Review on the Strategic Metals Recovery from Electrolytic Manganese Anode Slime (EMAS)
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摘要:
电解锰行业每年产生7.5~12万t的锰阳极泥固废, 其矿物组成与结构复杂, 有价金属组分多、含量高, 综合利用难度大, 目前大部分厂家廉价销售或大量堆存, 造成了严重的资源浪费和环境污染。文章分析了阳极泥的产生机理和资源特点, 综述了阳极泥中主要有价战略金属元素Mn、Pb、Sn、Se的分离回收技术, 对比了还原浸出法、焙烧浸出法、碱熔—浸出法等阳极泥处理方法的优缺点, 提出了硫转化综合回收锰铅锡硒新思路, 可为电解锰阳极泥固废的资源化利用提供技术参考。
Abstract:75 000-120 000 tons of electrolytic manganese anode slime (EMAS) are produced in the electrolytic manganese industry every year. The EMAS has high content of strategic metals, complex mineral compositions and complicated structure, and thus the comprehensive utilization is difficult. At present, most manufacturers sell the EMAS cheaply or take the stockpiling disposal, causing serious waste of resources and environmental pollution. This paper analyzed the production mechanism and resource characteristics of the EMAS, and also summarized the separation and recovery technologies of the valuable metals including Mn, Pb, Sn, and Se from the EMAS. The advantages and disadvantages of the reduction leaching method, roasting-leaching method, and alkali melting-leaching method were reviewed and compared. This paper puts forward a novel technique solution for the comprehensive recovery of Mn, Pb, Sn, and Se by sulfur conversion, which can provide technical reference for utilization of EMAS.
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图 2 电解锰阳极泥原料分析:(a), (b)光学显微镜;(c), (d)SEM;(e)XRD[64]
Figure 2.
表 1 典型电解锰阳极泥主要化学成分
/% Table 1. Chemical constituents of the typical electrolytic manganese anode slime
Mn (NH4)2SO4 Fe CaO Pb MgO Sn Se 40~50 5~10 0.1~6 0.1~6 3~6 0.1~6 0.1~0.5 0.1~0.4 表 2 不同还原剂与MnO2的反应方程式以及对应的ΔGθ-T方程式
Table 2. Reactions of different reducing agents and MnO2 and corresponding ΔGθ-T equations
编号 反应方程式 ΔGθ-T/(kJ·mol-1) 自发反应温度范围/K (1) 11MnO2+2FeS2=11MnO+Fe2O3+4SO2(g) ΔGTθ=-170.92-1.026T 自发反应 (2) 15MnO2+2FeS2+14H2SO4=15MnSO4+Fe2(SO4)3+14H2O ΔGθT=-2918.36-0.014T 自发反应 (3) 2MnO2+SO2(g)=Mn2O3+SO3(l) ΔGTθ=-15.01+0.018T T<834 (4) 3MnO2+2SO2(g)=Mn3O4+2SO3(l) ΔGTθ=-22.22+0.049T T<453 (5) MnO2+SO2(g)=MnSO4 ΔGTθ=-240.98+0.177T T<1361 (6) 3MnO2+2Fe+6H2SO4=3MnSO4+Fe2(SO4)3+6H2O ΔGTθ=-1020.13+0.047T 自发反应 表 3 电解锰阳极泥中锰铅分离方法
Table 3. Separation methods of manganese and lead from electrolytic manganese anode slime
分离方法 基本原理 优点 缺点 无机还原浸出法 采用低价硫化物将Mn4+还原为Mn2+进入溶液,铅富集于渣中 锰浸出率高,操作简单 产生酸性废水和废渣,产生SO2和H2S气体 有机还原浸出法 利用有机物的还原性将锰还原为低价进入溶液,铅不发生反应 锰铅分离效果好,原料价格低廉,易获得 操作复杂,反应周期长 固态焙烧浸出法(空气气氛) 高温焙烧活化,乙酸铵浸出铅,锰则不发生反应 铅浸出率高,操作简单 能耗高,反应时间长 固态焙烧浸出法(还原气氛) 利用还原性气体还原锰和铅,硫酸浸出后,固液分离 分离效果好,反应周期短 能耗高,会产生二次污染 碱熔浸出法 高温下碱溶液与MnO2反应生成锰酸根进入溶液,铅不发生反应,锰酸盐经还原得到初级二氧化锰 产品收率高,分离效果好 操作复杂,能耗高 表 4 SnO2转化过程中发生的主要反应[73]及对应的ΔGθ-T方程式
Table 4. Main chemical reactions[73] during the conversion of SnO2and corresponding ΔGθ-Tequations
编号 反应方程式 ΔGθ-T/(kJ·mol-1) 自发反应温度范围/K (32) SnO2+C=SnO+CO(g) ΔGθ-T=188.98-0.196T T>964 (33) SnO2+2C=Sn+2CO(g) ΔGθ-T=359.06-0.384T T>935 (34) 2SnO2+C=2SnO+CO2(g) ΔGθ-T=206.00-0.216T T>954 (35) SnO2+C=Sn+CO2(g) ΔGθ-T=187.10-0.208T T>900 (36) FeS2=FeS+0.5S2(g) ΔGθ-T=140.15-0.138T T>1 016 (37) SnO+FeS=FeO+SnS(g) ΔGθ-T=211.46-0.149T T>1 419 (38) 2Sn+S2=2SnS(g) ΔGθ-T=74.53-0.112T T>665 -
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