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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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Simultaneous CO

Jie ZHU,Wei WANG,Xiuning HUA,Zhou XIA,Zhou DENG

《环境科学与工程前沿（英文）》 2015年 第9卷 第6期   页码 1117-1129 doi: 10.1007/s11783-015-0812-z

摘要： The chemical looping concept provided a novel way to achieve carbon separation during the production of energy or substances. In this work, hydrogen generation with inherent CO capture in single packed bed reactor via this concept was discussed. Two oxygen carriers, Fe O 60 wt.% and Fe O 55 wt.%/CuO 5 wt.% supported by Al O , were made by ball milling method. First, according to the characteristics of the reduction breakthrough curve, a strict fuel supply strategy was selected to achieve simultaneous CO capture and H production. Then, in the long term tests using CO as fuel, it was proved that CuO addition improved hydrogen generation with the maximum intensity of 3700 μmol H ·g Fe O compared with Fe-Al of 2300 μmol H ·g Fe O . The overall CO capture efficiency remained 98%–98.8% over 100 cycles. Moreover, the reactivity of deactivated materials was recovered nearly like that of fresh ones by sintering treatment. Finally, two kinds of complex gases consist of CO, H , CH and CO were utilized as fuels to test the feasibility. The results showed all components could be completely converted by Fe-Cu-Al in the reduction stage. The intensity of hydrogen production and the overall CO capture efficiency were in the range of 2000–2400 μmol H ·g Fe O and 89%–95%, respectively.

关键词： CO2 capture     chemical looping hydrogen generation     iron based oxygen carriers     single packed bed reactor     long-term test     complex gases fuel    

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Influence of Fe on electrocatalytic activity of iron-nitrogen-doped carbon materials toward oxygen reduction

Lin LI, Cehuang FU, Shuiyun SHEN, Fangling JIANG, Guanghua WEI, Junliang ZHANG

《能源前沿（英文）》 2022年 第16卷 第5期   页码 812-821 doi: 10.1007/s11708-020-0669-0

摘要： The development of highly active nitrogen-doped carbon-based transition metal (M-N-C) compounds for the oxygen reduction reaction (ORR) in proton exchange membrane fuel cells (PEMFCs) greatly helps reduce fuel cell cost, thus rapidly promoting their commercial applications. Among different M-N-C electrocatalysts, the series of Fe-N-C materials are highly favored because of their high ORR activity. However, there remains a debate on the effect of Fe, and rare investigations focus on the influence of Fe addition in the second heat treatment usually performed after acid leaching in the catalyst synthesis. It is thus very critical to explore the influences of Fe on the ORR electrocatalytic activity, which will, in turn, guide the design of Fe-N-C materials with enhanced performance. Herein, a series of Fe-N-C electrocatalysts are synthesize and the influence of Fe on the ORR activity are speculated both experimentally and theoretically. It is deduced that the active site lies in the structure of Fe-N , accompanied with the addition of appropriate Fe, and the number of active sites increases without the occurrence of agglomeration particles. Moreover, it is speculated that Fe plays an important role in stabilizing N as well as constituting active sites in the second pyrolyzing process.

关键词： oxygen reduction reaction     Fe-N-C     active sites     Fe addition     second heat treatment    

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Heterometallic cluster-based organic frameworks as highly active electrocatalysts for oxygen reductionand oxygen evolution reaction: a density functional theory study

