Northeastern University1 is the cradle of the Chinese

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1 NEUI 600 ka prebaked potline in the Weiqiao aluminum smelter. Innovations in Aluminum Production Technology at Northeastern University, Shenyang, China By Dr. Gao Bingliang, School of Metallurgy, Northeastern University 26 Introduction Northeastern University1 is the cradle of the Chinese aluminum industry. It continues to make contributions in aluminum manufacturing R&D providing improvements in energy efficiency, green energy application, waste treatment, and advances in fundamental understanding. Some of these developments including a new uneven novel structure cathode, methods for spent pot lining disposal, wind power for electrolysis, and improvements on interfacial phenomena are discussed in this article. Furthermore, Northeastern University worked with Northeastern University Engineering and Research Institute Co., Ltd (NEUI) and other industry organizations to design and commercialize the world s first and highest amperage potline. The key performances of this 600 ka technology are also given in this paper. University and Institute Overview Northeastern University: Breakthrough technological innovations and advances in primary aluminum are being developed by formal research and development programs conducted at Northeastern University with the purpose of finding solutions to global challenges. Founded in 1923, it is located in the capital city of Liaoning Province, Shenyang, which is the political and economic center of Northeast China. Being a multi-discipline university focusing on engineering, it is famous for disciplines such as mining and metallurgy, as well as automation and computer science. At present, there are two groups working on aluminum electrolysis in the Institute of Nonferrous Metallurgy at Northeastern University. Both group leaders and some members have been PhD students of the renowned Prof. Qiu Zhuxian (see article page 40). One group is led by Professor Feng Naixiang, the other is led by Professor Wang Zhaowen. Northeastern University Engineering and Research Institute: NEUI was set up in 1981, having grown out of the Design Office of Northeastern University (known as the Northeast Institute of Technology, NEIT, at the time). With the development and expansion, the design office was updated to NEUI in The institute was registered in April 2004 as a joint-stock company. The shareholders consist of Northeastern University (shareholding ratio 31%), China Nonferrous Metal Industry s Foreign Engineering and Construction Co., Ltd. (shareholding ratio 20%), and company members (shareholding ratio 49%). Currently, NEUI is an integrated technology and consulting company headquartered in Shenyang, China. NEUI has a total of 370 staff members, including 260 engineers. Dr. Tu Ganfeng is the chairman of the board and Lü Dingxiong is the president and chief executive officer of NEUI. The company develops and sells techniques and equipment related to nonferrous metallurgy and consulting services. After decades of practice and experience, NEUI is making significant marks in nonferrous metals industries, especially in the primary aluminum industry. Development of Unique Cathodes to Reduce Energy Consumption It was in 2012 that Feng first reported that industrial tests of applying a new uneven novel structure cathode (NSC) was successful in three 168 ka prebaked cells at Chongqing Tiantai aluminum smelter. These cells were installed and put into production with a new raised cathode design (Figure 1a) in March The top surface of the new cathode is not flat, but has raised ridges (Figure 1b). During the first year of testing, the average cell voltage was 334 mv lower than that of conventional cells and also the current efficiency increased by 1.4%. As a consequence, the DC power consumption was lowered by 1,260 kwh/t Al. 2-3 A new generation of NSC 350

2 New Methods for Spent Pot Lining Disposal a b Figure 1. Industrial aluminum electrolysis cells installed with the NSC showing the new cathodes with raised small cylindrical columns (a) and raised transverse ridges (b). ka cells have been operating at the Qingtongxia smelter at 3.88 volts, a high ~96% current efficiency, and 12,044 kwh/t Al DC power consumption since In June 2009, ninety-four 200 ka prebaked cells were started at the Huadong aluminum smelter and installed with the new raised NSC cathode block design. During one year of operation, the cells showed good performance with an average DC energy consumption of 12,043 kwh/t Al. These test results are impressive as they indicate that more than 0.3 V can be saved on cell voltage together with a significant increase in current efficiency. 