煤炭是我国能源供给的压舱石，煤炭产业的可持续发展攸关国家能源安全和经济命脉。我国的低阶煤资源储量丰富，是煤炭生产和供应的重要组成部分。然而，采煤机械化程度的不断提高在满足产能需求的同时，也带来了细粒低阶煤含量和灰分急剧上升的严重问题。浮选是细粒煤泥降灰提质的有效手段，但由于低阶煤表面含氧基团丰富，润湿性强、可浮性差，其浮选过程回收率低、捕收剂用量大，难以实现它的高效经济回收，是煤炭行业迫切需要解决的重大技术难题。本文针对这一技术难题，以神东矿区长焰煤为研究对象，首先详细研究了煤样的基本性质和表面特征。针对低阶煤的浮选特性，提出了通过闪蒸-氧化法来改性烃类油捕收剂（柴油）以增强其吸附活性和浮选性能的创新思路，使用获得的改性柴油进行低阶煤的单因素浮选试验，初步探索长焰煤浮选的最佳工艺参数，并参考单因素试验结果利用Expert Design软件设计四因素三水平的浮选正交试验，对正交试验结果进行拟合分析，构建改性捕收剂条件下的低阶煤可燃体回收率模型，找到最优浮选工艺参数组合，评价捕收剂改性方案强化低阶煤回收的可行性。最后，通过界面相互作用能理论研究常规/改性捕收剂与低阶煤表面的相互作用，通过分析测试手段探讨常规/改性捕收剂对煤表面性质、可浮性的影响，进而从理论计算和实验研究两个层面来揭示柴油改性强化低阶煤浮选的作用机制。研究成果对突破低阶煤浮选的技术瓶颈，推动其浮选产业化进而实现其清洁高效资源化利用具有重要的现实意义。

对神东长焰煤进行煤质分析发现，原煤的氧元素含量23.52%，煤中的矸石矿物主要为石英、高岭石、白云母以及少量的黄铁矿等。通过XPS和FTIR对煤样表面官能团进一步分析测试，发现煤中的氧元素主要以羧基、羰基、羟基等含氧官能团存在，这些基团的总含量为34.89%，这导致煤样的表面亲水性强、可浮性极差。常规捕收剂浮选低阶煤的实验结果表明，当捕收剂柴油用量高达100 kg/t时，可燃体回收率仅达到了67.25%，此时浮选完善指标为38.84%，浮选效果仍不理想，说明常规捕收剂在低阶煤表面的吸附效果很差，无法有效改善低阶煤的可浮性。

通过自组装的氧化-冷凝装置对捕收剂柴油进行活化改性，成功地在捕收剂分子中引入了含氧官能团（极性亲固基），使部分捕收剂转变成了双亲分子。FTIR分析表明，改性处理后的柴油在3444 cm^-1、1090 cm^-1和1723 cm^-1处新增了羟基峰（–OH）和羰基峰（>C=O）。使用改性捕收剂进行煤样的浮选实验发现，当捕收剂用量为2 kg/t时，获得了可燃体回收率73.22%、灰分10.40%的良好指标。通过Box-Behnken试验设计和响应面分析，建立了低阶煤浮选可燃物回收率关于浮选条件的二次函数模型，并进一步求解浮选模型确定了改性捕收剂浮选低阶煤的最优工艺参数：当捕收剂用量4.179 kg/t、转速1718.636 r/min、矿浆浓度40 g/L、充气量0.02 m³/h时，浮选可燃体回收率达到了85.49%，远高于常规柴油用量为100 kg/t时的浮选指标，相当于把捕收剂用量降低了95.82%。通过常规捕收剂的活化改性实现了低阶煤的高效浮选。

界面相互作用能计算结果表明，常规/改性柴油-煤两相之间的相互作用自由能分别为-64.00 mJ和-84.90 mJ，说明改性柴油与煤表面间的相互引力更大，更容易在煤表面吸附，常规/改性捕收剂在煤表面的润湿速率实验也证实了这一计算结果，这与浮选实验结果一致。而在捕收剂-水-长焰煤三相体系中却出现了与之相反的计算结果，发现常规/改性柴油与煤表面间的相互能分别为-59.10 mJ和-31.88 mJ，出现这一现象的原因可能是因为，捕收剂改性引入了极性含氧基团提高了自身分子的极性，使得捕收剂分子与水分子的相互作用更强。同时还发现，相比于捕收剂分子来说，长焰煤煤与水分子的相互作用更强。因此，改性捕收剂取得更好浮选效果的作用机制可以解释为，改性捕收剂是通过水分子的架桥作用吸附在低阶煤的表面，以此来提高长焰煤的疏水性。对常规/改性捕收剂调浆后的煤样进行XPS和FTIR测试分析，发现经改性捕收剂处理后的煤样表面的亲水基团出现了更为显著的降低，表现出了更大的接触角，证实了改性捕收剂的有效吸附。更为重要的是，改性捕收剂同常规捕收剂一样对矸石矿物的疏水性影响很小，具有良好的选择性。

