Preparation of Ultrafine -Al2O3 Powder from Fly Ash by Ammonium Sulfate Roasting Technology

Yan Wu
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Ultrafine α-Al2O3 powder was prepared by calcining NH4Al(OH)2CO3 in 1200°C for 120min, which was characterized by XRD and SEM. Introduction Fly ash is generated during high temperature combustion of coal in coal-fired power plants [1-2]. Currently, about 800 million tons of coal fly ash has been generated in the world [3-4]. Since coal is still the major energy resource in China, the output of fly ash has increased continuously over the past several years, reaching 480 million tons in 2010 [5]. The annual fly ash discharge is more than 4×10 8 tons in China [6−7]. Presently, fly ash is consumed on a large scale in cement and concrete fillers as well as roadway and pavement utilization [8−11]. However, despite these positive uses, the production rate of fly ash is much greater than its consumption. There is still a proportion which is disposed of in ponds or landfill, so fly ash has become the main waste of power plant [12]. Fly ash contains significant amounts of alumina, typically about 20-50%, which presents an exciting new alternative source of alumina other than bauxite. Thus, extraction of aluminum from coal fly ash is environmentally and scientifically significant for disposing and utilizing waste materials and exploring new aluminum source, and has attracted extensive attention recently [13]. The Bayer process is the dominating method of refining alumina from bauxite ores throughout the world. The Bayer process mainly involves the bauxite digestion, solid-liquid separation, gibbsite precipitation and calcination [14]. In fly ash, the main form of alumina is mullite, and the alumina-silica ratio (mass ratio of alumina to silica) is approximately 1-1.5. With the low alumina-silica ratio and the stable mineral phase of mullite, a traditional Bayer Process is not suitable for the extraction of alumina from fly ash [15-18]. By using the acid method, alumina is dissolved in acids at high temperature. However, the acid method has not been used in industry because acid-resistant equipment is expensive and iron oxide had has to be separated from the alumina prior to treatment [19]. In the alkali method, fly ash is calcined with soda and lime at 1200°C, and the silica is converted into stable calcium silicate, thus separating the silica from the alumina. The alkali method is a relatively mature process, but the high sintering temperature consumes vast amounts of energy [17]. Recently, a new process for extracting alumina from coal fly ash has been established; where ammonium sulfate is used to roasting with coal fly ash [20]. Compared with acidic methods and alkali methods, this process results in fewer residues and less corrosive to equipment because ammoniums sulfate as a raw material. Ultrafine α-Al2O3 powder has received increasing attention due to its wide applications in transparent and electronic ceramics, single crystals, abrasives and catalysts [21]. Presently, the traditional methods for preparing α-Al2O3 powder are thermal decomposition of ammonium aluminum carbonate hydroxide (AACH) or ammonium aluminum sulfate hydroxide, Bayer process [22]. This research is therefore focused on the preparation of ultrafine α-Al2O3 powder from fly ash by ammonium sulfate roasting technology. The technology includes the extraction of Al2O3 from fly ash by roasted with (NH4)2SO4, Fe removal of solution, the synthesis of AACH and the preparation of ultrafine α-Al2O3. The effects of roasting process conditions on the extraction rate of Al2O3 were investigated and the product was characterized.","PeriodicalId":11324,"journal":{"name":"DEStech Transactions on Environment, Energy and Earth Sciences","volume":"21 1","pages":""},"PeriodicalIF":0.0000,"publicationDate":"2020-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"DEStech Transactions on Environment, Energy and Earth Sciences","FirstCategoryId":"1085","ListUrlMain":"https://doi.org/10.12783/dteees/peems2019/33935","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"","JCRName":"","Score":null,"Total":0}
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Abstract

