扩散受限的中间体富集增强CO2加氢合成重质烃: 半开放与开放系统对比

doi:10.1016/S1872-2067(26)65161-3

催化学报 ›› 2027, Vol. 92: 300-315.DOI: 10.1016/S1872-2067(26)65161-3

扩散受限的中间体富集增强CO₂加氢合成重质烃: 半开放与开放系统对比

郭立升^a^,¹^,^*(), 郑丽如^a^,¹, 张新宇^a, 王馨^a, 程杰^a, 蔡梦蝶^a, 刘娜^b^,^*(), 王凯歌^c^,^*(), 田友峰^d, 李杰^e, 孙松^a^,^*()

^a 安徽大学化学与化工学院, 安徽合肥 230601
^b 中南林业科技大学, 木本油料资源利用全国重点实验室, 湖南长沙 410004
^c 浙江大学, 能源清洁利用国家重点实验室, 浙江杭州 310027
^d 安徽中鼎密封件股份有限公司, 安徽宣城 341881
^e 扬州大学化学与材料学院, 江苏扬州 225002

收稿日期:2026-02-06 接受日期:2026-02-24 出版日期:2027-01-02 发布日期:2026-10-30
通讯作者: *电子信箱: lsguo@ahu.edu.cn (郭立升),
Liuna1912@163.com (刘娜),
kaigewang@zju.edu.cn (王凯歌),
suns@ustc.edu.cn (孙松).
作者简介:第一联系人：
¹共同第一作者.
基金资助:
国家自然科学基金(22102001);国家自然科学基金(22472001);木本油料资源利用国家重点实验室开放基金;浙江省重点研发计划(2025C01173);安徽省高校协同创新计划(GXXT-2023-009)

Enhanced CO₂ hydrogenation to heavy hydrocarbons through diffusion-limited intermediate enrichment: Semi-open vs. open systems

Lisheng Guo^a^,¹^,^*(), Liru Zheng^a^,¹, Xinyu Zhang^a, Xin Wang^a, Jie Cheng^a, Mengdie Cai^a, Na Liu^b^,^*(), Kaige Wang^c^,^*(), Youfeng Tian^d, Jie Li^e, Song Sun^a^,^*()

^a School of Chemistry and Chemical Engineering, Anhui University, Hefei 230601, Anhui, China
^b State Key Laboratory of Woody Oil Resources Utilization, Central South University of Forestry and Technology, Changsha 410004, Hunan, China
^c State Key Laboratory of Clean Energy Utilization, Zhejiang University, Hangzhou 310027, Zhejiang, China
^d Anhui Zhongding Sealing Parts Co., Ltd, Xuancheng 341881, Anhui, China
^e School of Chemistry and Materials, Yangzhou University, Yangzhou 225002, Jiangsu, China

Received:2026-02-06 Accepted:2026-02-24 Online:2027-01-02 Published:2026-10-30
Contact: *E-mail: lsguo@ahu.edu.cn (L. Guo),
Liuna1912@163.com (N. Liu),
kaigewang@zju.edu.cn (K. Wang),
suns@ustc.edu.cn (S. Sun).
About author:First author contact:
¹ Contributed equally to this work.
Author contributions
L. G., N. L., K. W., and S. S. directed the project. L. Z., X. Z., and X. W. carried out the experiments. M. C., N. L., J. C., J. L., and Y. T. assisted with characterization. L. G., and L. Z. drafted the manuscript. All authors discussed the results and commented on the manuscript.
Supported by:
National Natural Science Foundation of China(22102001);National Natural Science Foundation of China(22472001);Open Foundation of State Key Laboratory of Woody Oil Resources Utilization;Key R&D Program of Zhejiang(2025C01173);University Synergy Innovation Program of Anhui Province(GXXT-2023-009)

