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Materials · 2023 ·Vol. 16 ·期 6 ·2343 · IF 3.4

Enhanced Desulfurization by Tannin Extract Absorption Assisted by Binuclear Sulfonated Phthalocyanine Cobalt Polymer: Performance and Mechanism

Bing Wang,Huanyu Chen,Xingguang Hao,Kai Li,Xin Sun,Yuan Li,Ping Ning

Removal of hydrogen sulfide (H2S) from coke oven gas has attracted increasing attention due to economic and environmental concerns. In this study, tannin extract (TE) absorption combined with binuclear sulfonated phthalocyanine cobalt organic polymer (OTS) and binuclear sulfonated phthalocyanine cobalt (PDS) with a fixed bed reactor is used for removal of H2S. The effect of gas flow rate, concentration of H2S, co-existence of organic sulfide compounds and O2were investigated. Then, the effect of total alkalinity content of TE, NaVO3, OTS and PDS was studied in detail. The experimental results demonstrated that 100% H2S conversion could maintain for 13 h at a total alkalinity of 5.0 g/L, TE concentration of 4.0 g/L, NaVO3concentration of 5 g/L, and OTS and PDS concentration of 0.2 g/L and 0.2 g/L, respectively. The OTS and PDS showed synergistic effect on boosting TE desulfurization efficiency. The results provide a new route for the investigation of liquid catalyzed oxidation desulfurization in an efficient and low-cost way.Keywords:coke oven flue gas;flue gas desulfurization;tannin extract desulfurization;polymer

研究领域: 环境科学 · 化学工程
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FUEL · 2025 · IF 7.5

Gaseous arsenic capture and immobilization from incineration flue gas by MFe2O4 (M = Ca, Mn, Co, Ni, Cu and Zn) spinel sorbents

Dawei Wu,Aijia Zhang,Jing Liu,Yingju Yang

MFe 2 O 4 (M = Ca, Mn, Co, Ni, Cu and Zn) spinel sorbents were synthesized by a low-temperature sol–gel auto-combustion method for arsenic adsorption from flue gas. CuFe 2 O 4 spinel exhibited the highest arsenic removal performance among these sorbents, and the adsorption capacity reached 14.09 mg/g at 800 °C. The pseudo-first order, pseudo-second-order and Elovich kinetic models can well predict arsenic removal process, which indicates that the mass transfer and chemisorption processes are important during arsenic capture by CuFe 2 O 4 . The impact of incineration flue gas components on As 2 O 3 adsorption was elucidated. It was found that HCl showed negligible effect on arsenic removal by CuFe 2 O 4 sorbent while CO 2 , H 2 O, SO 2 and NO played inhibition roles. X-ray photoelectron spectroscopy results revealed that the adsorbed arsenic exists in the forms of As 3+ and As 5+ on the sorbent surface. The chemisorption and oxidation mechanisms are responsible for arsenic adsorption by CuFe 2 O 4 . The toxicity characteristic leaching procedure and sequential extraction experiments demonstrated that arsenic can be considerably immobilized in the CuFe 2 O 4 sorbent. The high arsenic capture capacity, excellent HCl resistance and low risk of secondary contamination make CuFe 2 O 4 an efficient sorbent for gaseous arsenic capture.

CAS / MDL: 7782-61-8
研究领域: 环境科学 · 材料科学
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Royal Society Open Science · 2019 ·Vol. 6 ·期 2 · IF 2.515

Molecular characterization of aldehydes and ketones in particle phase of mainstream and sidestream cigarette smoke

Xiu Chen,Quan Shi,Xibin Zhou,Xuezheng Liu

Aldehydes and ketones (AKs) in cigarette smoke are risk to humans and environment. Due to the complexity of itself and the interference of the smoke tar matrix, the aldehydes and ketones in particle phase (AKPs) of mainstream smoke (MSS) and sidestream smoke (SSS) have not been well investigated. In this study, the AKPs of MSS and SSS were derivatized into polar products by reaction with Girard T reagent. The derivatives were isolated rapidly by column chromatography and analysed by Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS). Fifteen species of aldehydes and ketones were detected by positive ion electrospray ionization (ESI) FT-ICR MS: O1–6, N1O1–4, N2O1–3 and N3O2–3. The total number of AKPs obtained by ESI FT-ICR MS in MSS and SSS is about 1100 and 970, respectively. After hydrolysis, the original AKPs were obtained and 63 carbonyls were identified and quantified by gas chromatography–mass spectrometry (GCMS). The nitrogen-containing and high-oxygen AKPs were further characterized by Orbitrap mass spectrometry. Structures of compounds with high relative abundance in the mass spectrum were speculated (e.g. a series of degradants of cembrenediol) by comparison with the results of GCMS.

