WO2024082838A1 - 一种矿山固废流态化充填处置协同二氧化碳封存方法 - Google Patents

一种矿山固废流态化充填处置协同二氧化碳封存方法 Download PDF

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WO2024082838A1
WO2024082838A1 PCT/CN2023/116687 CN2023116687W WO2024082838A1 WO 2024082838 A1 WO2024082838 A1 WO 2024082838A1 CN 2023116687 W CN2023116687 W CN 2023116687W WO 2024082838 A1 WO2024082838 A1 WO 2024082838A1
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filling
slurry
disposal
solid waste
carbon fixation
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PCT/CN2023/116687
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English (en)
French (fr)
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李百宜
龙康
郭宇鸣
张吉雄
马嘉源
周楠
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中国矿业大学
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Publication of WO2024082838A1 publication Critical patent/WO2024082838A1/zh

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    • E—FIXED CONSTRUCTIONS
    • E21—EARTH DRILLING; MINING
    • E21F—SAFETY DEVICES, TRANSPORT, FILLING-UP, RESCUE, VENTILATION, OR DRAINING IN OR OF MINES OR TUNNELS
    • E21F15/00—Methods or devices for placing filling-up materials in underground workings
    • E21F15/005—Methods or devices for placing filling-up materials in underground workings characterised by the kind or composition of the backfilling material
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
    • B01D53/34—Chemical or biological purification of waste gases
    • B01D53/46—Removing components of defined structure
    • B01D53/62—Carbon oxides
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
    • B01D53/34—Chemical or biological purification of waste gases
    • B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
    • B01D53/80—Semi-solid phase processes, i.e. by using slurries
    • E—FIXED CONSTRUCTIONS
    • E21—EARTH DRILLING; MINING
    • E21F—SAFETY DEVICES, TRANSPORT, FILLING-UP, RESCUE, VENTILATION, OR DRAINING IN OR OF MINES OR TUNNELS
    • E21F15/00—Methods or devices for placing filling-up materials in underground workings
    • E21F15/06—Filling-up mechanically
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02C—CAPTURE, STORAGE, SEQUESTRATION OR DISPOSAL OF GREENHOUSE GASES [GHG]
    • Y02C20/00—Capture or disposal of greenhouse gases
    • Y02C20/40—Capture or disposal of greenhouse gases of CO2

Definitions

  • the present invention relates to the field of green coal mining and carbon sequestration, and in particular to a method for fluidized filling disposal of mine solid waste and coordinated carbon dioxide sequestration.
  • coal gangue As a solid waste associated with coal mining, coal gangue is usually discharged and piled on the ground, accounting for 20% of coal production. It not only occupies a large amount of scarce land resources and has a huge impact on the ecological environment of the mining area, but also brings a series of safety hazards such as spontaneous combustion of gangue mountains. Faced with the pressure of ecological and environmental protection, how to efficiently dispose of solid waste such as coal gangue is one of the difficulties faced by coal enterprises in high-quality development.
  • CO2 storage refers to the process of injecting captured CO2 into deep geological reservoirs through engineering and technical means to achieve long-term isolation of CO2 from the atmosphere.
  • the main methods include geological storage, surface storage and marine storage.
  • the "Short-long wall intermittent filling mining and alkaline solid waste CO2 storage system and method” fills the prepared filling materials into the short wall working face underground and then injects carbon for storage, abandoning the advantages of large-scale equipment above ground to assist in the full mineralization of filling materials; for example, "A method for waste treatment and carbon dioxide storage at a pit-mouth coal-fired power plant” uses coal gangue, cement, and alkaline aqueous solution to treat the power plant The CO2 is directly captured and filled into an abandoned wellbore, and its filling space and storage volume are limited by the capacity of the abandoned wellbore.
  • the existing technology has the following problems: the amount of coal gangue consumed in surface sealing is small, the coal gangue and other wastes cannot be properly disposed of after surface sealing, the underground sealing abandons the advantageous conditions for full mineralization of auxiliary filling materials of large-scale equipment on the surface, and the underground sealing is limited by the storage space and can only achieve a smaller storage volume.