《化学科学与工程前沿（英文）》 2023年 第17卷 第5期   页码 570-580 doi: 10.1007/s11705-022-2247-y

摘要： Recently, metal–organic frameworks are one of the potential catalytic materials for electrocatalytic applications. The oxygen reduction reaction and oxygen evolution reaction catalytic activities of heterometallic cluster-based organic frameworks are investigated using density functional theory. Firstly, the catalytic activities of heterometallic clusters are investigated. Among all heterometallic clusters, Fe2Mn–Mn has a minimum overpotential of 0.35 V for oxygen reduction reaction, and Fe2Co–Co possesses the smallest overpotential of 0.32 V for oxygen evolution reaction, respectively 100 and 50 mV lower than those of Pt(111) and RuO2(110) catalysts. The analysis of the potential gap of Fe2M clusters indicates that Fe2Mn, Fe2Co, and Fe2Ni clusters possess good bifunctional catalytic activity. Additionally, the catalytic activity of Fe2Mn and Fe2Co connected through 3,3′,5,5′-azobenzenetetracarboxylate linker to form Fe2M–PCN–Fe2M is explored. Compared with Fe2Mn–PCN–Fe2Mn, Fe2Co–PCN–Fe2Co, and isolated Fe2M clusters, the mixed-metal Fe2Co–PCN–Fe2Mn possesses excellent bifunctional catalytic activity, and the values of potential gap on the Mn and Co sites of Fe2Co–PCN–Fe2Mn are 0.69 and 0.70 V, respectively. Furthermore, the analysis of the electron structure indicates that constructing a mixed-metal cluster can efficiently enhance the electronic properties of the catalyst. In conclusion, the mixed-metal cluster strategy provides a new approach to further design and synthesize high-efficiency bifunctional electrocatalysts.

关键词： bimetallic metal–organic frameworks     bifunctional electrocatalyst     density functional theory     oxygen reduction reaction     oxygen evolution reaction    

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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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A review of Pt-based electrocatalysts for oxygen reduction reaction

Changlin ZHANG, Xiaochen SHEN, Yanbo PAN, Zhenmeng PENG

《能源前沿（英文）》 2017年 第11卷 第3期   页码 268-285 doi: 10.1007/s11708-017-0466-6

摘要： Development of active and durable electrocatalyst for oxygen reduction reaction (ORR) remains one challenge for the polymer electrolyte membrane fuel cell (PEMFC) technology. Pt-based nanomaterials show the greatest promise as electrocatalyst for this reaction among all current catalytic structures. This review focuses on Pt-based ORR catalyst material development and covers the past achievements, current research status and perspectives in this research field. In particular, several important categories of Pt-based catalytic structures and the research advances are summarized. Key factors affecting the catalyst activity and durability are discussed. An outlook of future research direction of ORR catalyst research is provided.

关键词： oxygen reduction reaction (ORR)     electrocatalysis     platinum catalyst     activity     durability    

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Metal-free, carbon-based catalysts for oxygen reduction reactions

Zhiyi Wu,Zafar Iqbal,Xianqin Wang

《化学科学与工程前沿（英文）》 2015年 第9卷 第3期   页码 280-294 doi: 10.1007/s11705-015-1524-4

摘要： Developing metal-free, carbon-based catalysts to replace platinum-based catalysts for oxygen reduction reactions (ORRs) is an emerging area of research. In recent years, different carbon structures including carbon doped with IIIA-VIIA heteroatoms (C−M site-based, where M represents the doped heteroatom) and polynitrogen (PN) compounds encapsulated in carbon nanotubes (CNTs) (N−N site-based) have been synthesized. Compared to metallic catalysts, these materials are highly active, stable, inexpensive, and environmentally friendly. This review discusses the development of these materials, their ORR performances and the mechanisms for how the incorporation of heteroatoms enhances the ORR activity. Strategies for tailoring the structures of the carbon substrates to improve ORR performance are also discussed. Future studies in this area will need to include optimizing synthetic strategies to control the type, amount and distribution of the incorporated heteroatoms, as well as better understanding the ORR mechanisms in these catalysts.

关键词： oxygen reduction reaction     electrocatalysis     metal-free     carbon-based     polynitrogen    

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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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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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Removal of dissolved oxygen from water using a Pd-resin based catalytic reactor

Wenxin SHI, Chongwei CUI, Liye ZHAO, Shuili YU, Xia YUN

《化学科学与工程前沿（英文）》 2009年 第3卷 第1期   页码 107-111 doi: 10.1007/s11705-009-0154-0

摘要： The removal of dissolved oxygen (DO) from water was studied experimentally in a Pd-resin base catalyst reactor using purified hydrogen gas as a reducing agent. The effects of various operating conditions, such as hydrogen and water flow rates, height of the catalytic resin bed, temperature, pH value and run time, on the removal of DO, had been studied extensively. The results shows that DO could be removed by the reactor from ppm to ppb levels at ambient temperature. Increases of temperature, H gas rate and the height of the catalytic resin were helpful to improve the DO removal rate. The change of pH value from 4 to 12 resulted in no effect on DO removal. Reaction time was the key factor to control the DO removal efficiency. Only when the reaction time was longer than 2.3 minutes under the experimental conditions, could a very low DO level be achieved.