摘要/Abstract

摘要：

随着煤炭、石油等碳基资源的大量开发利用, 二氧化碳的大量排放引发了温室效应、海洋酸化等一系列环境问题. 在此背景下, 实现CO₂的资源化利用并定向转化为高附加值重质烃对推进“双碳”目标、构建碳循环体系具有重要意义. CO₂催化加氢是碳资源化利用的重要途径, 但传统催化体系存在重质烃选择性低、活性相易烧结、反应路径调控难等问题, 且多聚焦于广口开放非限域体系, 三维限域下双金属活性位点的研究十分匮乏. 通过纳米限域微环境调控多相催化反应路径, 成为提升CO₂转化效率与产物定向性的关键突破口, 开发兼具高活性、高选择性与高稳定性的催化体系已成为该领域的研究重点.

本文以调控纳米限域微环境、优化CO₂加氢反应路径为设计思路. 采用溶剂介导的聚合诱导自组装策略, 制备了孔径可调(0-100 nm)的半开放多孔碳球载体(MPCS_x), 并通过限域CoFe合金构筑了Fe₁₀Co₂@MPCS_x系列催化剂. 系统研究了半开放限域环境对CO₂加氢制重质烃性能的调控规律, 并结合有限元模拟与原位漫反射红外光谱技术, 揭示了限域调控的微观作用机制. X-射线衍射、透射电镜-能量散射谱、X-射线吸收光谱等多种表征手段证实了CoFe合金的成功合成与均匀分散. 通过对比不同限域孔径催化剂的结构特性与性能, 发现孔径为14 nm的Fe₁₀Co₂@MPCS₁₄性能最优, 其CO₂转化率为24.7%, C₅₊产率较开放体系提升约2倍, 且在100 h连续测试中性能稳定, 未观察到明显金属颗粒烧结现象. 研究机理表明, 14 nm的半开放孔域在活性位点周围形成了独特的“富集-扩散”动态平衡, 显著提升了CO₂/H₂的局部浓度, 并且稳定了HCOO^*, HCO₃^*, CO₃^*等关键C₁中间体, 延长了表面停留时间, 从而极大促进了C-C偶联. 反之, 孔径过小会导致传质阻力增加, 产物堆积并竞争性占据活性位点. 孔径过大则限域效应减弱, 中间体易脱附, 导致重质烃选择性下降.

综上, 本研究阐明了纳米限域微环境对CO₂加氢反应路径的调控规律, 不仅为CO₂加氢定向转化为高附加值烃类提供了设计思路, 也为通过空间限域调控多相催化反应的选择性建立了范例, 可为CO₂加氢催化剂的后续开发提供理论支撑.

关键词: CO₂加氢, 纳米孔域, 半开放系统, 钴铁合金, 自组装

Abstract:

Precisely tuning the nanoconfined microenvironment to optimize heterogeneous catalytic reaction pathways represents one of the critical challenges for achieving efficient and directional CO₂ conversion. In this study, we systematically investigated the impact of confinement dimensions on CO₂ hydrogenation performance by constructing a series of semi-open porous carbon spheres (MPCS_x) with tunable pore sizes (x = 0, 10, 14, 30, 100 nm) supported CoFe alloy catalysts. Experimental results revealed that the catalyst Fe₁₀Co₂@MPCS₁₄ with a pore size of 14 nm exhibits C₅₊ selectivity was twice that of open systems. To gain deeper insights into the structural origins of this optimal performance, we further elucidated the underlying microscopic mechanisms by combining Finite element method simulation with in-situ diffuse reflectance Fourier transform infrared spectroscopy. The 14 nm semi-open structure established a unique “enrichment-diffusion” dynamic equilibrium around the active sites, which not only substantially enhanced the local concentrations of CO₂/H₂ but also effectively stabilized key C1 intermediates such as HCOO^*, HCO₃^*, and CO₃^*. thereby promoting C-C coupling and carbon chain growth. This work provides important mechanistic insights into the regulation of selectivity in heterogeneous catalytic reactions through spatial confinement microenvironment modulation.

