原位载铁中孔活性炭吸附As和天然有机物效能
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摘要
采用配煤、原位浸渍和两步活化法制备了4种原位载铁活性炭(FGL1/2/3/4),并以空白炭C-GL为基础的表面铁浸渍后改性炭(Fe-GL-2/3/4)为对照,研究了原位载铁炭对水中As和腐植酸(HA)的同步吸附效能.结果表明,炭化料原位载铁促进了比表面积(S_(BET))和中孔结构的发育.其中,原位载铁炭FCL4(载铁量6.51%)在45?～480?的范围内的中孔容积(V_(mes))比C-GL增加了0.1146cm~3/g;而后改性载铁则造成S_(BET)和V_(mes)的显著降低.原位载铁同时促进了表面碱度的增加,保证了中性条件下更好的As离子吸附能力;FCL4对As(Ⅲ)和As(V)的Langmuir最大吸附量(L-Q_(max))分别达到2.566和2.825mg/g.原位载铁炭进一步发育的中孔结构促进了对HA(<10mg DOC/L)的吸附效能,FGL4对HA的Langmuir最大吸附量(Q_(HA))达到46.25mg DOC/g.As-HA共存体系内FGL4对各组分的吸附容量有所降低,但As(Ⅲ)和As(V)的吸附容量仍达到2.325和2.675mg/g.
Four types of iron in-situ-impregnated mesoporous activated carbons(FGL1/2/3/4)have been prepared by ironimpregnation and two-step steam activation using coal-blending as precursors.And surface modified carbons(Fe-GL-2/3/4)were prepared by iron impregnation based on finished blank carbon C-GL(without iron impregnation).Adsorption of arsenic ions(As(Ⅲ)and As(V))and humic acids(HA)from water by iron in-situ-impregnated carbons were investigated in comparison with surface modified carbons.Results suggested that iron in-situ-impregnation was beneficial for development of surface area(S_(BET))and mesoporous structures.When iron content reached to 6.51%,mesoporous volumes(V_(mes))from 45 to 480?of FCL4 increased by0.1146cm~3/g in comparison with C-GL.However,surface modified by iron impregnation resulted in the decrease of S_(BET) and V_(mes).Surface basicity ensured higher arsenic adsorption capacities by iron in-situ-impregnated carbons in neutral environment.Langmuir maximum adsorption capacities(L-Q_(max))of As(Ⅲ)and As(V)by FCL4 increased to 2.566 and 2.825mg/g,respectively.It indicated that adsorption capacity of HA(<10mg DOC/L)was significantly influenced by V_(mes),and iron in-situ-impregnated carbons achieved better capacities for HA.Langmuir maximum adsorption capacities of HA(Q_(HA))obtained by FGL4increased to 46.25mg DOC/g,but capacities by Fe-GL-4decreased to 22.15mg DOC/g.Adsorption capacities of arsenic and HA decreased in Arsenic-HA system.However,FGL4 still obtained higher capacities than C-GL and Fe-GL-2/3/4.And L-Q_(max) of As(Ⅲ)/As(V)by FGL4 was 2.325/2.675mg/g.Therefore,iron in-situ-impregnated mesoporous carbons prepared in present work are proved to be promising adsorbent for simultaneous removal of arsenic and humic acids.