  • the purpose of the present invention is to provide a method for fluidized filling disposal of mine solid waste and coordinated carbon dioxide sequestration.
  • a ground carbon fixation-underground well filling-underground carbon fixation system is formed in sequence, and filling slurry is prepared by coal gangue and additives.
  • the slurry and CO2 are fully mixed and stirred, and then filled into the underground production space, and then filled with CO2 again.
  • the mineralization sealing and physical sealing work together to dispose of mine solid waste and seal CO2 .
  • This method is safe, efficient, feasible, and low-cost, and realizes green mining of coal resources and CO2 storage in underground space, reduces the damage of coal mining to the ecological environment, and has broad application prospects.
  • CO2 mineralization principle is one of the main ways to achieve CO2 geological storage. That is, CO2 undergoes a rapid chemical reaction with rocks and forms new carbonate minerals. Through this method, CO2 is permanently "locked” in the rock formation, achieving CO2 mineralization geological storage.
  • the inventors discovered that calcium and magnesium compounds contained in solid wastes such as coal gangue can react with CO2 to form carbonate minerals. Therefore, they proposed a method for fluidized filling disposal of mine solid waste and coordinated carbon dioxide sequestration.
  • the coal gangue solid waste and CO2 are simultaneously disposed of and stored in the coal mine mining space, which is of great significance to reducing the damage to the environment caused by coal mining and reducing greenhouse gas emissions, and is in line with China's "dual carbon" strategic goal.
  • the present invention adopts the following technical solution:
  • One object of the present invention is a method for fluidized filling and disposal of mine solid waste in coordination with carbon dioxide sequestration, which is based on the characteristics of coal gangue solid waste and CO2 mineralization, and sequentially forms a ground carbon fixation-ground well filling-underground carbon fixation system, and fills the goaf formed after coal resource mining with mine solid waste-based filling slurry with the function of mineralization and CO2 sequestration to achieve mine solid waste disposal and CO2 sequestration, which specifically includes the following steps:
  • Preparation of filling materials First, the coal gangue is crushed in the crushing workshop and the grinding workshop, and then the crushed and ground coal gangue is mixed with the additives in each additive material bin and transported to the stirring carbon fixation reaction device;
  • the filling pump provides power to transport the stirred filling slurry through the filling pipeline of the ground-well borehole to the underground production space;
  • Underground carbon fixation process After the filling slurry fills the underground production space, open the CO2 ground-to-well injection system and inject CO2 into the underground filling slurry through the gas pipeline until the filling slurry solidifies, thereby realizing the fluidized solid waste filling disposal and CO2 storage of the underground production space in this mining area of the mine.
  • the crushing of the coal gangue needs to meet the filling slurry pumping requirements, the coal gangue particle size is less than 10 mm, and the proportion of particles below 2 mm is not less than 1/3.
  • the stirring reaction time of CO2 and the filling slurry in the stirring carbon fixation reaction device is determined according to the flow properties of the filling slurry and is monitored by an automatic viscosity measuring instrument.
  • the phase state of the filling material slurry can be determined by the CO 2 injection pressure and flow rate.
  • the CO 2 injection pressure increases sharply and the flow rate remains unchanged, it is determined that the filling material slurry has solidified and the injection of CO 2 can be stopped.
  • the additives include fly ash, quicklime and magnesium slag powder to increase the carbon fixation effect.
  • Another object of the present invention is to provide a system based on a fluidized filling disposal method for mining solid waste in coordination with a carbon dioxide sequestration method, specifically a ground carbon fixation-ground well filling-underground carbon fixation system, which is arranged near the ground gangue mountain corresponding to the middle of the mining area, and includes a feeder, a stirring carbon fixation reaction device, a filling pump and a filling pipeline connected in sequence, wherein the feeder is respectively connected to the grinding workshop, the water tank and each additive material tank, and the crushing workshop is connected to the grinding workshop;
  • the filling pipeline extends deep into the underground production space, and a filling pump is arranged on the filling pipeline; a well is drilled next to the filling pump to the underground production space, and the filling pipeline and gas pipeline are installed in the well; the CO2 gas source is connected to the gas pipeline, and the gas pipeline is divided into two sections, one section is connected to the stirring carbon fixation reaction device, and the other end extends deep into the underground production space.
