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1.中国科学院 大连化学物理研究所 低碳催化技术国家工程研究中心,辽宁 大连 116023
2.中国科学院 大连化学物理研究所 能源催化转化全国重点实验室,辽宁 大连 116023
3.中国科学院大学,北京 100049
刘一鸣(2003—),硕士研究生,研究方向为分子筛催化,E-mail:liuyiming@dicp.ac.cn。
郅玉春(1984—),博士,研究员,研究方向为分子筛催化与C1化学,E-mail:yuchunzhi@dicp.ac.cn;
刘中民(1964—),博士,研究员,中国工程院院士,研究方向为应用催化,E-mail:liuzm@dicp.ac.cn。
收稿:2026-06-01,
修回:2026-06-18,
网络首发:2026-07-28,
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刘一鸣,郅玉春,魏迎旭等.分子筛催化剂积炭失活与积炭调控策略[J].低碳化学与化工,
LIU Yiming,ZHI Yuchun,WEI Yingxu,et al.Coke-induced deactivation and coke regulation strategies of zeolite catalysts[J].Low-Carbon Chemistry and Chemical Engineering,
刘一鸣,郅玉春,魏迎旭等.分子筛催化剂积炭失活与积炭调控策略[J].低碳化学与化工, DOI:10.12434/j.issn.2097-2547.20260249.
LIU Yiming,ZHI Yuchun,WEI Yingxu,et al.Coke-induced deactivation and coke regulation strategies of zeolite catalysts[J].Low-Carbon Chemistry and Chemical Engineering, DOI:10.12434/j.issn.2097-2547.20260249.
积炭长期被视为导致分子筛催化剂失活的主要原因之一,工业上常需要对失活的分子筛催化剂采用空气烧炭的方式进行再生。通过梳理积炭领域的研究现状与面临的难题,发现积炭物种形态、结构与演变易受多种因素协同影响,并且积炭对反应过程的作用也不再被简单归结为单一的消极效应。一方面,积炭的过度沉积会覆盖催化剂表面活性位点,阻碍分子扩散,从而导致催化剂失活。另一方面,适量积炭可以在催化剂合成、反应路径调控等方面起到积极作用。随着对积炭认识的加深,积炭调控的整体思路正在从单纯的“被动去除”转向“主动调控”。具体而言,调变反应气氛可以显著延长催化剂寿命及优化产物分布,而预积炭、不完全再生等策略可在提高低碳烯烃选择性的同时降低CO
2
排放量。本研究可为实现工业催化过程中高产物选择性、低能耗和绿色可持续发展的目标提供参考。
Coke has long been regarded as a primary cause of deactivation of zeolite catalysts and it is often necessary to regenerate deactivation zeolite catalysts by air burn-off in industry. By reviewing the current research status and challenges of coke
it is found that the morphologies
structures and evolution are synergistically influenced by multiple factors. The role of coke in reaction processes can no longer be simply reduced to a purely negative effect. On the one hand
excessive deposition of coke can cover active sites on the catalyst surface and hinder molecular diffusion
leading to deactivation of catalysts. On the other hand
a moderate amount of coke can play a positive role in catalyst synthesis and the regulation of reaction pathways. With the deepening of understanding of coke
the coke regulation strategies are shifting from “passive removal” to “active regulation”. Specifically
adjusting the reaction atmospheres can significantly prolong catalysts’ lifetimes and optimize product distributions
while strategies like pre-coking and partial regeneration can increase the light olefin selectivity and reduce CO
2
emissions. This study can provide reference for achieving the goals of high product selectivities
low energy consumptions and green sustainable development in industrial catalysis.
BORODINA E , KAMALUDDIN H S H , MEIRER F , et al . Influence of the reaction temperature on the nature of the active and deactivating species during methanol-to-olefins conversion over H-SAPO-34 [J ] . ACS Catalysis , 2017 , 7 ( 8 ): 5268 - 5281 .
SHEN D Y , BAI Y , JIANG P Y , et al . Interfacial engineering of silica-anchored Ni nanoclusters for stable and efficient dry reforming of methane [J ] . Carbon and Hydrogen , 2025 , 27 ( 3 ): 328 - 334 .
MA J M , HE X Y , ZENG Y T , et al . Ni‐CeO 2 /AlSBA-15 with high H 2 production efficiency and potent coking resistance in methane steam reforming (SRM): Study the synergistic effects of Ni dispersion, redox property and surface alkalinity [J ] . Carbon and Hydrogen , 2025 , 27 ( 4 ): 495 - 506 .
WANG N , ZHI Y C , WEI Y X , et al . Molecular elucidating of an unusual growth mechanism for polycyclic aromatic hydrocarbons in confined space [J ] . Nature Communications , 2020 , 11 ( 1 ): 1079 .
HE Y J , ZHENG Y , CHEN Y Y , et al . Molecular routes of coke species on HZSM-5 zeolite with atomic-resolution structural identification [J ] . Journal of the American Chemical Society , 2025 , 147 ( 45 ): 41379 - 41389 .
LIN S F , ZHI Y C , ZHANG W N , et al . Hydrogen transfer reaction contributes to the dynamic evolution of zeolite-catalyzed methanol and dimethyl ether conversions: Insight into formaldehyde [J ] . Chinese Journal of Catalysis , 2023 , 46 : 11 - 27 .
赫英俊 , 陈祎瑶 , 林杉帆 , 等 . 甲醛对HZSM-5分子筛催化甲苯和苯转化反应积炭失活的影响 [J ] . 低碳化学与化工 , 2026 , 51 ( 2 ): 59 - 65 .