4 Mathematical simulation and industrial measurements confirmed that the new NSC cathode design significantly decreased the velocity of metal flow and increased the stability of the prebaked cell, which enabled the cell to run at lower voltage than cells with a flat cathode. 5 Consequently, energy consumption for aluminum production was reduced because heat loss was deceased to maintain the heat balance, which is different from the operational philosophy of forced heat dissipation. The cells with the new cathode have to be preheated with gas heating followed by metal preheating. The new preheating technology solved the problem of ridge failure that occurred during start up of the cells. At present, the gas preheating and the metal preheating technology have been widely used for restarting pots that were stopped because of power failure or occasional accidents. Since 2009, more than 50% of the smelters in China have tried this new technique. Some new cathode block concepts were also proposed and tried. In 2011, the new cathode technology was recognized with the TMS Light Metals Division Aluminum Reduction Technology Award. In 2014, the new cathode technique was recognized with the National Awards for Progress in Science and Technology. China has the largest aluminum production capacity in the world and, thus, it also has the largest amount of waste from failed cathodes. Spent pot linings (SPL) contain compounds that are toxic, hazardous, and environmentally undesirable, so it is becoming one of the aluminum industry s major environmental concerns. Qiu conducted basic research on spent pot lining treatment. He proposed to separate carbon from cryolite by the floatation method. The industrial scale test confirmed that it yields cryolite (>98% purity) and carbon powder (~75% C, ~7% oxides, and ~17% cryolite). Wang and Shi Zhongning further developed the process to purify the carbon extracted from the floatation process. 6 The carbon with fluorides is treated with a NaOH leaching operation. The filtrate is then sent to cryolite precipitation. The filtrated solids are washed and pressure leached to produce pure carbon powder with a purity higher than 95%. A pilot plant for spent pot lining treatment was built in Henan province. The annual design rate is 3,000 tpy of spent pot lining. Recently, Feng invented a new method for treatment of spent pot lining recycling. Spent carbon materials including spent pot lining and carbon dust are heated in a vacuum furnace at 1,000-1,400 C. The volatile materials including sodium metal and fluorides are then separated from the carbon. Because of the melting point difference, sodium metal will be solidified in the temperature region of below 500 C, and electrolyte will solidify in the 500-1,000 C region in the upper part of the vacuum chamber. After such treatment, the purity of the carbon can reach up to 92% and higher. The new method can also be used to recycle the spent insulating materials by addition of aluminum dust from the foundry shop. Aluminum reacts with sodium oxide to produce metallic sodium. During the step of distillation, cryolite-based electrolyte and metallic sodium are removed from the insulating materials, which can be used again in prebaked cells. Aluminum Electrolysis Using Wind Power China is rich in wind resources because of its long monsoon period. There are two main areas with rich wind resources in China (Figure 2): Northern areas (Xinjiang Province and Inner Mongolia Province) have wind energy densities reaching W/m 2 and 5,000-7,000 usable hours per year; coastal areas and islands have wind power densities above 500 W/m 2 and 7,000-8,000 usable hours per year. The wind power industry has increased rapidly and has reached 105 GW of electricity generating capacity installed in China in Legend Highest High Average Low Existing wind power plants Wind Power plants in progress Wind power plants in plan Herringbone wind power development zone Figure 2. Distribution of wind mills in China. 27

3 Wind power is very consistent from year to year, but has significant variation over shorter time periods. It is therefore used in conjunction with other electric power sources to give a reliable supply. Wind power may also be stored in a battery and electrical power provided on demand. Not all wind power capacity is connected to the power grid in China because the transmission capacity of the grid has not kept up with the growth of China s wind farms. Regarding this situation, Wang has proposed that aluminum electrolysis can be used as a special load for non-grid connecting wind power. A new process was designed and proceeded in laboratory scale in the period of During cell operation, DC electricity is supplied by grid power and non-grid connecting wind power together. With intelligent power management, the fluctuations in wind power can be overcome. When wind energy production is low, more energy from the grid can be used to balance the energy supply. A