研究领域: 化学 · 环境科学 · 公共卫生
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ENERGY & FUELS · 2024 · IF 5.2

Simultaneous Desulfurization and Denitrification by H2O2/FeSO4 Preoxidation Combined with Wet Flue Gas Desulfurization Postabsorption: Experimental Investigation and Process Simulation

Jia-tao Xiang,Jun-ting Li,Xiong Zhang,Han Zhang,Shao-hui Ren,Shi-hong Zhang

This study focused on the development of a novel process of H2O2/FeSO4 preoxidation combined with wet flue gas desulfurization (WFGD) postabsorption for simultaneous desulfurization and denitrification, and recovery of sulfur and nitrogen from flue gas. The results show that when no oxidant is added, the denitrification efficiency by WFGD is only 5.3%, while under the H2O2/FeSO4 preoxidation, the desulfurization and denitrification efficiency can reach 99.9% and 83.6%, respectively. When the liquid/gas ratio reaches 18 L·m–3, the desulfurization efficiency is nearly 100%, and the denitrification efficiency can reach 90.6% due to the increased liquid/gas contact area and improved heat and mass transfer. The absorption process of SO2 and NOx involves both physical and chemical absorption, which is dominated by physical absorption, and the absorption characteristics are multilayer absorption. The desulfurization products CaSO3 and CaSO4, and the denitrification products Ca(NO2)2 and Ca(NO3)2, are absorbed by the CaCO3 slurry. The Aspen Plus process simulation results show that the desulfurization and denitrification efficiencies are 99.5% and 89.6%, respectively, and the concentrations of SO2 and NOx in the flue gas are 21.4 mg·m–3 and 41.5 mg·m–3, respectively, which meet the ultralow emission standards. In addition, the H2O2/NO molar ratio, oxidation temperature, and SO2 concentration have an important effect on the NO conversion, which then affects the denitrification efficiency.

CAS / MDL: 471-34-1
研究领域: 环境工程 · 化学工程 · 过程模拟
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FUEL PROCESSING TECHNOLOGY · 2020 · IF 4.982

Capture of arsenic in coal combustion flue gas at high temperature in the presence of CaSiO3 with good anti-sintering

Yue Cao,Bing Song,Min Song,Fanyue Meng,Yuexing Wei,Qi Cao

Arsenic with high volatility and toxicity is usually generated during coal combustion and the capture of arsenic is restrained at high temperature since the sintering of adsorbents. Therefore, it is necessary to develop an adsorbent with sintering resistance for the arsenic removal at high temperature. In the study, the arsenic vapor capture by CaSiO 3 , CaO and SiO 2 was carried out in the flue gas with/without SO 2 and NO at high temperatures from 1000 °C to 1200 °C. The results showed that CaSiO 3 exhibited excellent arsenic capture with the capacity of 4.98 mg/g and the capture efficiency was increased with the temperature increasing. The effect of acid gases was also considered. A certain amount of CaSO 4 with poor capture performance was formed on CaSiO 3 surface in the presence of SO 2 , leading to the decrease of the amount of arsenic captured. On the other hand, the effect of NO was not obvious as SO 2 . Although arsenic capture was suppressed when introduced SO 2 and NO, it still remained considerable arsenic capture for the CaSiO 3 adsorbent. Additionally, the pivotal role of O 2 was also studied. Taking into account the high capture capacity and excellent anti-sintering property, CaSiO 3 was a good adsorbent suitable for the removal of arsenic from coal combustion flue gas.

