高等学校化学学报 ›› 2021, Vol. 42 ›› Issue (1): 40.doi: 10.7503/cjcu20200362
所属专题: 分子筛功能材料 2021年,42卷,第1期
王彬宇1, 李莉1, 李菁2, 靳科研1, 张少卿1, 张佳楠3, 闫文付1()
收稿日期:
2020-06-18
出版日期:
2021-01-10
发布日期:
2021-01-12
通讯作者:
闫文付
E-mail:yanw@jlu.edu.cn
基金资助:
WANG Binyu1, LI Li1, LI Jing2, JIN Keyan1, ZHANG Shaoqing1, ZHANG Jianan3, YAN Wenfu1()
Received:
2020-06-18
Online:
2021-01-10
Published:
2021-01-12
Contact:
YAN Wenfu
E-mail:yanw@jlu.edu.cn
Supported by:
摘要:
系统总结了以工业固体废料为原料合成沸石分子筛材料的最新研究进展, 讨论了以粉煤灰、 珍珠岩工业废料、 煤矸石、 流体催化裂化(FCC)废催化剂、 锂矿渣、 铝土矿渣、 废瓷料和废弃玻璃等工业固体废料为原料, 合成LTA, FAU, MFI, CHA, GIS, SOD, ANA和KFI沸石分子筛材料的工艺方法, 及其在污水中重金属离子的脱除、 空气中CO2的捕获、 氮氧化物的选择性还原等实际应用中的性能, 并对未来工业固体废料合成沸石分子筛的发展趋势进行了展望.
中图分类号:
TrendMD:
王彬宇, 李莉, 李菁, 靳科研, 张少卿, 张佳楠, 闫文付. 用工业固体废料合成沸石分子筛的研究进展. 高等学校化学学报, 2021, 42(1): 40.
WANG Binyu, LI Li, LI Jing, JIN Keyan, ZHANG Shaoqing, ZHANG Jianan, YAN Wenfu. Recent Progresses on the Synthesis of Zeolites from the Industrial Solid Wastes. Chem. J. Chinese Universities, 2021, 42(1): 40.
Raw material | Elemental composition(%, mass fraction) | Crystal phase | Ref. | |||||
---|---|---|---|---|---|---|---|---|
Fly ash | Al2O3 | SiO2 | CaO | Fe2O3 | K2O | MgO | Mullite, quartz | [ |
(40.26) | (48.97) | (2.29) | (3.07) | (0.49) | (0.4) | |||
MnO | Na2O | P2O5 | SO3 | TiO2 | LOI | |||
(0.02) | (0.11) | (0.3) | (0.27) | (1.52) | (2.26) | |||
Perlite industrial waste | O | Si | Al | K | Na | Fe | Mica, quartz, feldspars | [ |
(71.79) | (19.60) | (4.24) | (2.17) | (1.26) | (0.40) | |||
Ca | Mg | |||||||
(0.39) | (0.17) | |||||||
Coal gangue | SiO2 | TiO2 | Al2O3 | Fe2O3 | MgO | CaO | Kaolinite | [ |
(33.50) | (0.74) | (27.96) | (1.68) | (0.48) | (1.11) | |||
Na2O | K2O | H2O | P2O5 | MnO | LOI | |||
(0.17) | (0.35) | (0.43) | (0.079) | (0.02) | (34.24) | |||
Spent FCC catalyst | SiO2 | Al2O3 | NaO2 | Fe2O3 | TiO2 | La2O3 | FAU(Y) | [ |
(49.5) | (45.1) | (1.4) | (1.7) | (1.0) | (0.5) | |||
P2O5 | Other | |||||||
(0.5) | (0.2) | |||||||
Lithium slag | SiO2 | Al2O3 | SO3 | CaO | Fe2O3 | K2O | Quartz, spodumene | [ |
(71.73) | (25.16) | (1.58) | (0.21) | (0.58) | (0.38) | |||
Na2O | TiO2 | |||||||
(0.06) | (0.03) | |||||||
Bauxite residue | Na2O | MgO | Al2O3 | SiO2 | P2O5 | K2O | Gibbsite, calcite, hematite | [ |
(4.03) | (0.21) | (11.46) | (7.89) | (0.09) | (0.45) | |||
CaO | TiO2 | MnO | Fe2O | |||||
(3.53) | (4.82) | (0.21) | (36.8) | |||||
Waste porcelain | SiO2 | Al2O3 | Na2O | K2O | Fe2O3 | CaO | Mullite, quartz, trydimite | [ |
(65.1) | (23.0) | (4.40) | (1.89) | (1.80) | (1.26) | |||
