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1.太原理工大学 化学与化工学院,山西 太原 030024
2.清创人和生态工程技术有限公司,山西 太原 030031
夏利民(1999—),硕士研究生,研究方向为废水处理与多相催化,E-mail:xialimin2023@163.com。
丁传敏(1986—),博士,副教授,硕士研究生导师,研究方向为C1化学与多相催化,E-mail:dingchuanmin@tyut.edu.cn。
收稿:2025-03-10,
修回:2025-03-29,
纸质出版:2026-02-25
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夏利民,潘家奎,贾志怡等.改性无定形硅铝对焦化废水COD吸附性能的影响[J].低碳化学与化工,2026,51(2):107-116.
XIA Limin,PAN Jiakui,JIA Zhiyi,et al.Effect of modified amorphous silica-alumina on adsorption performance for COD in coking wastewater[J].Low-Carbon Chemistry and Chemical Engineering,2026,51(2):107-116.
夏利民,潘家奎,贾志怡等.改性无定形硅铝对焦化废水COD吸附性能的影响[J].低碳化学与化工,2026,51(2):107-116. DOI: 10.12434/j.issn.2097-2547.20250094.
XIA Limin,PAN Jiakui,JIA Zhiyi,et al.Effect of modified amorphous silica-alumina on adsorption performance for COD in coking wastewater[J].Low-Carbon Chemistry and Chemical Engineering,2026,51(2):107-116. DOI: 10.12434/j.issn.2097-2547.20250094.
焦化废水成分复杂,是一种典型的含高浓度化学需氧量(COD)、难生物降解的工业废水。目前大多数焦化厂的废水经处理后COD仍很难达标,因此亟需开发一种新型绿色高效且廉价吸附剂。采用共沉淀法制备了一系列改性无定形硅铝吸附剂并用于焦化废水中COD去除。通过比较原始与经晾干、焙烧和铵交换改性处理的吸附剂(ASA-1、ASA-2、ASA-3和ASA-4)的COD去除率,探究了不同改性方法
对吸附剂理化性质和吸附性能的影响机制。结果表明,与其他3种吸附剂相比,ASA-3的COD去除效果最佳,当其硅铝比(原子数之比)为4.50、焙烧温度为750 ℃和投加量为50 g/L时,在25 ℃下搅拌3 h,COD去除率可达62.40%。ASA-3的高吸附性能得益于其更优的织构性质(比表面积为271.0 m
2
/g)和丰富的酸性位点。ASA-4在酸性位点增加时吸附性能却较弱(COD去除率为32.54%),因为铵交换破坏了其结构(比表面积仅53.8 m
2
/g)。通过拟一级、拟二级和颗粒内扩散模型拟合改性吸附剂在不同吸附时间下的吸附量,并对吸附机理进行了探究,发现吸附过程符合拟二阶模型,受液膜扩散、化学吸附和颗粒内扩散机制控制。
Coking wastewater
characterized by its complex composition
is a typical industrial wastewater with a high concentration of chemical oxygen demand (COD)
which is resistant to biodegradation. Currently
most coking plants struggle to achieve compliance standards for COD even after wastewater treatment
thus there is an urgent need to develop a new type of green
efficient and low-cost adsorbent. A series of modified amorphous silica-alumina adsorbents were synthesized via the co-precipitation method and applied for COD removal in coking wastewater. By comparing the COD removal rates of the original adsorbent and modified adsorbents through drying
calcination
and ammonium exchange (ASA-1
ASA-2
ASA-3
and ASA-4)
the influence mechanisms of different modification methods on the physicochemical properties and adsorption performances of the adsorbents were explored. The results show that ASA-3 exhibits the best COD removal efficiency among the four adsorbents. At a ratio of silicon atoms number to aluminium atoms number of 4.50
calcination temperature of 750 ℃
and dosage of 50 g/L
COD removal reaches 62.40% after stirring for 3 h at 25 ℃. The excellent adsorption performance of ASA-3 is attributed to its enhanced textural properties (specific surface area of 271.0 m
2
/g) and abundant acidic sites. Conversely
although the acidic sites of ASA-4 increase
its adsorption performance is relatively poor (with a COD removal rate of only 32.54%). This is because the ammonium exchange process disrupt its structure (a specific surface area of merely 53.8 m
2
/g). Adsorption capacities of modifie
d adsorbents at different adsorption time were fitted using pseudo-first-order
pseudo-second-order
and intra-particle diffusion models. The adsorption mechanism was investigated
revealing that the adsorption process conforms to the pseudo-second-order model and is governed by liquid film diffusion
chemical adsorption
and intra-particle diffusion mechanisms.
