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

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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　gMeOH·kgcat–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-Ov-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.　©　2025　Dalian　Institute　of　Chemical　Physics,　the　Chinese　Academy　of　Sciences

Keyword：

Activation analysis Binary alloys Carbon dioxide Catalyst selectivity Cerium alloys Cerium compounds Copper alloys Copper compounds Hydrogenation II-VI semiconductors Metabolism Methanol Syngas production Ternary alloys Zinc alloys Zinc oxide

Community：

[ 1 ] [Chen, Yang]Key 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, Fujian, Fuzhou; 350108, China
[ 2 ] [Zhou, Diwen]Key Laboratory of Organic Compound Pollution Control Engineering (MOE), School of Environmental and Chemical Engineering, Shanghai University, Shanghai; 200444, China
[ 3 ] [Chang, Yongli]Key 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, Fujian, Fuzhou; 350108, China
[ 4 ] [Lin, Hongqiao]Key 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, Fujian, Fuzhou; 350108, China
[ 5 ] [Xu, Yunzhao]Key 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, Fujian, Fuzhou; 350108, China
[ 6 ] [Zhang, Yong]Key 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, Fujian, Fuzhou; 350108, China
[ 7 ] [Yuan, Ding]Key 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, Fujian, Fuzhou; 350108, China
[ 8 ] [Wu, Lizhi]Key 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, Fujian, Fuzhou; 350108, China
[ 9 ] [Tang, Yu]Key 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, Fujian, Fuzhou; 350108, China
[ 10 ] [Dai, Chengyi]School 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, Shaanxi, Xi'an; 710069, China
[ 11 ] [Li, Xingang]State 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
[ 12 ] [Wei, Qinhong]Department of Chemical Engineering, School of Petrochemical Engineering & Environment, Zhejiang Ocean University, Zhejiang, Zhoushan; 316022, China
[ 13 ] [Tan, Li]Key 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, Fujian, Fuzhou; 350108, China

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