TiO2 | ZrO2 | MgO | P2O5 | ZnO | BaO | |||
(0.88) | (0.87) | (0.133) | (0.096) | (0.227) | (0.133) | |||
Waste glass | SiO2 | CaO | Fe2O3 | Na2O | MgO | Bi2O3 | Amorphous | [ |
(66.1) | (24.9) | (2.4) | (1.7) | (1.2) | (0.5) | |||
Al2O3 | K2O | TiO2 | ||||||
(1.1) | (0.9) | (0.3) |
Table 1 Composition and crystal phase of industrial solid waste
Raw material | Elemental composition(%, mass fraction) | Crystal phase | Ref. | |||||
---|---|---|---|---|---|---|---|---|
Fly ash | Al2O3 | SiO2 | CaO | Fe2O3 | K2O | MgO | Mullite, quartz | [ |
(40.26) | (48.97) | (2.29) | (3.07) | (0.49) | (0.4) | |||
MnO | Na2O | P2O5 | SO3 | TiO2 | LOI | |||
(0.02) | (0.11) | (0.3) | (0.27) | (1.52) | (2.26) | |||
Perlite industrial waste | O | Si | Al | K | Na | Fe | Mica, quartz, feldspars | [ |
(71.79) | (19.60) | (4.24) | (2.17) | (1.26) | (0.40) | |||
Ca | Mg | |||||||
(0.39) | (0.17) | |||||||
Coal gangue | SiO2 | TiO2 | Al2O3 | Fe2O3 | MgO | CaO | Kaolinite | [ |
(33.50) | (0.74) | (27.96) | (1.68) | (0.48) | (1.11) | |||
Na2O | K2O | H2O | P2O5 | MnO | LOI | |||
(0.17) | (0.35) | (0.43) | (0.079) | (0.02) | (34.24) | |||
Spent FCC catalyst | SiO2 | Al2O3 | NaO2 | Fe2O3 | TiO2 | La2O3 | FAU(Y) | [ |
(49.5) | (45.1) | (1.4) | (1.7) | (1.0) | (0.5) | |||
P2O5 | Other | |||||||
(0.5) | (0.2) | |||||||
Lithium slag | SiO2 | Al2O3 | SO3 | CaO | Fe2O3 | K2O | Quartz, spodumene | [ |
(71.73) | (25.16) | (1.58) | (0.21) | (0.58) | (0.38) | |||
Na2O | TiO2 | |||||||
(0.06) | (0.03) | |||||||
Bauxite residue | Na2O | MgO | Al2O3 | SiO2 | P2O5 | K2O | Gibbsite, calcite, hematite | [ |
(4.03) | (0.21) | (11.46) | (7.89) | (0.09) | (0.45) | |||
CaO | TiO2 | MnO | Fe2O | |||||
(3.53) | (4.82) | (0.21) | (36.8) | |||||
Waste porcelain | SiO2 | Al2O3 | Na2O | K2O | Fe2O3 | CaO | Mullite, quartz, trydimite | [ |
(65.1) | (23.0) | (4.40) | (1.89) | (1.80) | (1.26) | |||
TiO2 | ZrO2 | MgO | P2O5 | ZnO | BaO | |||
(0.88) | (0.87) | (0.133) | (0.096) | (0.227) | (0.133) | |||
Waste glass | SiO2 | CaO | Fe2O3 | Na2O | MgO | Bi2O3 | Amorphous | [ |
(66.1) | (24.9) | (2.4) | (1.7) | (1.2) | (0.5) | |||
Al2O3 | K2O | TiO2 | ||||||
(1.1) | (0.9) | (0.3) |
Fig.3 Scheme showing preparation of the Ag NPs/4A?zeolite composite catalyst and the chemical equation of styrene epoxidation[59]Copyright 2015, Royal Society of Chemistry.
Fig.5 Co? and Mn?coimpregnated ZSM?5 prepared from recycled industrial solid wastes for low?temperature NH3?SCR[90]Copyright 2019, American Chemical Society.