SHI J X , XU C Y , HAN Y X , et al . Case study on wastewater treatment technology of coal chemical industry in China [J ] . Critical Reviews in Environmental Science and Technology , 2020 , 51 ( 10 ): 1003 - 1044 .
MISHRA L , PAUL K K , JENA S . Coke wastewater treatment methods: Mini review [J ] . Journal of the Indian Chemical Society , 2021 , 98 ( 10 ): 100133 .
WANG J L , WANG S Z , HU C Z . Advanced treatment of coking wastewater: Recent advances and prospects [J ] . Chemosphere , 2024 , 349 : 140923 .
TAMANG M , PAUL K K . Advances in treatment of coking wastewater—A state of art review [J ] . Water Science and Technology , 2021 , 85 ( 1 ): 449 - 473 .
HU J S , ZHANG P F , AN W J , et al . In-situ Fe-doped g -C 3 N 4 heterogeneous catalyst via photocatalysis-Fenton reaction with enriched photocatalytic performance for removal of complex wastewater [J ] . Applied Catalysis B: Environmental , 2019 , 245 : 130 - 142 .
LIU Y , WU Z Y , PENG P , et al . A pilot-scale three-dimensional electrochemical reactor combined with anaerobic-anoxic-oxic system for advanced treatment of coking wastewater [J ] . Journal of Environmental Management , 2020 , 258 : 110021 .
GONG B Z , DUAN K , CHEN S , et al . Enhanced nutrients removal and microbial mechanisms in a pilot-scale anaerobic-oxic-anoxic (A/O/A) system: Synergistic roles of denitrifying polyphosphate accumulating organisms and endogenous denitrifiers [J ] . Process Safety and Environmental Protection , 2023 , 179 : 47 - 56 .
ZHANG C C , GUISASOLA A , BAEZA J A . A review on the integration of mainstream P-recovery strategies with enhanced biological phosphorus removal [J ] . Water Research , 2022 , 212 : 118102 .
PERAMUNE D , MANATUNGA D C , DASSANAYAKE R S , et al . Recent advances in biopolymer-based advanced oxidation processes for dye removal applications: A review [J ] . Environmental Research , 2022 , 215 : 114242 .
LIN R Y , LI Y , YONG T Z , et al . Synergistic effects of oxidation, coagulation and adsorption in the integrated fenton-based process for wastewater treatment: A review [J ] . Journal of Environmental Management , 2022 , 306 : 114460 .
PUEYO N , MIGUEL N , MOSTEO R , et al . Synergistic effect of the presence of suspended and dissolved matter on the removal of cyanide from coking wastewater by TiO 2 photocatalysis [J ] . Journal of Environmental Science and Health , 2017 , 52 ( 2 ): 182 - 188 .
LAN D W , ZHU H W , ZHANG J W , et al . Adsorptive removal of organic dyes via porous materials for wastewater treatment in recent decades: A review on species, mechanisms and perspectives [J ] . Chemosphere , 2022 , 293 : 133464 .
鲍俊 , 曾双亲 , 杨清河 , 等 . 无定形硅铝材料的制备及应用研究进展 [J ] . 石油炼制与化工 , 2024 , 55 ( 03 ): 154 - 161 .
BAO J , ZENG S Q , YANG Q H , et al . Research progress on preparation and application of amorphous silicon-aluminum materials [J ] . Petroleum Processing and Petrochemicals , 2024 , 55 ( 3 ): 154 - 161 .
ZHENG J , GUO M , SONG C S . Characterization of Pd catalysts supported on USY zeolites with different SiO 2 /Al 2 O 3 ratios for the hydrogenation of naphthalene in the presence of benzothiophene [J ] . Fuel Processing Technology , 2008 , 89 ( 4 ): 467 - 474 .
李环宇 , 马辉 , 邢爱华 , 等 . 加氢裂化催化剂载体无定形硅铝制备研究进展 [J ] . 天然气化工—C1化学与化工 , 2021 , 46 ( 2 ): 15 - 20+38 .
LI H Y , MA H , XING A H , et al . Research progress on preparation of amorphous silicon-aluminum support for hydrocracking catalyst [J ] . Natural Gas Chemical Industry , 2021 , 46 ( 2 ): 15 - 20+38 .
SUGANUMA S , ARITA K , NAKANO F , et al . Adsorption kinetics in removal of basic nitrogen-containing compounds from practical heavy oils by amorphous silica-alumina [J ] . Fuel , 2020 , 266 : 117055 .
GAO L H , LI S L , WANG Y T , et al . Pretreatment of coking wastewater by an adsorption process using fine coking coal [J ] . Physicochemical Problems of Mineral Processing , 2016 , 52 ( 1 ): 422 - 436 .
