扩散-酸性协同效应调控ZnZrOx/SAPO-34串联催化剂实现高选择性CO2加氢制丙烯

doi:10.1016/S1872-2067(26)65189-3

催化学报 ›› 2026, Vol. 90: 145-157.DOI: 10.1016/S1872-2067(26)65189-3

扩散-酸性协同效应调控ZnZrO_x/SAPO-34串联催化剂实现高选择性CO₂加氢制丙烯

陈栋航^a, 刘俊辰^a, 邓威^b, 高彪^a, 王逸夫^a, 渡邊源規^c, 石原逹己^c, 郭利民^a^,^d^,^e^,^*()

^a 华中科技大学环境科学与工程学院, 绿色能源工业研究中心, 湖北武汉 430074, 中国
^b 江汉大学光电材料与技术学院, 湖北武汉 430056, 中国
^c 九州大学碳中和能源国际研究所, 福冈, 日本
^d 华中科技大学长江流域多介质污染协同控制湖北省重点实验室, 湖北武汉 430074, 中国
^e 朱拉隆功大学理学院化学技术系, 曼谷, 泰国

收稿日期:2026-01-18 接受日期:2026-03-30 出版日期:2026-11-18 发布日期:2026-09-09
通讯作者: *电子信箱: lmguo@hust.edu.cn (郭利民).
基金资助:
国家自然科学基金(22378152);国家自然科学基金(21878116);湖北省科技研究计划(2025CSA138);华中科技大学交叉研究计划(2024JCYJ018)

Diffusion-acidity cooperative effect in ZnZrO_x/SAPO-34 tandem catalysts for enhanced CO₂-to-propylene conversion

Donghang Chen^a, Junchen Liu^a, Wei Deng^b, Biao Gao^a, Yifu Wang^a, Motonori Watanabe^c, Tatsumi Ishihara^c, Limin Guo^a^,^d^,^e^,^*()

^a Green Energy Industry Research Centre, School of Environmental Science and Engineering, Huazhong University of Science and Technology, Wuhan 430074, Hubei, China
^b School of Optoelectronic Materials and Technology, Jianghan University, Wuhan 430056, Hubei, China
^c International Institute for Carbon-Neutral Energy Research, Kyushu University, Fukuoka 8190395, Japan
^d Hubei Key Laboratory of Multi-media Pollution Cooperative Control in Yangtze Basin, Huazhong University of Science and Technology, Wuhan 430074, Hubei, China
^e Department of Chemical Technology, Faculty of Science, Chulalongkorn University, Bangkok 10330, Thailand

Received:2026-01-18 Accepted:2026-03-30 Online:2026-11-18 Published:2026-09-09
Contact: *E-mail:lmguo@hust.edu.cn(L. Guo).
Supported by:
National Natural Science Foundation of China(22378152);National Natural Science Foundation of China(21878116);Hubei Provincial Science and Technology Research Project(2025CSA138);Interdisciplinary Research Program of Huazhong University of Science and Technology(2024JCYJ018)

摘要/Abstract

摘要：

在CO₂减排目标的驱动下, CO₂资源化利用成为催化领域的重要研究方向. CO₂加氢制烯烃, 尤其是丙烯, 因其在化工产业链中的重要地位而备受关注. 然而, 现有串联催化体系(如ZnZrO_x/SAPO-34)通常生成C₂-C₄烯烃混合物, 丙烯选择性受限(通常< 50%), 这主要受制于反应网络复杂性以及丙烯易发生二次加氢生成丙烷等副反应. 从原理上看, 分子在分子筛孔道中的扩散行为以及Brönsted酸位性质共同决定了产物分布. 因此, 发展兼顾分子扩散与酸性调控的协同催化策略, 有望突破丙烯选择性瓶颈.

