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废催化剂中铂族金属回收现状与研究进展

丁云集 张深根

丁云集, 张深根. 废催化剂中铂族金属回收现状与研究进展[J]. 工程科学学报, 2020, 42(3): 257-269. doi: 10.13374/j.issn2095-9389.2019.11.26.001
引用本文: 丁云集, 张深根. 废催化剂中铂族金属回收现状与研究进展[J]. 工程科学学报, 2020, 42(3): 257-269. doi: 10.13374/j.issn2095-9389.2019.11.26.001
DING Yun-ji, ZHANG Shen-gen. Status and research progress on recovery of platinum group metals from spent catalysts[J]. Chinese Journal of Engineering, 2020, 42(3): 257-269. doi: 10.13374/j.issn2095-9389.2019.11.26.001
Citation: DING Yun-ji, ZHANG Shen-gen. Status and research progress on recovery of platinum group metals from spent catalysts[J]. Chinese Journal of Engineering, 2020, 42(3): 257-269. doi: 10.13374/j.issn2095-9389.2019.11.26.001

废催化剂中铂族金属回收现状与研究进展

doi: 10.13374/j.issn2095-9389.2019.11.26.001
基金项目: 国家自然科学基金资助项目(51672024);工信部绿色制造系统集成资助项目;中央基本科研业务费资助项目(FRF-TP-19-003B1)
详细信息
    通讯作者:

    E-mail:zhangshengen@mater.ustb.edu.cn

  • 中图分类号: TF83;X742;X734.2

Status and research progress on recovery of platinum group metals from spent catalysts

More Information
  • 摘要: 我国铂族金属(Platinum group metals, PGMs)储量少,消费量大,对外依存度高,PGMs二次资源的回收利用是缓解我国PGMs短缺最重要的途径。废催化剂是PGMs最主要的来源,其回收成为研究的热点。本文详细介绍了PGMs消费结构与回收现状,全球PGMs回收量约占原矿产量的20%~30%,且将保持持续增长的趋势。样品的精准分析对PGMs回收有至关重要的作用,同时还原、焙烧、机械球磨等预处理能提高PGMs回收率。相对于传统氰化法和王水溶解,近年来开发出氯化浸出法、超临界萃取法、载体溶解法等较环保的浸出工艺。尽管部分湿法浸出工艺已经产业化应用,但存在废水量大、产生有毒气体及回收率低(特别是Rh)的问题。火法富集是以铅、铜、铁、镍锍为捕集剂,与PGMs形成合金富集,载体熔化造渣。本文对上述富集方法进行了综述并总结了优缺点,基于现有技术存在的污染严重、PGMs回收率不高等问题,展望了PGMs绿色高效回收技术,如活化预处理、协同提取有价金属和载体利用、贱金属协同冶炼和铁捕集–电解等,为从事该领域的科研工作者提供了良好的参考。
  • 图  1  2007—2018年全球主要国家原生Pt(a)和原生Pd产量(b)

    Figure  1.  Global mineral production of Pt (a) and Pd (b) during 2007—2018

    图  2  全球Pt和Pd在主要领域的消费结构分布

    Figure  2.  Main worldwide consumption distributions of Pt and Pd

    图  3  铁合金物相分析. (a)扫描透射电子显微镜微区;(b)能谱成分分析;(c)高分辨透射电镜;(d)选区电子衍射图谱

    Figure  3.  Analysis of Fe-PGMs alloy: (a) STEM; (b) EDS analysis; (c) HRTEM; (d) SAED

    表  1  不同废催化剂的分析方法及结果

    Table  1.   Determination of PGMs in spent catalysts by various methods

    Catalysts (carriers)ElementsAnalysis methodsRSD/%Ref
    Spent automotive catalystsPt, Pd, RhCarius tube+ICP–AES1~2[12]
    HCl–H2O2+ICP–AES4.5~5.1[13]
    Spent catalysts (Al2O3/SiO2)PtICP–AES standard curve method<3[14]
    Spent Oxo-alcohols CatalystRhH2SO4–H2O2–HCl+ICP–OES0.92[15]
    Spent catalysts (SiO2)RhChemical vapour generation+ICP–AES1.6[16]
    Spent catalyst (Al2O3/SiO2)Pt, PdFire assaying+ICP–AES<2[17]
    Spent dehydrogenation catalystPtAqua regia+FAAS<3.45[18]
    Spent Pd–C catalystPdH2SO4–HNO3+ICP–AES1.52[19]
    下载: 导出CSV

    表  2  25 ℃ PGMs的标准电极电位

    Table  2.   Standard electrode potentials of PGMs at 25 ℃

    Electrode reactionsε0/V
    ${\rm{PdBr}}_4^{2 - }$+2e=Pd+4Br0.60
    ${\rm{PdCl}}_4^{2 - }$+2e=Pd+4Cl0.62
    ${\rm{PdCl}}_6^{2 - }$+2e=${\rm{PdCl}}_4^{2 - }$+2Cl1.29
    ${\rm{PtBr}}_4^{2 - }$+2e=Pt+4Br0.58
    ${\rm{PtBr}}_6^{2 - }$+2e=${\rm{PtBr}}_4^{2 - }$+2Br0.59
    ${\rm{PtCl}}_6^{2 - }$+4e=Pt+6Cl0.74
    ${\rm{RhCl}}_6^{3 - }$+3e=Rh+6Cl0.43
    ${\rm{PdCN}}_4^{2 - }$+2e=Pd+4CN0.40
    ${\rm{PtCN}}_4^{2 - }$+2e=Pt+4CN0.09
    下载: 导出CSV

    表  3  部分典型贱金属捕集PGMs工艺

    Table  3.   Some typical pyrometallurgical processes for PGM recycling

    CountriesCompany namesFurnacesCollectors
    BelgiumUmicoreIsasmelt furnaceCopper
    AmericaMultimetcoDC electrical arc furnaceCopper
    JapanTanakaPlasma melting furnaceIron
    EnglandJohnson-MattheyPlasma melting furnaceIron
    ChinaSino-Platinum MetalsPlasma melting furnaceIron
    下载: 导出CSV
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  • 收稿日期:  2019-11-26
  • 刊出日期:  2020-03-01

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