Synergistic interface engineering in Cu-Zn-Ce catalysts for efficient CO2 hydrogenation to methanol

doi:10.1016/S1872-2067(25)64773-5

Chinese Journal of Catalysis ›› 2025, Vol. 77: 171-183.DOI: 10.1016/S1872-2067(25)64773-5

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Synergistic interface engineering in Cu-Zn-Ce catalysts for efficient CO₂ hydrogenation to methanol

Yang Chen^a^,¹, Diwen Zhou^b^,^*^,¹(), Yongli Chang^a, Hongqiao Lin^a, Yunzhao Xu^a, Yong Zhang^a, Ding Yuan^a, Lizhi Wu^a, Yu Tang^a, Chengyi Dai^c, Xingang Li^d, Qinhong Wei^e^,^*(), Li Tan^a^,^*()

^aKey Laboratory of Advanced Carbon-Based Functional Materials, Fujian Key Laboratory of Electrochemical Energy Storage Materials, State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou 350108, Fujian, China
^bKey Laboratory of Organic Compound Pollution Control Engineering (MOE), School of Environmental and Chemical Engineering, Shanghai University, Shanghai 200444, China
^cSchool of Chemical Engineering, International Science & Technology Cooperation Base for Clean Utilization of Hydrocarbon Resources, Chemical Engineering Research Center of the Ministry of Education for Advanced Use Technology of Shanbei Energy, Collaborative Innovation Center for Development of Energy and Chemical Industry in Northern Shaanxi, Northwest University, Xi’an 710069, Shaanxi, China
^dState Key Laboratory of Chemical Engineering, Collaborative Innovation Center of Chemical Science and Engineering (Tianjin), Haihe Laboratory of Sustainable Chemical Transformations, Tianjin Key Laboratory of Applied Catalysis Science and Engineering, School of Chemical Engineering and Technology, Tianjin University, Tianjin 300350, China
^eDepartment of Chemical Engineering, School of Petrochemical Engineering & Environment, Zhejiang Ocean University, Zhoushan 316022, Zhejiang, China

Received:2025-04-22 Accepted:2025-06-02 Online:2025-10-18 Published:2025-10-05
Contact: *E-mail: diwenzhou@shu.edu.cn (D. Zhou), weiqinhong@zjou.edu.cn (Q. Wei), tan@fzu.edu.cn (L. Tan).
About author:¹Contributed equally to this work.
Supported by:
National Key Research and Development Program of China(2022YFB4101800);National Natural Science Foundation of China(22172032);National Natural Science Foundation of China(U22A20431);National Natural Science Foundation of China(22202180)

Abstract

Abstract:

CO₂ hydrogenation to CH₃OH is of great significance for achieving carbon neutrality. Here, we show a urea-assisted grinding strategy for synthesizing Cu-Zn-Ce ternary catalysts (CZC-G) with optimized interfacial synergy, achieving superior performance in CO₂ hydrogenation to methanol. The CZC-G catalyst demonstrated exceptional methanol selectivity (96.8%) and a space-time yield of 73.6 g_MeOH·kg_cat^-1·h^-1 under optimized conditions. Long-term stability tests confirmed no obvious deactivation over 100 h of continuous operation. Structural and mechanistic analyses revealed that the urea-assisted grinding method promotes the formation of Cu/Zn-O_v-Ce ternary interfaces and inhibits the reduction of ZnO, enabling synergistic interactions for efficient CO₂ activation and selective stabilization of formate intermediates (HCOO*), which are critical for methanol synthesis. In-situ diffuse reflectance infrared Fourier transform spectra and X-ray absorption spectroscopy studies elucidated the reaction pathway dominated by the formate mechanism, while suppressing the reverse water-gas shift reaction. This work underscores the critical role of synthetic methodologies in engineering interfacial structures, offering a strategy for designing high-performance catalysts for sustainable CO₂ resource utilization.