研究领域: 环境科学 · 能源工程
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CHEMICAL ENGINEERING JOURNAL · 2022 · IF 16.744

A high efficiency and high capacity mercury adsorbent based on elemental selenium loaded SiO2 and its application in coal-fired flue gas

Rihong Xiao,Yili Zhang,Shuzhou Wei,Xing Chuai,Xiangzheng Cui,Zhuo Xiong,Junying Zhang,Yongchun Zhao

Massive Hg emissions from coal-fired units cause serious environmental pollution and result in a substantial waste of Hg resources. In this study, the prepared millimeter-grade Se/SiO 2 adsorbent was applied as a filler to adsorb mercury in a fixed-bed reactor to obtain the high value-added product HgSe, which solved the problem of short contact time and secondary pollution caused by the traditional injection mercury removal adsorbents. Experimental Hg removal showed that the 25 % Se-loaded adsorbent exhibited excellent Hg removal performance at 150 °C, with a saturation adsorption capacity of mercury was as high as 101.04 mg/g, nearly 300 times that of commercial activated carbons. Additionally, the influence of the flue gas composition on the Hg removal performance of Se/SiO 2 was studied. The results showed that O 2 , NO, and HCl increased the efficiency of Hg removal and SO 2 and SO 3 had trivial impact on the Hg removal performance. The Hg temperature-programmed desorption test results showed that the adsorbed Hg appeared predominantly as HgSe on the sample surface. DFT calculations verified that Se loading improved Hg removal performance and defined the adsorption mechanism. Moreover, the prepared Se/SiO 2 adsorbent carrier was soluble SiO 2 , which provided a good condition for the subsequent high-purity collection of HgSe. Finally, the technological process of Hg removal via Se-loaded adsorbents and the recovery of HgSe were proposed, which could offer a new way to achieve the resource utilization of Hg.

研究领域: 环境科学 · 材料科学
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FUEL · 2022 · IF 8.035

SO2 resistance of CeO2- and Co3O4-supported activated carbon during removal of mercury from flue gas: A comparative study

Shengji Wu,Yalun Ma,Wangsheng Yu,Hui Wang,Wei Yang,Lei Che,Zhongxi Han

How to enhance the SO 2 tolerance of transition metal oxide-supported activated carbon is one of the hottest issues in the field of mercury capture from flue gas. Addition of a foreign metal ion to prepare bimetallic adsorbent is a common method of improving the SO 2 tolerance of adsorbent. However, this approach suffers from high cost and a complex preparation process. In this study, CeO 2 - and Co 3 O 4 -supported activated carbon ( m %CeO 2 /AC and m %Co 3 O 4 /AC), with various loading values of active center, were prepared by an incipient wetness impregnation method, and their SO 2 tolerances were compared. The mercury removal performance and SO 2 tolerance of both CeO 2 /AC and Co 3 O 4 /AC could be remarkably improved through increasing the loading amount of the active center. Co 3 O 4 /AC exhibited high affinity with SO 2 , and the chemisorbed oxygen in Co 3 O 4 would be largely consumed, when SO 2 was present in the flue gas, resulting in a significant decrease of mercury removal efficiency. The mercury removal efficiencies of 20%CeO 2 /AC, 40%CeO 2 /AC and 60%CeO 2 /AC were 86.1%, 93.7% and 93.7%, respectively, during removal of mercury from flue gas at 150 °C in the presence of SO 2 . 20%CeO 2 /AC was the optimal adsorbent for mercury capture from flue gas, owing to its excellent mercury removal efficiency, strong SO 2 tolerance and relatively lower cost. The mercury species formed over spent 20%CeO 2 /AC were HgO and HgSO 4 . The HgO was generated through the reaction of mercury and chemisorbed oxygen, while the formation of HgSO 4 was due to the reaction between mercury, SO 2 and chemisorbed oxygen. The regeneration investigation indicated that the activity of spent 20%CeO 2 /AC could be almost fully recovered through a temperature-programmed decomposition and desorption process. The present study showed that the SO 2 tolerance of CeO 2 /AC could be easily improved through regulation of the loading amount of the active center.

