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Multi-Pollutant Formation and Control in Pressurized Oxy-Combustion: SOx, NOx, Particulate Matter, and

Gaofeng Dai,Jiaye Zhang,Zia ur Rahman,Yufeng Zhang,Yili Zhang,Milan Vujanović,Hrvoje Mikulčić,Nebojsa Manić,Aneta Magdziarz,Houzhang Tan,Richard L. Axelbaum,Xuebin Wang,

《工程(英文)》 doi: 10.1016/j.eng.2024.03.005

摘要: Oxy-combustion is a promising carbon-capture technology, but atmospheric-pressure oxy-combustion has a relatively low net efficiency, limiting its application in power plants. In pressurized oxy-combustion (POC), the boiler, air separation unit, flue gas recirculation unit, and CO2 purification and compression unit are all operated at elevated pressure; this makes the process more efficient, with many advantages over atmospheric pressure, such as low NOx emissions, a smaller boiler size, and more. POC is also more promising for industrial application and has attracted widespread research interest in recent years. It can produce high-pressure CO2 with a purity of approximately 95%, which can be used directly for enhanced oil recovery or geo-sequestration. However, the pollutant emissions must meet the standards for carbon capture, storage, and utilization. Because of the high oxygen and moisture concentrations in POC, the formation of acids via the oxidation and solution of SOx and NOx can be increased, causing the corrosion of pipelines and equipment. Furthermore, particulate matter (PM) and mercury emissions can harm the environment and human health. The main distinction between pressurized and atmospheric-pressure oxy-combustion is the former’s elevated pressure; thus, the effect of this pressure on the pollutants emitted from POC—including SOx, NOx, PM, and mercury—must be understood, and effective control methodologies must be incorporated to control the formation of these pollutants. This paper reviews recent advances in research on SOx, NOx, PM, and mercury formation and control in POC systems that can aid in pollutant control in such systems.

关键词: Pressurized oxy-combustion     Sulfur oxides     Nitrogen oxides     Particulate matter     Mercury     Direct contact cooler     Carbon capture and sequestration    

Selective catalytic reduction of NOx from exhaust of lean-burn engine over Ag-Al2O3/cordierite catalyst

LI Junhua, KANG Shoufang, FU Lixin, HAO Jiming

《环境科学与工程前沿(英文)》 2007年 第1卷 第2期   页码 143-146 doi: 10.1007/s11783-007-0025-1

摘要: A highly effective Ag-AlO catalyst was prepared using the sol-gel method, and characterized by surface area using nitrogen adsorption, scanning electron microscopy (SEM), and transmission electron microscopy (TEM) techniques. The catalyst performance was tested on a real lean-burn gasoline engine. Only unburned hydrocarbons and carbon monoxide in the exhaust were directly used as reductant (without any external reductant), the maximum NO conversion could only reach 40% at 450?C. When an external reductant, ethanol was added, the average NO conversion was greater than 60%. At exhaust gas temperature range of 350 500?C, the maximum NO conversion reached about 90%. CO and HC could be efficiently oxidized with Pt-AO oxidation catalyst placed at the end of SCR converter. However, NO conversion drastically decreased because of the oxidation of some intermediates to NO again. The possible reaction mechanism was proposed as two typical processes, nitration, and reduction in HC-SCR over Ag-AlO.

关键词: lean-burn gasoline     external reductant     nitrogen adsorption     conversion     catalyst performance    

Selective catalytic reduction of NO

Pavlo I. Kyriienko

《化学科学与工程前沿(英文)》 2020年 第14卷 第4期   页码 471-491 doi: 10.1007/s11705-019-1847-7

摘要: Research results regarding selective catalytic reduction (SCR) of NO with ethanol and other C oxygenates as reductants over silver-alumina catalysts are summarized. The aspects of the process mechanism, nature of active sites, role of alumina and silver (especially in the formation of bifunctional active sites), effects of reductants and reaction conditions are discussed. It has been determined that key stages of the process include formation of reactive enolic species, their interaction with NO and formation of nitroorganic compounds which transform to NCO species and further to N . The results obtained over various silver-alumina catalysts demonstrate the perspectives of their application for reducing the level of nitrogen oxides in engine emissions, including in the presence of water vapor and sulfur oxides. Ways to improve the catalysts for the SCR of NO with C oxygenates are outlined.

关键词: SCR     nitrogen oxides     silver-alumina catalyst     silver species     ethanol     oxygenates    

Precise regulation of acid pretreatment for red mud SCR catalyst: Targeting on optimizing the acidity and reducibility

《环境科学与工程前沿(英文)》 2022年 第16卷 第7期 doi: 10.1007/s11783-021-1447-x

摘要:

• The optimum SCR activity was realized by tuning the acid pretreatment.