  • the present invention fills the goaf formed after coal mining with mining solid waste-based filling slurry with the function of mineralization and CO2 storage, disposes of the coal gangue mining solid waste accumulated on the ground and stores CO2 on a large scale, reduces the environmental damage caused by the accumulation of solid waste on the ground, realizes green mining of coal resources, and effectively protects the ecological environment of the mining area;
  • This method forms a ground carbon fixation-ground well filling-underground carbon fixation system to treat solid waste and store CO2 .
  • Ground carbon fixation causes CO2 gas to move upward from the bottom of the filling slurry to increase the contact time and area between CO2 and the filling slurry, so that CO2 and the filling slurry fully react to mineralize and achieve the first CO2 storage.
  • the underground carbon fixation injects CO2 into the filling slurry to solidify it.
  • the porous adsorption properties and geological sealing properties of the filling slurry after solidification are utilized.
  • the mineralization storage and physical storage work together to achieve the second CO2 storage.
  • This method has a large CO2 storage capacity and mine solid waste disposal capacity, is safe and efficient, feasible, and low-cost, and has good prospects for promotion and application.
  • FIG1 is a schematic diagram of a method for fluidized filling disposal of mining solid waste in conjunction with carbon dioxide sequestration provided in Example 1 of the present invention
  • the present invention discloses a method for fluidized filling and disposal of mine solid waste in coordination with carbon dioxide sequestration, wherein a mine solid waste-based filling slurry 12 having the function of mineralizing and sequestering CO2 is filled into the goaf formed after coal resource exploitation, forming a ground carbon fixation-ground well filling-underground carbon fixation system, thereby realizing mine solid waste disposal and CO2 sequestration.
  • the present invention is divided into three steps: ground carbon fixation, ground well filling, and underground carbon fixation.
  • the present invention first completes the ground carbon fixation process. After coal gangue and other mining solid wastes are crushed and ground, they are mixed with fly ash, quicklime, magnesium slag powder and other additives in proportion, and the mass ratio of coal gangue to additives is 12-16:1, and transported to the stirring carbon fixation reaction device 7. The crushing of the coal gangue must meet the pumping requirements of the filling slurry 12. The coal gangue particle size must be less than 10mm, of which the proportion of particles below 2mm is not less than 1/3. A certain proportion of water is filled into the stirring carbon fixation reaction device 7, with 60-80% of coal gangue, 5% of additives, and the rest of water.
  • the CO2 gas source 8 is opened at the same time to continuously inject a certain concentration of CO2 from the bottom of the stirring carbon fixation reaction device 7, so that the CO2 gas moves upward from the bottom of the filling slurry 12 to increase the contact time and area between CO2 and the filling slurry 12, so that CO2 and the filling slurry 12 fully react and mineralize, and realize the carbon fixation of the filling slurry 12, so as to complete the ground carbon fixation process.
  • the stirring reaction time of CO 2 and the filling slurry 12 in the stirring carbon fixation reaction device 7 is determined according to the flow properties of the filling slurry and is monitored by an automatic viscosity measuring instrument.
  • the additives may be magnesium slag powder and quicklime powder.
  • the reaction equations thereof with CO 2 are respectively: MgO+H 2 O ⁇ Mg(OH) 2 (1) Mg(OH) 2 +CO 2 ⁇ MgCO 3 (2) CaO + CO 2 ⁇ CaCO 3 (3)
  • the present invention then performs the underground well filling process.
  • the filling slurry 12 that has fully reacted with CO2 is pumped to the underground production space 11 through the underground well borehole by the filling pump 9 and the filling pipeline 10, completing the underground well filling process;
  • the present invention finally performs an underground carbon fixation process.
  • CO 2 is continuously injected into the underground filling slurry 12 using the gas pipeline 13 until the filling slurry 12 solidifies.
  • the phase state of the filling slurry can be determined by the CO 2 injection pressure and flow rate. When the CO 2 injection pressure increases sharply and the flow rate remains unchanged, it is determined that the filling slurry 12 has solidified and the injection of CO 2 can be stopped.
