CaO sorbent pellets with the diameter range of 0.5 1.5 mm exhibited an excellent capacity for CO adsorption and adsorption rate due to the homogeneous dispersion of MgO in the sorbent pellets and its effects on the physical structure of sorbents. The results show that MgO can effectively inhibit the sintering of CaO and retain the adsorption capacity of sorbents during multiple adsorption-desorption cycles. The presence of mesopores and macropores resulted in appreciable change of volume from CaO (16.7 cm ∙mol ) to CaCO (36.9 cm ∙mol ) over repeated operation cycles. Ca2Mg1 sorbent pellets exhibited favorable CO capture capacity (9.49 mmol∙g ), average adsorption rate (0.32 mmol∙g ∙min ) and conversion rate of CaO (74.83%) after 30 cycles.

关键词： MgO doping CaO sorbent pellets gel-casting technique CO₂ capture

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Iron oxide nanoparticle-based theranostics for cancer imaging and therapy

Xiaoqing REN,Hongwei CHEN,Victor YANG,Duxin SUN

《化学科学与工程前沿（英文）》 2014年第8卷第3期页码 253-264 doi: 10.1007/s11705-014-1425-y

摘要： Theranostic platform, which is equipped with both diagnostic and therapeutic functions, is a promising approach in cancer treatment. From various nanotheranostics studied, iron oxide nanoparticles have advantages since IONPs have good biocompatibility and spatial imaging capability. This review is focused on the IONP-based nanotheranostics for cancer imaging and treatment. The most recent progress for applications of IONP nanotheranostics is summarized, which includes IONP-based diagnosis, magnetic resonance imaging (MRI), multimodal imaging, chemotherapy, hyperthermal therapy, photodynamic therapy, and gene delivery. Future perspectives and challenges are also outlined for the potential development of IONP based theranostics in clinical use.

关键词： theranostics iron oxide nanoparticles MRI drug delivery photothermal therapy photodynamic therapy

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Effects of humic acid and surfactants on the aggregation kinetics of manganese dioxide colloids

Xiaoliu HUANGFU,Yaan WANG,Yongze LIU,Xixin LU,Xiang ZHANG,Haijun CHENG,Jin JIANG,Jun MA

《环境科学与工程前沿（英文）》 2015年第9卷第1期页码 105-111 doi: 10.1007/s11783-014-0726-1

摘要： The aggregation of common manganese dioxide (MnO ) colloids has great impact on their surface reactivity and therefore on their fates as well as associated natural and synthetic contaminants in engineered (e.g. water treatment) and natural aquatic environments. Nevertheless, little is known about the aggregation kinetics of MnO colloids and the effect of humic acid (HA) and surfactants on these. In this study, the early stage aggregation kinetics of MnO nanoparticles in NaNO and Ca(NO ) solutions in the presence of HA and surfactants (i.e., sodium dodecyl sulfate (SDS), and polyvinylpyrrolidone (PVP)) were modeled through time-resolved dynamic light scattering. In the presence of HA, MnO colloids were significantly stabilized with a critical coagulation concentration (CCC) of ~300 mmol·L NaNO and 4 mmol·L Ca(NO ) . Electrophoretic mobility (EPM) measurements confirmed that steric hindrance may be primarily responsible for increasing colloidal stability in the presence of HA. Moreover, the molecular and/or chemical properties of HA might impact its stabilizing efficiency. In the case of PVP, only a slight increase of aggregation kinetics was observed, due to steric reactions originating from adsorbed layers of PVP on the MnO surface. Consequently, higher CCC values were obtained in the presence of PVP. However, there was a negligible reduction in MnO colloidal stability in the presence of 20 mg·L SDS.

关键词： humic acid surfactant aggregation kinetics drinking water manganese dioxide colloids

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标题作者时间类型操作

Desulfurization performance of iron-manganese-based sorbent for hot coal gas

Xiurong REN, Weiren BAO, Fan LI, Liping CHANG, Kechang XIE

期刊论文

Redox reactions of iron and manganese oxides in complex systems

Jianzhi Huang, Huichun Zhang

期刊论文

Migration of manganese and iron during the adsorption-regeneration cycles for arsenic removal

Fangfang CHANG, Jiuhui QU, Xu ZHAO, Wenjun LIU, Kun WU

期刊论文

Reaction mechanism of arsenic capture by a calcium-based sorbent during the combustion of arsenic-contaminated

Mei Lei, Ziping Dong, Ying Jiang, Philip Longhurst, Xiaoming Wan, Guangdong Zhou

期刊论文

Chemical composition and formation mechanisms in the cathode-electrolyte interface layer of lithium manganeseoxide batteries from reactive force field (ReaxFF) based molecular dynamics

Sahithya REDDIVARI, Christian LASTOSKIE, Ruofei WU, Junliang ZHANG

期刊论文

首座大型生物除铁除锰水厂的实践

李冬,杨宏,张杰

期刊论文

New nanostructured sorbents for desulfurization of natural gas

Lifeng WANG, Ralph T. YANG

期刊论文

Performance and kinetics of iron-based oxygen carriers reduced by carbon monoxide for chemical looping

Xiuning HUA,Wei WANG,Feng WANG

期刊论文

Preparation and selection of Fe-Cu sorbent for COS removal in syngas