CO竞争吸附和C-C偶联强化的PtCo合金催化剂调控CO2加氢产物选择性

doi:10.1016/S1872-2067(26)65159-5

催化学报 ›› 2026, Vol. 89: 378-389.DOI: 10.1016/S1872-2067(26)65159-5

CO竞争吸附和C-C偶联强化的PtCo合金催化剂调控CO₂加氢产物选择性

李文慧^a, 刘洋伯^a, 张依琳^a, 杨庆雯^a, 杨虹^b, 聂小娃^a^,^*(), 郭新闻^a^,^*()

^a大连理工大学化工学院,精细化工全国重点实验室, 智能材料前沿科学中心, PSU-DUT联合能源研究中心,辽宁大连 116024,中国
^b西澳大利亚大学工程学院,珀斯,澳大利亚

收稿日期:2025-12-31 接受日期:2026-02-28 出版日期:2026-10-18 发布日期:2026-09-01
通讯作者: *电子信箱: guoxw@dlut.edu.cn (郭新闻),
niexiaowa@dlut.edu.cn (聂小娃).
基金资助:
国家重点研发计划项目(2024YFB4105401);国家自然科学基金(22472017);辽宁省自然科学基金博士科研启动项目(2025-BS-0027);辽宁滨海实验室联合基金(LBLD-2025-08);中央高校基本科研业务费(DUT22LAB602);中央高校基本科研业务费(DUT24RC(3)071)

Regulation products selectivity on PtCo alloy catalyst in CO₂ hydrogenation through enhanced CO competitive adsorption and C-C coupling

Wenhui Li^a, Yangbo Liu^a, Yilin Zhang^a, Qingwen Yang^a, Hong Yang^b, Xiaowa Nie^a^,^*(), Xinwen Guo^a^,^*()

^aState Key Laboratory of Fine Chemicals, Frontier Science Center for Smart Materials, PSU‐DUT Joint Center for Energy Research, School of Chemical Engineering, Dalian University of Technology, Dalian 116024, Liaoning, China
^bSchool of Engineering, The University of Western Australia, Perth, WA 6009, Australia

Received:2025-12-31 Accepted:2026-02-28 Online:2026-10-18 Published:2026-09-01
Contact: *E-mail:guoxw@dlut.edu.cn(X. Guo),niexiaowa@dlut.edu.cn(X. Nie).
Supported by:
National Key Research and Development Program of China(2024YFB4105401);National Natural Science Foundation of China(22472017);Doctoral Research Startup Project of the Natural Science Foundation of Liaoning Province(2025-BS-0027);Liaoning Binhai Laboratory(LBLD-2025-08);Fundamental Research Funds for the Central Universities(DUT22LAB602);Fundamental Research Funds for the Central Universities(DUT24RC(3)071)

摘要/Abstract

摘要：

CO₂加氢转化为高附加值化学品是缓解温室效应和应对能源危机的最有效策略之一. Co基催化剂在费托合成反应中主要生成高碳烃产物, 而在CO₂加氢反应中其产物主要是CO或者CH₄. 研究表明, CO₂加氢生成的中间物种CO在催化剂表面继续加氢和脱附之间的竞争, 是影响产物选择性的关键因素. 另外, 在CO₂加氢反应体系中, 中间物种CO受反应物CO₂*覆盖度和CO₂活化产生的O*覆盖度影响, 其吸附能明显降低, 易脱附形成气相CO产物. 因此, 在CO₂加氢过程中, 增强中间物种CO的吸附, 是提高Co基催化剂上C₂₊产物选择性的关键.

本研究通过将Pt引入Co基催化剂, 构建了PtCo合金活性相, 调控了CO竞争吸附能力与反应路径, 显著增强了CO₂加氢过程中的C-C偶联进而提升了C₂₊烃类选择性. 扩展X-射线吸收精细结构拟合结果表明, 2% PtCo催化剂中存在Pt-Co配位键; 2% PtCo催化剂的近边吸收谱分析揭示了Pt与Co之间存在电子转移; X-射线光电子能谱结果显示, Pt和Co的电子结合能均发生显著偏移, 证实了催化剂中PtCo合金相的形成. CO-程序升温脱附, CO-(DRIFTS)和密度泛函理论(DFT)计算结果表明, 2% PtCo催化剂上的CO吸附强度显著高于纯Co催化剂, 但略低于纯Pt催化剂. 与此同时, PtCo合金相的存在改变了CO与CO₂在催化剂表面的竞争吸附行为, 促使CO取代CO₂成为催化剂表面的强吸附物种, 并且PtCo催化剂上的CO吸附速率和吸附量都强于CO₂. 原位DRIFTS结果表明, 2% PtCo催化剂上出现了归属于HCOO*物种的特征吸收峰, 而该吸收峰在纯Co催化剂上并未被检测到. DFT计算进一步表明, PtCo合金显著降低了甲酸盐中间体的生成能垒, 使得反应路径由纯Co催化剂上的CO₂经CO中间体的活化机制, 转变为PtCo催化剂上甲酸盐介导路径与CO中间体路径并存的协同机制. 由于CO-CO, HCOO-HCOO以及CO-HCOO的耦合能垒均较高, 因此, 在PtCo催化剂上中间物种CO和HCOO更倾向于先加氢生成CH_x, 再经由CH_x耦合路径生成C₂₊产物. 在350 °C和3 MPa的反应条件下, 2% PtCo催化剂实现了18.5%的C₂₊选择性, 显著高于纯Co催化剂上1.9%的C₂₊选择性. 另外, H/D交换实验结果表明, Pt的加入显著增强了H₂的吸附活化能力, CO₂转化率也进一步提升, PtCo催化剂的C₂₊收率最高达到83.6 mmol·g^-1·h^-1.

