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Removing carbonyl sulfide with metal-modified activated carbon

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Frontiers of Environmental Science & Engineering 2016年第1期10卷 11-18页

作者： Juan QIU Ping NING Xueqian WANG Kai LI Wei LIU Wei CHEN Langlang WANG Faculty of Environmental Science and Engineering Kunming University of Science and Technology Kunming 650093 China

A Cu-Co-K/activated carbon （AC） adsorbent has been developed for the removal of carbonyl sulfide （COS）. The effects of COS concentration, reaction temperature and relative humidity were closely examined. A breakthrough of 33.23 mg COS .gl adsorbent at 60℃, under 30% relative humidity and in presence of 1.0% oxygen was exhibited in the Cu-Co-K/AC adsorbent prepared. Competitive adsorption studies for COS in the presence of CS2, and H2S were also conducted. TPD analysis was used to identify sulfur-containing products on the carbon surface, and the results indicated that H2S, COS and SO2 were all evident in the effluent gas generated from the exhausted Cu-Co-K/AC. Structure of the activated carbon samples has been characterized using nitrogen adsorption, and their surface chemical structures were also determined with X-ray photoelectron spectroscopy （XPS）. It turns out that the modification with Cu（OH）2CO3- CoPcS-KOH can significantly improve the COS removal capacity, forming SO2/4 species simultaneously. Regenera- tion of the spent activated carbon sorbents by thermal desorption has also been explored.

关键词： carbonyl sulfide activated carbon removal,reactive adsorption

Effect of Fe/Cu/Ce loading on the coal-based activated carbons for hydrolysis of carbonyl sulfide

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Journal of Rare Earths 2010年第2期28卷 205-210页

作者：宁平于丽丽易红宏唐晓龙李华王红妍杨丽娜 Faculty of Environmental Science and Engineering Kunming University of Science and Technology

Fe/Cu/Ce modified coal-based activated carbon(AC) was prepared by the sol-gel method,and the effect of Fe/Cu/Ce on catalytic properties of Fe/AC,Fe-Cu/AC and Fe-Cu-Ce/AC was investigated in the hydrolysis of carbonyl sulfide(COS) at 50 °*** surface properties were evaluated by means of nitrogen adsorption and were characterized by using scanning electron microscopy(SEM),X-ray diffracto-metry(XRD) and X-ray photoelectron spectroscopy(XPS).The catalytic activities results showed that addition of Cu and Ce...

关键词： carbonyl sulfide activated carbons metal oxides rare earths

Influence of Gas Components on the Formation of carbonyl sulfide over Water-Gas Shift Catalyst B303Q

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Journal of Natural Gas Chemistry 2007年第1期16卷 53-59页

作者： Ju Shangguan Litong Liang Huiling Fan Fang Shen Key Laboratory of Coal Science and Technology Taiyuan University of Technology Ministry of Education and Shanxi Province Taiyuan 030024 Shanxi China

Water-gas shift reaction catalyst at lower temperature （200-400 ℃） may improve the conversion of carbon monoxide. But carbonyl sulfide was found to be present over the sulfided cobaltmolybdenum/alumina catalyst for water-gas shift reaction. The influences of temperature, space velocity, and gas components on the formation of carbonyl sulfide over sulfided cobalt-molybdenum/alumina catalyst B303Q at 200-400 ℃ were studied in a tubular fixed-bed quartz-glass reactor under simulated water-gas shift conditions. The experimental results showed that the yield of carbonyl sulfide over B303Q catalyst reached a maximum at 220 ℃ with the increase in temperature, sharply decreased with the increase in space velocity and the content of water vapor, increased with the increase in the content of carbon monoxide and carbon dioxide, and its yield increased and then reached a stable value with the increase in the content of hydrogen and hydrogen sulfide. The formation mechanism of carbonyl sulfide over B303Q catalyst at 200-400 ℃ was discussed on the basis of how these factors influence the formation of COS. The yield of carbonyl sulfide over B303Q catalyst at 200-400 ℃ was the combined result of two reactions, that is, COS was first produced by the reaction of carbon monoxide with hydrogen sulfide, and then the as-produced COS was converted to hydrogen sulfide and carbon dioxide by hydrolysis. The mechanism of COS formation is assumed as follows： sulfur atoms in the Co9Ss-MoS2/Al2O3 crystal lattice were easily removed and formed carbonyl sulfide with CO, and then hydrogen sulfide in the water-gas shift gas reacted with the crystal lattice oxygen atoms in CoO-MoOa/Al2O3 to form Co9S8-MoS2/Al2O3. This mechanism for the formation of COS over water-gas shift catalyst B303Q is in accordance with the Mars-Van Krevelen＇s redox mechanism over metal sulfide.