HE Y J , CHEN Y Y , LIN S F , et al . Effect of formaldehyde on coke-induced deactivation of HZSM-5 zeolite during catalytic conversion of toluene and benzene [J ] . Low-Carbon Chemistry and Chemical Engineering , 2026 , 51 ( 2 ): 59 - 65 .
VOGT E T C , FU D L , WECKHUYSEN B M . Carbon deposit analysis in catalyst deactivation, regeneration, and rejuvenation [J ] . Angewandte Chemie International Edition , 2023 , 62 ( 29 ): e202300319 .
张琴 , 陈祎瑶 , 牛晶 , 等 . 甲醇制烯烃(MTO)反应积炭演化和再生研究进展 [J ] . 化学学报 , 2026 , 84 ( 6 ): 987 - 1002 .
ZHANG Q , CHEN Y Y , NIU J , et al . Recent progress on coking and regeneration in the methanol-to-olefins (MTO) reaction [J ] . Acta Chimica Sinica , 2026 , 84 ( 6 ): 987 - 1002 .
HE Y J , CHEN Y Y , ZHANG W N , et al . Molecular elucidation of the deactivation mechanism of HZSM-22 zeolite-catalyzed methanol-to-hydrocarbons (MTH) reaction [J ] . Journal of Energy Chemistry , 2026 , 113 : 237 - 245 .
GUISNET M , COSTA L , RIBEIRO F R . Prevention of zeolite deactivation by coking [J ] . Journal of Molecular Catalysis A: Chemical , 2009 , 305 ( 1/2 ): 69 - 83 .
SCHULZ H . “Coking” of zeolites during methanol conversion: Basic reactions of the MTO-, MTP- and MTG processes [J ] . Catalysis Today , 2010 , 154 ( 3/4 ): 183 - 194 .
YU Y H , YU L L , JI Y X , et al . The Investigation of the deactivation of the metal-modified ZSM-5 zeolites for the catalytic dehydration of glycerol [J/OL ] . Carbon and Hydrogen : 1 - 14 [ 2026-06-17 ] . DOI: 10.1002/cbh2.70067 http://dx.doi.org/10.1002/cbh2.70067 .
WEI Y X , LI J Z , YUAN C Y , et al . Generation of diamondoid hydrocarbons as confined compounds in SAPO-34 catalyst in the conversion of methanol [J/OL ] . Chemical Communications , 2012 , 48 ( 25 ): 3082 - 3084 .
HOU J X , CHEN Y Y , LIU Y M , et al . Multiscale spatiotemporal heterogeneity of zeolite-catalyzed methanol-to-hydrocarbons (MTH) reaction [J ] . National Science Review , 2026 , 13 ( 12 ): nwag255 .
LIN S F , ZHI Y C , LIU Z Q , et al . Multiscale dynamical cross-talk in zeolite-catalyzed methanol and dimethyl ether conversions [J ] . National Science Review , 2022 , 9 ( 9 ): nwac151 .
谢宜委 , 彭诗超 , 李贵达 , 等 . 甲醇制烯烃过程中H-ZSM-5分子筛积碳对分子筛表面传质阻力的影响 [J ] . 中国科学: 化学 , 2024 , 54 ( 11 ): 2253 - 2262 .
XIE Y W , PENG S C , LI G D , et al . Effect of coke on surface barriers over H-ZSM-5 zeolites duringmethanol-to-olefins [J ] . Acta Chimica Sinica , 2024 , 54 ( 11 ): 2253 - 2262 .
ZHOU J B , ZHI Y C , ZHANG J L , et al . Presituated “coke”- determined mechanistic route for ethene formation in the methanol-to-olefins process on SAPO-34 catalyst [J ] . Journal of Catalysis , 2019 , 377 : 153 - 162 .
ZHU Z W , LI W J , ZHANG H X , et al . One-pot synthesis of metal-containing SSZ-13 nanocrystals by interzeolite transformation of spent FCC catalysts for the methanol-to-olefins reaction [J ] . Applied Catalysis B: Environment and Energy , 2025 , 365 : 124900 .
LI D B , LIU Z K , LIU Y , et al . The role of coke as the crystal structure protective agent in the synthesis of CHA zeolites from spent MFI [J ] . Catalysis Letters , 2019 , 150 ( 6 ): 1741 - 1748 .
ZHANG C W , WU X Q , ZHANG Y N , et al . Water-controlled coking dynamics during high-pressure methanol-to-olefins reaction over SAPO-34 [J ] . ACS Catalysis , 2025 , 15 ( 3 ): 1553 - 1562 .
ZHAO X B , LI J Z , TIAN P , et al . Achieving a superlong lifetime in the zeolite-catalyzed MTO reaction under high pressure: Synergistic effect of hydrogen and water [J ] . ACS Catalysis , 2019 , 9 ( 4 ): 3017 - 3025 .
WANG C , YANG L , GAO M B , et al . Directional construction of active naphthalenic species within SAPO-34 crystals toward more efficient methanol-to-olefin conversion [J ] . Journal of the American Chemical Society , 2022 , 144 ( 46 ): 21408 - 21416 .
ZHOU J B , GAO M B , ZHANG J L , et al . Directed transforming of coke to active intermediates in methanol-to-olefins catalyst to boost light olefins selectivity [J ] . Nature Communications , 2021 , 12 ( 1 ): 17 .
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