Chromium: A Double-Edged Sword in Preparation ... - ACS Publications

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Chromium: A Double-Edged Sword in Preparation of Refractory Materials from Ferronickel Slag Zhiwei Peng, Foquan Gu, Yuanbo Zhang, Huimin Tang, Lei Ye, Weiguang Tian, Guoshen Liang, Mingjun Rao, Guanghui Li, and Tao Jiang ACS Sustainable Chem. Eng., Just Accepted Manuscript • DOI: 10.1021/ acssuschemeng.8b01882 • Publication Date (Web): 25 Jun 2018 Downloaded from http://pubs.acs.org on July 5, 2018

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ACS Sustainable Chemistry & Engineering

Chromium: A Double-Edged Sword in Preparation of Refractory Materials from Ferronickel Slag

Zhiwei Peng*,†, Foquan Gu*,†, Yuanbo Zhang*,†, Huimin Tang†, Lei Ye†, Weiguang Tian‡, Guoshen Liang‡, Mingjun Rao†, Guanghui Li†, and Tao Jiang† †

School of Minerals Processing and Bioengineering, Central South University, Changsha, Hunan 410083, China ‡

Guangdong Guangqing Metal Technology Co. Ltd., Yangjiang, Guangdong 529500, China

Corresponding authors: [email protected] (Z. Peng), [email protected] (F. Gu), [email protected] (Y. Zhang).

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ABSTRACT: This study reports the role of chromium as a double-edged sword in the preparation of refractory materials from ferronickel slag with the addition of sintered magnesia based on the thermodynamic analysis and experimental exploration of the phase transformation of ferronickel slag during the sintering process. The results of thermodynamic calculation, X-ray diffraction and electron probe microanalysis revealed that in the presence of sintered magnesia (20 wt %) and Cr2O3 (0-6 wt%), forsterite, donathite (instead of magnesium chromate spinel generated without addition of Cr2O3), magnesium aluminate spinel, and enstatite were formed. The forsterite and spinel phases contributed to high refractoriness of the prepared material by sintering. However, with excessive addition of Cr2O3 (> 6 wt %), the quantity of enstatite increased obviously, which would lower the refractoriness of refractory material. For this reason, the addition of chromium or its content in the slag should be carefully controlled to fully exert its advantage in promoting the properties of the refractory material. Based on these findings, a superior refractory material with refractoriness of 1840 °C, bulk density of 2.68 g/cm3, apparent porosity of 15.19%, and compressive strength of 96.28 MPa was obtained by sintering at 1350 °C for 3 h with additions of 20 wt % sintered magnesia and 6 wt % Cr2O3. Because of its better comprehensive properties than the commercial counterparts and those obtained without addition of Cr2O3, the present study offers a very promising method for utilizing the hazardous element in preparing high-quality refractory materials from industrial waste, exhibiting great environmental and economic benefits.


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KEYWORDS: Ferronickel slag, Refractory material, Sintering, Chromium oxide, Spinel



INTRODUCTION Ferronickel slag is produced as a by-product from nickel smelters. Because of the very low percentage of nickel in the natural ores (1 wt % - 2 wt %), a significant quantity of slag is generated during the production of nickel.1 It was estimated that approximately 12-14 tons of nickel slag are generated in the production of 1 ton of nickel alloy.2 For this reason, massive ferronickel slag is produced worldwide and its annual global output is more than 11.934 Mt.3,4 At present, however, less than 10 wt % of ferronickel slag is utilized5 and most of ferronickel slag is disposed in an open environment, posing a great threat to ground and underground water due to its high contents of hazardous elements, including 1.08-3.07 wt % Cr.6,7 Apparently, there is an urgent need for safe disposal and utilization of ferronickel slag.8 For treatment of ferronickel slag, many efforts have been devoted to recovering the contained metals (Ni, Co, Cu, et al.),9-15 applying it in construction and building materials,16-25 and producing glass ceramics26-28 and geopolymers.29-36 Extracting metallic element usually demands harsh conditions such as high temperature and long processing time. Meanwhile, due to low contents of these elements, the process is considered uneconomic. When it is used as construction and building materials directly, there exists a risk of volume expansion of the material because of the high content of magnesia in the slag. Also, high contents of hazardous elements (e.g. Cr) in the slag may pose a potential danger to the environment and human health.37 For production of glass ceramics and geopolymers, relevant processes often require complex operations in the presence of various additives to maintain sufficient quality.