关键词： formation carbonyl sulfide sulfided cobalt-molybdenum/alumina catalyst water-gas shift

Characteristics and anthropogenic sources of carbonyl sulfide in Beijing

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Journal of Environmental Sciences 2015年第2期27卷 163-170页

作者： Ye Cheng Chenglong Zhang Yuanyuan Zhang Hongxing Zhang Xu Sun Yujing Mu Research Center for Eco-Environmental Sciences Chinese Academy of Sciences

Atmospheric mixing ratios of carbonyl sulfide（COS） in Beijing were intensively measured from March 2011 to June 2013. COS mixing ratios exhibited distinct seasonal variation, with a maximum average value of 849 ± 477 pptv in winter and a minimal value of 372 ± 115 pptv in summer. The seasonal variation of COS was mainly ascribed to the combined effects of vegetation uptake and anthropogenic emissions. Two types of significant linear correlations（R2〉 0.66） were found between COS and CO during the periods from May to June and from October to March, with slopes（ΔCOS/ΔCO） of 0.72 and 0.14 pptv/ppbv, respectively. Based on the emission ratios of COS/CO from various sources, the dominant anthropogenic sources of COS in Beijing were found to be vehicle tire wear in summer and coal burning in winter. The total anthropogenic emission of COS in Beijing was roughly estimated as 0.53 ± 0.02 Gg/year based on the local CO emission inventory and the ΔCOS/ΔCO ratios.

关键词： carbonyl sulfide Anthropogenic sources Vehicle tire wire Coal combustion Carbon monoxide

Surface characterization of metal oxides-supported activated carbon fiber catalysts for simultaneous catalytic hydrolysis of carbonyl sulfide and carbon disulfide

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Journal of Environmental Sciences 2020年第10期32卷 44-54页

作者： Kunlin Li Chi Wang Ping Ning Kai Li Xin Sun Xin Song Yi Mei Faculty of Environmental Science and Engineering Kunming University of Science and TechnologyKunming 650500China Faculty of Chemical Engineering Kunming University of Science and TechnologyKunming 650500China National-Regional Engineering Center for Recovery of Waste Gases from Metallurgical and Chemical Industries Kunming 650500China

The sol–gel method was used to synthesize a series of metal oxides-supported activated carbon fiber (ACF) and the simultaneous catalytic hydrolysis activity of carbonyl sulfide (COS)and carbon disulfide (CS2) at relatively low temperatures of 60°C was *** effects of preparation conditions on the catalyst properties were investigated,including the kinds and amount of metal oxides and calcination *** activity tests indicated that catalysts with 5 wt.%Ni after calcining at 400°C (Ni(5)/ACF(400)) had the best performance for the simultaneous catalytic hydrolysis of COS and *** surface and structure properties of prepared ACF were characterized by scanning electron microscope-energy disperse spectroscopy (SEM-EDS),Brunauer–Emmett–Teller (BET),X-ray diffraction (XRD),carbon dioxidetemperature programmed desorption (CO2-TPD) and diffuse reflectance Fourier transform infrared reflection (DRFTIR).And the metal cation defects were researched by electron paramagnetic resonance (EPR) *** characterization results showed that the supporting of Ni on the ACF made the ACF catalyst show alkaline and increased the specific surface area and the number of micropores,then improved catalytic hydrolysis *** DRFTIR results revealed that-OH species could facilitate the hydrolysis of COS and CS2;-COO and-C–O species could facilitate the oxidation of catalytic hydrolysate *** the EPR results showed that high calcination temperature conditions provide more active reaction center for the COS and CS2 adsorption.

关键词： Simultaneous catalytic hydrolysis carbonyl sulfide Carbon disulfide Ni(5)/ACF(400) Surface characterization Electron paramagnetic resonance

Removal of carbonyl sulfide from CO_2 stream using AgNO_3-modified NaZSM-5

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Journal of Energy Chemistry 2013年第6期22卷 902-906页

作者： Yanjun Wang Shaoyun Chen Heng Chen Xingzhou Yuan Yongchun Zhang State Key Laboratory of Fine Chemicals School of Chemical Engineering Dalian University of Technology

Removal of carbonyl sulfide(COS) from CO2 stream is significant for the production and utilization of food grade CO2. This study investigates the adsorption performance of Ag/NaZSM-5 as adsorbent prepared by incipient wetness impregnation for the removal of COS from a CO2 stream in a fixed-bed adsorption apparatus. Effects of various conditions on the preparation of adsorbent, adsorption and desorption were intensively examined. The results revealed that COS can be removed to below 1×10-9from a CO2stream(1000 ppm COS/CO2) using Ag/NaZSM-5(10 wt% AgNO3) with an adsorption capacity of 12.86 mg·g-1. The adsorbent can be fully regenerated using hot air at 450 C. The adsorption ability remained stable even after eight cycles of regeneration.