关键词： dissolved oxygen     palladium     catalytic reactor     hydrogen     resin    

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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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All-in-one functional supramolecular nanoparticles based on pillar[5]arene for controlled generation,storage and release of singlet oxygen

《化学科学与工程前沿（英文）》 2023年 第17卷 第3期   页码 307-313 doi: 10.1007/s11705-022-2216-5

摘要： The storage and controlled release of singlet oxygen (1O2) have attracted increasing attention due to the wide application and microsecond lifetime of 1O2 in water. Herein we provide an integrated nanoplatform consisting of a diphenylanthracene derivative, a water-soluble pillar[5]arene and a photosensitizer tetrakis(4-hydroxyphenyl)porphyrin (TPP), that may provide the controlled generation, storage and release of singlet oxygen. We design a new diphenylanthracene derivative with two trimethylammonium bromide groups on both ends that can be well recognized by the pillar[5]arene. The formed nanocarriers can be used to load TPP through their supramolecular self-assembly. The resulting nanoparticles show good water-solubility and uniform spherical morphology. After laser irradiation (660 nm), the nanoparticles exhibit excellent ability for the generation and storage of 1O2. When the irradiated nanoparticles are heated above 80 °C, 1O2 can be released from the system. Therefore, in this paper we pioneer the use of noncovalent interaction to integrate the diphenylanthracene derivatives and photosensitizers into one functional system, which provides a new strategy for the controlled generation, storage and release of singlet oxygen. We believe this groundbreaking strategy will have a great potential in providing necessary amounts of 1O2 for the photodynamic therapy of tumors in dark.

关键词： storage and controlled release of singlet oxygen     supramolecular nanoparticles     noncovalent interactions     pillararenes     diphenylanthracene     photosensitizers    

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Revealing the GHG reduction potential of emerging biomass-based CO utilization with an iron cycle system

《环境科学与工程前沿（英文）》 2023年 第17卷 第10期 doi: 10.1007/s11783-023-1727-8

摘要：

● Greenhouse gas mitigation by biomass-based CO2 utilization with a Fe cycle system.

关键词： Carbon dioxide utilization     Hydrothermal reactions     Biomass-based CO2 reduction     Simulation     Ex-ante LCA    

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Validation of polymer-based nano-iron oxide in further phosphorus removal from bioeffluent: laboratory

Ming HUA, Lili XIAO, Bingcai PAN, Quanxing ZHANG

《环境科学与工程前沿（英文）》 2013年 第7卷 第3期   页码 435-441 doi: 10.1007/s11783-013-0508-1

摘要： The efficient removal of phosphorous from water is an important but challenging task. In this study, we validated the applicability of a new commercially available nanocomposite adsorbent, i.e., a polymer-based hydrated ferric oxide nanocomposite (HFO-201), for the further removal of phosphorous from the bioeffluent discharged from a municipal wastewater treatment plant, and the operating parameters such as the flow rate, temperature and composition of the regenerants were optimized. Laboratory-scale results indicate that phosphorous in real bioeffluent can be effectively removed from 0.92 mg·L to<0.5 mg·L (or even<0.1 mg·L as desired) by the new adsorbent at a flow rate of 50 bed volume (BV) per hour and treatable volume of 3500–4000 BV per run. Phosphorous removal is independent of the ambient temperature in the range of 15°C–40°C. Moreover, the exhausted HFO-201 can be regenerated by a 2% NaOH+ 5% NaCl binary solution for repeated use without significant capacity loss. A scaled-up study further indicated that even though the initial total phosphorus (TP) was as high as 2 mg·L , it could be reduced to<0.5 mg·L , with a working capacity of 4.4–4.8 g·L HFO-201. In general, HFO-201 adsorption is a choice method for the efficient removal of phosphate from biotreated waste effluent.