new type of aluminum electrolysis cell was designed which has higher resolution for power fluctuation and was installed at Northeastern University. The test cell with sidewall heat recovery system is shown in Figure 3. Hitec salt is used as the heat exchange medium in this cell. When cells receive a higher energy input, more heat can be taken out to keep the sidewall ledge stable. This can be realized easily by tuning the flow rate of Hitec salt. In China, aluminum smelters are always built together with alumina refining plants. Therefore, the heat from the cells can be transferred to the alumina plant and used for bauxite digestion. Figure 3. A 3,000 amp aluminum electrolysis cell with sidewall heat recovery system. A 3,000 amp laboratory scale test was carried out at Northeastern University. The results showed that the temperature of the Hitec salt out from the heat exchanger can reach up to 400 C. A thermo-electric model of an aluminum reduction cell using non-grid connecting wind power was built using ANSYS. The impact of the flow rate of the Hitec salt on heat balance and ledge thickness was studied. The results showed that through control of the flow rate of the Hitec salt, they were capable of adjusting the cell heat balance easily and effectively. With the aid of mathematical simulation, Wang believes that the new cell can operate normally with variable current range of ±20%. 28 Further Improvement on Interfacial Phenomena in Molten Salt Electrolysis During the last decade the size of aluminum cells have become larger and larger. Alumina dissolution and anodic bubble behavior have become key points from the aspect of fundamental research. These problems were investigated systematically with the aid of the transparent cell invented by Qiu (Figure 4). Alumina Dissolution: Dr. Gao Bingliang and Wang investigated the dissolution behavior of secondary alumina and primary alumina with no stirring of the bath The dissolution behavior for the two kinds of alumina was almost the same during the 20 seconds, after addition. Alumina particles and small agglomerates dispersed through the bath gradually and dissolved quickly. However, the dissolution behavior was different for big agglomerates. Figure 4. Professor Qiu Zhuxian standing next to his laboratory-scale transparent aluminum electrolysis cell. During primary alumina dissolution, big agglomerates floated on the surface of the bath and were stable for over 2 minutes. Eventually the agglomerates went to the bottom of the crucible and dissolved slowly. Around 54-64% of the pot crust material is alumina at C. The dissolution rate of the crust material decreased greatly with the increase of the initial alumina concentration and decrease of operating temperature. The mass of the crust increased significantly at high initial alumina concentrations and decreased temperature, while the alumina content of the crust showed a slightly decreasing trend. The secondary alumina floated on the surface of the melt upon addition and penetrated through the melt gradually as particles and fine fragments. It dissolved faster than the primary alumina and no large lumps of alumina settled on the bottom of the crucible. On the other hand, gas bubbles were observed at the interface of the melt and floating agglomerate. The carbon dust in the secondary alumina generated some gas bubbles and played an important role in improving the dissolution behavior. However, HF and other fluorides had little effect on the dissolution behavior of the secondary alumina. Through the comparison of four different bath chemistries under the condition of no stirring, it has been found that the dissolution rate of alumina is relatively independent of the alumina concentration in the melts at Al 2 O 3 % 3%. A decrease of dissolution rate at Al 2 O 3 % > 3 was observed because of the lack of free fluoride solvent in the melts. The dissolution rate is also highly related to the operating temperature and alumina solubility contrasts to electrolyte superheat and minor changes of bath compositions. Anodic Bubble Behavior: Wang and Gao have improved the design of Qiu s transparent cell. 11 A new technique was applied, which enabled them to observe clearly the bubble behavior on the surface of the anode bottom. Anode gas bubbles were released in a cyclic pattern. When the bubble grew to a size as large as the anode bottom surface and to a maximum thickness of about 4 mm, it was released suddenly through the anode edge. The released bubble attached to the anode side walls and rose quickly in the cell channel. Tiny bubbles were generated at the anode bottom surface in many spots. These tiny bubbles grew through diffusion of gases. The formation of large bubbles was mainly driven by coalescence of surrounding bubbles when their edges were connected. The cell voltage is very consistent with the bubble coverage with a high voltage drop corresponding to high bubble coverage. The gas coverage decreased with increased current density. The anode slot affects the bubble behavior and the resultant voltage drop significantly. With the presence of a 4 mm wide longitudinal slot, the mean bubble coverage

