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活性外来矿物复合材料对高韦尔德部分氧化细煤矸石及其精选残渣热解过程中焦炭和焦油分布的催化作用

Catalytic Effect of Reactive Extraneous Mineral Composites on Char and Tar Distribution during Pyrolysis of Highveld Partially Oxidized Fine-Coal Reject and Its Beneficiated Residues.

作者信息

Mphahlele Katlego, Matjie Ratale Henry, Bunt John Reginald

机构信息

Centre of Excellence in Carbon-Based Fuels, School of Chemical and Mineral Engineering, North-West University, Potchefstroom Campus, Private Bag X6001, Potchefstroom 2520, South Africa.

出版信息

ACS Omega. 2023 Sep 20;8(39):36479-36492. doi: 10.1021/acsomega.3c05462. eCollection 2023 Oct 3.

Abstract

In this study, the South African partially oxidized fine-coal reject (FCR), which is associated with human health and environmental problems and sustains high disposal expenses, was subjected to density-separation, chemical fractionation, and demineralization experiments to isolate and evaluate the mode of occurrence of mineral-matter (MM) effects on the FCR pyrolysis. A unique composite of two reactive oxides (i.e., MgO and FeO) and a hydrated oxide [i.e., Ca(OH)] representing major extraneous coal-minerals were blended with either FCR, demineralized FCR, and its beneficiated samples to evaluate the yields of pyrolytic products and activation energy following a novel procedure. The properties of FCR samples and their pyrolytic products were determined by different analyses. Results indicate that the reactive oxides and a hydrated oxide composite addition increased the average activation energy (332.0-476.5 kJ/mol) for FCR due to the initial Ca(OH) decomposition and FeO reduction that took place under pyrolysis conditions. The FCR mineral-rich sink fractions achieved the highest carbon conversion (char yield = 78.8% and tar yield = 5.1%) compared to those of other samples (e.g., <1.9 g/cm float char yield = 87.3% and tar yield = 2.3%) evaluated due to higher proportions of calcite/dolomite/pyrite cleats and nonmineral inorganics (Ca, Mg, Na, and Fe) which catalyzed the pyrolysis reactions. On the other hand, CaCO, CaMg(CO), and metakaolinite formations in the char derived from a blend of reactive oxides and a hydrated oxide composite and FCR interfere with the pyrolysis reactions. Also, deoxygenation reactions were impeded by oxygen present in the reactive oxides and a hydrated oxide composite. The potent catalytic effects of cleat minerals and the extraneous minerals associated with cracking of heavy tars to lighter fractions open opportunities to further understand the mode of occurrence of MM present in FCR during utilization in global pyrolysis. This may reduce waste disposal costs, health-hazards, air-pollution, and FCR volumes and augments feed-coals.

摘要

在本研究中,南非部分氧化细煤矸石(FCR)存在与人类健康和环境相关的问题,且处置成本高昂,为此开展了密度分离、化学分级和脱矿质实验,以分离并评估矿物质(MM)对FCR热解影响的赋存方式。将两种活性氧化物(即MgO和FeO)与一种代表主要外来煤中矿物质的水合氧化物[即Ca(OH)]组成的独特混合物,与FCR、脱矿质FCR及其精选样品混合,按照一种新程序评估热解产物的产率和活化能。通过不同分析确定了FCR样品及其热解产物的性质。结果表明,由于热解条件下最初发生的Ca(OH)分解和FeO还原,活性氧化物和水合氧化物混合物的添加提高了FCR的平均活化能(332.0 - 476.5 kJ/mol)。与其他评估样品(例如,<1.9 g/cm浮选煤焦产率 =87.3%,焦油产率 =2.3%)相比,富含矿物质的FCR下沉级分实现了最高的碳转化率(煤焦产率 =78.8%,焦油产率 =5.1%),这是因为方解石/白云石/黄铁矿解理和非矿物无机物(Ca、Mg、Na和Fe)的比例较高,催化了热解反应。另一方面,由活性氧化物和水合氧化物混合物与FCR混合得到的煤焦中CaCO₃、CaMg(CO₃)₂和偏高岭石的形成干扰了热解反应。此外,活性氧化物和水合氧化物混合物中存在的氧阻碍了脱氧反应。解理矿物和与重焦油裂解为较轻馏分相关的外来矿物的强催化作用,为进一步了解FCR在全球热解利用过程中MM的赋存方式提供了机会。这可能会降低废物处置成本、健康危害、空气污染以及FCR的体积,并增加原料煤。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/1db8/10552492/5cdff68c1914/ao3c05462_0001.jpg

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