Key words: CO₂ hydrogenation, Methanol, Cu-based catalyst, Ternary interface, Formate mechanism

Yang Chen, Diwen Zhou, Yongli Chang, Hongqiao Lin, Yunzhao Xu, Yong Zhang, Ding Yuan, Lizhi Wu, Yu Tang, Chengyi Dai, Xingang Li, Qinhong Wei, Li Tan. Synergistic interface engineering in Cu-Zn-Ce catalysts for efficient CO₂ hydrogenation to methanol[J]. Chinese Journal of Catalysis, 2025, 77: 171-183.

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Figures/Tables 7

Fig. 1. (a,c) the CO2 conversion (red square star) and product selectivity (histogram) of CZC catalysts with different preparation method. (b,d) The methanol space-time yield and CO selectivity of catalysts. Reaction condition: 230 °C, 3.0 MPa, WHSV 8000 mL·gcat-1·h-1, CO2:H2 = 1:3. (f) the methanol space-time yield and CO selectivity of CZC-G catalysts under different WHSV. Reaction condition: 230 °C, 3.0 MPa, WHSV 2000/4000/8000 mL·gcat-1·h-1, CO2:H2 = 1:3 (e) Comparison of the CZC-G with the reported methanol synthesis catalysts. The reference data is cited below: Cat-1 [36], Cat-2 [37], Cat-3 [38], Cat-4 [39], Cat-5 [40], Cat-6 [41], Cat-7 [42], Cat-8 [43], Cat-9 [44], Cat-10 [45].

Fig. 2. Time on stream (TOS) evolution of CO2 conversion and product selectivity over the CZC-G. Reaction condition: 230 °C, 3.0 MPa, WHSV = 8000 mL·gcat-1·h-1, CO2:H2 = 1:3.

Fig. 3. (a) The TEM images of CZC-G after reaction. (b) EDS elemental mappings of CZC-G after reaction. (c) The TEM images of CZC-CP after reaction. (d) EDS elemental mappings of CZC-CP after reaction. (e) The TEM images of CZC-IWI after reaction. (f) EDS elemental mappings of CZC-IWI after reaction.

Fig. 4. (a) XRD patterns of CZC-G, CZC-CP and CZC-IWI before reaction. (b) XRD patterns of CZC-G, CZC-CP and CZC-IWI after reaction. (c) H2-TPR profile of CZC-G, CZC-CP and CZC-IWI. (d) CO2-TPD profile of CZC-G, CZC-CP and CZC-IWI.

Fig. 5. XPS spectra obtained from CZC-G, CZC-CP and CZC-IWI after reaction. (a) Cu 2p; (b) Cu LMM Auger spectra; (c) Ce 3d; (d) Zn 2p; (e) Zn LMM Auger spectra; (f) O 1s.

Fig. 6. (a) Cu K-edge XANES spectra of CZC-G catalysts and standard. (b) The Fourier transform of k2-weighted EXAFS spectra of CZC-G catalysts and standard. (c) Zn K-edge XANES spectra of CZC-G catalysts and standard. (d) The Fourier transform of k2-weighted EXAFS spectra of CZC-G catalysts and standard.

Fig. 7. (a,b) In-situ DRIFT spectroscopy of CZC-G catalysts from 2200-1000 and 3200-2500 cm-1. (c,d) In-situ DRIFT spectroscopy of CZC-CP catalysts from 2200-1000 and 3200-2500 cm-1. (e,f) In-situ DRIFT spectroscopy of CZC-IWI catalysts from 2200-1000 and 3200-2500 cm-1. Test condition: the sample was first pretreated under 10% H2 for 120?min, then mixed gas (CO2:H2 =? 1:3) was introduced into the cell to a pressure of 3 MPa, and data were recorded at 230 °C for 100 min.

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Synergistic interface engineering in Cu-Zn-Ce catalysts for efficient CO₂ hydrogenation to methanol

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