关键词： bioeffluent     phosphorus removal     nanocomposite adsorbent     hydrated ferric oxide    

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randomized, controlled, open label non-inferiority trial of intravenous ferric carboxymaltose versus ironsucrose in patients with iron deficiency anemia in China

《医学前沿（英文）》 doi: 10.1007/s11684-023-1001-2

摘要： Iron deficiency (ID) and ID anemia (IDA) pose significant public health concerns in China. Although iron sucrose (IS) treatment is well-established in the country, ferric carboxymaltose (FCM) offers the advantage of higher doses and fewer infusions. This open label, randomized, controlled, non-inferiority trial was conducted at multiple sites in China to compare the outcomes of FCM (maximum of 2 doses, 500 or 1000 mg iron) and IS (up to 11 infusions, 200 mg iron) treatments in subjects with IDA. The primary endpoint was the achievement of hemoglobin (Hb) response (an increase of ≥2 g/dL from baseline) within 8 weeks, whereas secondary endpoints included changes in Hb, transferrin saturation, and serum ferritin levels. Among the 371 randomized subjects, a similar percentage of subjects treated with FCM and IS achieved Hb-response (FCM 99.4%, IS 98.3%), thereby confirming the non-inferiority of FCM compared with IS (difference 1.12 (−2.15, 4.71; 95% confidence interval (CI))). Furthermore, a significantly higher proportion of FCM-treated subjects achieved early Hb-response at Week 2 (FCM 85.2%, IS 73.2%; difference 12.1 (3.31, 20.65; 95% CI)). Additionally, the increase in TSAT and serum ferritin levels from baseline was significantly greater at all time points for FCM-treated subjects. The safety profiles of FCM and IS were comparable, with the exception of transient hypophosphatemia and pyrexia, which are consistent with FCM’s known safety profile. In conclusion, FCM proves to be an efficacious treatment for IDA, providing faster Hb-response and correction of ID with fewer administrations than IS.

关键词： iron deficiency     anemia     intravenous iron     ferric carboxymaltose     iron sucrose     Hb response     early response    

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标题 作者 时间 类型 操作

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

Simultaneous CO

Jie ZHU,Wei WANG,Xiuning HUA,Zhou XIA,Zhou DENG

期刊论文

Influence of Fe on electrocatalytic activity of iron-nitrogen-doped carbon materials toward oxygen reduction

Lin LI, Cehuang FU, Shuiyun SHEN, Fangling JIANG, Guanghua WEI, Junliang ZHANG

期刊论文

Heterometallic cluster-based organic frameworks as highly active electrocatalysts for oxygen reductionand oxygen evolution reaction: a density functional theory study

期刊论文

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

A review of Pt-based electrocatalysts for oxygen reduction reaction

Changlin ZHANG, Xiaochen SHEN, Yanbo PAN, Zhenmeng PENG

期刊论文

Metal-free, carbon-based catalysts for oxygen reduction reactions

Zhiyi Wu,Zafar Iqbal,Xianqin Wang

期刊论文

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

期刊论文

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

期刊论文

Removal of dissolved oxygen from water using a Pd-resin based catalytic reactor

Wenxin SHI, Chongwei CUI, Liye ZHAO, Shuili YU, Xia YUN

期刊论文

Iron oxide nanoparticle-based theranostics for cancer imaging and therapy

Xiaoqing REN,Hongwei CHEN,Victor YANG,Duxin SUN

期刊论文

All-in-one functional supramolecular nanoparticles based on pillar[5]arene for controlled generation,storage and release of singlet oxygen

期刊论文

Revealing the GHG reduction potential of emerging biomass-based CO utilization with an iron cycle system

期刊论文

Validation of polymer-based nano-iron oxide in further phosphorus removal from bioeffluent: laboratory

Ming HUA, Lili XIAO, Bingcai PAN, Quanxing ZHANG

期刊论文

randomized, controlled, open label non-inferiority trial of intravenous ferric carboxymaltose versus ironsucrose in patients with iron deficiency anemia in China

期刊论文