Four types of iron in-situ-impregnated mesoporous activated carbons(FGL1/2/3/4)have been prepared by ironimpregnation and two-step steam activation using coal-blending as precursors.And surface modified carbons(Fe-GL-2/3/4)were prepared by iron impregnation based on finished blank carbon C-GL(without iron impregnation).Adsorption of arsenic ions(As(Ⅲ)and As(V))and humic acids(HA)from water by iron in-situ-impregnated carbons were investigated in comparison with surface modified carbons.Results suggested that iron in-situ-impregnation was beneficial for development of surface area(S_(BET))and mesoporous structures.When iron content reached to 6.51%,mesoporous volumes(V_(mes))from 45 to 480?of FCL4 increased by0.1146cm~3/g in comparison with C-GL.However,surface modified by iron impregnation resulted in the decrease of S_(BET) and V_(mes).Surface basicity ensured higher arsenic adsorption capacities by iron in-situ-impregnated carbons in neutral environment.Langmuir maximum adsorption capacities(L-Q_(max))of As(Ⅲ)and As(V)by FCL4 increased to 2.566 and 2.825mg/g,respectively.It indicated that adsorption capacity of HA(<10mg DOC/L)was significantly influenced by V_(mes),and iron in-situ-impregnated carbons achieved better capacities for HA.Langmuir maximum adsorption capacities of HA(Q_(HA))obtained by FGL4increased to 46.25mg DOC/g,but capacities by Fe-GL-4decreased to 22.15mg DOC/g.Adsorption capacities of arsenic and HA decreased in Arsenic-HA system.However,FGL4 still obtained higher capacities than C-GL and Fe-GL-2/3/4.And L-Q_(max) of As(Ⅲ)/As(V)by FGL4 was 2.325/2.675mg/g.Therefore,iron in-situ-impregnated mesoporous carbons prepared in present work are proved to be promising adsorbent for simultaneous removal of arsenic and humic acids.
引文
[1] Mondal M K, Garg R. A comprehensive review on removal of arsenic using activated carbon prepared from easily available waste materials[J]. Environmental Science and Pollution Research, 2017,24(15):13295-13306.
[2] Pawar R R, Lalhmunsiama, Kim M, et al. Efficient removal of hazardous lead, cadmium, and arsenic from aqueous environment by iron oxide modified clay-activated carbon composite beads[J].Applied Clay Science, 2018,162:339-350.
[3] Xiao J, Wang L, Deng L, et al. Characteristics, sources, water quality and health risk assessment of trace elements in river water and well water in the Chinese Loess Plateau[J]. Science of The Total Environment, 2019,650(Pt 2):2004-2012.
[4] Nieto-Delgado C, Gutierrez-Martinez J, Rangel-Mendez J R.Modified activated carbon with interconnected fibrils of ironoxyhydroxides using Mn2+, as morphology regulator, for a superior arsenic removal from water[J]. Journal of Environmental Sciences,2019,76:403-414.
[5] Lata S, Samadder S R. Removal of arsenic from water using nano adsorbents and challenges:A review[J]. Journal of Environmental Management, 2016,166:387-406.
[6] Holl W H. Mechanisms of arsenic removal from water[J].Environmental Geochemistry&Health, 2010,32(4):287-290.
[7] Luong V T, Canas Kurz E E, Hellriegel U, et al. Iron-based subsurface arsenic removal technologies by aeration:A review of the current state and future prospects[J]. Water Research, 2018,133:110-122.
[8] Safi S R, Gotoh T, Iizawa T, et al. Development and regeneration of composite of cationic gel and iron hydroxide for adsorbing arsenic from ground water[J]. Chemosphere, 2019,217:808-815.
[9]公绪金.适宜松花江源水特性及生物增强的活性炭优选[J].水处理技术, 2018,44(6):120-125.Gong X. Optimization of Bio-enhanced Activated Carbon for Songhua River Treatment[J]. Technology of Water Treatment, 2018,44(6):120-125.
[10]公绪金,李伟光,张多英,等.负载金属捕获剂改性PAC吸附低温水中低浓度Cr(Ⅵ)特性[J].化工学报, 2012,(11):3680-3687.Gong X, Li W, Zhang D, et al. Adsorption characteristics of metal-capture-agent immobilized PAC for low concentration Cr(VI)in water at low temperature[J]. CIESC Journal, 2012,(11):3680-3687.
[11] Gong X, Li W, Wang K, et al. Study of the adsorption of Cr(VI)by tannic acid immobilised powdered activated carbon from micro-polluted water in the presence of dissolved humic acid[J].Bioresource Technology, 2013,141:145-151.
[12] GB/T 7702.15-2008煤质颗粒活性炭试验方法-灰分的测定[S].Yin C Y, Aroua M K, Ashi W M, et al. Review of modifications of activated carbon for enhancing contaminant uptakes from aqueous solutions. Separation and Purification Technology, 2007,52:403-415.