关键词: Air pollution control     Nitrogen oxides     Selective catalytic reduction     Red mud     Solid waste utilization    

4 on HZSM-5 support: designing applicable catalysts for selective catalytic reduction of nitrogenoxides by ammonia

《化学科学与工程前沿(英文)》 2023年 第17卷 第11期   页码 1741-1754 doi: 10.1007/s11705-023-2332-x

摘要: Based on monolayer dispersion theory, Co3O4/ZSM-5 catalysts with different loadings have been prepared for selective catalytic reduction of nitrogen oxides by ammonia. Co3O4 can spontaneously disperse on HZSM-5 support with a monolayer dispersion threshold of 0.061 mmol 100 m–2, equaling to a weight percentage around 4.5%. It has been revealed that the quantities of surface active oxygen (O2) and acid sites are crucial for the reaction, which can adsorb and activate NOx and NH3 reactants effectively. Below the monolayer dispersion threshold, Co3O4 is finely dispersed as sub-monolayers or monolayers and in an amorphous state, which is favorable to generate the two kinds of active sites, hence promoting the performance of ammonia selective catalytic reduction of nitrogen oxide. However, the formation of crystalline Co3O4 above the capacity is harmful to the reaction performance. 4% Co3O4/ZSM-5, the catalyst close to the monolayer dispersion capacity, possesses the most abundant active O2 species and acidic sites, thereby demonstrating the best reaction performance in all the samples. It is proposed the optimal Co3O4/ZSM-5 catalyst can be prepared by loading the capacity amount of Co3O4 onto HZSM-5 support.

关键词: Co3O4/ZSM-5     NOx-SCR by NH3     monolayer dispersion threshold effect     surface acid sites     surface active O2 anions    

Study on the NOx release rule along the boiler during pulverized coal combustion

JIN Jing, ZHANG Zhongxiao, LI Ruiyang

《能源前沿(英文)》 2007年 第1卷 第1期   页码 91-95 doi: 10.1007/s11708-007-0009-7

摘要: Numerical simulation and experimental study on NO release along the boiler during pulverized coal combustion have been conducted. With the increase of temperature the NO emission increased and the peak value of NO release moved forward. But when the temperature increased to a certain degree, NO emission began to reduce. NO emission increased with the increase of nitrogen content of coal. The peak value of NO release moved backwards with the increase of coal rank. NO emission increased obviously with the increase of stoichiometric ratio. There existed a critical average diameter of the pulverized coal (). If "d, NO emission reduced with the decrease of pulverized coal size. If >, NO emission reduced with the increase of the pulverized coal size. The results showed that the simulation results are in agreement with the experimental results for concentration distribution of NO along the axis of the furnace.

Design and operational considerations for selective catalytic reduction technologies at coal-fired boilers

Jeremy J. SCHREIFELS, Shuxiao WANG, Jiming HAO

《能源前沿(英文)》 2012年 第6卷 第1期   页码 98-105 doi: 10.1007/s11708-012-0171-4

摘要: By the end of 2010, China had approximately 650 GW of coal-fired electric generating capacity producing almost 75% of the country’s total electricity generation. As a result of the heavy reliance on coal for electricity generation, emissions of air pollutants, such as nitrogen oxides (NO ), are increasing. To address these growing emissions, the Ministry of Environmental Protection (MEP) has introduced new NO emission control policies to encourage the installation of selective catalytic reduction (SCR) technologies on a large number of coal-fired electric power plants. There is, however, limited experience with SCR in China. It is therefore useful to explore the lessons from the use of SCR technologies in other countries. This paper provides an overview of SCR technology performance at coal-fired electric power plants demonstrating emission removal rates between 65% and 92%. It also reviews the design and operational challenges that, if not addressed, can reduce the reliability, performance, and cost-effectiveness of SCR technologies. These challenges include heterogeneous flue gas conditions, catalyst degradation, ammonia slip, sulfur trioxide (SO ) formation, and fouling and corrosion of plant equipment. As China and the rest of the world work to reduce greenhouse gas emissions, carbon dioxide (CO ) emissions from parasitic load and urea-to-ammonia conversion may also become more important. If these challenges are properly addressed, SCR can reliably and effectively remove up to 90% of NO emissions at coal-fired power plants.

