准东煤水热提质过程中煤质特性变化对CO<sub>2</sub>气化影响

张小培; 张成; 余圣辉; 李鑫; 冯小飞; 马亚飞; 陈刚

准东煤水热提质过程中煤质特性变化对CO₂气化影响

华中科技大学煤燃烧国家重点实验室, 湖北武汉 430074

基金项目:

国家自然科学基金 51676076

国家国际科技合作专项 2015DFA60410

华中科技大学自主创新研究基金 5003120003

详细信息

通讯作者:
张成, Tel:027-87542417-8321;Fax:027-87545526;E-mail:chengzhang@mail.hust.edu.cn

中图分类号: TQ536.1
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出版历程
- 收稿日期: 2017-06-09
- 修回日期: 2017-07-25
- 网络出版日期: 2021-01-23
- 刊出日期: 2017-10-10

Changes of Zhundong coal properties by hydrothermal upgrading and its impacts on CO₂ gasification

State Key Laboratory of Coal Combustion, Huazhong University of Science and Technology, Wuhan 430074, China

Funds:

National Natural Science Foundation of China 51676076

National Program of International Science and Technology Cooperation 2015DFA60410

Graduates' Innovation Fund of HUST 5003120003

摘要

摘要: 选取准东高钠煤为研究对象，在高压反应釜中进行了不同温度（150-350℃）下的水热提质处理实验，依托电感耦合等离子体质谱（ICP-MS）、氮气等温吸附模型（BET）和X射线衍射（XRD）等技术，分析了煤样的煤质特性变化以及对CO₂气化的综合影响规律。结果表明，水热提质处理后煤样成熟度增加，煤阶上升，钠的脱除效果显著，在300-350℃时脱除率均大于95%。煤焦化学结构致密、有序、稳定；煤样CO₂气化曲线向高温区偏移，气化活性指数呈下降趋势且300-350℃时下降明显。水热提质过程中煤样气化反应活性受到煤阶、碱金属钠含量、物理孔隙结构、化学微晶结构等多个因素的综合影响。
- 准东煤 /
- 水热提质 /
- 煤质特性 /
- 脱钠 /
- CO₂气化
Abstract: The Zhundong high sodium coal was hydrothermally upgraded at 150-350℃ in an autoclave. The inductively coupled plasma mass spectrometer (ICP-MS), nitrogen adsorption isotherm (BET) and X-ray diffraction (XRD) were used to investigate the changes of coal properties and the impacts on the CO₂ gasification characteristics. The results indicate that the coal quality is increased after the hydrothermal upgrading. The removal effect of sodium is obvious, reaching to more than 95% at 300-350℃. The pore structure of the chars changes significantly, the specific surface area and total pore volume increase initially at 150-300℃ and then decrease at 300-350℃. The crystalline structure tends to be aromatic and graphitized, and the chemical structure becomes dense, orderly and stable. Additionally, the gasification reactivity exhibits a decreasing trend, especially for the chars treated at 300-350℃. The CO₂ gasification reactivity during the process of hydrothermal upgrading is comprehensively influenced by different factors containing coal rank, sodium content, physical pore structure and chemical microcrystalline structure.
- Zhundong coal /
- hydrothermal upgrading /
- coal properties /
- sodium removal /
- CO₂ gasification

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图 1 水热改性提质实验装置示意图

Figure 1 Schematic diagram of hydrothermal upgrading experimental apparatus

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图 2 不同水热温度下钠的脱除率

Figure 2 Removal of sodium under different hydrothermal temperatures

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图 3 原煤及提质煤焦的孔隙结构

Figure 3 Pore structure parameters of the raw and upgraded chars

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图 4 原煤及提质煤焦的XRD谱图

Figure 4 XRD spectra of the raw and upgraded chars

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图 5 原煤焦XRD的分峰谱图

Figure 5 Gauss fitting-curves of WCW-raw char

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图 6 煤焦气化反应曲线

Figure 6 Gasification curves during 600-950℃

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图 7 煤焦CO₂气化活性指数(R_0.5)

Figure 7 CO₂ gasification reactivity index (R_0.5) of coal chars

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图 8 CO₂气化活性影响机制分析示意图

Figure 8 Analysis on the mechanism of CO₂ gasification reactivity

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表 1 煤样的工业分析、元素分析

Table 1 Proximate and ultimate analysis of samples

Sample	Proximate analysis w/%				Ultimate analysis w_daf/%					Q_{net, d} / (MJ·kg^-1)	Atomic ratio (daf)
Sample	M_ad	A_d	V_d	FC_d	C	H	O^*	N	S	Q_{net, d} / (MJ·kg^-1)	H/C	O/C
Raw	10.95	5.61	31.90	62.49	73.95	3.97	20.90	0.54	0.64	25.52	0.644	0.212
H150	9.02	5.15	31.86	62.99	74.42	3.92	20.77	0.56	0.40	25.59	0.632	0.209
H200	5.56	5.43	31.15	63.42	74.52	3.90	20.62	0.58	0.38	25.60	0.628	0.208
H250	4.82	5.03	29.86	65.11	74.92	3.80	20.38	0.58	0.32	25.76	0.608	0.204
H300	4.24	5.22	28.48	66.31	76.31	3.79	19.02	0.60	0.29	26.28	0.595	0.187
H350	2.41	5.38	25.36	69.26	78.47	3.73	16.98	0.59	0.23	27.08	0.570	0.162
^*：by difference

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表 2 焦样的XRD参数

Table 2 XRD parameters of coal chars

Sample	2 θ₀₀₂/(°)	2 θ₁₀₀/(°)	d₀₀₂/nm	L_c/nm	L_a/nm
Raw	24.93	43.89	0.357	1.556	1.897
H150	25.04	43.79	0.355	1.557	2.299
H200	25.17	43.95	0.354	1.705	2.376
H250	25.26	43.84	0.352	1.850	2.382
H300	25.34	44.06	0.351	1.905	2.389
H350	25.58	43.44	0.348	2.243	2.411

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准东煤水热提质过程中煤质特性变化对CO₂气化影响

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准东煤水热提质过程中煤质特性变化对CO2气化影响

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Changes of Zhundong coal properties by hydrothermal upgrading and its impacts on CO2 gasification

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2023年《燃料化学学报（中英文）》评优结果公布！

准东煤水热提质过程中煤质特性变化对CO₂气化影响

通讯作者:
张成, Tel:027-87542417-8321;Fax:027-87545526;E-mail:chengzhang@mail.hust.edu.cn

Changes of Zhundong coal properties by hydrothermal upgrading and its impacts on CO₂ gasification