综上, 本研究提出了通过调控中间体与反应物竞争吸附来提高产物选择性的催化剂设计新概念, 推动了Co基催化剂上CO₂加氢制C₂₊烃的进一步发展. 这不仅为CO₂高值化利用提供了新型催化剂设计策略, 更为深入理解多相催化中吸附竞争与反应路径的调控机制奠定了基础.

关键词: CO₂加氢, Co基催化剂, CO竞争吸附, PtCo合金, C₂₊产物

Abstract:

The hydrogenation of CO₂ into high-value-added chemicals represents one of the most effective strategies for mitigating the greenhouse effect and addressing the energy crisis. In this study, the incorporation of Pt into Co-based catalysts is utilized to modulate the CO competitive adsorption capacity and reaction pathways, thereby significantly enhances the C-C coupling and the selectivity of C₂₊ hydrocarbons during CO₂ hydrogenation. The formation of PtCo alloy in the catalysts is confirmed by X-ray absorption spectroscopy, in-situ X-ray diffraction, X-ray photoelectron spectroscopy and scanning transmission electron microscopy analyses. The study reveals that the presence of PtCo alloy alters the competitive adsorption behavior of CO and CO₂ on the catalyst, and enables CO to replace CO₂ as the strongly adsorbed species on the catalyst. Density functional theory calculations demonstrate that the PtCo alloy exhibits enhanced CO adsorption energy and reduced formation energy barrier for formate compared with pure Co. This is responsible for the emergence of an additional formate pathway on the PtCo catalyst. Consequently, the 2%PtCo catalyst achieves a C₂₊ selectivity of 18.5% under conditions of 350 °C and 3 MPa, markedly higher than the 1.9% over the pure Co catalyst. PtCo catalysts possesses 83.6 mmol·g^-1·h^-1 C₂₊ yield, outperforming the Fe-based reference catalyst by a factor of 4. The study presents a novel catalyst design concept for increasing C₂₊ selectivity through regulating the competitive adsorption between intermediate and reactant.

Key words: CO₂ hydrogenation, Co-based catalysts, CO competitive adsorption, PtCo alloy, C₂₊ products

李文慧, 刘洋伯, 张依琳, 杨庆雯, 杨虹, 聂小娃, 郭新闻. CO竞争吸附和C-C偶联强化的PtCo合金催化剂调控CO₂加氢产物选择性[J]. 催化学报, 2026, 89: 378-389.

Wenhui Li, Yangbo Liu, Yilin Zhang, Qingwen Yang, Hong Yang, Xiaowa Nie, Xinwen Guo. Regulation products selectivity on PtCo alloy catalyst in CO₂ hydrogenation through enhanced CO competitive adsorption and C-C coupling[J]. Chinese Journal of Catalysis, 2026, 89: 378-389.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(26)65159-5

https://www.cjcatal.com/CN/Y2026/V89/I10/378

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Fig. 1. (a) Catalytic performance over Co and PtCo catalysts in CO2 hydrogenation. Arrhenius plots of CO2 and C2+ over Co (b) and 2%PtCo (c). Reaction conditions: 0.04 g catalyst, H2/CO2 = 4:1 or 1:1, GHSV = 90000 mL·g-1·h-1, T = 350 °C, and P = 3 MPa.

Fig. 2. XRD patterns taken in-situ during hydrogen reduction of the 2%PtCo catalyst from 50 to 600 °C at 50 °C intervals. Reduction conditions: pure H2 atmosphere at 0.8 MPa.

Fig. 3. HAADF-STEM images of 2%PtCo catalyst before (a-d) and after (e-i) the H2 reduction at 400 °C.

Fig. 4. Co 2p XPS spectra of the reduced 2% PtCo and Co catalysts.

Fig. 5. XANES spectra (a), RDFs from the EXAFS data taken at Pt L3 edge (b), and Wavelet transform contour plots at Pt L3 edge of 2%PtCo (c) and Pt foil (d).

Fig. 6. (a) H2-TPR curves of the PtCo catalysts with 0.1 wt%, 0.5 wt% and 2.0 wt% Pt loading. (b) H/D exchange curves of 2%PtCo and Co.

Fig. 7. (a) CO-TPD curves of Co and PtCo catalysts with 0.1 wt%, 0.5 wt% and 2.5 wt% Pt loading. (b) In-situ CO DRIFT spectra of Co and 2%PtCo. (c) CO adsorption energy on Pt (111), PtCo (101-0) and Co (101-0).

Fig. 8. Breakthrough curves (a), adsorption rate-time curves (b), and adsorption capacity-time curves (c) for the competitive CO?/CO adsorption on Co. Breakthrough curves (d), adsorption rate-time curves (e), and adsorption capacity-time curves (f) for the competitive CO?/CO adsorption on 2%PtCo. Competitive adsorption conditions: 25 °C, 0.1 bar, and CO/CO2 = 1:1.

Fig. 9. In-situ DRIFT spectra collected over wavenumber range of 3200 to 1000 cm-1 during CO2 hydrogenation on Co and 2%PtCo. Reaction conditions: H2/CO2 = 1:1, T = 50-400 °C, and P = 3 MPa.

Fig. 10. Energy diagrams of different CO2 reaction routes on Co (101-0) and PtCo (101-0).

Fig. 11. Mechanism diagram of CO2 hydrogenation to C2+ hydrocarbons on PtCo catalyst.

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CO竞争吸附和C-C偶联强化的PtCo合金催化剂调控CO₂加氢产物选择性

Regulation products selectivity on PtCo alloy catalyst in CO₂ hydrogenation through enhanced CO competitive adsorption and C-C coupling

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