  • the underground carbon fixation process mainly uses the porous adsorption properties and geological sealing properties of the filling slurry 12 after solidification to seal CO 2. At this point, the underground carbon fixation process is completed, and solid waste disposal and CO 2 sealing are finally achieved.
  • basic filling facilities are arranged near the ground gangue mountain 1 corresponding to the middle of the mining area, including a crushing workshop 2, a grinding workshop 3, various additive material bins 4, a water bin 5, a feeder 6, a stirring carbon fixation reaction device 7, a CO2 gas source 8, and a filling pump 9.
  • the feeder 6, the stirring carbon fixation reaction device 7, the filling pump 9 and the filling pipeline 10 are connected in sequence, and the filling pipeline 10 goes deep into the underground mining space 11;
  • the feeder 6 is respectively connected to the grinding workshop 3, the water bin 5 and the various additive material bins 4;
  • the crushing workshop 2 is connected to the grinding workshop 3, and solid wastes such as coal gangue are crushed in the crushing workshop 2 and then input into the grinding workshop 3 for grinding, and then the gangue, various additive materials and water are transported to the stirring carbon fixation reaction device 7 according to the proportion through the feeder 6 for mixing and stirring.
  • a well is drilled next to the filling pump station to the underground production space 11, and two pipelines, a filling pipeline 10 and a gas pipeline 13, are installed in the well.
  • the CO2 gas source 8 is connected to the gas pipeline 13, and the gas pipeline 13 is divided into two sections when passing through the stirring carbon fixation reaction device 7, one section of the pipeline is passed into the stirring carbon fixation reaction device 7, and the other end goes deep into the underground production space 11.