本工作提出并构建了一种扩散-酸性协同效应调控策略, 通过调控SAPO-34分子筛的形貌与酸性位点, 实现ZnZrO_x/SAPO-34串联催化体系中丙烯选择性的显著提升. 首先, 通过共沉淀法制备ZnZrO_x催化剂, 表征结果表明, Zn和Zr物种均匀分布, 并实现电子转移(Zr→Zn), 表明ZnZrO_x催化剂的成功合成. 随后构建不同形貌SAPO-34 (微米级、纳米颗粒及纳米片), 并系统研究了它们的扩散性能. 动态吸附实验结果表明, 纳米片SAPO-34中甲醇和丙烯的扩散速率分别提高约2-2.5倍, 显著缩短分子停留时间, 从而有效抑制丙烯二次加氢反应. 在370 °C, 3 MPa条件下, 相比ZnZrO_x/SAPO-34-COM, ZnZrO_x/SAPO-34-NS催化剂上丙烯选择性由29.4%提升至46.3%, 同时轻烯烃选择性提高至78.6%. 在此基础上, 通过调控Si配位环境构建了富含Si(0Si,4Al)与Si(1Si,3Al)结构的SAPO-34-NS-BE, 显著提升了强Brönsted酸位比例. NH₃-程序升温脱附与固体核磁表征显示, 该结构有效提升强酸位密度. 催化性能评价结果显示, 该协同体系实现19.2%的CO₂转化率, 丙烯选择性提升至52.6%. 进一步, 在高空速条件下可提高至57.4%. 机理研究(原位漫反射红外光谱)表明, CO₂在ZnZrO_x上经甲酸盐(HCOO*)路径转化为甲氧基(CH₃O*), 后者可迁移至SAPO-34表面并参与C-C偶联反应生成烯烃. 纳米片结构促进中间体快速迁移与转化, 而强Brönsted酸位促进C₃分子生成, 两者协同作用提升丙烯选择性. 此外, 该催化体系表现出优异稳定性, 150 h反应后仍保持较高烯烃选择性.

综上, 本工作提出的扩散-酸性协同调控策略为CO₂加氢制丙烯性能提升提供了可能, 并验证了其在多种金属氧化物体系中的可行性. 未来, 可进一步从界面耦合及反应动力学角度优化金属氧化物组分, 实现更高活性与稳定性. 本工作为高选择性烯烃合成及CO₂高值转化提供了可供选择的路径.

关键词: CO₂加氢, 串联反应, C-C偶联, 轻烯烃, 丙烯选择性

Abstract:

Achieving carbon neutrality requires the development of rational catalytic strategies for efficient CO₂ utilization, particularly toward propylene, which global demand continues to increase. Herein, a diffusion-acidity cooperative effect strategy is proposed and implemented using ZnZrO_x/SAPO-34 tandem catalysts to enhance propylene selectivity in CO₂ hydrogenation. Compared with a ZnZrO_x/conventional SAPO-34 catalyst, which exhibits 29.4% propylene selectivity among hydrocarbons, the optimized ZnZrO_x/SAPO-34 system delivers a CO₂ conversion of 19.2% with a substantially improved propylene selectivity of 52.6%, further rising to 57.4% at higher gas hourly space velocity. The results reveal that accelerating molecular diffusion within SAPO-34 promotes the rapid transport and transformation of hydrogenated intermediates formed on ZnZrO_x, thereby suppressing undesired secondary hydrogenation pathways. Simultaneously, an increased content of strong Brönsted acid sites associated with Si(0Si,4Al) and Si(1Si,3Al) facilitates selective propylene formation. These findings suggest diffusion-acidity cooperative effect as a possible design principle for efficient CO₂-to-propylene conversion over ZnZrO_x/SAPO-34.

Key words: CO₂ hydrogenation, Tandem process, C-C coupling, Light olefins, Propylene selectivity1. Introduction

陈栋航, 刘俊辰, 邓威, 高彪, 王逸夫, 渡邊源規, 石原逹己, 郭利民. 扩散-酸性协同效应调控ZnZrO_x/SAPO-34串联催化剂实现高选择性CO₂加氢制丙烯[J]. 催化学报, 2026, 90: 145-157.