(NH4)2SO4 roasting technology was used for extracting alumina from fly ash which located in Shandong Zibo power plant. The roasting temperature, the mole ratio of Al2O3 to (NH4)2SO4 and roasting time on the effect of the extraction rate of alumina was studied. The optimal roasting technology condition is 380°C for 120min with mole ratio of Al2O3 to (NH4)2SO4 of 1:6. Under the optimal roasting condition, the extraction rate of Al2O3 can reached 82% and a new phase NH4Al(SO4)2 was formed in clinker. NH4Al(SO4)2 in clinker was dissolved by distilled water and then separated from silicon-rich residue by filtration. Iron in NH4Al(SO4)2 solution was removed by goethite process, and then, NH4Al(OH)2CO3 was synthesized by adding (NH4)2CO3 in NH4Al(SO4)2 solution. Ultrafine α-Al2O3 powder was prepared by calcining NH4Al(OH)2CO3 in 1200°C for 120min, which was characterized by XRD and SEM. Introduction Fly ash is generated during high temperature combustion of coal in coal-fired power plants [1-2]. Currently, about 800 million tons of coal fly ash has been generated in the world [3-4]. Since coal is still the major energy resource in China, the output of fly ash has increased continuously over the past several years, reaching 480 million tons in 2010 [5]. The annual fly ash discharge is more than 4×10 8 tons in China [6−7]. Presently, fly ash is consumed on a large scale in cement and concrete fillers as well as roadway and pavement utilization [8−11]. However, despite these positive uses, the production rate of fly ash is much greater than its consumption. There is still a proportion which is disposed of in ponds or landfill, so fly ash has become the main waste of power plant [12]. Fly ash contains significant amounts of alumina, typically about 20-50%, which presents an exciting new alternative source of alumina other than bauxite. Thus, extraction of aluminum from coal fly ash is environmentally and scientifically significant for disposing and utilizing waste materials and exploring new aluminum source, and has attracted extensive attention recently [13]. The Bayer process is the dominating method of refining alumina from bauxite ores throughout the world. The Bayer process mainly involves the bauxite digestion, solid-liquid separation, gibbsite precipitation and calcination [14]. In fly ash, the main form of alumina is mullite, and the alumina-silica ratio (mass ratio of alumina to silica) is approximately 1-1.5. With the low alumina-silica ratio and the stable mineral phase of mullite, a traditional Bayer Process is not suitable for the extraction of alumina from fly ash [15-18]. By using the acid method, alumina is dissolved in acids at high temperature. However, the acid method has not been used in industry because acid-resistant equipment is expensive and iron oxide had has to be separated from the alumina prior to treatment [19]. In the alkali method, fly ash is calcined with soda and lime at 1200°C, and the silica is converted into stable calcium silicate, thus separating the silica from the alumina. The alkali method is a relatively mature process, but the high sintering temperature consumes vast amounts of energy [17]. Recently, a new process for extracting alumina from coal fly ash has been established; where ammonium sulfate is used to roasting with coal fly ash [20]. Compared with acidic methods and alkali methods, this process results in fewer residues and less corrosive to equipment because ammoniums sulfate as a raw material. Ultrafine α-Al2O3 powder has received increasing attention due to its wide applications in transparent and electronic ceramics, single crystals, abrasives and catalysts [21]. Presently, the traditional methods for preparing α-Al2O3 powder are thermal decomposition of ammonium aluminum carbonate hydroxide (AACH) or ammonium aluminum sulfate hydroxide, Bayer process [22]. This research is therefore focused on the preparation of ultrafine α-Al2O3 powder from fly ash by ammonium sulfate roasting technology. The technology includes the extraction of Al2O3 from fly ash by roasted with (NH4)2SO4, Fe removal of solution, the synthesis of AACH and the preparation of ultrafine α-Al2O3. The effects of roasting process conditions on the extraction rate of Al2O3 were investigated and the product was characterized.
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硫酸铵焙烧法制备粉煤灰超细-Al2O3粉体
采用(NH4)2SO4焙烧技术从山东淄博电厂飞灰中提取氧化铝。研究了焙烧温度、Al2O3与(NH4)2SO4的摩尔比和焙烧时间对氧化铝提取率的影响。最佳焙烧工艺条件为380℃、120min, Al2O3与(NH4)2SO4的摩尔比为1:6。在最佳焙烧条件下,Al2O3提取率可达82%,熟料中形成新相NH4Al(SO4)2。将熟料中的NH4Al(SO4)2用蒸馏水溶解,过滤出富硅渣。采用针铁矿法去除NH4Al(SO4)2溶液中的铁,然后在NH4Al(SO4)2溶液中加入(NH4)2CO3合成NH4Al(OH)2CO3。采用NH4Al(OH)2CO3在1200℃下煅烧120min的方法制备了超细α-Al2O3粉体,并用XRD和SEM对其进行了表征。粉煤灰是燃煤电厂煤在高温燃烧过程中产生的[1-2]。目前,全世界已产生约8亿吨粉煤灰[3-4]。由于煤炭仍是中国的主要能源,近年来粉煤灰的产量不断增加,2010年达到4.8亿吨[5]。中国年粉煤灰排放量超过4×10 8吨[6−7]。目前,粉煤灰在水泥和混凝土填料以及巷道和路面利用中被大量消耗[8−11]。然而,尽管有这些积极的用途,粉煤灰的生产量远远大于它的消耗量。仍有一定比例的粉煤灰被弃入池塘或填埋,因此粉煤灰已成为电厂的主要废弃物[12]。粉煤灰含有大量的氧化铝,通常约为20-50%,这是一种令人兴奋的氧化铝替代铝土矿的新来源。因此,从粉煤灰中提取铝对于废弃物的处理利用和寻找新的铝源具有环保和科学意义,近年来受到了广泛关注[13]。拜耳法是世界上从铝土矿矿石中提炼氧化铝的主要方法。拜耳法主要包括铝土矿溶出、固液分离、三水铝石沉淀和煅烧[14]。粉煤灰中氧化铝的主要形态为莫来石,氧化铝-二氧化硅比(氧化铝与二氧化硅的质量比)约为1-1.5。由于铝硅比低,莫来石矿物相稳定,传统拜耳法不适合从粉煤灰中提取氧化铝[15-18]。采用酸法,氧化铝在高温下溶解于酸中。然而,酸法尚未在工业中使用,因为耐酸设备昂贵,并且在处理之前必须将氧化铁从氧化铝中分离出来[19]。碱法是将粉煤灰与纯碱、石灰在1200℃下煅烧,二氧化硅转化为稳定的硅酸钙,从而将二氧化硅与氧化铝分离。碱法是一种比较成熟的工艺,但烧结温度高,能耗大[17]。建立了一种从粉煤灰中提取氧化铝的新工艺;其中硫酸铵用于与粉煤灰一起焙烧[20]。与酸法、碱法相比,以硫酸铵为原料,废渣少,对设备腐蚀小。超细α-Al2O3粉体因其在透明陶瓷和电子陶瓷、单晶、磨料和催化剂等方面的广泛应用而受到越来越多的关注[21]。目前,制备α-Al2O3粉体的传统方法有热分解碳酸铝铵氢氧化物(AACH)或硫酸铝铵氢氧化物,拜耳法[22]。因此,本文主要研究了以粉煤灰为原料,采用硫酸铵焙烧技术制备超细α-Al2O3粉体。该工艺包括(NH4)2SO4焙烧法从粉煤灰中提取Al2O3、去除溶液中的铁、合成AACH和制备超细α-Al2O3。研究了焙烧工艺条件对氧化铝提取率的影响,并对焙烧产物进行了表征。
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