  • the filling material preparation process begins. First, the coal gangue is crushed to a particle size of less than 10 mm in the crushing workshop and the grinding workshop, and the proportion of particles less than 2 mm is not less than 1/3. Then, 70 kg of crushed and ground coal gangue is mixed with 3.5 kg of quicklime and magnesium slag powder in each additive material bin and transported to the stirring carbon fixation reaction device 7;
  • Fluidized filling process Next, the fluidized filling process begins.
  • the filling pump 9 provides power to transport the stirred filling slurry 12 to the underground production space 11 through the filling pipeline 10;

Abstract

公开了一种矿山固废流态化充填处置协同二氧化碳封存方法及基于这种方法的系统。该方法形成地面固碳-地井充填-井下固碳系统，在煤炭资源开采后形成采空区内充入具有矿化封存CO 2功能的矿山固废基充填料浆(12)，实现矿山固废处置与CO 2封存，步骤具体包括：将破碎的煤矸石与添加剂混合输送至搅拌固碳反应装置(7)，向其中加入水并搅拌，从底部注入CO 2气体，待料浆流动性能达到泵送要求的最低限度后，停止注入CO 2；充填泵(9)将充填料浆通过充填管路(10)输送至井下采出空间(11)，待充填料浆充满井下采出空间后，通过气体管路(13)向井下料浆内部注入CO 2，直至料浆固结。该方法安全高效、切实可行、成本低，实现煤炭资源绿色开采、井下空间CO 2封存，减少了煤炭开采对生态环境的损害。

Description

一种矿山固废流态化充填处置协同二氧化碳封存方法 技术领域
本发明涉及煤矿绿色开采及碳封存领域，具体涉及一种矿山固废流态化充填处置协同二氧化碳封存方法。
背景技术
我国富煤贫油少气的能源禀赋特征决定了煤炭作为我国主体能源地位，而作为煤炭开采伴生的固体废弃物，煤矸石通常排放堆积在地面，占比达到煤炭产量的20％，不仅占用了大量稀缺土地资源，给矿区生态环境造成巨大的影响，同时会带来矸石山自燃等一系列安全隐患。面对生态环境保护的压力，如何高效处置煤矸石等固废是煤炭企业高质量发展面临的难题之一。
另一方面，气候变化是人类面临的全球性问题，CO2排放量与日俱增，对生命系统构成了威胁。大力发展CO2捕集利用与封存(CCUS)技术不仅是未来我国减少CO2排放、保障能源安全的战略选择，而且是构建生态文明和实现可持续发展的重要手段。CO2封存是指通过工程技术手段将捕集的CO2注入深部地质储层，实现CO2与大气长期隔绝的过程，主要方式有地质封存、地表封存和海洋封存等。
目前，地表利用煤矸石、尾矿等材料进行矿化、吸附二氧化碳的技术关键主要集中在添加有效添加剂等环节，但这类方法往往只能消耗少量煤矸石或结束CO2封存工序的废弃煤矸石难以得到合理处置，如“一种利用改性煤矸石脱除电厂烟气CO2的系统及其实施方法”利用有机胺活性组分喷淋负载于改性的破碎煤矸石上对CO2进行捕获，CO2捕获效果良好，但最终作为载体的CO2依旧难以得到合理处置。
而涉及到地下处理煤矸石且同步封存的技术往往将充填材料输送至井下后再进行注碳等工序而失去了井上矿化的优势条件，或受限于封存空间而只能实现较小的封存量。如“短长壁间断充填开采协同碱基固废CO2封存系统及方法”将配制好的充填材料充填入井下短壁工作面后进行注碳封存，舍弃了井上大型设备辅助充填材料充分矿化的优势条件；如“一种坑口燃煤电厂废物处理及二氧化碳封存的方法”采用煤矸石、水泥、碱性水溶液对电厂 的CO2直接捕获后充填入废弃井筒，其充填空间和封存量均受到了该废弃井筒的容量限制。