研究领域: 环境科学 · 化学工程 · 材料科学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2022 · IF 9.136

Thermal conductivity analysis of ceramic membranes for recovering water from flue gas

Zhaohao Li,Run Qi,Zheng Zhang,Heng Zhang,Haiping Chen,Dan Gao

Condensation is the common mechanism of water intake from gases. Transport membrane condenser is a newly proposed technology to recover water from flue gas based on the mechanism of condensation. Most of the existing heat transfer research on transport membrane condenser focuses on water vapor phase change or fluid convection heat transfer, and there is a lack of research on the thermal conductivity of ceramic membranes. The significance of studying thermal conductivity is to optimize the overall heat transfer performance. The thermal conductivity of alumina ceramic solid materials is not good enough, which can affect the industrial application performance to a certain extent. There is currently a lack of experimental measurements or theoretical calculations to quantitatively characterize the thermal conductivity of ceramic membranes. This affects the optimization of overall heat transfer performance of transport membrane condenser. In this paper, coal fly ash is used as the raw materials to prepare macroporous ceramic membranes. Coal fly ash is a very cheap material. It can greatly reduce the manufacturing cost of transport membrane condenser using coal fly ash to prepare ceramic membranes. The classical theoretical model of thermal conductivity of porous materials is introduced, the calculation and experimental results are compared, and the validity and limitation of the classical models in analyzing the heat transfer problem of transport membrane condenser are discussed. Finally, based on the composite effective medium theory, combining with the experimental results, a modified model is proposed. The modified model reduces the average theoretical error to 7.20%, and enriches the research on the heat transfer theory of transport membrane condenser.

研究领域: 材料科学 · 热力学 · 环境工程
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ENERGY & FUELS · 2024 · IF 5.2

Multiscale Investigation of 3D Morphology SnSe2 for Mercury Removal from Flue Gas: Experimental and Simulation Studies

Rihong Xiao,Yili Zhang,Kaiyan Long,Zhuo Xiong,Junying Zhang,Yongchun Zhao

Mercury, a toxic heavy metal, poses significant risks to human health. Coal-fired power plants are the largest anthropogenic sources of mercury emissions, making mercury removal from flue gas imperative. Among various mercury adsorbents, metal selenides show promising potential in mercury capture. Here, we reported the synthesis of a novel three-dimensional hierarchical flower-like material, SnSe2, and its debut application in flue gas mercury capture. Under the influence of low-coordinated selenium, the introduction of abundant selenium vacancy defects led to the exposure of additional active sites in the adsorbent. Additionally, the presence of Sn enhanced gas selectivity and promoted electron transfer processes, thereby augmenting Hg0 adsorption and oxidation performance. Benefiting from these advantages, SnSe2 exhibited superior mercury removal performance over a wide temperature range (30–180 °C), with a saturated mercury adsorption capacity of 2027.23 μg/g, surpassing that of commercial activated carbon. Furthermore, the presence of NO in flue gas improved mercury adsorption performance, while high concentrations of SO2 do not affect mercury removal efficiency, as elucidated by adsorption kinetics models. Moreover, the mercury adsorption mechanism was demonstrated through mercury temperature-programmed desorption (Hg-TPD) and density functional theory (DFT) calculations. Finally, toxicity characteristic leaching procedure (TCLP) experiments confirmed SnSe2 as an efficient and permanent adsorbent for mercury, offering insights into the application of novel mercury removal materials.

研究领域: 环境科学 · 材料科学
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Journal of Cleaner Production · 2021 · IF 9.297

Highly efficient sorption and immobilization of gaseous arsenic from flue gas on MnO2/attapulgite composite with low secondary leaching risks

