电解煤浆制氢过程中煤阶及矿物的影响与煤结构演化研究进展

doi:10.16085/j.issn.1000-6613.2023-2256

化工进展 ›› 2024, Vol. 43 ›› Issue (5): 2294-2310.DOI: 10.16085/j.issn.1000-6613.2023-2256

• 化石能源的清洁高效转化利用 • 上一篇

电解煤浆制氢过程中煤阶及矿物的影响与煤结构演化研究进展

周安宁¹^,²(), 江雨寒¹, 刘墨宣¹^,², 赵伟¹^,², 李振¹^,²

^1.西安科技大学化学与化工学院，陕西西安 710054
^2.自然资源部煤炭资源勘查与综合利用重点实验室，陕西西安 710021

收稿日期:2023-12-25 修回日期:2024-02-28 出版日期:2024-05-15 发布日期:2024-06-15
通讯作者: 周安宁
作者简介:周安宁（1962—），教授，博士生导师，研究方向为能源化工、功能纳米材料、二氧化碳捕集与转化、电解煤浆制氢等。 E-mail：psu564@139.com。
基金资助:
中国博士后基金(2023TQ0269);陕西省博士后科研项目(2023BSHEDZZ302);国家自然科学基金-新疆联合基金(U2003133)

Research progress in hydrogen production from electrolytic coal slurry: Effects of coal rank and minerals, and the evolution of coal structure

ZHOU Anning¹^,²(), JIANG Yuhan¹, LIU Moxuan¹^,², ZHAO Wei¹^,², LI Zhen¹^,²

^1.College of Chemistry and Chemical Engineering, Xi’an University of Science and Technology, Xi’an 710054, Shaanxi, China
^2.Key Laboratory of Coal Resources Exploration and Comprehensive Utilization, Ministry of Natural Resources, Xi’an 710021, Shaanxi, China

Received:2023-12-25 Revised:2024-02-28 Online:2024-05-15 Published:2024-06-15
Contact: ZHOU Anning

摘要/Abstract

摘要：

电解煤浆制氢（CSE）是一种在温和条件下实现电化学制氢与煤炭低碳清洁利用的新技术。电解煤浆制氢的理论分解电压仅为0.21V，实际消耗的能量约为电解水制氢的1/3~1/2，具有能耗低、污染小，可与煤基精细化学品制备、煤岩显微组分分离等过程集成的优点，但煤转化率低、煤浆电解机理不清晰等问题仍具有极大挑战性。本文讨论了CSE机理研究现状，概述了煤阶及矿物质对CSE的电氧化活性的影响，总结了CSE过程中煤表面元素、官能团结构、煤碳骨架结构在阳极区电化学氧化的变化规律，讨论了阴极区电化学还原对煤表面润湿性、Zeta电位等煤表面性质的影响，以及阴极区添加煤浆的电还原制氢及其耦合技术，以期为CSE制氢与煤低碳清洁利用提供理论支撑。此外，本文还展望了CSE的发展方向，提出了高性能CSE电极催化材料开发及煤氧化-还原反应调控机理研究是该技术获得突破的关键。

关键词: 电解, 制氢, 电化学, 煤浆氧化, 煤结构

Abstract:

Coal slurry electrolysis for hydrogen production (CSE) is a novel technology that enables electrochemical hydrogen production and the low-carbon clean utilization of coal under mild conditions. The theoretical decomposition voltage of hydrogen production from electrolyzed coal slurry is only 0.21V, and the actual energy consumption is about 1/3—1/2 of that of hydrogen production from electrolyzed water. This method has the advantages of low energy consumption, minimal pollution, and being integrated with the process of separating coal macerals and preparing coal-based fine chemicals. However, the challenges of low coal conversion rate and unclear mechanism of coal slurry electrolysis remain extremely daunting. This review discussed the current status of research on CSE mechanism, outlined the influence of coal rank and minerals on the electrooxidizing activity of CSE, summarized the changing rules of coal surface elements, functional group structure, and coal carbon skeleton structure during CSE in the anode zone, and expound the effects of electrochemical reduction in the cathode zone on the coal surface properties such as coal surface wettability and Zeta potential, as well as hydrogen production by electroreduction with the addition of coal slurry in the cathode zone and its coupling technology. The aim was to provide theoretical support for CSE in hydrogen production and low-carbon clean utilization of coal. In addition, this review also anticipated the future development direction of CSE and suggested that achieving a breakthrough in this technology relied on the development of high-performance electrode catalytic materials for CSE and the investigation of the regulation mechanism behind coal oxidation-reduction reactions.

Key words: electrolysis, hydrogen production, electrochemistry, coal slurry oxidation, coal structure

中图分类号:

TQ536

周安宁, 江雨寒, 刘墨宣, 赵伟, 李振. 电解煤浆制氢过程中煤阶及矿物的影响与煤结构演化研究进展[J]. 化工进展, 2024, 43(5): 2294-2310.

ZHOU Anning, JIANG Yuhan, LIU Moxuan, ZHAO Wei, LI Zhen. Research progress in hydrogen production from electrolytic coal slurry: Effects of coal rank and minerals, and the evolution of coal structure[J]. Chemical Industry and Engineering Progress, 2024, 43(5): 2294-2310.

图/表 8

图1 电解煤浆制氢机理示意图[(a)，R n+/O m–为氧化还原电对][43]及不同氧化电子对的煤电氧化机理[Fe3+[27](b)，Fe(CN)63-[60](c)；碱性条件下电解煤浆制氢机理[64] (d)及有机碳形成机制[40] (e)]

图2 在标准状态下酸性介质中水电解和碳辅助电解的电化学电势窗口内的电解活性[25](a)；水电解和煤辅助电解产生的每摩尔H2的能量需求[47] (b)

图3 霍林河褐煤、准东次烟煤和鸡西烟煤三种不同煤变质程度煤的I-V曲线(a)，I-t曲线(b)[71]；不同种类的煤、活性炭、石墨与初始电流密度的关系(c)[39]a—印尼煤（泥炭）；b—新疆煤（褐煤）；c—明佳煤（烟煤）；d—阳泉煤（无烟煤）；e—活性炭；f—石墨

图4 电解煤浆及产品分离过程示意图[75] (a)；碱性环境中电解煤浆机理[75] (b)；原煤和脱矿煤进行恒电流电解[75] (c)；电解前后煤的SEM图[26] (d)：右上电解后原煤比右下电解后脱矿煤多一层钝化膜

图5 不同温度下电解前后煤样的XPS谱图[85](a)；CSE与电化学脱硫联合工艺示意图[88](b)；不同温度下电解前后煤中各元素的质量分数[51](c)；不同温度下电解前后煤样的XRD谱图[51](d)

图6 煤样品的FTIR光谱[85](a)；使用FTIR光谱计算获得的结构参数[85](b)；电解不同时间煤的FTIR谱图[26](c)；机械球磨制备羧基化石墨烯模型化合物原理示意图[90](d)

图7 不同温度锡盟褐煤电解前后的13C NMR及分峰拟合谱图[85]

图8 经电化学阳极处理的SMV(a)和SMI(b)的红外光谱图；经电化学阴极处理的SMV(c)和SMI(d)的红外光谱图；电化学阳极(e)和阴极(f)处理时间对SMV和SMI接触角的影响[91]

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电解煤浆制氢过程中煤阶及矿物的影响与煤结构演化研究进展

Research progress in hydrogen production from electrolytic coal slurry: Effects of coal rank and minerals, and the evolution of coal structure

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