因此，现有技术存在井上封存消耗煤矸石量小、井上封存后煤矸石等废弃物不能合理处置、井下封存舍弃了井上大型设备辅助充填材料充分矿化的优势条件、井下封存受限于封存空间只能实现较小的封存量。
发明内容
针对上述存在的技术不足，本发明的目的是提供一种矿山固废流态化充填处置协同二氧化碳封存方法，基于煤矸石固废与CO2发生矿化的特征，依次形成地面固碳-地井充填-井下固碳系统，将煤矸石与添加剂制备充填料浆，料浆与CO2充分混合搅拌后充入井下采出空间，再次充入CO2，矿化封存和物理封存共同作用将矿山固废处置与CO2封存，该方法安全高效、切实可行、成本低，实现煤炭资源绿色开采、井下空间CO2封存，减少了煤炭开采对生态环境的损害，具有广泛的应用前景。
目前利用CO2矿化原理是实现CO2地质封存的主要路径之一，即CO2与岩石发生了快速的化学反应并形成了新的碳酸盐矿物，通过这一方法，CO2被永久的“禁锢”在岩层里，实现了CO2的矿化地质封存。
发明人发现煤矸石等固废中含有的钙镁化合物，可与CO2反应形成碳酸盐矿物，因此提出一种矿山固废流态化充填处置协同二氧化碳封存方法，将煤矸石固废与CO2同时在煤矿采出空间中处置封存，对减小煤炭开采对环境的损害、减少温室气体排放具有重要意义，符合我国“双碳”的战略目标。
为实现上述目的，本发明采用如下技术方案：
本发明的一个目的是一种矿山固废流态化充填处置协同二氧化碳封存方法，其基于煤矸石固废与CO2发生矿化的特征，依次形成地面固碳-地井充填-井下固碳系统，在煤炭资源开采后形成的采空区内充入具有矿化封存CO2功能的矿山固废基充填料浆，实现矿山固废处置与CO2封存，具体包括以下步骤：
a、充填材料制备：首先在破碎车间和研磨车间中将煤矸石破碎，然后将破碎研磨后的煤矸石与各添加剂材料仓中的添加剂混合输送至搅拌固碳反应装置；
b、地面固碳工序：向搅拌固碳反应装置中加入一定量的水，开始搅拌，并开始通过CO2 气源从搅拌固碳反应装置底部注入CO2气体，待充填料浆流动性能达到泵送要求的最低限度后，停止搅拌并停止注入CO2；
c、流态化充填工序：通过充填泵提供动力，将搅拌好的充填料浆通过地-井钻孔的充填管路输送至井下采出空间；
d、井下固碳工序：待充填料浆充满井下采出空间后，开启CO2地-井注入系统，通过气体管路向井下充填料浆内部注入CO2，直至充填料浆固结，实现该矿该采区井下采出空间的流态化固废充填处置与CO2封存。
优选地，步骤b中，所述的煤矸石破碎需满足充填料浆泵送要求，煤矸石粒径小于10mm，且2mm以下占比不低于1/3。
优选地，步骤b中，所述搅拌固碳反应装置中CO2与充填料浆搅拌反应时间根据充填料浆流动性能决定，由粘度自动测量仪监测。
优选地，步骤d中，充填料浆物相状态可通过CO2注入压力和流量进行判定，当CO2注入压力急剧增加且流量不变时，则判定充填料浆已经固结，可以停止注入CO2。
优选地，所述添加剂包括粉煤灰、生石灰和镁渣粉，用于增加固碳效果。
本发明的另一个目的是提供基于一种矿山固废流态化充填处置协同二氧化碳封存方法的系统，具体为地面固碳-地井充填-井下固碳系统，布设在该采区中部对应的地面矸石山附近，包括顺次连接的给料机、搅拌固碳反应装置、充填泵和充填管路，所述给料机分别与所述研磨车间、水仓和各添加剂材料仓连接，破碎车间与研磨车间连接；
充填管路深入到井下采出空间，充填管路上设有充填泵；在充填泵旁钻井至井下采出空间，井内安设有所述充填管路和气体管路；CO2气源连接有气体管路，所述气体管路分为两段管路，一段通入搅拌固碳反应装置，另一端深入到井下采出空间。
本发明的有益效果在于：
1、本发明在煤炭资源开采后形成的采空区内充入具有矿化封存CO2功能的矿山固废基充填料浆，规模化处置地面堆积的煤矸石矿山固废与封存CO2，减小固废地面堆积对环境损害，实现煤炭资源绿色开采、有效地保护了矿区生态环境；
2、本方法通过形成地面固碳-地井充填-井下固碳系统进行固废处理与封存CO2，地面固碳使CO2气体从充填料浆底部向上运动，以增加CO2与充填料浆的接触时间和面积，使CO2与充填料浆充分反应而发生矿化实现第一次CO2封存；井下固碳向充填料浆内部注入CO2使其固结，同时利用充填料浆凝固后的多孔吸附性质和地质密闭性质，矿化封存和物理封存共同作用实现第二次封存CO2，该方法CO2封存量和矿山固废处置量大，安全高效、切实可行，成本低，具有较好的推广应用前景。
