由甲烷化变为链增长: Co-ZrOx催化剂上钠诱导的分叉机理

doi:10.1016/S1872-2067(26)65033-4

催化学报 ›› 2026, Vol. 85: 394-411.DOI: 10.1016/S1872-2067(26)65033-4

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由甲烷化变为链增长: Co-ZrO_x催化剂上钠诱导的分叉机理

Syeda Sidra Bibi^a, Sheraz Ahmed^b, Heuntae Jo^b, Jaehoon Kim^a^,^b^,^c^,^d()

^a 成均馆大学化学工程学院, 京畿道水原市, 韩国
^b 成均馆大学机械工程学院, 京畿道水原市, 韩国
^c 成均馆大学纳米技术高级研究所(SAINT), 京畿道水原市, 韩国
^d 成均馆大学低碳能源工程系, 京畿道水原市, 韩国

收稿日期:2025-10-14 接受日期:2025-12-09 出版日期:2026-06-18 发布日期:2026-05-18
通讯作者: *电子信箱: jaehoonkim@skku.edu (J. Kim).

Turning methanation into chain growth: Na-induced mechanistic bifurcation on Co-ZrO_x catalyst

Syeda Sidra Bibi^a, Sheraz Ahmed^b, Heuntae Jo^b, Jaehoon Kim^a^,^b^,^c^,^d()

^a School of Chemical Engineering, Sungkyunkwan University, Suwon, Gyeonggi-do 16419, Republic of Korea
^b School of Mechanical Engineering, Sungkyunkwan University, Suwon, Gyeonggi-do 16419, Republic of Korea
^c SKKU Advanced Institute of Nano Technology (SAINT), Suwon, Gyeonggi-do 16419, Republic of Korea
^d Department of Low-Carbon Energy Engineering, Sungkyunkwan University, Suwon, Gyeonggi-do 16419, Republic of Korea

Received:2025-10-14 Accepted:2025-12-09 Online:2026-06-18 Published:2026-05-18
Contact: *E-mail: jaehoonkim@skku.edu (J. Kim).
About author:CRediT authorship contribution statement
Syeda Sidra Bibi: Conceptualization, methodology, formal analysis, data curation, and writing - original draft. Sheraz Ahmed: Methodology, Validation, formal analysis, and investigation. Heuntae Jo: Methodology, formal analysis, and investigation. Jaehoon Kim: Supervision, project administration, resources, writing - review and editing, and funding acquisition.

摘要/Abstract

摘要：

二氧化碳直接加氢制备长链碳氢化合物是碳中和燃料生产的重要技术路线, 但同时实现高选择性和高催化剂稳定性仍面临巨大挑战. 本文系统地研究了碱金属(Li, Na, K)对钴-氧化锆催化剂的促进作用, 揭示碱金属种类直接决定催化剂的氧化还原稳定性与产物分布. 无碱助剂和K促进的催化剂在二氧化碳加氢过程中会发生严重的表面再氧化, 抑制C-C偶联并主导甲烷的形成; 而Na促进的催化剂保留了金属Co⁰相, 并在与工业相近的反应条件下实现了优异的C₅₊烃选择性(39.4%)和收率(22.4%). 机理研究表明, Na可特异性促进羟基和甲酰基中间体的形成, 有利于C-C键的形成, 同时避免了在Li体系中出现的碳酸盐钝化的现象. 本文首次发现了Na在稳定催化剂活性位点和选择反应路径方面的作用, 为设计稳定性好、选择性高的钴基催化剂提供了一种合理的策略, 用于将二氧化碳转化为可用作可持续运输燃料的液态烃.

关键词: CO₂加氢, 碱金属促进作用, 钴的氧化还原性能, C₅₊烃类

Abstract:

Direct hydrogenation of CO₂ to long-chain hydrocarbons represents a promising route for carbon-neutral fuel production, yet achieving high selectivity and catalyst stability remains a formidable challenge. In this study, we systematically investigate the promotional effect of alkali metals (Li, Na, K) on cobalt-zirconia catalysts, revealing that the nature of the alkali promoter governs both redox stability and product distribution. While unpromoted and K-promoted catalysts undergo extensive surface reoxidation during CO₂ hydrogenation, suppressing C-C coupling and favoring methane formation, the Na-promoted catalyst preserves the metallic Co⁰ phase and achieves exceptional C₅₊ hydrocarbon selectivity (39.4%) and yield (22.4%) under industrially relevant conditions. Mechanistic investigations reveal that Na uniquely facilitates the formation of hydroxyl and formyl intermediates conducive to C-C bond formation, while avoiding carbonate passivation observed in the Li-promoted catalyst. This work highlights a previously unrecognized role of Na in simultaneously stabilizing active sites and directing reaction pathways, offering a rational strategy for designing robust, selective cobalt-based catalysts for CO₂ conversion to liquid hydrocarbons that can be used as sustainable transportation fuel.