[13] Gong X J, Li W G, Wang G Z, et al. Characterization and performance evaluation of an innovative mesoporous activated carbon used for drinking water purification in comparison with commercial carbons[J].Environmental Science and Pollution Research, 2015,22:13291-13304.
[14] Gong X J, Li W G, Zhang D Y, et al. Adsorption of arsenic from micro-polluted water by an innovative coal-based mesoporous activated carbon in the presence of co-existing ions[J]. International Biodeterioration&Biodegradation, 2015,102:256-264.
[15] Wang J, Bi L, Ji Y, et al. Removal of humic acid from aqueous solution by magnetically separable polyaniline:adsorption behavior and mechanism[J]. Journal of Colloid and Interface Science, 2014,430:140-146.
[16] Gao Z, Li M, Sun Y, et al. Effects of oxygen functional complexes on arsenic adsorption over carbonaceous surface[J]. Journal of Hazardous Materials, 2018,360:436-444.
[17]陈维芳,程明涛,张道方,等.有机酸-铁改性活性炭去除饮用水中的As[J].中国环境科学, 2011,31(6):910-915.Chen W, Cheng M, Zhang D, et al. Granular activated carbon tailored by organic acid-Fe for arsenic removal. China Environmental Science,2018,360:436-444.
[18] Li W G, Gong X J, Wang K, et al. Adsorption characteristics of arsenic from micro-polluted water by an innovative coal-based mesoporous activated carbon[J]. Bioresource Technology, 2014,165:166-173.
[19] Lodeiro P, Kwan S M, Perez J T, et al. Novel Fe loaded activated carbons with tailored properties for As(V)removal:Adsorption study correlated with carbon surface chemistry[J]. Chemical Engineering Journal, 2013,215(2):105-112.
[20] Chang Q, Lin W, Ying W C. Preparation of iron-impregnated granular activated carbon for arsenic removal from drinking water[J]. Journal of Hazardous Materials, 2010,184(1):515-522.
[21] Arcibar-Orozco J A, Rios-Hurtado J C, Rangel-Mendez J R.Interactions between reactive oxygen groups on nanoporous carbons and iron oxyhydroxide nanoparticles:effect on arsenic(V)removal[J].Adsorption, 2016,22(2):181-194.
[22] Asadullah M, Jahan I, Ahmed M B, et al. Preparation of microporous activated carbon and its modification for arsenic removal from water[J]. Journal of Industrial and Engineering Chemistry, 2014,20(3):887-896.
[23]公绪金.基于表面修饰及孔结构调控的活性炭饮用水处理强化技术[M].北京:中国建筑工业出版社, 2019:60-64.
[2] Pawar R R, Lalhmunsiama, Kim M, et al. Efficient removal of hazardous lead, cadmium, and arsenic from aqueous environment by iron oxide modified clay-activated carbon composite beads[J].Applied Clay Science, 2018,162:339-350.
[3] Xiao J, Wang L, Deng L, et al. Characteristics, sources, water quality and health risk assessment of trace elements in river water and well water in the Chinese Loess Plateau[J]. Science of The Total Environment, 2019,650(Pt 2):2004-2012.
[4] Nieto-Delgado C, Gutierrez-Martinez J, Rangel-Mendez J R.Modified activated carbon with interconnected fibrils of ironoxyhydroxides using Mn2+, as morphology regulator, for a superior arsenic removal from water[J]. Journal of Environmental Sciences,2019,76:403-414.
[5] Lata S, Samadder S R. Removal of arsenic from water using nano adsorbents and challenges:A review[J]. Journal of Environmental Management, 2016,166:387-406.
[6] Holl W H. Mechanisms of arsenic removal from water[J].Environmental Geochemistry&Health, 2010,32(4):287-290.
[7] Luong V T, Canas Kurz E E, Hellriegel U, et al. Iron-based subsurface arsenic removal technologies by aeration:A review of the current state and future prospects[J]. Water Research, 2018,133:110-122.