Donghang Chen, Junchen Liu, Wei Deng, Biao Gao, Yifu Wang, Motonori Watanabe, Tatsumi Ishihara, Limin Guo. Diffusion-acidity cooperative effect in ZnZrO_x/SAPO-34 tandem catalysts for enhanced CO₂-to-propylene conversion[J]. Chinese Journal of Catalysis, 2026, 90: 145-157.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(26)65189-3

https://www.cjcatal.com/CN/Y2026/V90/I11/145

图/表 7

Fig. 1. XRD pattern (a), N2 sorption isotherm (b), HRTEM image (c), aberration-corrected scanning TEM-high-angle annular dark-field images and element distribution (d) of the ZnZrOx catalyst. (e) Zn LMM Auger spectra for ZnZrOx and ZnO. (f) XPS spectra of Zr 3d for ZnZrOx catalysts and ZrO2.

Fig. 2. (a) Schematic illustration of the diffusion enhancement strategy. (b) Intra-diffusion rates of methanol in SAPO-34 zeolites with different morphologies. (c) Intra-diffusion rates of propylene in SAPO-34 zeolites with different morphologies. (d) CO2 hydrogenation performance and product selectivity of the three ZnZrOx/SAPO-34 catalysts under reaction conditions of 370 °C, 3 MPa, and 6000 mL/(g·h).

Fig. 3. NH3-TPD profiles (a), 31P MAS NMR spectra (b), 27Al MAS NMR spectra (c), 1H MAS NMR spectra (d), and 29Si MAS NMR spectra (e) of the SAPO-34-COM, SAPO-34-NS, and SAPO-34-NS-BE samples. (f) Schematic illustration of the changes of acid sites.

Fig. 4. (a) Relationship between propylene selectivity and Si/Al ratio. (b) Comparison of propylene selectivity between different strategies (based on ZnZrOx/SAPO-34-COM). CO2 hydrogenation performance and product selectivity of ZnZrOx/SAPO-34-NS-BE at different reaction temperatures (3 MPa, 6000 mL/(g·h)) (c), at various GHSVs (370 °C, 3 MPa) (d), at different reaction pressures (370 °C, 6000 mL/(g·h)) (e). (f) Propylene selectivity among hydrocarbon products over ZnZrOx/SAPO-34-NS-BE at varying GHSVs and pressures. (g) Comparison of the catalytic performance in this work with previously reported catalysts. (h) Diffusion-acidity cooperative effect applied in other metal oxide catalysts.

Fig. 5. (a) In-situ DRIFTS spectra of CO2 hydrogenation. In-situ DRIFTS spectra collected after switching off the CO2 feed (b) and temporal evolutions of formate and methoxy species (c) over ZnZrOx/SAPO-34-COM. (d) In-situ DRIFTS spectra of CO2 hydrogenation. In-situ DRIFTS spectra collected after switching off the CO2 feed (e), and temporal evolutions of formate and methoxy species (f) over ZnZrOx/SAPO-34-NS-BE (300 °C and 0.1 MPa).

Fig. 6. (a) Stability test of ZnZrOx/SAPO-34-COM over 60 h on stream. (b) Stability test of ZnZrOx/SAPO-34-NS-BE over 60 h on stream. (c) TGA results of the samples after the 60 h stability tests. Stability test of ZnZrOx/SAPO-34-NS-BE over 150 h on stream (d), and TGA results (e) of the samples after the 150 h stability tests.

Fig. 7. Schematic illustration of the proposed reaction mechanism of CO2 hydrogenation over the ZnZrOx/SAPO-34.

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扩散-酸性协同效应调控ZnZrO_x/SAPO-34串联催化剂实现高选择性CO₂加氢制丙烯

Diffusion-acidity cooperative effect in ZnZrO_x/SAPO-34 tandem catalysts for enhanced CO₂-to-propylene conversion

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