EL-KHAIARY M I , MALASH G F , HO Y S . On the use of linearized pseudo-second-order kinetic equations for modeling adsorption systems [J ] . Desalination , 2010 , 257 ( 1 ): 93 - 101 .
ANSARI K B , DANISH M , MESFER M K A , et al . Biosorption of cobalt (II) from an aqueous solution over acid modified date seed biochar: An experimental and mass transfer studies [J ] . Environmental Science and Pollution Research , 2025 , 32 ( 5 ): 2561 - 2576 .
WANG Z C , JIANG Y J , JIN F Z , et al . Strongly enhanced acidity and activity of amo rphous silica-alumina by formation of pentacoordinated Al V species [J ] . Journal of Catalysis , 2019 , 372 : 1 - 7 .
张浅 , 定明月 , 张玉兰 , 等 . 无定形硅铝催化生物质热裂解气齐聚合成汽油的特性 [J ] . 高等学校化学学报 , 2016 , 37 ( 11 ): 2060 - 2067 .
ZHANG Q , DING M Y , ZHANG Y L , et al . Oligomerization of biomass cracking gas to gasoline distillates over amorphous silica-alumina [J ] . Chemical Journal of Chinese Universities , 2016 , 37 ( 11 ): 2060 - 2067 .
BAO J , YANG Q H , ZENG S Q , et al . Synthesis of amorphous silica-alumina with enhanced specific surface area and acidity by pH-swing method and its catalytic activity in cumene cracking [ J ] . Microporous and Mesoporous Materials , 2022 , 337 : 111897 .
ZHANG D Q , ZHANG X H , YIN H , et al . Production of aromatic hydrocarbons from lignin derivatives by catalytic cracking over a SiO 2 -Al 2 O 3 catalyst [J ] . RSC Advances , 2023 , 13 ( 16 ): 10830 - 10839 .
LI T , ZHANG L , TAO Z C , et al . Synthesis and characterization of amorphous silica-alumina with enhanced acidity and its application in hydro-isomerization/cracking [J ] . Fuel , 2020 , 279 : 118487 .
HUANG Z H , LI Y Z , CHEN W J , et al . Modified bentonite adsorption of organic pollutants of dye wastewater [J ] . Materials Chemistry and Physics , 2017 , 202 : 266 - 276 .
KLAVARIOTI M , KOSTARELOS K , POURJABBAR A , et al . In situ sensing of subsurface contamination—Part I: Near-infrared spectral characterization of alkanes, aromatics, and chlorinated hydrocarbons [J ] . Environmental Science and Pollution Research , 2014 , 21 ( 9 ): 5849 - 5860 .
WU M L , DING L , LIAO J , et al . Preparation of novel porous Al 2 O 3 -SiO 2 nanocomposites via solution-freeze-drying-calcination method for the efficient removal of uranium in solution [J ] . Nanotechnology , 2022 , 33 ( 9 ): 095705 .
KONG Y L , ZHOU Y H , ZHANG P J , et al . Coagulation performance and mechanism of different novel covalently bonded organic silicon-aluminum/iron composite coagulant for As(V) removal from water: The role of hydrolysate species and the effect of coexisting microplastics [J ] . Journal of Hazardous Materials , 2024 , 480 : 135819 .
GEHRKE L , BLÄKER C , PASEL C , et al . Structural and energetic characterization of silica-alumina gels for adsorption processes [J ] . Microporous and Mesoporous Materials , 2024 , 365 : 112891 .
SHIBATA S , MASUI Y , NARUKAWA N , et al . Synthesis of N-unprotected diaryl ketimines and alkyl ketimines from ketones and ammonia using porous solid acids with analysis of their adsorption behavior [J ] . Bulletin of the Chemical Society of Japan , 2023 , 96 ( 6 ): 555 - 567 .
LI T , XU D , SUN Z Y , et al . Influence of calcination temperature on Brønsted acidity and activity of amorphous silica-alumina for n -hexadecane hydroisomerization [J ] . Fuel , 2025 , 381 : 133222 .
GAO Y , ZOU D L , LIU Y Z , et al . Degradation of coking wastewater under microwave irradiation in the presence of modified activated carbon [J ] . CLEAN-Soil, Air, Water , 2019 , 47 ( 10 ): 1900095 .
TOFIGHY M A , MOHAMMADI T . Adsorption of divalent heavy metal ions from water using carbon nanotube sheets [J ] . Journal of Hazardous Materials , 2011 , 185 ( 1 ): 140 - 147 .
AHMARUZZAMAN M , SHARMA D K . Adsorption of phenols from wastewater [J ] . Journal of Colloid and Interface Science , 2005 , 287 ( 1 ): 14 - 24 .
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