关键词: nitrogen oxides (NOx)     coal     selective catalytic reduction (SCR)     air pollution control    

Catalytic combustion of volatile organic compounds using perovskite oxides catalysts—a review

《化学科学与工程前沿(英文)》 2023年 第17卷 第11期   页码 1649-1676 doi: 10.1007/s11705-023-2324-x

摘要: With the rapid development of industry, volatile organic compounds (VOCs) are gaining attention as a class of pollutants that need to be eliminated due to their adverse effects on the environment and human health. Catalytic combustion is the most popular technology used for the removal of VOCs as it can be adapted to different organic emissions under mild conditions. This review first introduces the hazards of VOCs, their treatment technologies, and summarizes the treatment mechanism issues. Next, the characteristics and catalytic performance of perovskite oxides as catalysts for VOC removal are expounded, with a special focus on lattice distortions and surface defects caused by metal doping and surface modifications, and on the treatment of different VOCs. The challenges and the prospects regarding the design of perovskite oxides catalysts for the catalytic combustion of VOCs are also discussed. This review provides a reference base for improving the performance of perovskite catalysts to treat VOCs.

关键词: perovskite oxides     volatile organic compounds     catalytic combustion     reaction mechanism    

Multi-stage ammonia production for sorption selective catalytic reduction of NO

Chen ZHANG, Guoliang AN, Liwei WANG, Shaofei WU

《能源前沿(英文)》 2022年 第16卷 第5期   页码 840-851 doi: 10.1007/s11708-021-0797-1

摘要: Sorption selective catalytic reduction of nitrogen oxides (NOx) (sorption-SCR) has ever been proposed for replacing commercial urea selective catalytic reduction of NOx (urea-SCR), while only the single-stage sorption cycle is hitherto adopted for sorption-SCR. Herein, various multi-stage ammonia production cycles is built to solve the problem of relative high starting temperature with ammonia transfer (AT) unit and help detect the remaining ammonia in ammonia storage and delivery system (ASDS) with ammonia warning (AW) unit. Except for the single-stage ammonia production cycle with MnCl2, other sorption-SCR strategies all present overwhelming advantages over urea-SCR considering the much higher NOx conversion driven by the heat source lower than 100°C and better matching characteristics with low-temperature catalysts. Furthermore, the required mass of sorbent for each type of sorption-SCR is less than half of the mass of AdBlue for urea-SCR. Therefore, the multifunctional multi-stage sorption-SCR can realize compact and renewable ammonia storage and delivery with low thermal energy consumption and high NOx conversion, which brings a bright potential for efficient commercial de-NOx technology.

关键词: selective catalytic reduction (SCR)     nitrogen oxides (NOx)     ammonia     composite sorbent     chemisorption    

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    

以氮氧化物深度减排为抓手,推动细颗粒物和臭氧协同控制 Views & Comments

楚碧武, 丁焰, 高翔, 李俊华, 朱廷钰, 余运波, 贺泓

《工程(英文)》 2022年 第15卷 第8期   页码 13-16 doi: 10.1016/j.eng.2021.09.006

Multivalent manganese oxides with high electrocatalytic activity for oxygen reduction reaction

Xiangfeng Peng, Zhenhai Wang, Zhao Wang, Yunxiang Pan

《化学科学与工程前沿(英文)》 2018年 第12卷 第4期   页码 790-797 doi: 10.1007/s11705-018-1706-y

摘要: A noble-metal-free catalyst based on both Mn O and MnO was prepared by using the dielectric barrier discharge technique at moderate temperature. The prepared catalyst shows a higher electrocatalytic activity towards the oxygen reduction reaction than the catalyst prepared by using the traditional calcination process. The enhanced activity could be due to the coexistence of manganese ions with different valences, the higher oxygen adsorption capacity, and the suppressed aggregation of the catalyst nanoparticles at moderate temperature. The present work would open a new way to prepare low-cost and noble-metal-free catalysts at moderate temperature for more efficient electrocatalysis.

关键词: oxygen reduction reaction     manganese oxides     mixed valences of manganese     oxygen adsorption     dielectric barrier discharge    

The role of manganese oxides in the activation of peroxymonosulfate (PMS)

Jianzhi Huang, Huichun Zhang

《环境科学与工程前沿(英文)》 2019年 第13卷 第5期 doi: 10.1007/s11783-019-1158-8

摘要: Manganese oxides (MnOx) have been demonstrated to be effective materials to activate Oxone (i.e., PMS) to degrade various contaminants. However, the contribution of direct oxidation by MnOx to the total contaminant degradation under acidic conditions was often neglected in the published work, which has resulted in different and even conflicting interpretations of the reaction mechanisms. Here, the role of MnOx (as both oxidants and catalysts) in the activation of Oxone was briefly discussed. The findings offered new insights into the reaction mechanisms in PMS-MnOx and provided a more accurate approach to examine contaminant degradation for water/wastewater treatment.