关键词： carbonyl sulfide adsorption π-complexation completely regeneration Ag-modified adsorbents

Catalytic hydrolysis of carbonyl sulfide over modified coal-based activated carbons by loading metal

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Journal of Central South University 2010年第5期17卷 985-990页

作者：易红宏于丽丽唐晓龙宁平李华王红妍杨丽娜 Faculty of Environmental Science and Engineering Kunming University of Science and Technology

A novel type of metal oxide/activated carbon catalyst was prepared by sol-gel method for the hydrolysis of carbonyl sulfide （COS）. The influences of the calcination temperature, additive content （2.5%-10.0% Fe2O3, mass fraction） and the basic density of the activation process were thoroughly investigated. The surface of catalysts was characterized by Boehm titration. The products were characterized by scanning electron microscopy （SEM）, X-ray diffractometry （XRD） and X-ray photoelectron spectroscopy （XPS）. The results show that catalysts with 2.5%-5.0% Fe2O3 after calcining at 500 ℃ have superior activity. The conversion rate of COS increases with increasing the relative density of basic capacity loaded onto activated carbon（AC）, and the activity follows the order： KOH〉Na2CO3 〉NaHCO3. Boehm titration data clearly show that the total acidity increases （from 0.06 to 0.48 mmol/g） and the basic groups decrease （from 0.78 to 0.56 mmol/g） after COS hydrolysis and H2S adsorption. The XPS results show that the product of HzS may be absorbed by the interaction with metal compounds and 02 to form sulfate （171.28 eV） and element sulfur （164.44 eV）, which lead to catalysts poisoning.

关键词： carbonyl sulfide activated carbon metal oxide hydrolysis

Anionic Copolymerization of carbonyl sulfide with Epoxides via Alkali Metal Alkoxides

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Chinese Journal of Chemistry 2018年第7期36卷 625-629页

作者： Cheng-Jian Zhang Jia-Liang Yang Lan-Fang Hu Xing-Hong Zhang MOE Key Laboratory of Macromolecular Synthesis and Functionalization Department of Polymer Science and Engineering Zhejiang University Hangzhou Zhejiang 310027 China

carbonyl sulfide （COS）, an analogue of carbon dioxide （CO2）, can be converted to CO2 via the carbonic anhydride enzymes widely existing in nature. COS is an ideal monomer for making poly（monothiocarbonate）s, which are difficult to synthesize by traditional methods. Herein, for the first time, we describe an anionic copolymerization of COS with epoxides using alkali metal alkoxides as the catalysts （initiators）, affording poly（monothiocarbonate）s with 100% alternating degree, 〉99% tail-to-head （T-H） content, high number-average molecular weights （Mns, up to 90.3 kg/mol） with narrow molecular weight distributions （D=Mw/Mn, 1.05-1.31 for COS/propylene oxide copolymers） under solvent-free and mild conditions. Oxygen-sulfur exchange reaction （O/S ER）, which can result in the production of contaminated dithiocarbonate and carbonate units in the main chain, was nearly completely depressed at 0 ℃. In addition, in contrast to previously reported salen chromium （iron） complexes that required multiple synthetic steps, this work provides simple, low-cost, and effective catalysts for making colorless sulfur-containing polymers.

关键词： carbonyl sulfide copolyrnerization alkali metal alkoxides sulfur-containing polymer

Tuning the growth of Cu-MOFs for efficient catalytic hydrolysis of carbonyl sulfide

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Chinese Journal of Catalysis 2017年第8期38卷 1373-1381页

作者： Lijuan Shen Gaojie Wang Xiaoxiao Zheng Yanning Cao Yufeng Guo Ke Lin Lilong Jiang National Engineering Research Center of Chemical Fertilizer Catalyst Fuzhou University Fuzhou 350002 Fujian China

Development of the high activity,promoter‐free catalysts for carbonyl sulfide(COS)hydrolysis is important for the efficient utilization of various *** this study,the Cu‐based metal‐organic framework HKUST‐1is synthesized by a simple and mild anodic‐dissolution electrochemical *** physical and chemical properties of the samples are characterized by several techniques,including scanning electron microscopy,X‐ray diffraction,Brunauer‐Emmett‐Teller analysis and X‐ray photoelectron *** results reveal that the synthesis voltage plays a crucial role in controlling the morphology of the resulting HKUST‐*** obtained samples function as novel catalysts for the hydrolysis of COS.A high efficiency,approaching100%,can be achieved for the conversion of COS at150oC over the optimal HKUST‐1synthesized *** is significantly higher than that of the sample prepared by the traditional hydrothermal ***,the effects of the water temperature and the flow velocity on the hydrolysis of COS are also investigated in ***,a possible reaction pathway of COS hydrolysis over HKUST‐1is also *** work represents the first example of MOFs applied to the catalytic hydrolysis of *** results presented in this study can be anticipated to give a feasible impetus to design novel catalysts for removing the sulfur‐containing compounds.

关键词： Metal‐organic framework carbonyl sulfide Electrochemical synthesis Catalytic hydrolysis HKUST‐1