4 was reduced by about 38% and the maximum coverage by 33% at a current density of 0.9 A/cm 2. The bubble induced voltage drop and its fluctuation were reduced consequently, while the mean fluctuation was reduced by 37%. The bubble coverage on the slotted anode was much lower than that on the un-slotted anode when the current density was less than 1.1 A/cm 2. At the highest current density of 1.3 A/cm 2 performed in this experiment, the difference was reduced. Since 2010, Wang has been cooperating with Dr. Feng Yuqing at CSIRO in Australia They conducted investigations on bubble dynamics based on a computational fluid dynamics (CFD) model with the volume-of-fluid (VOF) method. Using a two-dimensional geometry of part of a real cell as the testing bed, the motion of different sized bubbles has been simulated in an air-water system and a CO 2 -cryolite system. Comparisons between the two systems were conducted through the three periods of bubble motion: bubble sliding under the anode, bubble releasing at the anode edge, and bubble rising in the side channel. It was found that both systems showed similar trends in bubble dynamics, such as an increase in the bubble sliding velocity as the bubble size increased and the appearance of a thick head at large bubble sizes. Quantitatively, there are differences between the two systems, evidenced in terms of the detailed bubble dynamics at each period of bubble motion, such as the bubble morphology, the bubble sliding velocity, the bubble layer thickness, and the bubble-induced liquid flow. The detailed microscale modeling provided useful information for the development of a multiscale modeling methodology by building constitutive correlations to support the macro/process scale modeling. Molten Salt Chemistry: In many Chinese aluminum smelters, the bath contains high contents of KF and LiF, which come as potassium oxide and lithium oxide impurities in the alumina. These cells always perform poorly with low current efficiency and poor cell stability. Thus, it was important to conduct investigations on alumina dissolution, aluminum solubility, electrical conductivity, and bath analysis of cryolite-based melts containing KF and LiF. Gao carried out a measurement campaign for physicochemical properties of complex aluminum electrolyte. First, using XRD/XRF analysis, he found that both KF and LiF have a significant effect on determination of bath ratio. KF also influences the accuracy of the CaF 2 concentration determined with XRF. 14 The impact of KF on aluminum solubility and alumina dissolution can be neglected in the range of less than 5%. In Chinese smelters using complex electrolytes, the cryolite ratio is usually in the range of , which may be one of the reasons for the loss of current efficiency in industrial cells. Bath analysis problems can lead to poorer aluminum fluoride control in all cells. Operation temperature goes to below 930 C, but with superheat higher than 15 C, which results in many problems, such as poor alumina solubility, sludge formation, and unstable side ledge. Consequently, the industrial cell will be operated in an unstable state, which may be another important reason for the loss in current efficiency. Recently, Gao developed a new room temperature molten salt chemistry for aluminum deposition. This is a eutectic solvent based on AlCl 3 and amide compounds, which are much cheaper than imidazole ionic liquids. 15 The electrodeposition of aluminum was successfully carried out on a copper cathode from AlCl 3 /acetamide (r = 1.3) eutectic solvent at different temperatures (40 C and 60 C). The morphology of the electrodeposited aluminum depends on the temperature. Uniform, dense, and compact deposit was formed at lower temperature. Development of Large High Amperage Cell at NEUI During 1986 to 1994, Aluminum Corporation of China Limited (Chalco), Northeastern University, and Central South University (CSU) worked together to successfully develop 280 ka prototype technology in the Qinyang pilot smelter. Shenyang Aluminum and Magnesium Engineering & Research Institute (SAMI), Guiyang Aluminum and Magnesium Engineering and Research Institute (GAMI), and NEUI have been the three main designers for the aluminum industry, including for alumina plants and primary aluminum smelters during the last twenty years. Cooperation between these organizations has enabled continued development of NEUI cell technology. The first NEUI potline was put into operation at Xichuan smelter in 1998; this 200 ka potline had a capacity