Coal is the ballast stone of China's energy supply, the sustainable development of coal industry is vital to national energy security and economic lifeline. China's low rank coal resources are rich in reserves, which is an important part of coal production and supply. However, the continuous improvement of coal mining mechanization not only meets the demand of production capacity, but also brings about the serious problem of the sharp rise of fine low rank coal content and ash. Flotation is an effective means of reducing ash and improving quality of fine coal slime. However, due to the rich oxygen-containing groups on the surface of low-rank coal, strong wettability and poor floatability, its flotation process has low recovery rate and large amount of collector, so it is difficult to realize its efficient and economic recovery, which is a major technical problem urgently needed to be solved in the coal industry. Aiming at this technical problem, this paper takes the long-flame coal of Shendong mining area as the research object, and firstly studies the basic properties and surface characteristics of the coal sample in detail. According to the flotation characteristics of low-rank coal, the innovative idea of modifying hydrocarbon oil collector by flash-oxidation method to enhance its adsorption activity and flotation performance was put forward. The single factor flotation test of low-rank coal was carried out by using the modified collector, and the optimal flotation test conditions were obtained. And refer to the single factor test results using the Expert Design software design of four factors three levels orthogonal experiment of flotation and fitting analysis, the result of the orthogonal experiment to build modified collector under the condition of low rank coal burning body recovery model, to find the optimal flotation process parameters combination, evaluation of collector modification method to strengthen the feasibility of low rank coal recovery. Finally, through the interface interaction energy theory research routine/modification on the surface of the collector and the low rank coal interaction, through the analysis of testing methods conventional/modified collector for coal, the influence of the floatability of surface properties, and then from two aspects: theoretical calculation and experimental study to reveal collector modification to strengthen the mechanism of action of low rank coal flotation. The research results have important practical significance for breaking through the technical bottleneck of low-rank coal flotation, promoting its flotation industrialization and realizing its clean and efficient resource utilization.

The coal quality analysis of Shendong long-flame coal shows that the content of oxygen element in raw coal is 23.52%, and the gangue minerals in coal are mainly quartz, kaolinite, muscovite and a small amount of pyrite. XPS and FTIR were used to further analyze and test the surface functional groups of coal samples. It was found that oxygen elements in coal mainly existed in oxygen-containing functional groups such as carboxyl group, carbonyl group and hydroxyl group, and the total content of these groups was 34.89%, which resulted in strong hydrophilicity and poor floatability of coal samples. The experimental results of low-rank coal flotation with conventional collector show that when the amount of collector diesel oil is as high as 100 kg/t, the recovery rate of combustible body only reaches 67.25%. At this time, the flotation perfect index is 38.84%, and the flotation effect is still not ideal, indicating that the adsorption effect of conventional collector on the surface of low-rank coal is very poor, and the floatability of low-rank coal cannot be effectively improved.

A self-assembled oxidation-condensation device was used to activate and modify the collector diesel oil. Oxygen-containing functional groups (polar solid loving groups) were successfully introduced into the collector molecule, and some collectors were converted into parental molecules. FTIR analysis showed that hydroxyl peak (–OH) and carbonyl peak (＞C=O) increased at 3444 cm^-1, 1090 cm^-1 and 1723 cm^-1. Flotation experiments on coal samples with modified collector show that when the collector dosage is 2 kg/t, the good indexes of combustible body recovery of 73.22% and ash content of 10.40% are obtained. Through Box-Behnken test design and response surface analysis, the quadratic function model of fuel recovery in low-rank coal flotation was established, and the optimal process parameters of low-rank coal flotation with modified collector were determined by further solving the flotation model: When the amount of collector was 4.179 kg/t, the speed was 1718.636 r/min, the pulp concentration was 40 g/L, and the gas volume was 0.02 m³/h, the recovery rate of flotation combustible reached 85.49%, which was far higher than the flotation index when the conventional diesel consumption was 100 kg/t. It is equivalent to reducing the amount of collector by 95.82%. High efficiency flotation of low rank coal was realized by activation modification of conventional collector.

Calculated interface interaction energy shows that the conventional/modified diesel oil coal the interaction of two free energy of -64.00 mJ and -84.90 mJ respectively, it shows that the mutual attraction between modified diesel oil and coal surface is larger, more easily in the coal surface adsorption, experiments on wettability rate of conventional/modified collector on coal surface also confirm this calculation result, this is consistent with the flotation experiment results. However, in the three-phase system of collector-water- long flame coal, the calculation results are opposite, and it is found that the mutual energy between conventional/modified diesel oil and coal surface is -59.10 mJ and -31.88 mJ respectively. This phenomenon may be caused by the introduction of polar oxygen-containing groups by collector to improve the polarity of its own molecules. The interaction between the collector molecule and the water molecule is stronger. It is also found that the interaction between long-flame coal and water molecules is stronger than that of collector molecules. Therefore, the mechanism of the modified collector to achieve better flotation effect can be explained as that the modified collector is adsorbed on the surface of long-flame coal through the bridging action of water molecules, so as to improve the hydrophobicity of long-flame coal. XPS and FTIR tests were carried out on the coal samples treated with the conventional/modified collector, it was found that the hydrophilic groups on the surface of the coal samples treated with the modified collector decreased more significantly and showed a larger contact angle, which confirmed the effective adsorption of the modified collector. More importantly, the modified collector has little effect on the hydrophobicity of gangue minerals, and has good selectivity.

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