Key words: CO₂ hydrogenation, Alkali metal -promotion, Cobalt redox behavior, C₅₊ hydrocarbons

Syeda Sidra Bibi, Sheraz Ahmed, Heuntae Jo, Jaehoon Kim. 由甲烷化变为链增长: Co-ZrO_x催化剂上钠诱导的分叉机理[J]. 催化学报, 2026, 85: 394-411.

Syeda Sidra Bibi, Sheraz Ahmed, Heuntae Jo, Jaehoon Kim. Turning methanation into chain growth: Na-induced mechanistic bifurcation on Co-ZrO_x catalyst[J]. Chinese Journal of Catalysis, 2026, 85: 394-411.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(26)65033-4

https://www.cjcatal.com/CN/Y2026/V85/I6/394

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Fig. 1. Catalytic CO2 conversion of the catalysts. (a) Catalytic performance, hydrocarbon product selectivity (excluding CO), and C5+ yield of various CZOx-8 with different alkali metals. (b) Catalytic performance, hydrocarbon product selectivity (excluding CO), and C5+ yield of various CZOx-8 catalysts having different Na loadings. (c) Long-term stability of Na1.8-CZOx-8 catalyst. Reaction conditions: 270 °C, 4.0 MPa, a H2/CO2 ratio of 3, and GHSV of 4000 mL g-1 h-1 for 30 h.

Fig. 2. (a) XRD patterns of spent unpromoted and alkali-promoted CZOx-8 catalyst. (b) Enlarged XRD pattern indicating the formation of Li2CO3. Reaction conditions: 270 °C, 4.0 MPa, a H2/CO2 ratio of 3, and GHSV of 4000 mL g-1 h-1 for 30 h.

Fig. 3. XAS analysis of reduced and spent unpromoted and alkali-promoted CZOx-8 catalysts. Normalized Co K-edge XANES spectra of the reduced (a) and spent (c) catalysts. k3-weighted Fourier transforms of normalized Co K-edge EXAFS spectra (κ3 χ(k)) for the reduced (b) and spent (d) catalysts. (e) Linear combination fitting data of reduced and spent catalysts. Reduction conditions: 350 °C for 6 h at a flow of 50 mL min-1 H2 and 4.0 MPa. Reaction conditions: 270 °C, 4.0 MPa, a H2/CO2 ratio of 3, and GHSV of 4000 mL g-1 h-1 for 30 h.

Fig. 4. Raman spectra of the spent unpromoted and alkali-promoted catalysts. Reaction conditions: 270 °C, 4.0 MPa, a H2/CO2 ratio of 3, and GHSV of 4000 mL g-1 h-1 for 30 h.

Fig. 5. XPS profiles of the spent unpromoted and alkali-promoted catalysts in the C 1s (a), O 1s (b), Zr 3d (c), and Co 2p (d) regions. Reaction conditions: 270 °C, 4.0 MPa, a H2/CO2 ratio of 3, and GHSV of 4000 mL g-1 h-1 for 30 h.

Fig. 6. HR-TEM and corresponding EDX images of the calcined (a)-(d), reduced (e)-(h), and spent (i)-(t) unpromoted and alkali-promoted catalysts. Calcination conditions: 330 °C and 100 mL min-1 air flow for 3 h. Reduction conditions: 350 °C and 50 mL min-1 H2 flow for 6 h under 4.0 MPa. Reaction conditions: 270 °C, 4.0 MPa, a H2/CO2 ratio of 3, and GHSV of 4000 mL g-1 h-1 for 30 h.

Fig. 7. H2-TPR (a), H2-TPD (b), and CO2-TPD (c) profiles of the unpromoted and alkali-promoted catalysts. Amount of H2 consumption (d), H2 desorption (e), and CO2 desorption (f) in mmol g-1 of the unpromoted and alkali-promoted catalysts. Calcination conditions: 330 °C and 100 mL min-1 air flow for 3 h. Reduction conditions: 350 °C and 50 mL min-1 H2 flow for 6 h under 4.0 MPa.

Fig. 8. In-situ CO2 hydrogenation DRIFT profiles of BC-CZOx-8 (a), Li1.8-CZOx-8 (b), Na1.8-CZOx-8 (c), and K1.8-CZOx-8 (d). CO2 and H2 were injected into the cell at flow rates of 16.7 and 50 mL min−1, respectively, under the conditions of 3.0 MPa and 270 °C for 2 h. Pretreatment reduction conditions: 350 °C (ramping rate of 2.5 °C min-1), 3.0 MPa, 50 mL min-1 H2 flow for 6 h. (e) Proposed reaction mechanism on unpromoted and alkali-promoted CZOx-8 catalyst.

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由甲烷化变为链增长: Co-ZrO_x催化剂上钠诱导的分叉机理

Turning methanation into chain growth: Na-induced mechanistic bifurcation on Co-ZrO_x catalyst

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由甲烷化变为链增长: Co-ZrOx催化剂上钠诱导的分叉机理

Turning methanation into chain growth: Na-induced mechanistic bifurcation on Co-ZrOx catalyst

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由甲烷化变为链增长: Co-ZrO_x催化剂上钠诱导的分叉机理

Turning methanation into chain growth: Na-induced mechanistic bifurcation on Co-ZrO_x catalyst