Key words: CO₂ hydrogenation, Nanopore domain, Semi-open system, CoFe alloy, Self-assembly

郭立升, 郑丽如, 张新宇, 王馨, 程杰, 蔡梦蝶, 刘娜, 王凯歌, 田友峰, 李杰, 孙松. 扩散受限的中间体富集增强CO₂加氢合成重质烃: 半开放与开放系统对比[J]. 催化学报, 2027, 92: 300-315.

Lisheng Guo, Liru Zheng, Xinyu Zhang, Xin Wang, Jie Cheng, Mengdie Cai, Na Liu, Kaige Wang, Youfeng Tian, Jie Li, Song Sun. Enhanced CO₂ hydrogenation to heavy hydrocarbons through diffusion-limited intermediate enrichment: Semi-open vs. open systems[J]. Chinese Journal of Catalysis, 2027, 92: 300-315.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(26)65161-3

https://www.cjcatal.com/CN/Y2027/V92/I1/300

图/表 6

Fig. 1. FEMS results of the concentration and distribution of CO2 and C1-C3 species on Fe10Co2@MPCS0 (A), Fe10Co2@MPCS10 (B), Fe10Co2@MPCS14 (C), and Fe10Co2@MPCS30 (D).

Fig. 2. (A) Schematic diagram of solvent-mediated PISA strategy for synthesizing porous carbon spheres and subsequent active metal site anchoring. (B-K) SEM images of MPCS0, MPCS10, MPCS14, MPCS30 and MPCS100.

Fig. 3. (A,B) SEM images of fresh Fe10Co2@MPCS14 and Fe10Co2@MPCS0. TEM image (C) and corresponding EDS elemental maps (D-H) of the fresh Fe10Co2@MPCS14. (I) XRD patterns of the fresh catalysts. (J) XRD patterns of the spent catalysts. (K) Raman spectra of the spent catalysts. Fe 2p (L) and Co 2p (M) XPS spectra of spent catalysts. (N) 57Fe Mössbauer spectra of spent MPCS0 and MPCS14. For clarity, the Fe10Co2@MPCSx samples are denoted simply as MPCSx (where x = 0, 10, 14, 30, 100). Unless specified otherwise, MPCSx refers to the Fe-based catalysts supported on porous spherical carbon.

Fig. 4. Coordination environment analysis of spent catalyst. Normalized XANES spectra of the spent catalyst at Fe K-edge (A) and Co K-edge (C). k3-weighted Fourier transformed EXAFS spectra of spent catalyst (B) and (D). (E-H) Wavelet transform spectra of the catalysts.

Fig. 5. (A) STY values of C5+ over different catalysts. (B) Catalytic performances of the Fe10Co2@MPCSx catalysts. (C) Chain growth factor α of different catalysts. (D,E) Catalytic performances over different catalysts. (F) The catalytic performance of the Fe10Co2@MPCS14 catalyst under different reaction temperatures (with all other conditions kept consistent). (G) The long-term experimental performance plot of the Fe10Co2@MPCS14 catalyst over 100 h of reaction. Reaction conditions: weight of catalyst = 0.25 g, 2.0 MPa, 320 °C, 4800 mL/(g·h), H2/CO2 = 3, TOS = 100 h. To simplify the presentation, the Fe10Co2@MPCSx shown in the Fig. is uniformly named as MPCSx (where x = 0, 10, 14, 30, 100). Unless otherwise specified, MPCSx consistently refers in this Fig. to the iron catalysts supported on porous spherical carbon.

Fig. 6. The in-situ DRIFTS spectra of Fe10Co2@MPCS0 (A) and Fe10Co2@MPCS14 (B). (C) Proposed reaction pathways for the directional synthesis of different hydrocarbons from CO2 hydrogenation over different catalysts.

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扩散受限的中间体富集增强CO₂加氢合成重质烃: 半开放与开放系统对比

Enhanced CO₂ hydrogenation to heavy hydrocarbons through diffusion-limited intermediate enrichment: Semi-open vs. open systems

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