Raw material | Pre?treatment method | Crystallization method | Main product | Crystal size/μm | Ref. |
---|---|---|---|---|---|
Fly ash | NaOH solution pretreatment | Microwave hydrothermal | LTA | 2—5 | [ |
crystallization | |||||
Alkali fusion | Hydrothermal crystallization | LTA | 8—10 | [ | |
Alkali fusion | Ultrasonic hydrothermal | FAU(X) | 0.5 | [ | |
crystallization | |||||
Alkali fusion(Na2CO3), acid leaching | Hydrothermal crystallization | GIS | 2.84—5.82 | [ | |
Roasting, alkali fusion, acid leaching | Hydrothermal crystallization | ZSM?5 | 2—3 | [ | |
Acid leaching | Hydrothermal crystallization | ZSM?5 | 5—8 | [ | |
Acid leaching | Hydrothermal crystallization | ZSM?5 | 0.4—0.5 | [ | |
Alkali fusion(KOH) | Hydrothermal crystallization | CHA | 4—8 | [ | |
Alkali fusion(KOH) | Hydrothermal crystallization | CHA | 5—8 | [ | |
Alkali fusion | Hydrothermal crystallization | FAU(Y) | 7—8 | [ | |
Perlite industrial waste | No treatment | Hydrothermal crystallization | Zeolite?Pc | 1 | [ |
No treatment | Hydrothermal crystallization | FAU(X) | 10—25 | [ | |
No treatment | Hydrothermal crystallization | FAU(X) | 1 | [ | |
Coal gangue | Roasting, alkali fusion | Hydrothermal crystallization | LTA | 1.7 | [ |
Roasting | Hydrothermal crystallization | LTA | 1—1.5 | [ | |
Roasting | Hydrothermal crystallization | LTA | 1.5 | [ | |
Roasting | Hydrothermal crystallization | LTA | 1.5—2 | [ | |
Roasting, alkali fusion | Hydrothermal crystallization | FAU(X) | 2.5—3 | [ | |
Alkali fusion | Hydrothermal crystallization | FAU(X) | 12—17 | [ | |
No treatment | Hydrothermal crystallization | CHA | 2—7 | [ | |
No treatment | Ultrasonic hydrothermal | CHA | 1.5—7 | [ | |
crystallization | |||||
Roasting, acid leaching | Hydrothermal crystallization | ZSM?5 | 2—4 | [ | |
Spent FCC catalyst | Alkali fusion(Na2CO3) | Hydrothermal crystallization | LTA | 2 | [ |
Acid leaching | Hydrothermal crystallization | LTA | 1—2.5 | [ | |
Ball milling | Hydrothermal crystallization | FAU(X) | 1 | [ | |
Alkali fusion | Hydrothermal crystallization | FAU(Y) | 0.2 | [ | |
Ammonium sulfate activation method, | Hydrothermal crystallization | FAU(Y) | 0.4—1.2 | [ | |
acid leaching | |||||
Microwave acid treatment | Microwave hydrothermal | FAU(Y) | 0.1—0.3 | [ | |
crystallization | |||||
Lithium slag | No treatment | Dynamic hydrothermal | SOD | 20 | [ |
crystallization | |||||
Alkali fusion | Hydrothermal crystallization | FAU(X) | 1—3 | [ | |
Bauxite residue | Alkali fusion | Hydrothermal crystallization | LTA | 0.2—1 | [ |
Acid leaching, alkali fusion | Hydrothermal crystallization | LTA | 5—10 | [ | |
No treatment | Hydrothermal crystallization | ZSM?5 | 2—5 | [ | |
Alkali fusion | Hydrothermal crystallization | ZSM?5 | 1—2 | [ | |
Alkali fusion, acid leaching | Hydrothermal crystallization | LTA | 1—10 | [ | |
Waste porcelain | Alkali fusion | Hydrothermal crystallization | EMT | 0.3—1 | [ |
Alkali fusion | Hydrothermal crystallization | FAU | 0.5 | [ | |
Alkaline Liquor | Hydrothermal crystallization | LTA | 2—4 | [ | |
Waste glass | Acid leaching | Hydrothermal crystallization | LTA | 2—3 | [ |
NaOH solution pretreatment, | Hydrothermal crystallization | LTA | 2—5 | [ | |
Sodium sulfide treatment | |||||
Roasting | Hydrothermal crystallization | GIS | 2—5 | [ | |
No treatment | Hydrothermal crystallization | ANA | 5—10 | [ |
Table 2 Activation methods, crystallization methods and size distribution of synthetic zeolites from industrial solid wastes