of 100,000 tpy. This was followed by the first NEUI 300 ka potline in 2005, which was put into operation in Nanshan smelter with a capacity of 200,000 tpy. In August 2008, the first NEUI 400 ka potline with a capacity of 230,000 tpy was put into operation in Henan Zhongfu Industry Co. Ltd. On December 11, 2014, the first NEUI 600 ka potline and also the first complete 600 ka potline in the world was put into operation at Weiqiao smelter, operated by Weiqiao Pioneering Group located in Shandong province, China. This line has 186 cells and a capacity of 300,000 tpy. Over a six-month period of operation, the new 600 ka potline showed excellent performance (Table I). The average DC consumption is 12,482 kwh/t Al, with an average current efficiency of 94.3%. The big cell adopts the design of bridge for designing superstructure, which fulfilled the designer s dream to create a big structure with a simple and elegant configuration. The success of the NEUI 600 ka technology was due to many years of work on MHD stability, thermo-electric balance, thermo-mechanical, computer control, materials selection, and handling. The 600 ka aluminum electrolytic technology is an important global milestone. Current (ka) 600 Anodic Current Density (A/cm 2 ) 0.81 Current Efficiency (%) Anode Effect Frequency (ae/cell-day) 0.01 Cell Voltage (V) 3.95 Gross Anode Consumption (kg/t Al) 480 Specific Energy Consumption (kwh/t Al) Roof Vent Fluoride Emissions (kg F/t Al) 0.55 Table I. Key performance indicators of NEUI 600 ka prebaked cell. Currently, 33 potlines using different NEUI technologies are in operation, which have a total capacity of 6.6 million tonnes. In addition, NEUI has designed 107 lines for alumina refining production, which occupy 65% of the total production capacity of alumina in China. Acknowledgments The author would like to express his thanks to Mao Jihong and Dr. Ban Yungang, both at NEUI, for their valuable information and suggestions. Special thanks goes to Prof. Feng Naixiang and Dr. Peng Jianpin for their valu- 29

5 able discussions and suggestions. In addition, thanks goes to Dr. Alton Tabereaux, consultant, in Muscle Shoals, AL; Dr. Xiangwen Wang, at the Alcoa Technical Center, Alcoa Inc.; and Dr. Halvor Kvande, professor emeritus at Norwegian University of Science and Technology in Trondheim, Norway for their review and editing of the manuscript. References 1. Northearstern University website, 2. Feng Naixiang. Chinese Patent Feng Naixiang, Peng Jianping, Wang Yaou, Di Yuezhong, You Jin, and Liao Xian an, Light Metals 2012, pp Feng Naixiang, Peng Jianping, Wang Yaowu, Di Yuezhong, You Jin, and Liao Xian an, Light Metals 2013, pp Baokuan Li, Fang Wang, Xiaobao Zhang, Fengsheng Qi, and Naixiang Feng, Light Metals 2012, pp Shi Zhongning, Li Wei, Hu Xianwei, Ren Bijun, Gao Bingliang, and Wang Zhaowen, Transaction of Nonferrous Metals of China, Vol. 22, No. 1, 2012, pp Cuiping Liao, Eberhard Jochem, Yi Zhang, and Nida R. Farid, China Renewable Energy 35, 2010, pp. 1,879-1, Youjian Yang, Bingliang Gao, Zhaowen Wang, Zhongning Shi, and Xianwei Hu, Metallurgical and Materials Transactions B, Vol. 44B, No. 5, 2013, pp. 1,296-1, Youjian Yang, Bingliang Gao, Zhaowen Wang, Zhongning Shi, Xianwei Hu, and JIangyu Yu, Metallurgical and Materials Transactions B, Vol. 45B, No. 6, 2014, pp. 1,150-1, Youjian Yang, Bingliang Gao, Zhaowen Wang, Zhongning Shi, Xianwei Hu, JOM, Vol. 67, No. 9, 2015, pp. 2,170-2, Zhibin Zhao, Zhaowen Wang, Bingliang Gao, Yuqing Feng, Zhongning Shi, and Xianwei Hu, Light Metals 2015, pp Kaiyu Zhang, Doctoral thesis, Northeastern University, Shenyang, February Kaiyu Zhang, Yuqing Feng, Phil Schwarz, Zhaowen Wang, and Mark Cooksey, Ind. Eng. Chem. Res., Vol. 52, 2013, pp.11,378 11, Dong Shi, Doctoral thesis, Northeastern University, Shenyang, January Min Li, Bingliang Gao, Chengyuan Liu, Wenting Chen, Zhongning Shi, Xianwei Hu, and Zhaowen Wang, Electrochimica Acta, Vol. 180, 2015, pp Yungang Ban, Zhuo Zhang, Xiquan Qi, Yu Mao, Zhaowen Wang, Zhongning Shi, Bingliang Gao, and Xianwei Hu, Light Metals 2010, pp Lu Dingxiaong, Mao Jihong, Ban Yonggang, Qi Xiquan, Yang Qingchen, and Dong Hui, Light Metals 2011, pp Bingliang Gao obtained his Ph.D. in Non-ferrous Metallurgy from the Northeastern University in China. He is a full professor at Northeastern University, where he started his career in Gao has been working on molten salts electrochemistry, especially in aluminum reduction technology, for over 20 years. His work mainly focuses on the theory of molten salts electrolysis as well as electrochemical preparation of Al-based alloys in high temperature molten salts and room temperature molten salts. Gao is the author or co-author of more than 100 scientific and technical papers, as well as two books on molten salts. 30

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