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Overall, the above methods for treatment of ferronickel slag still face many challenges. It is essential to seek viable applications of the ferronickel slag to ensure its maximal utilization due to the rapid increase of slag discharge. As ferronickel slag is mainly composed of magnesia and silica, exhibiting a similar composition to forsterite refractory materials, a route for preparing forsterite refractory materials from ferronickel slag with the addition of sintered magnesia was proposed in our recent studies.38,39 It showed that a good refractory material with the refractoriness of 1660 °C could be successfully prepared after sintering at 1350 °C for 3 h with the utilization ratio of ferronickel slag of 80 wt % (addition of 20 wt % sintered magnesia). This method was considered promising for treatment of the slag because of its smaller energy consumption (1350 °C, 3 h versus 1500-1650 °C, 3-6 h) 40-42

and lower production cost43 in comparison with traditional processes for

production of commercial counterparts. However, the influence of main impurities in the ferronickel slag, such as chromium oxide, on the preparing refractory materials from ferronickel slag was still uncertain although their promoting effect may exist regarding the possibility of formation of Cr-bearing spinel. In fact, refractory materials containing chromium (III) oxide are featured by excellent corrosion resistance, thermal shock resistance, relatively low cost and long durability,44-46 with wide applications in waste melting furnaces, gasification furnaces, glass tank furnaces, tapping channels and many other furnaces in ferrous and non-ferrous (e.g., copper and lead) metallurgy.47-53 It should be mentioned that when chromium is stabilized as Cr (III) in the spinel phase, it becomes nontoxic.54-56 The conversion of Cr (III) to Cr (VI)



is also restrained when the furnaces are operated in low oxygen atmosphere ( 6 wt %), the spinel phases, mainly donathite, were preferably


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formed. Meanwhile, a large amount of SiO2 was released and its reaction with MgO speeded up the formation of enstatite, which would lower the refractoriness of refractory material. When the slag was sintered at 1350 °C for 3 h with additions of 20 wt % magnesia and 6 wt % chromium oxide, a high-quality refractory material with refractoriness of 1840 °C, bulk density of 2.68 g/cm3, apparent porosity of 15.19%, and compressive strength of 96.28 MPa was obtained. Overall, it is highly promising to improve the property of refractory materials derived from ferronickel slag by controlling the amount of chromium-bearing additives, including various chromium-rich wastes. The novel route proposed in this study not only contributes to sustainable ferronickel production, but also serves as an effective means for comprehensive utilization of Cr-containing and other relevant hazardous wastes, creating pronounced environmental and economic benefits.

AUTHOR INFORMATION Corresponding Authors *E-mail: [email protected] Tel.: +86-731-88877656. Fax: +86-731-88830542 (Z. Peng). *E-mail: [email protected] Tel.: +86-731-88877542. Fax: +86-731-88830542 (F. Gu). *E-mail: [email protected] Tel.: +86-731-88877214. Fax: +86-731-88830542 (Y. Zhang).



ORCID Zhiwei Peng: 0000-0003-1720-0749 Foquan Gu: 0000-0002-0257-8530 Notes The authors declare no competing financial interest.

ACKNOWLEDGEMENTS This work was partially supported by the National Natural Science Foundation of China under Grants 51774337, 51504297 and 51811530108, the Natural Science Foundation of Hunan Province, China, under Grant 2017JJ3383, the Key Laboratory for Solid Waste Management and Environment Safety (Tsinghua University) Open Fund under Grant SWMES2017-04, the Open Project of State Key Laboratory Cultivation Base for Nonmetal Composites and Functional Materials under Grant 17kffk11, the Fundamental Research Funds for the Central Universities of Central South University under Grants 502221803 and 502211823, the Co-Innovation Center for Clean and Efficient Utilization of Strategic Metal Mineral Resources under Grant 2014-405, the Guangdong Guangqing Metal Technology Co. Ltd. under Grant 738010210, the Innovation-Driven Program of Central South University under Grant 2016CXS021, and the Shenghua Lieying Program of Central South University under Grant 502035001.


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TOC/Abstract graphic Ferronickel slag (800 o C decomposition)

Transitional products Cr2 O3

Refractory material Chromium additive

(Addition of 6 wt % Cr2 O3)

5μ m

Cr2 O3 Al2 O3

Donathite

Magnesium aluminate spinel

Enstatite

Forsterite

Fe2O3

MgO SiO2 Mg2 SiOz4

Sintered magnesia

5μ m

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Synopsis The role of chromium as a double-edged sword in the preparation of refractory materials from ferronickel slag was verified.


Chromium: A Double-Edged Sword in Preparation ... - ACS Publications

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