附图说明
为了更清楚地说明本发明实施例或现有技术中的技术方案，下面将对实施例或现有技术描述中所需要使用的附图作简单地介绍，显而易见地，下面描述中的附图仅仅是本发明的一些实施例，对于本领域普通技术人员来讲，在不付出创造性劳动的前提下，还可以根据这些附图获得其他的附图；
图1为本发明实施例1提供的一种矿山固废流态化充填处置协同二氧化碳封存方法示意图；
附图标记说明：
图中：1-地面矸石山；2-破碎车间；3-研磨车间；4-各添加剂材料仓；5-水仓；6-给料机；7-搅拌固碳反应装置；8-CO2气源；9-充填泵；10-充填管路；11-井下采出空间；12-充填料浆；13-气体管路。
具体实施方式
下面将结合本发明实施例中的附图，对本发明实施例中的技术方案进行清楚、完整地描述，显然，所描述的实施例仅仅是本发明一部分实施例，而不是全部的实施例。对于本领域技术人员已知的技术、方法和设备可能不作详细讨论，但在适当情况下，所述技术、方法和设备应当被视为授权说明书的一部分。
本发明公开的一种矿山固废流态化充填处置协同二氧化碳封存方法，在煤炭资源开采后形成的采空区内充入具有矿化封存CO2功能的矿山固废基充填料浆12，形成地面固碳-地井充填-井下固碳系统，实现矿山固废处置与CO2封存。本发明分为地面固碳、地井充填、井下固碳三个步骤。
本发明首先完成地面固碳流程。将煤矸石等矿山固废破碎磨细后，与粉煤灰、生石灰和镁渣粉等添加剂按比例混合，煤矸石与添加剂混合质量比例为12～16：1，运输至搅拌固碳反应装置7中，所述煤矸石破碎需满足充填料浆12泵送要求，煤矸石粒径要小于10mm，其中2mm以下占比不低于1/3。在搅拌固碳反应装置7内充入一定比例的水，煤矸石60-80％，添加剂占煤矸石5％，其余为水，持续搅拌后，同时打开CO2气源8从搅拌固碳反应装置7底部持续注入一定浓度的CO2，使CO2气体从充填料浆12底部向上运动，以增加CO2与充填料浆12的接触时间和面积，使CO2与充填料浆12充分反应而发生矿化，实现充填料浆12的固碳作用，至此完成地面固碳流程。搅拌固碳反应装置7中CO2与充填料浆12搅拌反应时间根据充填料浆流动性能决定，由粘度自动测量仪监测。
优选的，为增加固碳效果，添加剂可优选为镁渣粉和生石灰粉。其与CO2的反应方程式分别为：
MgO+H2O→Mg(OH)2      (1)
Mg(OH)2+CO2→MgCO3       (2)
CaO+CO2→CaCO3             (3)
本发明接下来进行地井充填流程。首先准确定位井下采出空间11，在井下采出空间11的中部位置布设地-井钻孔，在地-井钻孔内安设充填管路10和气体管路13。将与CO2充分反应后的充填料浆12，利用充填泵9与充填管路10，通过地-井钻孔泵送至井下采出空间11，完成地井充填流程；
本发明最后进行井下固碳流程。将充填料浆12充满井下采出空间[11]后，利用气体管路13持续向井下充填料浆12内部注入CO2，直至充填料浆12凝固，充填料浆物相状态可通过CO2注入压力和流量进行判定，当CO2注入压力急剧增加且流量不变时，则判定充填料浆12已经固结，可以停止注入CO2。井下固碳流程主要利用充填料浆12凝固后的多孔吸附性质和地质密闭性质来封存CO2。至此完成井下固碳流程，最终实现固废处置与CO2封存。
实施例1
依据对发明内容中的说明，结合某煤矿工程地质条件，进行实施例的说明。该矿某采区已经开采完毕，针对该采区开采结束后的所有采出空间实施本发明。
如图1所示，首先在该采区中部对应的地面矸石山1附近布设基础充填设施，包括破碎车间2、研磨车间3、各添加剂材料仓4、水仓5、给料机6、搅拌固碳反应装置7、CO2气源8、充填泵9。其中给料机6、搅拌固碳反应装置7、充填泵9和充填管路10顺次连接，充填管路10深入到井下采出空间11；所述给料机6分别与所述研磨车间3、水仓5和各添加剂材料仓4连接；破碎车间2与研磨车间3连接，煤矸石等固废经破碎车间2破碎后输入研磨车间3进行研磨，然后通过给料机6按照比例将矸石、各添加剂材料和水输送至搅拌固碳反应装置7进行混合搅拌。
在充填泵站旁钻井至井下采出空间11，井内安设有充填管路10和气体管路13两个管路。CO2气源8连接有气体管路13，所述气体管路13经过搅拌固碳反应装置7时分为两段管路，一段通入搅拌固碳反应装置7，另一端深入到井下采出空间11。
