Yao Shuo, Du Wei, Chen Changshuai, Pan Yinhai, Meng Weijie, Zhang Zhen, Zhang Haijun, Tian Quanzhi
State Key Laboratory of Coking Coal Resources Green Exploitation, China University of Mining and Technology, Xuzhou 221116, China.
National Engineering Research Center of Coal Preparation and Purification, China University of Mining and Technology, Xuzhou 221116, China.
ACS Omega. 2025 May 25;10(22):22769-22778. doi: 10.1021/acsomega.4c11336. eCollection 2025 Jun 10.
Gasification slag has been viewed as a secondary resource for preparing various high-value-added materials with enormous potential. Residual silicon in gasification slag can be used to prepare mesoporous silica materials, such as MCM-41. However, it is challenging to avoid doping impurities from gasification slag, including metal impurities, such as Fe, Mg, and Ca, in the synthesis of MCM-41. This study used the supernatant of leached gasification slag to synthesize MCM-41 with a controllable Si/Al atomic ratio, and MCM-41 synthesized from chemical agents was used as a control group. In addition, XRD characterized two kinds of mesoporous molecular sieves: SEM-EDS, N adsorption/desorption isotherm, Al, and Si solid-state NMR spectroscopy. It has been found that the crystallinity of the MCM-41 crystal structure decreased due to the doping of metal impurities. No octahedral aluminum was observed in MCM-41 synthesized by gasification slag, which may be related to the change of charge pairing cations (partial substitution of Na by Ca) in the aluminosilicate framework of MCM-41. On the other hand, the specific surface area, pore size, and pore volume of MCM-41 synthesized from gasification slag were affected by metal impurities. This can be attributable to partial mesopores blocked by metal oxide nanoparticles. This study provides a new understanding of the structural change of molecular sieve MCM-41 due to the metal impurities of gasification slag. These results also provided insight into the efficient recycling of gasification slag and the production of high-value-added materials from solid waste.
气化炉渣被视为一种具有巨大潜力的制备各种高附加值材料的二次资源。气化炉渣中的残余硅可用于制备介孔二氧化硅材料,如MCM-41。然而,在合成MCM-41时,要避免掺杂来自气化炉渣的杂质(包括金属杂质,如铁、镁和钙)具有挑战性。本研究使用浸出气化炉渣的上清液合成具有可控硅/铝原子比的MCM-41,并将由化学试剂合成的MCM-41用作对照组。此外,采用X射线衍射仪(XRD)对两种介孔分子筛进行表征:扫描电子显微镜-能谱仪(SEM-EDS)、氮气吸附/脱附等温线、铝和硅的固态核磁共振光谱。研究发现,由于金属杂质的掺杂,MCM-41晶体结构的结晶度降低。在由气化炉渣合成的MCM-41中未观察到八面体铝,这可能与MCM-41硅铝酸盐骨架中电荷配对阳离子的变化(钙部分取代钠)有关。另一方面,由气化炉渣合成的MCM-41的比表面积、孔径和孔体积受到金属杂质的影响。这可归因于部分介孔被金属氧化物纳米颗粒堵塞。本研究为气化炉渣金属杂质导致分子筛MCM-41结构变化提供了新的认识。这些结果也为气化炉渣的高效回收利用以及从固体废物中生产高附加值材料提供了见解。