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1.宁夏大学 化学化工学院 省部共建煤炭高效利用与绿色化工国家重点实验室,宁夏 银川 750021
2.宁夏计量质量检验检测研究院, 国家煤及煤化工产品质量检验检测中心(宁夏), 宁夏 银川 750200
3.富山大学 工学部 应用化学系,富山 930-8555
4.聊城市特种设备检验研究院,山东 聊城 252000
贾菲(1999—),硕士研究生,研究方向为CO2催化转化,E-mail:2485204147@qq.com。
李海鹏(1999—),硕士,研究方向为CO2催化转化,E-mail:lihp_nxu@163.com;
高新华(1990—),博士,研究员,研究方向为碳一化学,E-mail:gxh@nxu.edu.cn。
收稿:2025-11-25,
修回:2026-01-05,
网络首发:2026-05-07,
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贾菲,李海鹏,王家琪等.SSZ-13分子筛硅铝比调控及其甲醇选择性制烯烃催化性能研究[J].低碳化学与化工,
JIA Fei,LI Haipeng,WANG Jiaqi,et al.Study on regulation of silica-alumina ratios of SSZ-13 zeolites and their catalytic performances for methanol to olefins reaction[J].Low-Carbon Chemistry and Chemical Engineering,
贾菲,李海鹏,王家琪等.SSZ-13分子筛硅铝比调控及其甲醇选择性制烯烃催化性能研究[J].低碳化学与化工, DOI:10.12434/j.issn.2097-2547.20250450.
JIA Fei,LI Haipeng,WANG Jiaqi,et al.Study on regulation of silica-alumina ratios of SSZ-13 zeolites and their catalytic performances for methanol to olefins reaction[J].Low-Carbon Chemistry and Chemical Engineering, DOI:10.12434/j.issn.2097-2547.20250450.
甲醇制烯烃(MTO)反应作为一条非石油路线生产低碳烯烃(C
2
=~C
4
=)备受关注。具有CHA拓扑结构的SSZ-13分子筛因其孔道结构有序和Brønsted酸位点丰富,在MTO反应中展现出优异的催化潜力。然而,强Brønsted酸位点导致SSZ-13分子筛在反应过程中易积炭失活。采用脱铝改性策略,制备了不同浓度HNO
3
改性SSZ-13分子筛,通过XRD、SEM和N
2
物理吸/脱附等技术对HNO
3
改性前后SSZ-13分子筛进行了表征,并在固定床反应器上对其进行了MTO催化性能评价。结果表明,在350 °C、0.1 MPa下,改性前后SSZ-13分子筛的甲醇初始转化率接近100%,低碳烯烃选择性超过91.0%。随着HNO
3
溶液浓度从0.5 mol/L升高至5.0 mol/L,SSZ-13分子筛的硅铝比(
n
(SiO
2
)/
n
(Al
2
O
3
))从16(SSZ-13-0.5H)升高至21(SSZ-13-5.0H)。在MTO反应中,改性后的SSZ-13-5.0H的催化寿命延长至8.0 h。本研究可为延长SSZ-13分子筛在MTO反应中的催化寿命提供理论支撑。
The methanol to olefins (MTO) reaction has attracted significant attention as a non-petroleum route for producing light olefins (C
2
=~C
4
=). SSZ-13 zeolites with CHA topology exhibit excellent catalytic potential in the MTO reaction due to their well-ordered pore structures and abundant Brønsted acid sites. However
the strong Brønsted acid sites leads to the inactivation of carbon deposition of SSZ-13 zeolites during the reaction. By dealuminization and modification strategy
SSZ-13 zeolites modified by HNO
3
with different concentrations were prepared. The SSZ-13 zeolites before and after modification were characterized by XRD
SEM
N
2
physical adsorption/desorption
etc.
and the catalytic performances for MTO of the SSZ-13 zeolites were evaluated on a fixed-bed reactor. The results show that under conditions of 350 ℃ and 0.1 MPa
initial methanol conversion rates of SSZ-13 zeolites before and after modification are close to 100% and the selectivities of low-carbon olefins exceed 91.0%. As the concentration of the HNO
3
solution increases from 0.5 mol/L to 5.0 mol/L
the silica-alumina ratio (
n
(SiO
2
)/
n
(Al
2
O
3
)) increases from 16 (SSZ-13-0.5H) to 21 (SSZ-13-5.0H). The catalytic lifetime of SSZ-13-5.0H after modification is extended to 8.0 h in the MTO reaction. This study can provide theoretical support for achieving long catalytic lifetime of SSZ-13 zeolites in MTO reactions.
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