矿山固废流态化充填处置协同二氧化碳封存的具体步骤如下：
a、充填材料制备工序：做好上述基础准备工作后开始进行充填材料制备工序，首先在破碎车间和研磨车间中将煤矸石破碎至10mm粒径以下，且2mm以下占比不低于1/3，然后将破碎研磨后的70kg煤矸石与各添加剂材料仓中的3.5kg生石灰和镁渣粉混合输送至搅拌固碳反应装置7；
b、地面固碳工序：接下来在搅拌固碳反应装置7中进行第一步固碳工序，首先向搅拌固碳反应装置7中加入26.5kg水，开始搅拌，并开始通过CO2气源8从搅拌固碳反应装置7底部注入CO2气体，待充填料浆流动性能达到泵送要求的最低限度后，可停止搅拌并停止注入CO2。
c、流态化充填工序：接下来开始流态化充填工序，通过充填泵9提供动力，将搅拌好的充填料浆12通过充填管路10输送至井下采出空间11；
d、井下固碳工序：待充填料浆12充满井下采出空间11后，开启CO2地-井注入系统，通过气体管路13向井下充填料浆12内部注入CO2，当CO2注入压力急剧增加且流量不变时，则判定充填料浆12已经固结，至此实现该矿该采区井下采出空间11的流态化固废充填处置与CO2封存。
显然，本领域的技术人员可以对本发明进行各种改动和变型而不脱离本发明的精神和范围。这样，倘若本发明的这些修改和变型属于本发明权利要求及其等同技术的范围之内， 则本发明也意图包含这些改动和变型在内。

Claims (7)

  1. 一种矿山固废流态化充填处置协同二氧化碳封存方法，其特征在于，基于煤矸石固废与CO2发生矿化的特征，依次形成地面固碳-地井充填-井下固碳系统，在煤炭资源开采后形成的采空区内充入具有矿化封存CO2功能的矿山固废基充填料浆，实现矿山固废处置与CO2封存，具体包括以下步骤：
    a、充填材料制备：在破碎车间和研磨车间中将煤矸石破碎，给料机将破碎研磨后的煤矸石与各添加剂材料仓中的添加剂混合输送至搅拌固碳反应装置；
    b、地面固碳：给料机向搅拌固碳反应装置中加入一定量的水，开始搅拌，并开始通过CO2气源从搅拌固碳反应装置底部注入CO2气体，待充填料浆流动性能达到泵送要求的最低限度后，停止搅拌并停止注入CO2；
    c、流态化充填：通过充填泵提供动力，将搅拌好的充填料浆通过地-井钻孔的充填管路输送至井下采出空间；
    d、井下固碳：待充填料浆充满井下采出空间后，开启CO2地-井注入系统，通过气体管路向井下充填料浆内部注入CO2，直至充填料浆固结，实现该矿采区井下采出空间的流态化固废充填处置与CO2封存。
  2. 如权利要求1所述的一种矿山固废流态化充填处置协同二氧化碳封存方法，其特征在于，步骤b中，所述的煤矸石破碎需满足充填料浆泵送要求，煤矸石粒径小于10mm，且2mm以下占比不低于1/3。
  3. 如权利要求1所述的一种矿山固废流态化充填处置协同二氧化碳封存方法，其特征在于，步骤b中，所述搅拌固碳反应装置中CO2与充填料浆搅拌反应时间根据充填料浆流动性能决定，由粘度自动测量仪监测。
  4. 如权利要求1所述的一种矿山固废流态化充填处置协同二氧化碳封存方法，其特征在于，步骤b中，所述煤矸石60-80wt％，添加剂占煤矸石5wt％，其余为水。
  5. 如权利要求1所述的一种矿山固废流态化充填处置协同二氧化碳封存方法，其特征在于，步骤d中，充填料浆物相状态可通过CO2注入压力和流量进行判定，当CO2注入压力急剧增加且流量不变时，则判定充填料浆已经固结，可以停止注入CO2。
  6. 如权利要求1所述的一种矿山固废流态化充填处置协同二氧化碳封存方法，其特征在于，所述添加剂包括粉煤灰、生石灰、镁渣粉，优选为镁渣粉和生石灰粉，用于增加固碳效果。
  7. 一种基于权利要求1所述一种矿山固废流态化充填处置协同二氧化碳封存方法的系统，具体为地面固碳-地井充填-井下固碳系统，布设在该采区中部对应的地面矸石山附近，包括顺次连接的给料机、搅拌固碳反应装置、充填泵和充填管路，所述给料机分别与所述研磨车间、水仓和各添加剂材料仓连接，破碎车间与研磨车间连接；
    充填管路深入到井下采出空间，充填管路上设有充填泵；在充填泵旁钻井至井下采出空间，井内安设有所述充填管路和气体管路；CO2气源连接有气体管路，所述气体管路分为两段管路，一段通入搅拌固碳反应装置，另一端深入到井下采出空间。
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