关键词: Peroxymonosulfate     Manganese oxides     Catalyst     Oxidant    

Review on research and application of mesoporous transitional metal oxides in water treatment

Minghao SUI, Lei SHE

《环境科学与工程前沿(英文)》 2013年 第7卷 第6期   页码 795-802 doi: 10.1007/s11783-013-0521-4

摘要: This paper reviews the application of mesoporous transitional metal oxides in water treatment on basis of the catalysis and adsorption. Mesoporous transitional metal oxides are characterized by their intrinsic features, such as a high surface area, a highly ordered array of unidimensional pores with a very narrow pore size distribution, and highly dispersed active sites. Finally, the suggestions of further study on application are proposed.

关键词: mesoporous materials     transitional metal oxides     catalysis     adsorption     water treatment    

NOx removal by non-thermal plasma reduction: experimental and theoretical investigations

《化学科学与工程前沿(英文)》 2022年 第16卷 第10期   页码 1476-1484 doi: 10.1007/s11705-022-2165-z

摘要: Green and efficient NOx removal at low temperature is still desired. NOx removal via non-thermal plasma (NTP) reduction is one of such technique. This work presents the experimental and theoretical study on the NOx removal via NTP reduction (NTPRD) in dielectric barrier discharge reactor (DBD). The effect of O2 molar fraction on NOx species in the outlet of DBD, and effects of NH3/NO molar ratio and discharge power of DBD on NOx removal efficiency are investigated. Results indicate that anaerobic condition and higher discharge power is beneficial to direct removal of NOx, and the NOx removal efficiency can be up to 98.5% under the optimal operating conditions. It is also found that adding NH3 is favorable for the reduction of NOx to N2 at lower discharge power. In addition, the NOx removal mechanism and energy consumption analysis for the NTPRD process are also studied. It is found that the reduced active species ( N, N, N+, N2, NH2+, etc.) generated in the NTPRD process play important roles for the reduction of NOx to N2. Our work paves a novel pathway for NOx removal from anaerobic gas in industrial application.

关键词: ${\rm{NO}}_x $ removal     NTP reduction     mechanism     energy consumption    

标题 作者 时间 类型 操作

Multi-Pollutant Formation and Control in Pressurized Oxy-Combustion: SOx, NOx, Particulate Matter, and

Gaofeng Dai,Jiaye Zhang,Zia ur Rahman,Yufeng Zhang,Yili Zhang,Milan Vujanović,Hrvoje Mikulčić,Nebojsa Manić,Aneta Magdziarz,Houzhang Tan,Richard L. Axelbaum,Xuebin Wang,

期刊论文

Selective catalytic reduction of NOx from exhaust of lean-burn engine over Ag-Al2O3/cordierite catalyst

LI Junhua, KANG Shoufang, FU Lixin, HAO Jiming

期刊论文

Selective catalytic reduction of NO

Pavlo I. Kyriienko

期刊论文

Precise regulation of acid pretreatment for red mud SCR catalyst: Targeting on optimizing the acidity and reducibility

期刊论文

4 on HZSM-5 support: designing applicable catalysts for selective catalytic reduction of nitrogenoxides by ammonia

期刊论文

Study on the NOx release rule along the boiler during pulverized coal combustion

JIN Jing, ZHANG Zhongxiao, LI Ruiyang

期刊论文

Design and operational considerations for selective catalytic reduction technologies at coal-fired boilers

Jeremy J. SCHREIFELS, Shuxiao WANG, Jiming HAO

期刊论文

Catalytic combustion of volatile organic compounds using perovskite oxides catalysts—a review

期刊论文

Multi-stage ammonia production for sorption selective catalytic reduction of NO

Chen ZHANG, Guoliang AN, Liwei WANG, Shaofei WU

期刊论文

Redox reactions of iron and manganese oxides in complex systems

Jianzhi Huang, Huichun Zhang

期刊论文

以氮氧化物深度减排为抓手,推动细颗粒物和臭氧协同控制

楚碧武, 丁焰, 高翔, 李俊华, 朱廷钰, 余运波, 贺泓

期刊论文

Multivalent manganese oxides with high electrocatalytic activity for oxygen reduction reaction

Xiangfeng Peng, Zhenhai Wang, Zhao Wang, Yunxiang Pan

期刊论文

The role of manganese oxides in the activation of peroxymonosulfate (PMS)

Jianzhi Huang, Huichun Zhang

期刊论文

Review on research and application of mesoporous transitional metal oxides in water treatment

Minghao SUI, Lei SHE

期刊论文

NOx removal by non-thermal plasma reduction: experimental and theoretical investigations

期刊论文