[8] Safi S R, Gotoh T, Iizawa T, et al. Development and regeneration of composite of cationic gel and iron hydroxide for adsorbing arsenic from ground water[J]. Chemosphere, 2019,217:808-815.
[9]公绪金.适宜松花江源水特性及生物增强的活性炭优选[J].水处理技术, 2018,44(6):120-125.Gong X. Optimization of Bio-enhanced Activated Carbon for Songhua River Treatment[J]. Technology of Water Treatment, 2018,44(6):120-125.
[10]公绪金,李伟光,张多英,等.负载金属捕获剂改性PAC吸附低温水中低浓度Cr(Ⅵ)特性[J].化工学报, 2012,(11):3680-3687.Gong X, Li W, Zhang D, et al. Adsorption characteristics of metal-capture-agent immobilized PAC for low concentration Cr(VI)in water at low temperature[J]. CIESC Journal, 2012,(11):3680-3687.
[11] Gong X, Li W, Wang K, et al. Study of the adsorption of Cr(VI)by tannic acid immobilised powdered activated carbon from micro-polluted water in the presence of dissolved humic acid[J].Bioresource Technology, 2013,141:145-151.
[12] GB/T 7702.15-2008煤质颗粒活性炭试验方法-灰分的测定[S].Yin C Y, Aroua M K, Ashi W M, et al. Review of modifications of activated carbon for enhancing contaminant uptakes from aqueous solutions. Separation and Purification Technology, 2007,52:403-415.
[13] Gong X J, Li W G, Wang G Z, et al. Characterization and performance evaluation of an innovative mesoporous activated carbon used for drinking water purification in comparison with commercial carbons[J].Environmental Science and Pollution Research, 2015,22:13291-13304.
[14] Gong X J, Li W G, Zhang D Y, et al. Adsorption of arsenic from micro-polluted water by an innovative coal-based mesoporous activated carbon in the presence of co-existing ions[J]. International Biodeterioration&Biodegradation, 2015,102:256-264.
[15] Wang J, Bi L, Ji Y, et al. Removal of humic acid from aqueous solution by magnetically separable polyaniline:adsorption behavior and mechanism[J]. Journal of Colloid and Interface Science, 2014,430:140-146.
[16] Gao Z, Li M, Sun Y, et al. Effects of oxygen functional complexes on arsenic adsorption over carbonaceous surface[J]. Journal of Hazardous Materials, 2018,360:436-444.
[17]陈维芳,程明涛,张道方,等.有机酸-铁改性活性炭去除饮用水中的As[J].中国环境科学, 2011,31(6):910-915.Chen W, Cheng M, Zhang D, et al. Granular activated carbon tailored by organic acid-Fe for arsenic removal. China Environmental Science,2018,360:436-444.
[18] Li W G, Gong X J, Wang K, et al. Adsorption characteristics of arsenic from micro-polluted water by an innovative coal-based mesoporous activated carbon[J]. Bioresource Technology, 2014,165:166-173.
[19] Lodeiro P, Kwan S M, Perez J T, et al. Novel Fe loaded activated carbons with tailored properties for As(V)removal:Adsorption study correlated with carbon surface chemistry[J]. Chemical Engineering Journal, 2013,215(2):105-112.
[20] Chang Q, Lin W, Ying W C. Preparation of iron-impregnated granular activated carbon for arsenic removal from drinking water[J]. Journal of Hazardous Materials, 2010,184(1):515-522.
[21] Arcibar-Orozco J A, Rios-Hurtado J C, Rangel-Mendez J R.Interactions between reactive oxygen groups on nanoporous carbons and iron oxyhydroxide nanoparticles:effect on arsenic(V)removal[J].Adsorption, 2016,22(2):181-194.
[22] Asadullah M, Jahan I, Ahmed M B, et al. Preparation of microporous activated carbon and its modification for arsenic removal from water[J]. Journal of Industrial and Engineering Chemistry, 2014,20(3):887-896.
[23]公绪金.基于表面修饰及孔结构调控的活性炭饮用水处理强化技术[M].北京:中国建筑工业出版社, 2019:60-64.
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