Kai-Qiang He,Chun-Gang Yuan,Yang-Hong Jiang,Yan Li,Xue-Lei Duan,Qi Guo

Some sorbents have been developed for arsenic (As) compounds capture from flue gas . However, most of the conventional sorbents have cost constraints and can cause secondary pollution due to the leaching of arsenic after use. To solve this problem, a new and highly efficient adsorbent for gaseous arsenic was successfully developed in this paper with excellent immobilization performance and low-cost. A series of Mn-supported attapulgite (ATP) composites were fabricated, characterized, and investigated for arsenic capture. The modification of ATP with Mn not only considerably enhanced the adsorption efficiency but also stabilized the adsorbed As in the spent sorbents. SO 2 in flue gas promoted the adsorption performance through As-sulfate binding, whereas NO was beneficial for the oxidation of As(III) to As(V) on the surface of Mn-modified ATP. The incorporation of Mn with ATP generated abundant hydroxylate (OH − ) from hydration and accelerated the formation of As-sulfate compounds, which was beneficial for physical encapsulation. The results of the toxicity characteristic leaching procedure and sequential extraction test revealed that adsorbed As could be considerably immobilized by the sorbent with low leaching ability. Mn modification changed more As into inert fractions and consequently inhibited release from spent sorbents, which considerably reduced the risks of secondary pollution. The developed composite can be potentially used as a new efficient sorbent for gaseous arsenic capture in flue gas.

研究领域: 环境科学 · 材料科学
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NEW JOURNAL OF CHEMISTRY · 2021 ·Vol. 45 ·期 30 ·13329-13339 · IF 3.591

Preferred zinc-modified melamine phytate for the flame retardant polylactide with limited smoke release

Dong Wang,Yang Wang,Xuhui Zhang,Ting Li,Mingliang Du,Mingqing Chen,Weifu Dong

Bio-based flame retardants (FRs) have drawn increasing attention for FR polylactide (PLA). Hence, a green and facile method was presented in this work for the synthesis of melamine phytate (MPA), melamine copper phytate (MPACu), melamine zinc phytate (MPAZn), and melamine magnesium phytate (MPAMg). In general, the PLA/MPAZn composite exhibited a better flame retardancy and smoke suppression with an acceptable mechanical property. With the addition of 20 phr MPAZn, the peak of heat release rate (PHRR) was decreased by 45.0% compared with that of neat PLA. Also, TSR of the PLA/MPAZn composite was the lowest among the FR PLA composites in this study. Furthermore, the higher quality char residues played the key role in the synergistic flame retardancy and smoke suppression for the PLA/MPAZn composites. In addition, in this work, we found that the mass loss rate (MLR) was highly related to the heat release rate (HRR).

研究领域: 材料科学 · 环境科学
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FUEL · 2024 · IF 6.7

Demineralization effects on physicochemical and combustion characteristics of biomass: Insights into distributed kinetics, flue gas evolution, and slag formation

Peiyong Ma,Bowen Li,Rui Diao,Xiaohao Liu,Zhusong Cheng,Fenglei Qi

Biomass as the only carbon-bearing renewable energy has enormous potential to challenge the established energy structure dominated by fossil resources, and incineration technology is one of the most direct and efficient pathways for utilizing biomass resources, unfortunately enduring the inevitable sintering and slagging problems owing to the excessive alkali metals. Herein, we comparatively investigated the effects of five leaching solvents (water, acetic acid, wood vinegar, hydrochloric acid, and oxalic acid) on the physicochemical properties and ash-removal capabilities of wheat straw (WS) and rice husk (RH), with a view to achieving better performance in the subsequent combustion characteristics, kinetic examination, flue gas, and slag evolution. Results indicated with ionization ability increased (water < acetic acid < hydrochloric acid), the WS exhibited a strong demineralization performance (maximum 61.1%), further leading to a steep weight loss in its combustion characteristic curve at approximately 350 °C and a delayed peak temperature after the removal of alkali metal. Multiple distributed activation energy model and sensitivity analysis revealed that leaching pretreatment enhanced the activation energy (189–191.8 kJ mol −1 ) and optimized energy distribution at the preliminary stage of the combustion reaction. In addition, the absence of alkali metals suppressed the catalytic oxidation reaction in the flue gas, remarkably limiting the formation of CO 2 but facilitating the release of CO and CH 4 . Meanwhile, a considerable optimal in biomass ash slagging, in which the initial temperature of the liquid phase slag for WS ash increased to 991 °C. Notably, HCl showed the strongest demineralization performance among the five leaching solvents during pretreatment, but the high-temperature slag content was still higher than that of acetic acid. Therefore, slagging performance is not only associated with the demineralization ability of leaching solvents, but also with ash composition.

研究领域: 能源与环境科学 · 化学工程
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