Raw material | Pre?treatment method | Crystallization method | Main product | Crystal size/μm | Ref. |
---|---|---|---|---|---|
Fly ash | NaOH solution pretreatment | Microwave hydrothermal | LTA | 2—5 | [ |
crystallization | |||||
Alkali fusion | Hydrothermal crystallization | LTA | 8—10 | [ | |
Alkali fusion | Ultrasonic hydrothermal | FAU(X) | 0.5 | [ | |
crystallization | |||||
Alkali fusion(Na2CO3), acid leaching | Hydrothermal crystallization | GIS | 2.84—5.82 | [ | |
Roasting, alkali fusion, acid leaching | Hydrothermal crystallization | ZSM?5 | 2—3 | [ | |
Acid leaching | Hydrothermal crystallization | ZSM?5 | 5—8 | [ | |
Acid leaching | Hydrothermal crystallization | ZSM?5 | 0.4—0.5 | [ | |
Alkali fusion(KOH) | Hydrothermal crystallization | CHA | 4—8 | [ | |
Alkali fusion(KOH) | Hydrothermal crystallization | CHA | 5—8 | [ | |
Alkali fusion | Hydrothermal crystallization | FAU(Y) | 7—8 | [ | |
Perlite industrial waste | No treatment | Hydrothermal crystallization | Zeolite?Pc | 1 | [ |
No treatment | Hydrothermal crystallization | FAU(X) | 10—25 | [ | |
No treatment | Hydrothermal crystallization | FAU(X) | 1 | [ | |
Coal gangue | Roasting, alkali fusion | Hydrothermal crystallization | LTA | 1.7 | [ |
Roasting | Hydrothermal crystallization | LTA | 1—1.5 | [ | |
Roasting | Hydrothermal crystallization | LTA | 1.5 | [ | |
Roasting | Hydrothermal crystallization | LTA | 1.5—2 | [ | |
Roasting, alkali fusion | Hydrothermal crystallization | FAU(X) | 2.5—3 | [ | |
Alkali fusion | Hydrothermal crystallization | FAU(X) | 12—17 | [ | |
No treatment | Hydrothermal crystallization | CHA | 2—7 | [ | |
No treatment | Ultrasonic hydrothermal | CHA | 1.5—7 | [ | |
crystallization | |||||
Roasting, acid leaching | Hydrothermal crystallization | ZSM?5 | 2—4 | [ | |
Spent FCC catalyst | Alkali fusion(Na2CO3) | Hydrothermal crystallization | LTA | 2 | [ |
Acid leaching | Hydrothermal crystallization | LTA | 1—2.5 | [ | |
Ball milling | Hydrothermal crystallization | FAU(X) | 1 | [ | |
Alkali fusion | Hydrothermal crystallization | FAU(Y) | 0.2 | [ | |
Ammonium sulfate activation method, | Hydrothermal crystallization | FAU(Y) | 0.4—1.2 | [ | |
acid leaching | |||||
Microwave acid treatment | Microwave hydrothermal | FAU(Y) | 0.1—0.3 | [ | |
crystallization | |||||
Lithium slag | No treatment | Dynamic hydrothermal | SOD | 20 | [ |
crystallization | |||||
Alkali fusion | Hydrothermal crystallization | FAU(X) | 1—3 | [ | |
Bauxite residue | Alkali fusion | Hydrothermal crystallization | LTA | 0.2—1 | [ |
Acid leaching, alkali fusion | Hydrothermal crystallization | LTA | 5—10 | [ | |
No treatment | Hydrothermal crystallization | ZSM?5 | 2—5 | [ | |
Alkali fusion | Hydrothermal crystallization | ZSM?5 | 1—2 | [ | |
Alkali fusion, acid leaching | Hydrothermal crystallization | LTA | 1—10 | [ | |
Waste porcelain | Alkali fusion | Hydrothermal crystallization | EMT | 0.3—1 | [ |
Alkali fusion | Hydrothermal crystallization | FAU | 0.5 | [ | |
Alkaline Liquor | Hydrothermal crystallization | LTA | 2—4 | [ | |
Waste glass | Acid leaching | Hydrothermal crystallization | LTA | 2—3 | [ |
NaOH solution pretreatment, | Hydrothermal crystallization | LTA | 2—5 | [ | |
Sodium sulfide treatment | |||||
Roasting | Hydrothermal crystallization | GIS | 2—5 | [ | |
No treatment | Hydrothermal crystallization | ANA | 5—10 | [ |
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